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Recent advances in additive manufacturing of
engineering thermoplastics: challenges and
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Cite this: RSC Adv., 2020, 10, 36058
opportunities
ab *ab and Manjusri Misra *ab
Maisyn Picard, Amar K. Mohanty
There are many limitations within three-dimensional (3D) printing that hinder its adaptation into industries
such as biomedical, cosmetic, processing, automotive, aerospace, and electronics. The disadvantages of 3D
printing include the inability of parts to function in weight-bearing applications, reduced mechanical
performance from anisotropic properties of printed products, and limited intrinsic material performances
Received 1st June 2020
Accepted 17th August 2020 such as flame retardancy, thermal stability, and/or electrical conductivity. Many of these shortcomings
have prevented the adaptation of 3D printing into product development, especially with few novel
DOI: 10.1039/d0ra04857g
researched materials being sold commercially. In many cases, high-performance engineering
rsc.li/rsc-advances thermoplastics (ET) provide a basis for increased thermal and mechanical performances to address the
a
School of Engineering, University of Guelph, Thornbrough Building, Guelph, N1G b
Bioproducts Discovery and Development Centre, Department of Plant Agriculture,
2W1, ON, Canada. E-mail: mohanty@uoguelph.ca; mmisra@uoguelph.ca University of Guelph, Crop Science Building, Guelph, N1G 2W1, ON, Canada
Maisyn Picard has completed Dr Amar Mohanty is a Professor
her Bachelor's degree in and OAC Distinguished
Biomedical Engineering (with Research Chair in Sustainable
distinction) from the University Biomaterials and holds
of Guelph. Currently, she has a University Research Leader-
completed her Master of Applied ship Chair at the University of
Science degree under the advice Guelph. He is an international
of Professor Amar Mohanty and leader in the eld of biomate-
Professor Manjusri Misra in rials with a focus on engineering
Biological Engineering at the new sustainable materials. Prof.
University of Guelph (Guelph, Mohanty's research interests
Ontario, Canada). Ms Picard's have focused on the bioeconomy
research interests include addi- related to bioplastics, biobased
tive manufacturing, polymer processing and characterization, and materials, and sustainable composites. He has more than 800
sustainable materials development via a circular economic publications to his credit, including 396 peer-reviewed journal
approach. papers and 61 patents awarded/applied. He has 34399 citations of
his research with an h-index of 83 (Google Scholar). Prof. Mohanty
has received many awards, including the JL White Innovation
Award from the Polymer Processing Society; Synergy Award for
Innovation from Natural Sciences and Engineering Research
Council of Canada (NSERC); Lifetime Achievement Award from the
BioEnvironmental Polymer Society (BEPS); Andrew Chase Forest
Products Division Award from the American Institute of Chemical
Engineers (AIChE) and OAC Alumni Distinguished Researcher
Award. Prof. Mohanty has been named a Fellow of the American
Institute of Chemical Engineers, a Fellow of Royal Society of
Chemistry (UK) and a Fellow of the Society of Plastic Engineers.
Prof. Mohanty is the Editor-in-Chief of Sustainable Composites,
Composites Part C: Open Access.
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shortcomings or limitations of both selective laser sintering and extrusion 3D printing. The first strategy to
combat these limitations is to fabricate blends or composites. Novel printing materials have been
implemented to reduce anisotropic properties and losses in strength. Additives such as flame retardants
generate robust materials with V0 flame retardancy ratings, and compatibilizers can improve thermal or
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dimensional stability. To serve the electronic industry better, the addition of carbon black at only 4 wt%,
to an ET matrix has been found to improve the electrical conductivity by five times the magnitude.
Surface modifications such as photopolymerization have improved the usability of ET in automotive
applications, whereas the dynamic chemical processes increased the biocompatibility of ET for medical
device materials. Thermal resistant foam from polyamide 12 and fly ash spheres were researched and
fabricated as possible insulation materials for automotive industries. These works and others have not
Open Access Article. Published on 01 October 2020. Downloaded on 10/6/2020 11:47:43 PM.
only generated great potential for additive manufacturing technologies, but also provided solutions to
critical challenges of 3D printing.
1. Introduction
Currently, the additive manufacturing (AM) market is in
Dr Manju Misra is a Professor at
demand for a larger variety of feedstock materials with novel
the School of Engineering and
thermal, mechanical, electrical, or biocompatible characteris-
holds a joint appointment in the
tics. In this review, feedstock materials refer to those that are
Dept. of Plant Agriculture at the
commercially available for industries for the use of printing.
University of Guelph. She is also
The addition of more printing materials with unique mechan-
the Research Program Director of
ical performances might better serve wider range of applica-
the Plant – Technology Panel for
tions and industries that currently cannot implement the AM
the Ontario Agri-Food Innovation
technologies. A comprehensive review of the current market
Alliance, a program between the
solutions discovered in academia could bridge this knowledge
Ontario Ministry of Agriculture
gap for industry and suggest novel materials. Three-
and Rural Affairs (OMAFRA) and
dimensional (3D) printing is an additive manufacturing
the University of Guelph. She is
process where complex geometric parts can be made in a short
a Fellow of the Royal Society of
period of time (i.e., without the need for tools and die fabrica-
Chemistry (UK) and the American Institute of Chemical Engineers
tion) in a layer-by-layer fashion.1,2 This technology has reduced
(AIChE). Dr Misra's current research focuses primarily on novel bio-
the need for machining or tooling products/prototypes, and has
based composites and nanocomposites from agricultural, forestry
resulted in cost and time saving.3 Since the inception of this
and recycled resources for the sustainable bio-economy moving
technology in 1986, various methods of 3D printing have been
towards a circular economy. She has authored more than 700
created.4 The most common methods are extrusion 3D printing
publications, including 369 peer-reviewed journal papers, 21 book
(E3DP) i.e., fused lament fabrication, big area additive
chapters, and 51 patents. She was an editor of the CRC Press
manufacturing, and selective laser sintering (SLS).4 However,
volume, “Natural Fibers, Biopolymers and Biocomposites”, Taylor
other methods include stereolithography, direct energy depo-
& Francis Group, Boca Raton, FL (2005); American Scientic
sition, and ink jetting.3
Publishers volume “Packaging Nanotechnology”, Valencia, Cal-
Extrusion 3D printing can be further categorized as either
ifornia (2009); “Polymer Nanocomposites”, Springer (2014) and
small-scale or large-scale printers. Small-scale printers were
“Fiber Technology for Fiber-Reinforced Composites”, Woodhead
referred to as fused deposition modelling (FDM) prior to
Publishing (2017). She was the chief editor of “Biocomposites:
trademarking; however, the same process has been renamed
Design and Mechanical Performance” Woodhead Publishing
fused lament fabrication (FFF). These desktop-sized printers
(2015). She was the President of the BioEnvironmental Polymer
extrude thermoplastic polymer laments through a heated
Society (BEPS) in 2009. She serves on the editorial board of “Journal
nozzle and deposit the extrudate on to a heated bed,5 building
of Applied Polymer Science”, “Composites Part A: Science and
components by the bottom up method. The printer and its
Manufacturing”, “Polymer Testing”, and “Composites Part C: Open
products are created at a comparatively low cost to that of SLS.4
Access”. In 2012, Dr Misra received the prestigious “Jim Hammar
However, the limitations of these printers include a minimal
Memorial Award” from BEPS and University of Guelph's Innovation
lament diameter and a smaller print area that is limited by the
of the year award in 2016 for her involvement in developing the
size of the printer's bed. When developing materials, the size
“Compostable single-serve coffee pods”. In 2017, Professor Misra
constraint of the lament diameter may result in needed
also received the Andrew Chase Division Award in Chemical Engi-
additives (increasing costs) or increased time to optimize the
neering from the Forest Bioproducts Division of AIChE. In 2019,
processing conditions.6 However, to overcome these challenges,
Professor Misra was awarded the Woman of Distinction in Science,
large-scale extrusion printers were fabricated, which offer the
Technology, Engineering & Math (STEM) from the Guelph YWCA-
option for pellet or lament feed systems. Big-area-additive-
YMCA. Total citations: 32818; h-index: 81; i10-index: 345 (Goo-
manufacturing (BAAM) is another name for these large scale
gle Scholar, July 23, 2020).
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extrusion printers7–9 and they are able to increase the produc- fabrication. Although the material was not tested for its FFF
tion rates and times in hopes of adapting 3D printing into mass properties, based on the injection molding properties, it was
production. determined that 90PEI/10PC was a prime substitute. The
Selective laser sintering, also known as a powder bed fusion authors determined that the mechanical performance was
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process,10 requires the use of a powder bed and a laser to melt similar to that of commercially available laments but obtained
the polymer such that each layer connects to the surrounding at about half the cost.22
ones. This process can generate larger parts than FFF but Once the materials are blended, via extrusion or reactive
requires more space and resources to do so; i.e., space for the extrusion, they are collected as laments. The collected la-
large powder bed and substantial le-over materials that are not ments can be size-reduced to powder or pellets before use in AM
solidied by the laser. The most common thermoplastic used equipment. Since FFF uses laments without further modi-
Open Access Article. Published on 01 October 2020. Downloaded on 10/6/2020 11:47:43 PM.
for FFF is poly(lactic acid) (PLA) but its use is limited in SLS due cations, the experimental material can be collected immediately
to its thermal stability and mechanical properties.11 Similarly, following the extrusion process and maintained in lament
SLS is limited to resins or other materials that offer minimal form. This would be benecial since no other resources (i.e.,
variability in performance.12 Engineering thermoplastics, as time, energy, or labour) would be required to transform the
well as blends or composites of engineering thermoplastics, can materials.24 The same is true for the large-scale extrusion 3D
address some limitations in 3D printing associated with printers that operate on a lament system. However, the pellet
mechanical and thermal performances. However, a limited feed systems underwent the size reduction of laments prior to
number of polymers have been investigated and transitioned to use.7 Although this can be benecial since it removes the la-
industry to date. ment diameter limitations as mentioned above, it does require
Some of the most common printing materials that are additional energy input and time. This may have an increased
commercially available are engineering thermoplastics. Engi- associated cost and would have to be investigated by industry
neering thermoplastics are noteworthy because they provide prior to use. Experimental materials used in SLS require the
high mechanical performances and high chemical stability.13 most modications aer extrusion. The laments must be cry-
Some commonly used engineering thermoplastics include PAs omilled to generate ne powders25 to function well in SLS.
(also referred to as polyamides), poly(ether-block-amide), poly- Although the purpose of blending materials is to diversify
etherimides (PEIs), polyimides (PIs),14 and polycarbonates and optimize particular aspects like mechanical perfor-
(PCs).13 Substantial work has been completed in researching mances,26 lament consistency,6 and surface nish.27 There are
engineering thermoplastics for injection and compression other methods to optimize the extrusion output quality as well
molding. Engineering thermoplastics have been used in the as print quality. This can be completed through trial-and-error
automotive industry,15 the biomedical industry,16 and many processes, strategic experimental design28 and tailored
more because of their versatile nature. In some cases, these printing parameters. Irrespective of the optimization methods,
materials are blended with other polymeric materials to vary the such methods are required to generate complete parts without
characteristics such as mechanical performance, biocontent, warpage or delamination and materials with diversied
and/or cost.17 mechanical performances.
The use of blending polymers for injection molding practices Another technique being studied to generate a greater variety
has been studied extensively since the resulting novel materials of feedstock materials and improved mechanical performance
display traits that are a combination of both starting materials. is through the implementation of composite materials. The
Various engineering thermoplastics have been blended to make composites fabricated for 3D printing can vary from lignocel-
new materials with tailorable properties. For example, Asadi- lulosic materials29–31 to carbon-based materials32 and even
nezhad et al.18 blended poly(trimethylene terephthalate) (PTT) inorganic llers.33 The combinations of composites, blends, or
and polyamide (PA)12;18 PTT and poly(butylene terephthalate) rened printing materials can assist with the generation of the
(PBT) were blended for unique performances between those of materials, and 3D printing technology can expand to the 4-
both neat polymers,19,20 and PBT/PC blends21 were studied to dimensional (4D) printing market and fabricate novel
determine their unique properties. In some cases, engineering products.34
thermoplastics have been blended with commodity polymers. The scope of this literature review is to focus on the use of
Codou et al.123 examined PA 6/polypropylene blends with the engineering thermoplastics for 3D printing via E3DP (small and
addition of biocarbon to generate thermally stable and large scale) and SLS methods. A critical review will summarize
sustainable composites.22 Other sustainable blends include what has been done with these materials, how engineering
combining PLA and PBT.23 Blending has been quite successful thermoplastics could address some shortcomings of traditional
in injection molding to generate tailor-made, sustainable, or thermoplastics, as well as examine the feasibility of the mate-
unique materials and the same strategy has provided consid- rials for large-scale production. The optimization and imple-
erable potential to the 3D printing market as well. Blends of PEI mentation of engineering thermoplastics have the potential to
and one of PC or glycol-modied PET (PETG) were studied by generate feedstock materials with larger variability in mechan-
Cicala et al.22 The studied materials displayed potential as ical performance. The newly discovered polymers with
alternatives to other commercialized PEI polymers or blends improved performance can better serve the biomedical, elec-
such as Ultem 9085, which is a commercially available PEI trical and automotive industries.
blend manufactured by Stratasys22 for fused lament
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2. Methods
2.1 Methods for preparing materials
Filaments are oen produced using an extrusion or reactive
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extrusion (Fig. 1) that operates via twin-screw or single-screw
congurations. Screws function by either rotating in the same
or opposite directions, referred to as counter- or co-rotating. If
laments require a specic diameter for use in 3D printing,
then processing conditions such as feed rate, collection rate,
screw speed and melt temperature require optimization.6
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2.2 Methods of 3D printing
There are several methods for 3D printing, which have been
implemented to assist the generation of complex designs or
prototypes in a short period of time. The most common
methods include (1) E3DP, which includes fused lament
fabrication (FFF) and big area additive manufacturing
(BAAM);4 (2) selective laser sintering (SLS);4 (3) stereo-
lithography (SLA);4 (4) laminated object modelling.4 Although
SLS was the rst commercially available process, E3DP and
SLS are the more commonly studied AM processes with engi- Fig. 2 Schematic representation of fused filament fabrication.39
Reprinted with permission from Elsevier: Additive Manufacturing,
neering thermoplastics. The diversity of printing parameters
Copyright 2020, License: 4743160219820.
and operational practices offers a unique means of generating
complex products over injection or compression molding
practices.
materials to be used for a wide range of products functioning in
2.2.1 Extrusion 3D printing
the automotive,36 electrical37 and biomedical38 industries.
Fused lament fabrication. Fused lament fabrication is an
However, more work is required to generate economically and
E3DP method where a lament is extruded through a heated
environmentally-friendly feedstock printing materials. The ease
nozzle and placed onto a heated bed/platform (Fig. 2). The
of use of FFF printers has led to their personal use with desktop
molten lament is referred to as the extrudate and is relatively
computers, and a general variety of commercially available
simple to place during the print since the computer-aided
feedstocks. However, there are denite drawbacks and limita-
design is spliced into layer-by-layer instructions for the printer
tions to this technology.
to follow. For this type of printing, there are many functional
Fig. 1 Extrusion set-up for filament processing.35 Reprinted with permission from Elsevier: Additive Manufacturing, Copyright 2020, License:
4838260364616.
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This method of printing requires support for extremely building from the bottom up. Unlike E3DP, the feedstock
complicated designs with projections above the bed.4 Unfortu- materials for print are stored in a secondary bed that serves as
nately, the requirements of the support material increase the the reservoir. Both beds are held on a piston system to adjust to
cost slightly and increase the waste generated. The optimization the required height and a roller sends powder from the reserve
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of prints can reduce waste and time. Other challenges with FFF to the print area when needed (Fig. 4). One disadvantage of SLS
include (1) limited or specically supported lament diame- is the resultant rough surface nish. It is recommended that
ters,37 which can create challenges for new experimental mate- SLS be used when aesthetics and appearance are less crucial.
rials for E3DP; (2) relatively small print areas.8 As a result, an However, this printer is very accurate and would be good for
additional method of E3DP has been created and it is referred to manufacturing large parts. It is important to note that larger
as big-area-additive manufacturing.9 parts require more space and this may be a limiting factor for
Open Access Article. Published on 01 October 2020. Downloaded on 10/6/2020 11:47:43 PM.
Big-area additive manufacturing. In industry, large-scale SLS in some cases.4 The aerospace, biomedical and automotive
custom printers have been designed for larger volume prints industries have beneted from the diverse uses of SLS printers
and increased printing speeds.40 This process of E3DP has been to generate parts for aircra, hearing aids, race cars, and many
coined big-area-additive manufacturing (BAAM).41 Unique to more structures. However, the materials used are limited for
BAAM printers is their ability to use either lament feedstocks other applications because of the current mechanical properties
or pellets to deposit onto the bed. Pellet-based systems require and lack of reproducibility of parts.45
the hopper to be lled with dried pellets and then fed into
a heated channel with a single screw inside. The channel for the 2.3 Methods of optimization prints
polymers is oen covered in thermal jackets and monitored by
thermocouples. The heated channel is set to the desired print Both SLS and E3DP have specic parameters for optimization to
temperature then the screw ensures that the polymer, blends or print samples based on the printing instructions, sample size
composites are efficiently melted and mixed prior to extrusion and orientation. For FFF/BAAM the major optimized printing
through the nozzle. parameters include bed temperature, melt temperature, print
Large-scale printers have the added benet of printing speed, percent ll, inll type (orientation and pattern), and layer
products with a wider range of dimensions than that of FFF.8 height.5,47 Parameters oen optimized for SLS include laser
The BAAM printer in Fig. 3 displays the extruder assembly and power, laser scan speed, and particle size of the powder.48
common conguration for these printers. Like all technologies, Further modications to printed samples can be implemented
BAAM is also subject to some challenges. Since there is such to optimize the mechanical performance. These post-print
a drastic increase in the print rate, the BAAM printer can treatments include sintering48 or annealing.5 This requires
struggle to maintain the intended geometry and has decreased holding the samples at elevated temperatures for extended
surface resolution.42 The BAAM is also likely to be far more periods of time. However, said processes are time-consuming
expensive and requires a larger production area. and require more energy input. Due to the increased time and
2.2.2 Selective laser sintering. Parts are formed in SLS by cost, sintering/annealing is less likely to be implemented in
solidifying powder with a laser in a layer-by-layer fashion,44 large-scale printing processes. The combination of print opti-
mization can lead to function-specic parts. To systematically
optimize prints and observe the inuence or dependence of
printing parameters, statistical analyses are performed.
2.3.1 Statistical analysis. The design of experiments (DOE)
is a method of selecting optimal values or ranges of values,
planning and executing a designed plan. Once executed, the
Fig. 3 Big-area-additive-manufacturing extrusion 3D printer.43 Fig. 4 Selective laser sinter schematic.46 Reprinted with permission
Reprinted with permission from Elsevier: Procedia Manufacturing, from Elsevier: Journal of Manufacturing Processes, Copyright 2020,
Copyright 2020, License: 4743161414193. License: 4743141319375.
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collected products are tested, and the obtained results are 2.4.1 Finite elemental analysis. Finite elemental analysis
analyzed. Many works have been completed on DOE with the (FEA) requires the implementation of computational and
injection molding of composites49 and blends50 to generate analytical practices to model materials and their properties.60
novel materials. The same process is now being implemented in These models can be used to study uid dynamics, heat transfer
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3D printing to generate tailor-made products to serve a wider in correlation to the nozzle temperature and dimensional
variety of purposes. aspects of the printed parts.60 Many models have been created
For composites and polymer blends, a mixtures design of and analyzed with respect to the kinematics of layer deposi-
experiments can be implemented to optimize samples for tion.61 A FEA can also assist with determining the thermal and
a given quality.49 This method systematically varies the content mechanical stability of printed samples.62 Such analysis could
of each constituent and then analyzes the properties obtained be implemented to further reduce the warpage in samples.63 An
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by each combination of materials.50 This type of DOE focuses on extended FEA can also be used to model the fracture behaviour
blending,20 compatibilizing,17 or making composites.51 The of the samples. This assists in determining which internal
most common uses for the mixtures design include the printing structure is the most effective for product application.64
following: (1) optimizing the ller/bre/blending polymer Such analyses are very important when designing prints for
content such that the mechanical properties are maintained or mass production.
enhanced, (2) replacing the more expensive polymer with a cost- Finite element analysis has been implemented with 3D
effective replacement (i.e., lower cost ller, polymer).52 printing of the engineering thermoplastic, PEI, to predict the
For 3D printing, the optimization of printing parameters is linear elastic behaviour of the printed samples.65 The FEA
oen of greater importance; more works have focused on using soware was able to accurately determine Poissons ratio, as well
the Taguchi DOE.53–55 In many cases, parameters such as layer as elastic and shear moduli. This is essential in understanding
height, print speed and extrusion temperature are correlated to whether a part can function safely and wholly for the intended
other properties such as dimensional accuracy.54 These sorts of purpose. This process can also be used to optimize the 3D
correlations are important for understanding and implement- printed part based on its design. Space frame and shell analysis
ing in other works such that materials have tailorable are models within the FEA soware that analyze the PEI parts
mechanical properties or desired aesthetics. containing an internal lattice structure; these methods are cost-
Design of experiments has also been used in 3D printing to effective for optimizing prints.
optimize the waste generated and the input required to produce
samples.56 One of the most important inputs for optimization is
the energy required for the print.57 However, the input of 3. Types of printing materials
materials, which is correlated to the cost of the product, can
also be optimized.57 One important difference between energy This section categorizes the printing materials for both E3DP
usage regarding E3DP and SLS arises when SLS requires sin- and SLS. The rst type is the neat polymer, which means that
tering aer printing. This requires additional energy to form the the virgin or recycled polymer is printed alone and oen
nal product. A comparison of the energy consumption for SLS requires optimization of processing and printing parameters to
and E3DP could be benecial when determining the best generate functional products. The second material type,
printing method. The production of parts via 3D printing referred to as blends, is a combination of polymers or polymers
methods has been noted to reduce the cost and production time and additives, which offer unique property differences as
by 30% and 40% respectively.58 The major energy consumption compared to the neat polymer. In some cases, this may include
for SLS is directly related to the volume and height of the nal improved dimensional or thermal stability or unique mechan-
product.59 A comparative life cycle assessment (LCA) would be ical performances; such aspects are discussed in the sections
important for comparing the energy consumption as well as below. The last category of printing materials is composites.
waste materials of the SLS and E3DP methods. Further details Composites are made from a combination of a distributive
are highlighted below in Section 6.5. Both the energy phase and a continuous phase. In many cases, composites are
consumption and waste have associated costs, which could be formed with bers or llers and polymer matrices for unique
reduced if possible to improve the sustainability of the printing mechanical performances of printed parts.
processes.58
3.1 Neat polymers
2.4 Optimization and exploration of printing parameters Although engineering thermoplastics offers superior thermal
Oen researchers start to test the printability of the materials stability and mechanical performances4 as compared to
through a trial-and-error process to generate complete, commodity thermoplastics, printing can be challenging due to
warpage-free samples. The optimization of printing parameters a combination of high melting temperatures, crystallization
is not effective unless a range of parameters is known that characteristics and viscoelastic properties.66 However, there is
reduces the warpage (lack of adhesion to bed) and delamination substantial potential for the use of engineering thermoplastics to
(lack of adhesion between layers). In some cases, only one set of address the current limited variability in mechanical properties
parameters will print aer determining the ideal set of param- between commercially available feedstocks. To allow 3D printing
eters.6 This is referred to as the trial-and-error process. to serve a larger variety of applications, there is a demand for
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materials that are economically feasible, sustainable and that can feedstock materials, either blends or composites, for novel
fabricate high-quality products each time. printing applications.67 One of the drawbacks to blending alone
relates to the immiscibility of some polymers. Essentially the
3.2 Blends combined polymers remain as separate and distinctive phases,
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which could hinder their performance. In this case, further
Blending polymers is a method for generating diverse feedstock additives are needed to compatibilize and improve the cohesion
materials for 3D printing applications and can be used to between the materials. In some cases, the blending materials
counteract the anisotropic properties that currently limit the are chemicals or polymeric materials considered to be additives
performance of many 3D printed products.67 The use of since they either function as an elastomer as compared to the
blending technologies has been used in the injection molding major system, impact modier, or compatibilizer. Such mate-
Open Access Article. Published on 01 October 2020. Downloaded on 10/6/2020 11:47:43 PM.
industry with engineering plastics to obtain properties between rials will be discussed in the additives section below.
those of each neat polymer. 3.2.1 Additive materials. Additives, like blending with
For example, engineering thermoplastics have been polymers, are used to tailor the performances such as thermal
combined with commodity plastics such as polypropylene stability or mechanical properties. Blends with thermoplastic
(PP),68 and high-density polyethylene (HDPE).69 Other combi- elastomers such as thermoplastic polyurethane (TPU) can help to
nations with engineering thermoplastics are formed from give a balance of toughness and stiffness.79 This could be bene-
binary or ternary blends of only engineering thermoplastics cial for applications such as biomedical applications, where
such as blending polyesters,18,70 polycarbonates,71,72 poly- there are oen the requirements of exibility and strength. Other
amides,73,74 ABS,71,72 and polyether-derived polymers.75,76 More important blending materials include compatibilizing agents
recently, research has also looked into combining virgin mate- such as maleic anhydride-graed polymers and styrene–
rial with recycled material to form the same polymer.66 The ethylene–butadiene–styrene (SEBS). Other compatibilizing
process of SLS produces a lot of waste powder that could be agents work to improve the miscibility of blended polymers.7
affected by thermal degradation. It has been studied and proven Compatibilizers and other additives are important to mention
that recycled materials exhibit some differences in mechanical since they have the added benets of (1) diversifying mechanical
performance as compared to virgin materials. However, blends performance, improving dimensional stability and thermal
with these materials could improve the renewability content of stability during extrusion, as well as reducing the melt ow index
the materials and also give new purpose to wastes. As an such that it is within a printable range (i.e., near 10 g/10 min 80).
example, recycled ABS and high-impact polystyrene from elec- There has been some research with these materials in 3D
trical components were combined to make value-added prod- printing as displayed in Table 1; however, this process was
ucts.77 This diverted waste from potential landll applications commonly used in extrusion for injection molding in the past.
and increased its sustainability via a circular economic Identied below are also additives that have been implemented
approach.78 In addition to increasing the sustainability of in injection molding and may show promise for use in E3DP.
printing materials, blending polymers has many other benets. In Table 1, there are also compatibilizing materials that have
The benets of blending engineering thermoplastics with been implemented in injection molding and may have
polymers or polymer-based additives include the following: (1) a purpose in 3D printing. More research is needed to conrm
developing materials with improved mechanical performance, their functionality, economic viability and success.
(2) reducing the cost of materials since used materials can be
obtained at little to no cost, (3) improving renewable content,
and (4) improving the processability of polymers. If these 3.3 Composites
strategies are adopted into 3D printing, there is potential Composites offer benets in 3D printing, especially E3DP,
growth for this industry to commercialize new polymer because the addition of bre can reduce warpage and the
Table 1 Compatibilizers used in polymer blends and composites
Family Compatibilizer Description Use
Implemented in 3D
printing
Styrene Styrene–ethylene–butylene–styrene (SEBS) Thermoplastic elastomer81 With ABS82
Glycidyl methacrylate Poly(ethylene-n-butylene- acrylate-co-glycidyl methacrylate) Impact modier6 EBA–GMA with PTT6
(GMA) (EBA–GMA)
Styrene maleic anhydride (SMA) Chain extender6 SA–GMA with PTT6
Poly(ethylene-co-glycidyl methacrylate) (PE-c-GMA) Graing co-polymer83 PE-c-GMA with PC83
Anhydride Maleic anhydride (MA) Coupling agent7 SMA with ABS/PA blends7
Implemented in injection
molding
Phosphite Tris(nonylphenyl) phosphite (TNPP) Stabilizer/crosslinker84 TNPP with PA/PLA84
85
Diisocyanate Polymeric methylene diphenyl diisocyanate (PMDI) Compatibilizer
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coefficient of thermal expansion.86 This is a possible solution Traditionally, ABS would not have been used for medical
for generating products that can better serve load-bearing or implants as it lacked native biocompatibility as compared to
structural applications such as those in the automotive silicones or polyurethanes. However, the lower cost, ease of use
industry. Since composites have been used extensively in the and versatility of ABS resulted in efforts to increase its
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automotive industry via injection molding,87,88 there is potential biocompatibility.105 As a result, the FFF parts from ABS were rst
for 3D printing to be used for customizable jigs, xtures, and sealed via submersion in acetone, then treated with poly(-
other assembly parts.89,90 Composites are also used extensively ethylene glycol) methacrylate and subjected to photoinduced
in the biomedical industry for replacement cartilage products, gra polymerization. This process enhanced the biocompati-
bones, implants, gras, screws, and many more.91 The adapta- bility and hydrophilicity of the samples.105 Surface modication
tion of these materials into 3D printing could foster a more to ABS then allowed for its potential use in the medical device
Open Access Article. Published on 01 October 2020. Downloaded on 10/6/2020 11:47:43 PM.
personalized approach to medicine, further diversifying the industry where it had otherwise not been used before. Metalized
uses of AM technologies.44,92 automotive plastics parts were created through dynamic
Like injection molding practices, some additives used in 3D chemical processing that mixed two substrates to successfully
printing can be bres or llers. Most oen, the addition of these make a conductive lm on the outside of non-conductive ABS.104
materials in both instances serves one or more features including This was completed through OH* and super-radical suspen-
the following: (1) increasing renewability content,93,94 (2) reduc- sions mixed closely with ABS, followed by the implementation
tion of the cost by the replacement of expensive polymers with of a titanium dioxide suspension that was subjected to UV
low-cost llers/bres,95,96 (3) acting as a reinforcing agent97 and irradiation.104 The successful manufacture of electrically
improving mechanical properties. Unique composite materials conductive ABS allowed ABS to better serve the automotive
that combine polymer/metal powder are of increasing interest in industry.104 Surface modications to neat ABS have been found
3D printing applications.98 Also, blends of polymers are to increase the performance and use of FFF products in
combined with metal powders to make hybrid materials for 3D industries that have not previously used ABS for the described
printing.99 The research of these combinations of materials is applications.
recent but there are hopes for these materials to serve the 4.1.2 Neat ABS in SLS. The use and success of printing ABS
biomedical implants industry as well as electrical industry.99 in SLS required the optimization of the laser power and scan-
ning speed. To further improve the print quality, Chen et al.106
found that pre-heating the powder to 100 C was benecial for
4. 3D printing of engineering improved surface nish. To implement ABS in industry, where
thermoplastics surface nish is a crucial requirement, the researchers sug-
gested a laser power of 24 W, a scan speed of 2000 mm s1, and
4.1 Acrylonitrile butadiene styrene a layer height of 0.2 mm.106 The printed parts would have the
Acrylonitrile butadiene styrene (ABS) is an engineering ther- potential for non-structural components of a car, such as
moplastic derived from a combination of three petroleum dashboards and cup holders, which require a smooth surface
sources. The major constituents include acrylonitrile, buta- nish to maintain the appearance/aesthetics with traditional
diene and styrene in weight percentages of 15–35, 5–30 and 40– injection moulded parts. Parameter optimization studies are
60, respectively.100 The mixture of these copolymers generates very helpful in learning what factors impact product quality and
parts that have a balance of rigidity and light-weight traits. The production times. These are important aspects to consider
versatility of ABS has made this polymer one of the most when the mass production of a part is required.
popular to use since its development in the 1950s.100 The poly- 4.1.3 ABS blends used in E3DP. One strategy to modify and
mer has been studied for its use in biomedical applications potentially improve the viscoelastic properties of ABS is to blend
such as printing handles for scalpels and forceps, as well as with a thermoplastic elastomer. One of the most common
other surgical tools.101 However, this material also functions thermoplastic elastomers used in FFF is TPU. In one work, ABS
well in the industrial and electronics sectors. The adaptability of was combined with TPU in varying weight concentrations.79 The
ABS has resulted in its use with various other materials for 3D prints were generated through a trial-and-error process to
printing. determine optimized printing parameters. The printing
4.1.1 Neat ABS in E3DP. The use of ABS in 3D printing was parameters are described in Table 2. The mechanical perfor-
extensively studied in the early 2000s, which has led to much of mances of the blends are displayed in Table 3. The relative
its use to date.102,103 Designs of experiments were completed to maintenance of mechanical properties was attributed to
compare which printing parameters were of the greatest supramolecular interactions induced by hydrogen bonding
importance in relation to the mechanical performances.102 between the aromatic and polar groups of ABS and TPU,
These works laid the foundation for the research completed to respectively. Two interesting aspects of this work were as
date. follows: (1) the increased presence of elastomer increased the
Since there have been many works completed with ABS in bond strength of the materials, and (2) the presence of elas-
FFF, there has been a shi in focus to printing neat ABS and tomer at the highest studied content of 30 wt% was able to
then adding surface treatments. The surface treatments allow improve the adhesion to the bed and, therefore, result in the
the ABS to be used in areas where it had not been used previ- ability to print ABS at room temperature.79 Since ABS material
ously, such as the automotive104 and medical industries.105 blends can be printed at room temperature, there is no need for
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Table 2 Optimal properties for 3D printing engineering thermoplastics
Materials Method Parameters Ref.
ABS/PA 6 and ABS/PA 6/SMA BAAM Speed: 1.795 in per s, melting temperature: 220–280 C 7
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ABS FFF Melting temperature: 230 C, speed: 90 mm s1, bed
temperature: 100 C, layer height: 0.1 mm
PA Melting temperature: 260 C, speed: 72 mm s1, bed
temperature: 80 C, layer height 0.1 mm
ABS/PA/SMA Melting temperature: 245 C, speed: 30 mm s1, bed
temperature: 80 C, layer height 0.1 mm
ABS FFF Layer thickness: 0.127–0.3302 mm, raster angle 0 –45 , 177
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raster width: 0.2032–0.5588 mm, air gap: 0.00254 to
0.5588 mm, part orientation 0–90
PA 12 FFF Nozzle: 245 C, bed temperature: 98 C, layer height: 0.1 168
mm, speed: 25 mm s1, inll density: 75%
ABS Nozzle: 240 C, bed temperature: 80 C, layer height: 0.1
mm, speed: 25 mm s1, inll density: 75%
Poly(methyl methacrylate) (PMMA) Nozzle: 240 C, bed temperature: 90 C, layer height: 0.1
mm, speed: 25 mm s1, inll density: 75%
PEEK Nozzle: 420 C, bed temperature: 110 C, layer height: 0.1
mm, speed: 20 mm s1, inll density: 75%
PC Raster width: 0.432 mm
PA 12 SLS Optimized properties for mechanical performance: 45
0.15 mm layer thickness, feed powder temperature 50 C,
heated platform, 45.7 W ll laser power, 10.9 W outline
laser power, 4000 mm s1 speed, 0.3 mm scan spacing
Optimized properties for accuracy: 0.10 mm layer
thickness, feed powder temperature +100 C, unheated
platform, 11 W ll laser power, 5 W outline laser power,
5000 mm s1 speed, 0.15 mm scan spacing
PBT SLS Wavelength: 10.6 mm; laser beam diameter: 0.3 mm; 25
laser power for ll and outline: 5, 11, 20 or 30 W; scan
speed 5 m s1; powder bed temperature: 190, 193 C;
layer thickness: 0.1 mm
ABS/SEBS 100/0, 95/5, 90/10, 80/20, 50/50 ME3DP Inll: 100%, layer height: 0.2 mm & 0.27 mm, number of 12
shells: 1, feed rate: 40 mm s1, travel speed: 55 mm s1,
nozzle diameter: 0.4 mm & 0.8 mm, print temperature
230 C & 240 C
ABS/UHMWPE/SEBS 75/25/10, 90/10/10 ME3DP Inll: 100%, layer height: 0.2 mm, number of shells: 1, 82
feed rate: 40 mm s1, travel speed: 55 mm s1, nozzle
diameter: 0.8 mm, print temperature 230 C
ABS MG47/SEBS-g-MA ME3DP Nozzle: 230–280 C, bed temperature: 110 C, inll
density: 100%, print speed: 30 or 60 mm s1, nozzle
diameter: 0.6 mm
ABS MG94/SEBS-g-MA Nozzle: 230–265 C, bed temperature: 110 C, inll
density: 100%, print speed: 30 or 60 mm s1, nozzle
diameter: 0.6 mm
PA/ABS/SMA (85/10.5/4.5) BAAM (pellets) Extrudate temperature: 250 C, print speed: 1.795 inch 7
per s, bead width: 0.289, wall thickness: 0.530 in
PA/ABS/SMA 60/40 with 5 to 20 phr of SMA FFF Neat ABS: nozzle temperature: 230 C, layer height: 0.1
mm, bed temperature: 100 C, print speed: 90 mm s1
Neat PA: nozzle temperature: 260 C, layer height: 0.1
mm, bed temperature: 80 C, print speed: 72 mm s1
Compatibilized blends: nozzle temperature: 245 C, layer
height: 0.1 mm, bed temperature: 80 C, print speed:
30 mm s1
ABS/TPU 90/10, 80/20, 70/30 FFF Nozzle: 230 C, bed temperature: 110 C, inll density: 79
100%, print speed: 30 mm s1, layer height: 0.2 mm, bed
temperature 25 to 90 C
PEK virgin/used: 80/20 & 70/30 SLS Laser temperature: 368 C, layer thickness: 0.12 mm, CO2 48
laser, exposure time: 12 s, laser power: 15 and 16.5 W,
scan speed: 2250 mm s1
PP/PA 6 80/20 SLS Layer thickness: 100 mm, scan speed: 1257 mm s1, 68
powder roller: 80 mm s1, laser power: 6, 7, 8, or 9 W
PA 12/HDPE 80/20, 50/50, 20/80 SLS Laser beam diameter: 250 mm, layer thickness: 150 mm, 69
wavelength 10.6 mm, scan speed: 80 mm s1, laser power:
3, 6, or 12 W
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Table 3 Properties of 3D printing engineering thermoplastics, their blends and composites
Sample Method Composition (%) TS (MPa) TM (GPa) Strain at break Ref.
PA 6 BAAM 100 92a 5.2a 0.022a 7
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PA/ABS/SMA 85/10.5/4.5 84a 3.4a 0.032a
PA FFF 100 42a 0.225a 2.6a
ABS 100 32a 0.320a 0.85a
PA 6/ABS/SMA 95 (60/40)/5 52a 0.305a 0.50a
ABS FFF 100 10.44–34.61 — — 177
PA 12 FFF 100 43.08 (1.54) 0.757 (0.194) — 168
ABS 100 28.97 (0.53) 2.760 (0.050) —
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Poly(methyl methacrylate) (PMMA) 100 56.25 (1.95) 2.750 (0.050) —
PEEK 100 68.04 (7.01) 3.530 (0.010) —
PC 100 56a 2.01a —
PA 12 SLS (Lboro) Used 40 1600 12.5 45
Virgin 35 1600 4
SLS (TNO) Used 50 1700 17
Virgin 50 1700 13
PBT (LD: laser density (kJ m2)) SLS 100 (LD: 6.7) 18a 1.3 (at 25 C) 2a 25
100 (LD: 14.7) 55a 1.95 (at 25 C) 3.75a
100 (LD: 26.7) 51a 2.0 (at 25 C) 3.5a
100 (LD: 40.0) 42a 2.25 (at 25 C) 3.25a
ABS/SEBS ME3DP 100 : 0 34.0 (1.74) — 8.6 (3.3) 12
95 : 5 25.5 (2.3) — 3.6 (0.7)
90 : 10 26.2 (2.5) — 4.0 (1.1)
80 : 20 25.2 (1.8) — 11.9 (2.1)
50 : 50 18.0 (0.03) — 47.6 (5.0)
ABS/UHMWPE/SEBS 75 : 25 : 10 14.7 (0.7) — 5.7 (0.7)
90 : 10 : 10 23.19 (0.8) — 8.4 (1.0)
ABS MG47/SEBS-g-MA ME3DP 100 : 0 34.01 (1.3) 2161 (247) 5 82
75 : 25 17.34 (1.1) 1391 (140) 20
50 : 50 12.86 (0.3) 675.7 (151) 30
25 : 75 7.33 (0.8) 70.70 (21.3) 500
ABS MG94/SEBS-g-MA ME3DP 100 : 0 33.04 (2.14) 2280 (341) 5
75 : 25 25.09 (1.2) 1484 (141) 9
50 : 50 13.21 (0.3) 690.3 (88.4) 65
25 : 75 11.55 (0.2) 43.08 (4.46) 850
10 : 90 10.16 (0.5) 14.98 (3.69) 1100
PA/ABS/SMA (x-direction) BAAM (pellets) 85/10.5/4.5 86 3400 3.2 7
PA/ABS/SMA wt%/wt%/phr (x-direction) FFF (lament) 60/40/5 52 300 5
60/40/10 16 160 2
60/40/20 34 240 2.5
ABS/TPU FFF (lament) Neat ABS 28.5b 800 6 79
90/10 30b 830 5
80/20 27.5b 750 6.5
70/30 20.2b 725 15
Neat TPU 20.5b 8 795
PEK virgin/used blends SLS (15 W laser power) 100/0 90 — 3.6 48
80/20 80 — 3.6
70/30 75 — 3.0
PP/PA 12 SLS (6 W laser power) Neat PP 30 1950 — 68
Neat PA 12 47 1800 —
80/20 10.5 1750 —
ABS 1,3,5 wt% OMM (XY print direction) FFF 100/0 27.59 1900 1.2 114
99/1 31.59 2600 1.4
97/3 36.33 3000 2.8
95/5 39.48 3200 3.6
a
Values were approximated from graphical data. b Yield strength.
a heated chamber. Chambers are structures that surround the associated reductions in cost since less energy (electricity) is
printer and maintain elevated temperatures to reduce the required to heat and maintain elevated temperatures. Bene-
warpage of the samples. The chamber is oen maintained at the cially, the reduced need for a chamber by implementing ABS
glass transition temperature of the polymer.107 There are blends resulted in reductions in the associated cost from energy
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consumption. Potentially, the ability to produce ABS blends 3D printing, more work is required to improve the perfor-
without a chamber could improve the circular economic aspects mances of the materials before implementation on a larger
of this process by reducing resource consumption. Further- scale.
more, the reduced energy consumption has the potential to Sized macadamia nut shells were used as natural ller in
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slightly reduce the greenhouse gas emissions for each print. compatibilized ABS-based composites for FFF. The matrix
Siqueiros et al.82 also studied the effects of SEBS on two ABS contained 3 wt% maleic anhydride and 68 or 78 wt% ABS.110
samples of different molecular weights in attempts to develop Filaments with 1.75 mm diameter were printed with 100% inll
blends that can function under an array of applications.82 The through a 0.5 mm nozzle. This work showed promise since the
mission of this paper was to fabricate new printable materials addition of macadamia shells reduced the density of the printed
with a wide variety of physical properties. The blends were samples in comparison to the other wood llers used in this
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optimized through a mixtures design and the chosen parame- study, as well as maintained or enhanced the mechanical
ters are displayed in Table 2. Many successful blends were performance110 as compared to other wood-lled materials. The
printed and a wide range of properties were obtained (Table 3). performances of the macadamia composite prints were
One of the most unique outcomes was that the lower molecular compared to PLA and ABS-printed samples and found to have
weight ABS (MG94) with 90 wt% SEBS was able to improve the lesser mechanical performances. The challenges with some
percent elongation at break by 1500% over that of neat ABS.82 composites, as conrmed in this work, arise from the formation
The success of the prints and unique blends demonstrated of voids during printing. The voids around the ller reduce the
properties strong enough to support shock absorbers and stress dissipation and result in the localized bucking of samples
actuators, which would be a novel application for 3D printed when compressed. Macadamia shells can be obtained at little to
parts.82 This method was noted to be an economically feasible no cost since they are a food-industry waste. This means that the
alternative to thermoplastic elastomer printing materials that nutshells are a by-product of processing the nuts that are then
are currently on the market.82 prepared for packaging and consumption. The shell and other
4.1.4 E3DP of ABS bre-reinforced composites. Contin- remnants le behind are waste biomass. Waste biomass from
uous carbon bre (CF) composites made with thermoplastics the food-processing industry is essential for generating
are also advantageous for the potential recycling of the mate- sustainable products that align with a circular economy.111,112
rials at the end of their intended life.86 Thus, the implementa- This offers a comparative cost or advantage for mass
tion of these materials could improve the sustainability through production.
recycling and could also address concerns about the limited 4.1.5 E3DP of ABS nanocomposites. Nanocomposites in
mechanical performance. The continuous bres showed the additive manufacturing industry have attracted increasing
promise for load-bearing parts86 that would better serve indus- interest because the resulting products are oen lighter and
tries such as automotive and aerospace. The obtained proper- stiffer than neat polymers alone.113,114 Lignin-coated cellulose
ties are customizable based upon bre distribution and nanocrystals (L-CNC) in combination with ABS were fabricated
orientation.86 and studied as a novel material with unique thermal and
A combination of ABS and CFs was used to synthesize la- mechanical properties. Combinations of L-CNC from 0 to
ments with 10, 20, 30, and 40 wt% CF loading. The CFs and ABS 10 wt% were melt-compounded with ABS with a twin-screw
were mixed then placed into a hopper at 220 C. The print extruder at a co-rotating conguration to optimize mixing and
conditions included a nozzle temperature of 205 C, nozzle dispersion. Aer laments were made, samples were printed via
diameter 0.5 mm, bed temperature of 85 C and a layer height of FFF. One of the critical aspects of this work was the dependency
0.2 mm. Samples of 40 wt% CF could not be printed due to of ow during 3D printing since the temperature of the extru-
clogging. For the samples that were printed successfully, it was date impacted the ller mobility and the overall porosity of the
determined that the CFs were oen oriented in the ow direc- samples. Increased porosity in the samples resulted in reduced
tion, which was assumed to happen during extrusion. The mechanical performance as compared to injection-molded
strength of the composites was also found to increase for the 3D samples and is one of the limitations with printing
and compression moulded samples with CF showing promising nanocomposites.113
potential for these materials in load-bearing applications.108 In work conducted by Weng et al.,114 ABS was combined with
The use of 3D printing parts in load-bearing applications would organically modied montmorillonite (OMM) and prepared for
be an advancement for this technology to serve a greater FFF. Like most 3D printing samples, there was a large decrease
number of applications. in the mechanical properties from the injection-moulded to 3D
Additional materials that are oen used to fabricate sample values. The loss in mechanical performance was
composites include natural llers or natural bres. These attributed to a lack of polymer chain entanglement between
materials have been used to increase the biocontent or vary the layers, as well as gaps and voids created by the circular nature of
mechanical performances. Osman et al.109 used ABS in combi- the molten polymer. Interestingly, for this work, the addition of
nation with rice straw as a method to generate value-added ller was able to increase the tensile strength and modulus as
products from waste material. However, this work experienced noted in Table 3. Furthermore, the ller was able to decrease the
a decrease in mechanical properties with the addition of natural linear coefficient of thermal expansion.114 This is a benecial
bre. Also, the water absorption in the samples increased.109 trait as it ensures better dimensional stability at elevated
Although this work was one of the early uses of natural llers in temperatures, i.e., maintaining geometry during printing.
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Filaments of ABS and up to 10 wt% multiwalled carbon prosthetics because of the tough, versatile and durable nature
nanotubes (MWCNT) were generated on a twin-screw extruder of these materials.92 Some mentionable PAs in this paper
and resulted in a lament diameter of 1.7 mm.115 The 3D include PA 6,6, PA 6, PA 12 and PA 11.
printing parameters for these samples were as follows: 0.4 mm PA 6,6 is formed from a combination of diacids and
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nozzle diameter, 30 mm s1 print speed, bed temperature diamines. It was the rst commercialized polyamide and was
110 C, melt temperature of 245 C and layer thickness of 0.2 synthesized at Dupont in 1935.117 It is formed from the
mm. The strength was highest in samples with 10 wt% loading. condensation reaction of adipic acid and hexane-1,6-diamine.
Overall, successful composites were generated.115 The studied This material is oen used for small brous parts such as
materials were suggested for applications where electrical and toothbrush bristles and clothing.117
thermal conduction were required since the MWCNT increases PA 6 was the second polyamide synthesized and became
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both these aspects. commercially available shortly aer PA 6,6.117 The monomer
4.1.6 SLS of ABS composites. In another work, ABS was unit of PA 6, called caprolactam, is a ring-shaped structure that
used in SLS and was combined with a compatibilizer, impact is polymerized by a ring-opening reaction120 to form the poly-
modier, thermoplastic starch (30 wt%) and colourant. The mer. Each monomer has the chemical formula C6H11NO.
preparation of composites required several steps to product PA 12, an aliphatic engineering thermoplastic, is formed by
laments. The rst step focused on the plasticization of the the ring-opening polymerization or condensation reaction of
starch with water and glycerol and compounding (70 C, 500 lauryl lactam or an u-amino acid, respectively.124 Uniquely, PA
rpm). Pelletized starch was then melt-compounded (180 C, 600 12 has two stable crystal structures, a- or g-, where the g-form is
rpm) with ABS, compatibilizer, and impact modier to generate the more stable crystal with a higher melting temperature.45 The
laments with the 1.75 mm required diameter for FFF. Samples crystalline characteristics are the largest factors that hinder the
were successfully printed with a printed melt temperature of printability of PA 12.
210 C. It was anticipated that the combination of materials Polyamide 11 (PA11) is made up of monomer units of 11-
could better serve the industrial, mechanical, electronics and aminoundecanoic acid, which is made from castor beans.125
automotive sectors based upon (1) the high thermal stability of Not only is this a biologically-based polyamide, but it is very
the composites, (2) good mechanical properties, and (3) versatile. PA 11 has been used in applications ranging from
reduced volatile organic compound (VOC) emissions.116 To aerospace to automotive and textiles to sports equipment.125
validate this experiment and recommend the materials for Further applications of PA 11 include AM, which is most oen
commercial use, a cost comparison of these materials with implemented in SLS technologies.125
existing market products would need to be conducted. This 4.2.1 E3DP of neat PAs. Polyamides are an exceptionally
means that if the total cost for raw materials to fabricate these versatile material that has fostered their use in many industries.
composites is greater than that of the neat polymer (which is Part of the diversity is correlated to the many PA materials
commercially available), there needs to be an incentive for available such as PA 12, PA 6, PA 6,6, and many others. One of
industry or the consumer. Essentially, the implementation of the unique polyamides studied in E3DP was PA 1012.126 The
new printing materials oen requires materials to be econom- success of the print (dimensional stability, completeness and
ically feasible, viable and sustainable. a lack of warpage) was largely inuenced by the bed and nozzle
temperatures. Other recent works have focused on FFF with PA
12. One of the challenges with PA 12 is that it is semi-crystalline,
4.2 Polyamides which can result in more warpage or challenges during
Polyamides (PAs) are formed from condensation reactions printing. It has an optimal nozzle temperature of 250 C, raster
between acids and amines. Traditionally, PAs implemented in angle of 45 and 100% inll density, samples with good
commercial production were made from petroleum-based interlayer bonding and only 4% less ultimate tensile strength
resources.117 However, a push for green chemistry and than injection molding samples.126 This work shows great
sustainable product development resulted in some PA polymers promise for the potential use of PA 12 in commercial and reli-
now synthesized from biological sources. Examples of biobased able materials for E3DP.
sources used to produce PAs include the diacids like succinic 4.2.2 SLS of neat PAs. Although there have been works that
acid or sebacic acid. For instance, bio-succinic acid is made have successfully printed PA 12 and PA 11 via SLS, there tends to
from microorganisms where succinic acid is a by-product of be a lack of reproducibility in parts.45 A lack of consistency may
their natural Krebs cycle.118 As for diamines, the counterpart of include reduced dimensional stability or surface appearance,127
polyamide synthesis, in some cases is based on organic thus, resulting in less consistent products, which may be chal-
compounds. An example of this is hexamethylenediamine, lenging for mass production where identical parts are impor-
which is used in the synthesis of PA 6,6.119 The relative amounts tant. This may also increase waste since many replicates are
of diacid and diamine used in the synthesis are the basis for the required. Oen, the lack of reproducibility is a result of the
naming convention of polyamides.120 shrinkage of the samples and is largely inuenced by the crystal
Diversity within the polyamide family of polymers has structure. Zarringhalam et al.45 addressed these concerns by
resulted in polymers that are crystalline, amorphous and taking a closer look at the crystal structure, chemical structure
brous;119 for this reason, it has been studied extensively.84,121–123 and microstructure of PA 12. The authors found that the g-form
Polyamides have more recently been studied for use in of the crystals was most impacted by the processing conditions.
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This work also provided insight into the mechanical perfor-
mance of PA 12 in SLS; the used powder possessed an increased
molecular weight as compared to virgin powder. The increase in
the molecular weight of the particle was attributed to better
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elongation at break properties.45 Researchers demonstrated
that the optimized properties for the SLS process were tailored
for the nal product based upon mechanical performance or
accuracy (Table 3). The optimization of the laser properties for
either the accuracy or the mechanical performance was unique
for this work since most work is only optimized for one purpose.
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Other challenges with SLS have been summarized by Schmid
et al.,128 who suggest that SLS can be improved through the
optimization of (1) particle size and shape; (2) aging, distribu-
tion and owability of the powder; (3) optics and thermal Fig. 6 Optical microscopy image displaying the crystal structure of PA
characteristics of the powder, and (4) rheological properties of 12.45 Reprinted with permission from Elsevier: Materials Science and
Engineering: A, Copyright 2019, License: 4838261169022.
the bulk material128 (Fig. 5).
To improve the sustainability of the SLS process, it would be
important to reuse the powders that were present during the
printing but not sintered. Researchers found that the tensile Engineering thermoplastics can also be used to address yet
strength and elongation of samples prepared via SLS with used another shortfall of SLS; that is, the thermal degradation of non-
powders were equal, if not better than that of the SLS-printed sintered powders and their limited re-use. In the long run, if
samples fabricated from virgin polymer.45 Optical microscopy properly addressed and used samples were no longer a waste
determined that there were various cores present in the PA 12 product, then the use of SLS in mass production could be
samples and this likely affected the mechanical performances allowed.129,130 Since there is an accumulation of aged/used
(Fig. 6). The more cores present indicated that there was a better powders in SLS, it is more advantageous to use recycled
melting of the polymer, correlating to better particle fusion and powder in combination with non-sintered materials to improve
superior mechanical performance. The increased number of cost efficiency and sustainability. To implement used powders,
crystals, by samples printed on the machine trademarked by the a greater understanding of the chemical and physical effects of
name TNO, likely resulted in the improved mechanical perfor- aging on the powder's performance and the printed parts is also
mance.45 Although the authors only looked at PA, similar trends required. Wudy and Drummer129 discussed that studying the
could likely be found in other polymers. The reuse of materials effects of time and temperature on the thermal properties and
is both economically and environmentally favourable and molecular characteristics could lead to a solution.129 Although
should be implemented when possible. both the build time and temperature affect the molecular
weight, the effect of the chamber temperature on aged samples
Fig. 5 Parameters of powder and processing conditions that influence SLS printed products.128 Reprinted with permission from Cambridge
University Press: Journal of Materials Research, Copyright 2014, License: 4840231185789.
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is more substantial. Ultimately, researchers determined that the Interestingly, the tensile modulus was the only property that
increased molecular weight results in reduced chain mobility, remained relatively similar for the blend and neat polymers
which is a disadvantage for SLS.129 This work highlighted the (Table 3).68
importance of temperature and its correlation with build time Another work combined PA 12 with a more traditional
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based upon the molecular structures present. With a greater thermoplastic called high-density polyethylene (HDPE).69 The
understanding of print temperature, build time, molecular microcrystalline structures of the blends were measured and
structure and their dependence on each other could be taken to compared to the mechanical performances of samples. The
industry to further optimize the printing process. This then printing parameters, noted in Table 2, were optimized to
addresses the shortcomings of SLS, which have prohibited its improve the cohesion between materials. The authors deter-
adaptation to large-scale production to date. mined that the HDPE remained as a co-continuous phase and
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4.2.3 E3DP of PA blends. Polyamide 6 was combined at oen remained separated from PA. To improve the laser sin-
30 wt% with a polypropylene (PP) blend. The PP blend was tering between materials, the viscosity of HDPE required focus.
1.5 : 1 for PP to maleic anhydride graed poly(ethylene-octene) Overall, the blends could be used as new materials with tailor-
(MA-g-PEO). Therefore, the overall blends were 30 wt% PA and able properties to improve the applications of SLS.69
70 wt% of the 1.5 to 1 blend.131 Samples were printed at melt 4.2.5 Polyamide composites in E3DP. Carbon bre is
temperatures between 220 and 250 C, bed temperature of debatably the most common bre used with engineering ther-
110 C, 0.1 mm layer height and speed of 30 mm s1. This moplastics for 3D printing. Many works have been completed
material was studied for its shape memory characteristics and with this combination of materials.108,133,134 Carbon bre as
reduced warpage with the presence of the compatibilizer, MA-g- a reinforcing agent in various polymers for injection molding
PEO. Essentially, the compatibilizer fosters improved bonding practices has been of interest due to the enhanced properties as
between the non-polar PP and polar PA 6.131 If shape memory is compared to the neat polymer.135 In hopes of achieving similar
a requirement of a printed part, this strategy has the potential to improvements to that of injection molding, researchers have
also be applied with other engineering thermoplastics. combined carbon bre with PAs for E3DP. Researchers wanted
4.2.4 Selective laser sintering of PA blends. Used PA to conrm that the combination of carbon bre in a PA matrix
powder is described as a powder that has been used in the could improve the impact strength and load capabilities of the
sintering process but has not been solidied into a part. Used printed parts.136 This paper highlighted a substantial improve-
powders oen experience thermal degradation and possess ment in impact strength based upon the build orientation of the
reduced properties. As a result, researchers have explored the samples, as well as increased impact strength with a greater
reuse of PA powder for cost savings benets.132 However, to volume fraction of bres.136 This work is important since we are
generate viable nal products, the layer thickness, laser speed all aware that in most cases, extrusion 3D printed products are
and power, as well as build temperature must be optimized for affected by anisotropic properties and cannot function well in
a desired mechanical performance (such as ultimate tensile load-bearing applications. It is important to note the correlation
strength).132 The authors determined that the reuse of PA would between parameters such as print direction and bre orienta-
be possible without compromising the quality of the fabricated tion such that products can be developed with desired
part, such as mechanical performance and dimensional accu- mechanical performance and can serve a greater number of
racy of the print. This further suggests that this material could applications. Other works with polyamide-based composites
be used in the biomedical industry to optimize performance, have also helped to address the limitations of E3DP such as
cost and sustainability,132 where PAs most oen are used in anisotropic properties and lack of weight-bearing capabilities.
prosthetics.80 Continuous carbon bres combined with PA 6 were studied
The purpose of this work was to design tailor-made and based on the optimization of the interface between the bre and
graded feedstock materials for SLS. Blending is a more cost- matrix.137 By sizing the bres, there was reduced pull-out and
effective and industrially implemented strategy to develop improved interfacial adhesion; these materials are more likely
novel printing materials as compared to trying to synthesize to succeed in industrial applications.137 Another work only
new polymers.68 Drummer et al.68 combined polypropylene and required 10 wt% of carbon bre with PA 12 to result in more
PA 12, an immiscible blend, to form samples through varied than 100% increase in both exural and tensile strengths.138
laser power. This work provided fundamental insight as to how The implementation of carbon bres is one way to address the
the building temperature can be determined from DSC anal- limitations in the strength of extrusion 3D printer materials and
ysis.68 Blends of 20 wt% PA 12 and 80 wt% PP were mixed and reduce the impact of anisotropic properties.
placed in the bed and printed with the parameters discussed in Other brous materials such as glass bre and Kevlar have
Table 2. The authors found that the increased laser power been used in engineering thermoplastics for traditional injec-
resulted in better adhesion between layers as conrmed by tion molding. These materials oen function in structural
microscopic analysis. According to the SEM analysis of the components and the bres act as reinforcing agents to dissipate
fracture surface, the dispersed phase was noted to have less the load. The same concept is being adapted to 3D printing as
adhesion to the continuous phase but was also slightly mentioned previously. Caminero et al.136 also studied the
improved through increased laser power. The lack of adhesion addition of glass bres, carbon bres and Kevlar to PA for FFF.
between phases was used to explain the reduced mechanical There are two orientations compared for printing such
performance of the blends as compared to either neat polymer. composites which were found to impact their performance. The
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rst of which is the at orientation, where the largest face of the the preliminary stage of research, it does show promise for
impact sample adheres to the bed. The second orientation electronic applications. This would potentially increase the use
requires the placement of the sample on-edge, where the of SLS for parts that are traditionally injection-moulded. To
surface opposite to the notch is in contact with the bed. All further increase the electrical nature of materials, the research
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samples were printed with a rectangular inll pattern at 0 and has focused on the development, adaptation and success of
in every case, the samples printed in the on-edge formation hybrid materials.
resulted in superior performance. The authors offered a partial Inorganic additives are used in SLS and other 3D printing
solution to the limited impact performance of 3D printing methods to diversify the mechanical performances. Diversied
samples, which is a short-coming of this technology. The solu- mechanical performance, thermal performance or printability
tion is to print samples in the on-edge orientation to orient the may allow 3D printing objects to better serve structural
Open Access Article. Published on 01 October 2020. Downloaded on 10/6/2020 11:47:43 PM.
bres to improve the impact properties.136 Although this is one components or other applications where 3D printing is
viable solution to improve the impact strength of the printed currently not implemented. Hybrid systems can be made from
parts, there is still a requirement for improved mechanical a combination of two or more llers in one polymer matrix. As
performances overall. Researchers continue to address these an example, BaTiO3 was combined with PA 11 and carbon
concerns in hopes of developing 3D printing parts with nanotubes to form a unique nanocomposite material.139
enhanced mechanical performance and improved impact Samples were printed with 7.5 W laser power, 0.1 mm layer
strength. thickness and a laser scanning speed of 7.6m s1. The combi-
4.2.6 Selective laser sintering PA composites. In SLS, it is nation of ller and polymer showed promise with an increased
common to combine polyamides with inorganic additives.139,140 sintering window and higher laser absorption. These materials
Inorganic additives are those that do not contain carbon, such resulted in improved dielectric properties and possess the
as silica-based materials, minerals, or metals. Many works also potential to serve a unique purpose in energy storage devices or
combine llers derived from petroleum sources such as carbon energy harvesting.139 This is yet another industry where AM has
black or carbon bre. The combination of llers helps to the potential to benet from greatly.
fabricate novel materials with varying mechanical,139 elec-
trical,139 morphological and thermal properties.121 This fosters
the use of SLS in the automotive, aerospace, thermal,141 elec-
tronics,121 and energy139 sectors. 4.3 Engineering thermoplastic polyesters
A unique work worth noting is focused on the use of y ash Polyesters are formed from the condensation reaction of an
hollow spheres (FAHS) with PA 12.141 Fly ash is an inorganic acid, oen adipic or sebacic, with an alkanediol.143 Like PAs,
material made from carbonaceous particulate spheres in some precursors are now sustainably sourced to improve the
combination with ash spheres (containing silica). These mate- biocontent of the polymers.
rials are oen generated as a by-product contained in the ue Polybutylene terephthalate (PBT) is a linear aromatic poly-
gas from burnt fossil fuels.142 Polyamide 12 was combined in ester synthesized from 1,4-butanediol and terephthalic acid.
varying amounts (from 10–25 wt%) with FAHS to make light- PBT is a versatile engineering thermoplastic with a semi-
weight ceramic foams. These foams can be 3D printed for crystalline structure.19 Some of the benecial properties of
novel applications. One of the fundamental ndings in this PBT include excellent electrical properties, good chemical
work was the reduction in the thermal conductivity of the resistance, good processability, and good modulus and
materials141 as would be expected when combining a silica- strength, even at elevated temperatures.144 PBT is most
based ller with a polymer. The ceramic foams made in this commonly used in the automotive sector as a functional
work could be used to fabricate custom and intricate insulating material in housing, panels and electrical components.144
materials, which suggest that there is potential for this material The synthesis of polyethylene terephthalate (PET) requires
in high-temperature applications such as automotive and the combination of ethylene glycol with terephthalic acid. The
aerospace because of the improved heat transfer. In high- exceptional thermal and chemical stabilities of PET have led to
temperature applications, the transfer of heat must be mini- its use in automotive applications such as canopy covers.145
mized such that there are no changes to the geometric shape or Furthermore, PET is widely used in the beverage and packaging
performance of the materials. However, more work is required industry but also serves as a material for components in the
with FAHS and PA 12 composites to improve the control over the electrical industry.146 Other important properties of PET include
pore size since this directly relates to the strength of the its resistance to shattering, its relatively light-weight nature,
materials. and exceptional barrier properties.146 The combination of the
The combination of PAs with inorganic llers like carbon properties of this semi-crystalline polymer makes it one of the
black could better serve the electronic industry by fostering the most used engineering thermoplastics to date.
development of electrically conductive materials. Carbon black The combination of 1,3-propanediol (PDO) and terephthalic
(CB) was combined at 4 wt% with PA 12 to generate121 an acid is used to synthesize poly(trimethylene terephthalate)
increase in the electrical conductivity by 5 orders of magnitude (PTT), a high-melting-point polyester.70 The exceptional thermal
as compared to the neat polymer. The mechanical properties of stability and elastic recovery have indicated that PTT is suitable
these materials were further rened by the optimization of the for use in engineering and textile applications.70 Over the last
laser powder and scanning speed.121 Although this material is in decade, the PDO content of this polymer has been renewably
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sourced, resulting in a 37% renewable content as compared to compared to some engineering thermoplastics.25 Likewise, PBT
100% petroleum-based polyesters.147 also offers good mechanical performance and high chemical
4.3.1 Neat engineering thermoplastic polyesters in E3DP. resistance,25 which has led to its adaptation in SLS.149 Arai
In addition to improved thermal stability and mechanical et al.149 studied the use of PBT in SLS with careful attention to
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performances, improved sustainability content has been the printing conditions (Table 2) since the conditions strongly
important for product development and can be done through impact the mechanical performance.25 The milling process of
the implementation of renewably-sourced or recycled engi- PBT resulted in metal contaminants present in the samples.
neering thermoplastics. Recycled polymers oen experience Benecially, the metal contaminants acted as nucleating agents
a decrease in mechanical performance or changes in other (Fig. 7a) to increase the crystallization temperature25 and
characteristics, such as thermal stability and appearance, as mechanical performance (Table 3). Crystallization of the poly-
Open Access Article. Published on 01 October 2020. Downloaded on 10/6/2020 11:47:43 PM.
compared to the neat polymer.24 However, there is a desire to mer is a fundamental aspect of 3D printing and should be
generate products that fulll aspects of the circular economy, considered prior to printing because it oen affects the quality
where waste is repurposed for value-added products. The of the print. The addition of the metal contaminants may have
adaptation of used polyester engineering thermoplastics for 3D been ideal for sample quality but are not ideal where these
printing is a promising method to repurpose recycling. contaminants could cause a risk during use.25 Arai et al.,25 were
In FFF, Zander et al.66 used recycled PET bottles to generate successful at displaying a connection between laser power and
lament feedstocks. The mechanical performance of the prin- mechanical performance. Laser power affected the formation of
ted samples displayed only a small loss in elongation at break as crystals (Fig. 7b and c). For tensile strength, tensile modulus
compared to injection-moulded samples. However, the tensile and elongation at break, the increased laser power resulted in
strength was comparable to other commercially available la- superior performance.25 Essentially, the industry could prepare
ments that are blends of neat PC–ABS.66 The success of the tailor-made samples through adjusting the laser power, further
recycled material was in part attributed to additives that form allowing the same material to be used in a wide range of
the PET into bottles prior to the initial use. The additives applications.
functioned as nucleating sites that impact crystal growth and One of the greatest challenges of printing polyesters is that
size, further improving the printability of the recycled PET. This they are crystalline, which creates more dened melting char-
work provided fundamental insight into how to generate acteristics but results in delamination, warpage/curling as well
sustainable and diverse laments to serve a wider range of as limited dimensional stability during the re-crystallization
industrial applications if the material was commercialized. process.6,150 Such limitations have been investigated for SLS of
4.3.2 Neat engineering thermoplastic polyesters in SLS. PET. Bashir et al.150 were able to successfully print the PET
Historically, injection molding has been used to make powder through the implementation of ideal printing parame-
consumer goods or products rather than SLS since the samples ters and overcome the limitations mentioned above. The ideal
generally possess superior mechanical performances. However, printing parameters with a CO2 laser included part bed
injection molding is not well suited for circumstances where temperature of 225 C, feed temperature of 160 C, laser scan
complex geometries are required, since complex parts oen speed of 4 m s1 and layer thickness of 100 mm. Aer printing,
require post-production modications. It has been suggested in the bed plates were le at 200 C to anneal the samples and
the literature that the use of polyesters like PET has been of benecially increase the crystallinity. From the process and
interest in SLS because they offer the potential to replace PA 12 print optimization, the authors found that PET had a wider
(one of the most common commercially used materials).148 processing window, improved part denition, better surface
Poly(butylene terephthalate), commonly used in injection nish, and larger particle size tolerance as compared to PA 12.150
molding, offers high heat resistance and relatively low cost as This was an important discovery for this work as traditionally,
Fig. 7 Polarized optical microscopy images of room temperature (a) pellets, (b) powder, (c) powder with 0.1 wt% silica.25 Reprinted with
permission from Elsevier: Materials & Design, Copyright 2019, License: 4694240888567.
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PA 12 was the most commonly used material in SLS. The of biobased materials. When heated, biobased materials are
improved part denition is the ability of the printer to maintain converted to carbon-based black material (also referred to here
the dimensional accuracy of the computer-aided design and as biocarbon), syngas and bio-oil. In work by Idrees et al.,47
a smooth or desired surface nish. Such aspects would make starch-based packing materials were pyrolyzed to generate
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printing this material commercially possible. llers to combine with recycled PET.47 All biocarbon was sized
4.3.3 Engineering thermoplastic polyester blends for E3DP to be less than 100 mm, which assists in the reduction of nozzle
Neat polymer with compatibilizer. Polyesters can be chal- clogging. Filaments were fabricated with weight loadings from
lenging to print via E3DP based on the crystalline nature of the 0.5 to 5%. The tensile modulus was highest for the 5 wt%
polymer. To combat this, PTT was combined with a chain loaded samples, whereas 0.5 wt% resulted in the greatest
extender and an impact modier for the rst time use of PTT in strength composites.47 This suggests that the biocarbon content
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FFF.6 The additives fullled two major criteria that allowed for can be tailored for commercialization, dependent on the func-
successful printing. For starters, the additives increased the tional requirements such as strength modulus or a strength-
dimensional stability of the laments such that they were stiffness balance.
consistent and met the minimum required thickness. The use Polyester nanocomposites. Carbon nanotubes (CNT) and PBT
of the compatibilizer further reduced the crystallinity, resulting laments were prepared via compounding and extruding
in less warpage during printing. This work shows a method for (240 C, 50 rpm, 5 min mix time) for FFF by Gnanasekaran
improving the printability of novel materials through a smooth et al.37 The authors also combined graphene with other
and easily implemented change during melt extrusion in Fig. 8. composites to fabricate products that were mechanically stable
This work also highlights the importance of print parameter and electrically conductive. Samples were printed through
optimization. Samples were only able to be printed under one a 0.4 mm nozzle at 20 mm s1 print speed and nozzle temper-
set of printing conditions, which were comprised of nozzle ature range of 240–260 C. The CNT biocomposites were found
temperature at the maximum value of the printer at 290 C, to outperform the graphene composites, however, both mate-
print layer orientation of 45 and 135 in alternating rows, as rials were successful at producing functional objects at a low
well as the use of a brim. The brim is the portion of the printed fabrication cost.37 This work also highlights a unique applica-
part outside of the actual sample, which was only deposited in tion for 3D printing multi-material products. This was
the rst layer. The brim is used to improve adhesion to the bed completed with a dual nozzle/head extruder so two materials
by covering a larger surface area and ensuring consistent ow can be printed simultaneously. For example, the PBT/CNT
before printing the part. This strategy is recommended for parts composites could be printed as one segment of a part, along
that have trouble adhering to the bed or tend to warp. with neat PLA to make an integrated product.37 Similar products
4.3.4 Selective laser sintering polyester blends. Blends of have been suggested for use in electrical components.151
PBT, copolymer and ame retardants were combined to make 4.3.6 Engineering thermoplastic polyester composites in
unique blends for SLS of ame-retardant applications. The SLS. The implementation of composites in SLS technologies
optimal blends were able to achieve a UL test ration of V0.149 The requires careful attention to bre orientation as this affects the
use of such materials could foster the growth of SLS technology thermal, mechanical and dimensional accuracy of the mate-
into other applications where higher ammability perfor- rials.152 A promising study combined PBT with 30 wt% short
mances are required. A cost comparison would be needed to test glass bre and subjected the samples to single and double
the economic feasibility of these blends in comparison to scanning motions during the print process. The double scan-
existing AM materials. ning practice, depicted in Fig. 9, was able to improve the
4.3.5 Engineering thermoplastic polyester composites in product quality by reducing the porosity and increasing the
E3DP mechanical performance.152 It was suggested that improved
Fiber-reinforced polyester composites. Biocarbon, also referred mechanical performance, especially in the z-direction, was due
to as biochar, is produced from the thermochemical conversion to reduced resin deterioration. If implementing PBT short glass
Fig. 8 Optimization of PTT/impact modifier/chain extender blends to make complete samples as novel use for PTT in 3D printing.6
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Single versus double scanning for SLS.152 Reprinted with permission from Elsevier: Optics and Laser Technology, Copyright 2019, License
Fig. 9
number: 4838260880549.
bre composites commercially, it is recommended to use Corporation. The polymer is semi-crystalline and possesses
double scan SLS as well, since there was a slight increase in high impact resistance and natural ame retardation. The
HDT.152 synthesis of PEK was not only costly but also produced signi-
The implementation of this strategy in other composites cant toxic wastes. This resulted in the reduced production of
fabricated via SLS may offer commercial viability and enhanced this polymer initially.13 Since the creation of PEK, the process
performance to increase the use of SLS parts in various has been optimized and is now synthesized at a more reason-
industries. able cost with reduced environmental concerns. The melting
temperature of this polymer is 364 C,13 which is much greater
than many other engineering thermoplastics and offers
4.4 Polyether-derived polymers a greater advantage for high-temperature applications.
Polyether-derived polymers are those containing aryl esters and Polyetheretherketone is also a semi-crystalline polymer.
can include polymers like polyetherketone (PEK), poly- Unlike PEK, the synthesis conditions require milder condi-
etheretherketone (PEEK), and polyetherimide (PEI). The struc- tions,13 making this the more sought aer polyketone. The
ture of the polymers can be found in Fig. 10. melting point of PEEK is 335 C and the glass transition
Polyketones are engineering thermoplastics synthesized temperature is 145 C,13 suggesting that PEEK may be used
from a mixture of ketones, aromatic moieties and aryl ethers. instead of PEK for the same applications. The extremely stable
This family of polymers is well-known for their exceptional nature of PEEK has led to its use in chemical processing
mechanical performance, thermal stability, and resistance to applications, aerospace and electrical industries.13 Also, PEEK
environmental and chemical factors.13 Another polymer in this has been proven as a useful material for biomedical applica-
family is polyetherimide, which is discussed in greater detail tions due to its inert nature and biocompatibility.16 This has
below. been of interest for 3D printing tissue scaffolds and other
Polyetherimide is an engineering thermoplastic with an implants. For example, PEEK has been used to make craniofa-
amorphous structure, excellent dimensional stability, high heat cial skin tissue scaffolds for personalized medicine.155
resistance, good optical properties and reduced ammability.153 4.4.1 Neat polyether-derived polymers in E3DP. Wu et al.156
The exceptional properties of this material have led to its use in printed neat PEEK and neat ABS as a comparative study. The
injection moulded products154 and more recent use in 3D authors highlighted that both raster angle and layer height
printing applications. affected the mechanical performance of FFF samples. The
Polyetherketone was the rst polyketone produced and optimal goal of the paper was to highlight the exceptional
became commercially available in the 1970s through Raychem properties of PEEK. The tensile, bending and compressive
Fig. 10 Chemical structure for PEI, PEK and PEEK which are polyether-based polymers; chemical structures were drawn by the author.
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strengths of PEEK were greater than 100% of those of ABS. The in processability but losses in mechanical performance.161 This
use of PEEK may prove to be a promising alternative to ABS for research would benet from the blend optimization through
high-strength and high-temperature applications, broadening a DOE or a compatibilization study.
the overall use of E3DP technology.156 4.4.4 Polyether blends in SLS. Poly(ether ketone) was used
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The use of PEEK has been more common in FFF than SLS in combination with a high-temperature laser to produce
due to challenges with printing since there is such a high samples from virgin and recycled polymers. In this work, opti-
melting temperature. In general, PEEK is a relatively expensive mization was essential to develop parts that were less affected
polymer that struggles to be penetrated by the laser in SLS.157 by their porosity and had improved surface nish. The opti-
Further challenges with the printing material result from its mized parameters are displayed in Table 2. The authors found
semi-crystalline nature and high melting temperature.158 To that particle size greatly impacted the quality of the products. If
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overcome these challenges, it oen requires the use of the powder particles are too large, the product is very porous
a custom-built fused lament fabrication printer that reaches and has a rougher surface, whereas smaller powders cause poor
higher melting temperatures than standard desktop-sized powder owability. Poor powder owability could have resulted
printers. The materials can be printed for high-temperature in incomplete prints. The optimal size of powder particles was
applications like automotive and aerospace.158 In works from between 75–150 mm.48 Unique to this work, researchers also
Deng et al.,157 the printed samples were tailored for high-impact looked at the re-ordering between the virgin and used materials
and high-strength applications. Other works have demon- during the sintering process. There are two proposed re-
strated potential in the manufacturing industry for FFF parts.159 ordering mechanisms described in Fig. 11 below. Scenario A
To obtain PEEK parts with the highest tensile strength, it was was conrmed in this work; in this case, optimized tempera-
suggested that they be printed with 100% inll and at an inll tures resulted in a cross-linked site across the entire span of the
direction of 45 . If PEEK were adapted to the manufacturing necking region. This conrmed that the crystalline regions were
industries in FF, modications would be required since the able to merge and form a strongly sintered part. The potential to
current strength of cast materials are 1.3 times greater.159 re-use materials can be a sustainable and feasible alternative
Methods such as blending, composites, or other additives as when sintering conditions are optimized, thereby reducing
outlined in the review could be added to PEEK in FFF to waste and increasing the renewability content of parts. This sort
manufacture parts with modiable properties, which may of material valorisation is important for a circular economic
better serve the automotive, aerospace and electronics approach to sustainable product development. Through
industries. parameter optimization in this work, the authors were also able
4.4.2 Neat polyether-derived polymers in SLS. The imple- to determine that there were no signicant changes in the
mentation of polyether-derived polymers has been challenging tensile properties or elongation at break for different laser
at times due to the high melting temperature. To overcome this, powers (Table 3).48 This suggests that a lower laser power of
high temperature (HT) SLS machines (HT-SLS) have been 15 W, rather than 16.5 W, can achieve the same properties at
fabricated. Such technologies have been used in the aerospace a higher laser power where the increased laser power would
and medical industries to generate highly complex parts.160 consume more energy to operate. Therefore, if used in industry,
Although the cost of PEEK is comparatively high, the material is a lower power laser could save some energy costs and slightly
of high strength, ame resistance and exibility, which are very reduce the nal cost of the part.
important for 3D technologies to better serve an array of func-
tions159 such as in the aerospace, electrical and energy sectors.
Materials that are made via SLS have the added benet of not
requiring additional tooling costs as compared to the current
manufacturing process. Tooling costs are associated with
modications to the product that are required to prepare it for
function. This may include removing material or adding further
details. The HT-SLS machines have been used to fabricate parts
from PEEK.160 The benet of using PEEK is that it offers
improved mechanical performance as compared to other
materials, and performance comparable to injection moulded
samples;160 this suggests that the use of PEEK in SLS may have
a better performance than in FFF, since the product perfor-
mance was similar to those of current market materials.
Although the print conditions were not provided in the litera-
ture, the use of HT-SLS and the strong mechanical performance
of PEEK in SLS have been attributed to the semi-crystalline
nature since the nal product was 35% crystalline.160
Fig. 11 Two scenarios for re-ordering between virgin and used PEK
4.4.3 Polyether blends in E3DP. Blends of PEI and poly(- powders during SLS.48 Reprinted with permission from Elsevier:
ethylene terephthalate)-glycol (PETG) were combined for FFF. At Journal of Materials Processing Technology, Copyright 2019, License:
compositions of 5 and 10 wt% PETG, there were improvements 4632510363502.
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The work by Ghita et al.48 also combined used and virgin PEK 4.5.1 Neat PC IN E3DP. Research of blends and print
to determine how SLS performance is hindered by the porosity optimization is good for generating new feedstock materials.
of the samples, such that higher porosity leads to stress However, if the material is not economically feasible, it cannot
concentration factors that further enhance the crack propaga- be used on a large scale. Cicala et al.168 looked into the use of PC
This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence.
tion within the printed sample. Porous samples perform less for FFF because it is cheaper to use than PEEK or PLA. This
favourably and oen have a poor surface nish. The concerns paper would have beneted from providing the printing
for porosity can be addressed as follows: (1) careful material temperatures of the PC as a comparison to the other data (Table
selection to ensure that effective bonding and sintering can 2). However, the products were successfully printed via this
occur; (2) optimization of laser power and (3) effective particle process where the maximal strength and modulus were 55 MPa
size (possibly best between 75–100 mm).48,162 Surface nish is and 2.14 GPa, respectively.168 In this work and others, alter-
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important not only to avoid defects but also to improve the look nating layers were printed on raster angles of 30 and 60 . For
of the product. This is also important for SLS in the pharma- printing neat PC, it was suggested that these raster angles would
ceutical industry.163 achieve the best mechanical properties, therefore, suggesting
4.4.5 Polyether composites in E3DP. Many of the high- that there could be the potential for commercialization of this
performance engineering thermoplastics are complicated to material if feasible.
implement in E3DP due to their high melt viscosity. If the 4.5.2 Neat PC IN SLS. The use of PC in SLS was studied over
viscosity is too high them there is limited ow from the nozzle. the last decade to determine the effect of printing parameters
To overcome this challenge; PEEK was combined with inor- on the nal printed product.169 The structural integrity of the
ganic fullerene tungsten sulde at 2 wt%. The authors sug- printed samples was found to be largely impacted by the size of
gested that the smooth spherical nature of the ller provided the powder particles,169 as well as laser power.170 Essentially,
a lubricating effect on the polymer and resulted in reduced high laser power is required to improve the strength and density
melt viscosity. Once viscosity was improved, printed samples of the materials. If the power is too high, it can result in the
exhibited improved mechanical performance and print degradation of the printed materials, and if the power is too
quality.164 On gauging the viscosity of the melt ow index, the low, it results in samples that are prone to fracturing. In the
optimal value was around 10 g min1 for E3DP.80 Further literature, the optimal laser energy density was 0.1 J mm2 for
research is required to assess the cost comparison and envi- developing parts with the greatest tensile strength.170 The
ronmental impact of the materials. However, the researched improvement in mechanical performance is strongly illustrated
materials showed promise with more diverse feedstock for FFF via the comparison of Fig. 12a and b below. The increased laser
applications. power improved the cohesion of particles as noted by reduced
4.4.6 Polyether composites in SLS. Inorganic compounds voids and a more solid surface. Simple modications to the
have been used in SLS for biomedical applications. Since PEEK printing such as laser power can improve the strength and
is a biocompatible material,16 it has been adapted for use in surface quality of a part. This has led to the success of PC in SLS
tissue scaffolds. Tan et al.165 further added hydroxyapatite to for commercial or large-scale applications.
improve the biogenesis and functionality through the 4.5.3 PC blends in E3DP. Diversity refers to a larger vari-
controlled pore structure.165 The laser power and bed tempera- ability in mechanical performances for printed materials such
ture were the most important tailored parameters for SLS. that they could be used in a greater number of industries, as
When adjusted, the designed scaffolds were produced with well as have improved or optimized mechanical performance
desirable characteristics and appearance. The use of PEEK in and dimensional stability. To better fulll the desire for diver-
biomedical applications may foster the growth of personalized sity amongst printing materials, Zhou et al.83 studied the
medicine. viability of PC and PP blends, as well as their compatibilization.
As compared to commodity plastics, the exceptional perfor- The compatibilizer was made of PE-c-GMA with 8 wt% GMA.
mance of PEEK has also indicated its applicability in CF This work conrms that the addition of compatibilizers
composites to generate materials t for aerospace.166 Prelimi- increases mechanical performance.83 The optimal tensile
nary works by Yan et al.166 modelled the viscoelastic properties, strength was approximately 33 MPa and allowed for greater
correlated with temperature, to determine effective printing material diversity. The addition of compatibilizers or other
parameters.166 The success of the model demonstrated that additives has proven that 3D printing can be adapted to other
more work is required to be able to implement these technol- applications that it does not currently operate on.
ogies in commercial use. 4.5.4 PC composites in E3DP. As mentioned earlier, there
has been signicant interest in studying materials made from
a combination of metals and polymers. Metals like aluminum
4.5 Polycarbonate
have been studied due do the enhanced mechanical perfor-
Polycarbonate (PC) is an engineering thermoplastic derived mance of printed parts with a lower density and lower cost than
from carbonic acid and polyhydroxy compounds. It is extremely other inorganic llers.171 Chemical mixing, which occurs during
tough and amorphous with a heat deection of 130 C, which is the combination of the metal and the polymer matrix, was
good for many high-temperature applications. It has excellent found to improve the metallographic, thermal, and mechanical
resistance to scratches and ultra-violet radiation. This polymer properties through reduced porosity and improved molecular
also has excellent ame retardant properties.167
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Fig. 12 SLS of PC under (a) 0.036 J mm1 and (b) 0.094 J mm1 laser density, respectively.170 Reprinted with permission from Elsevier: Journal of
Materials Processing Technology, Copyright 1999, License number: 4838261399886.
packing.172 The combination of aluminum (30–60 volume frac- addition of HA. However, porosity is important for tissue scaf-
tion) and PC powders was studied to determine the printability folds since the pores foster the adhesion of cells to the
of the materials. Samples were printed via FFF while optimizing sample.175 This work highlights important aspects of the
and correlating resin viscosity, nozzle diameter, volume content implementation of engineering thermoplastic composites for
of the ller, and its corresponding size.171 An interesting nding tissue engineering applications.
of this work was how clogging occurs during the nozzle ow of
composites (Fig. 13). This work displayed that printing PC 4.6 Binary and ternary engineering thermoplastic blends
composites was possible but further work is needed to optimize There are blends of multiple engineering thermoplastics that
the printing parameters and reduce the clogging. are not able to be classied as solely belonging to a group above.
4.5.5 PC composites in SLS. Composites from PC in SLS Here, such studies are discussed for the unique mechanical
have been studied for some time with some of the older works properties that are between both precursor polymers. The
focusing on inorganic powders like graphite powder with SLS;173 blending of engineering thermoplastics is used to generate
more recent advances for PC composites involve research for more diverse feedstock materials that offer a greater range of
medical applications. Tissue scaffold research has been of mechanical properties, variable surface nishes and maintain
interest in the combination of AM and biomedical indus- thermal stability for higher temperature applications. The
tries.33,174 Tissue scaffolds are easily fabricated by SLS since it is strategy of blending polymers has been widely studied in
a more rapid process than the existing commercial opera- injection molding.21,154,176 Similar processes are being adapted
tions.175 To generate scaffolds that are biocompatible and in the additive manufacturing industry to generate tailor-made
interactive with the human body, hydroxyapatite (HA) is oen materials to serve a wider range of applications such as medical,
added to make composites. Hydroxyapatite is a biocompatible electronics, automotive, electronics and consumer product
mineral that increases cell adherence. In literature, HA was industries. Many times, blends of engineering thermoplastics
milled to a very ne powder for many hours before being also include the use of compatibilizing agents to improve the
included at concentrations of 5, 10 and 15 wt% in a PC matrix. compatibility of used polymers in the blends. In some cases, the
The printed materials were optimized and correlations were materials may be immiscible and thus hinder mechanical
made between porosity, scan speed, scan spacing, and laser performances.
thickness. This study showed that increased porosity and 4.6.1 E3DP of binary and ternary blends. Binary blends are
decreased compressive strength were associated with the a combination of two polymers; this section will focus on the
Fig. 13 Modelled clog formation for PC composites via FFF.171 Reprinted with permission from John Wiley and Sons: Journal of Applied Polymer
Science, Copyright 2019, License: 4732631260702.
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binary blends of two engineering thermoplastics. Ternary linking and branching of polymer chains. The use of poly-
blends with two engineering thermoplastics and an additional styrene–maleic-anhydride (SMA) improved the performance of
polymer or compatibilizer will also be discussed. The blending blends of ABS and PA (Table 3). Although this strategy
of engineering thermoplastics leads to a balance of mechanical addressed one challenge of FFF, other strategies can be imple-
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and thermal properties. There are also further concerns that can mented to improve the quality of FFF products.
be addressed by blending engineering thermoplastics as dis- The mechanical performance of ABS, PA and compatibilized
cussed below. ABS/PA blends that exhibited improved mechanical perfor-
In regards to the surface nish, reproducibility and accuracy mances were conrmed by SEM. Under microscopic analyses,
for FFF printed products, Onwubolu et al.177 determined that samples displayed exceptional layer adhesion (Fig. 14a and b).
printing parameters play a crucial role; optimizing these The BAAM printers produced samples with superior perfor-
Open Access Article. Published on 01 October 2020. Downloaded on 10/6/2020 11:47:43 PM.
parameters can tailor the product's aesthetics and mechanical mance with the added benet of the pellet feed system7 as noted
performance. Aesthetics refers to the surface nish and visual in Fig. 14c. The compatibilizer used was not only able to func-
quality of the product. Higher quality products maintain tion properly but it allowed for two immiscible blends to
dimensional accuracy and are smooth textured visually. The generate samples with enhanced tensile strength (for SS-FFF
major contributors that affect the mechanical performance and systems) as compared to the neat polymer.7 As suggested by
appearance of the product are as follows: part orientation, raster the work of Spreeman et al.,7 the diversity of the pellet-feed
angle, layer thickness, raster width and ll density (referred to systems as compared to the lament feed systems offered
as the air gap) (Table 2). Moreover, Onwubolu et al.177 found that a larger variety of printable materials. Moreover, a larger range
the smaller layer thickness of samples resulted in increased of printing temperatures also led to improvements in the
tensile strength.177 Tensile strength was improved through modulus of the printed samples.
smaller raster widths, negative air gaps, and increased raster The reasons for the difference in the quality of the products
angles.177 However, this strategy may be less favourable for between FFF and BAAM are related to (1) the diversity of the
BAAM as more materials are required and the cost of the feedstocks, pellets and/or laments; (2) improved chamber
samples would increase. This work determined that aestheti- heating, which holds the atmosphere at the desired tempera-
cally pleasing samples with desirable tensile strength and ture to reduce warpage;178 (3) screw extrusion to mix heated
design of experiments were required. polymeric materials more evenly before deposition;40 (4)
As mentioned above, there are different scales of E3DP that improved print resolution.42
can impact the product performance over the size ranges of Rocha et al.12 fabricated binary and ternary polymeric blends
industrial-sized machines and home-printing set-ups. Spree- of ABS/SEBS and ABS/UHMWPE/SEBS, respectively, where
man et al.7 used the term BAAM for industrial printing small- UHMWPE was ultra-high molecular weight polyethylene. The
scale platforms FFF for small printers. This work discusses aim of this paper was to discover new compatible blends of
the implementation of engineering thermoplastics blends to materials for FFF to generate greater variability in lament
generate tailor-made materials with a wider variety of feedstocks to serve a greater number of purposes. The printing
mechanical properties as displayed in Fig. 14c. The printing parameters were optimized for both the binary and ternary
parameters are summarized in Table 2. To ensure adhesion blends and are displayed in Table 2. When adding SEBS to ABS,
between constituents and to successfully fabricate blends, Rocha et al.12 found a slight decrease in the tensile strength of
a compatibilizing agent is required. Compatibilizing agents the ABS/SEBS blends but there was an improvement in the
improve the cohesion between materials by inducing the cross- elongation at break (Table 3). The ternary blends experienced
Fig. 14 SEM analysis of the fracture surfaces for BAAM samples (a) PA, (b) PA/ABS compatibilized and (c) a comparison of moduli for small scale
versus large scale printing.7 Reprinted with permission from Elsevier: Additive Manufacturing, Copyright 2019, License: 4694241403414.
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increased tensile strength and elongation at break with used to address concerns such as the limited variability in
increasing UHMWPE content, but the properties were still less current materials and diversied mechanical performances.
than that of the neat ABS polymer. The authors used SEM to
explain the decrease in the mechanical properties. The ternary
5. Summary of parameters and
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blends had a lack of adhesion between components. Overall,
complete and warpage free-samples were printed, which sug- materials design to improve 3D printing
gested that this material could be further used as a new lament
To summarize these works and strategies, a point-form list of
feedstock material with tailorable mechanical performances.12
methods is provided. As noted in Fig. 15, many technical
Blends of PC and PEI highlighted an important aspect of 3D
aspects tailor the performance of 3D printed products.
printing. To successfully print via FFF, the laments need to be
To improve lament consistency
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easy to process such that they have a consistent and uniform
B Optimize melt-compounding and extrusion
thickness. The addition of PC (at 5 to 40 wt%) to PEI was able to
processes6,37,116
lower the viscosity, which improved the lament processability.
- Increase the feed rate
If PC/PEI blends were to be used in FFF the addition of com-
- Decrease the collection rate of lament
patibilizers or additives to improve miscibility needs to be
B Add a compatibilizing agent or impact modier to
studied to avoid phase separation.179
increase the molecular weight
Dual polymer lament systems. Rather than blending mate-
To improve ow during E3DP
rials through extrusion to diversify the mechanical properties of
B Blend polymers for unique melt characteristics
printed objects, two distinctive neat polymers can be printed
B Optimize nozzle diameter
simultaneously through dual extrusion. For toughened parts,
B Use BAAM rather than E3DP due to increase melting and
ABS has been printed in combination with PC, where a star-
mixing before extrusion onto bed7,178
shaped internal structure is continuous and encapsulated in
B Modify viscosity182
ABS. Such material combinations were found to have greater
- Check the melt ow index (MFI). Extremely high or low
strength as compared to the existing commercially available
values will not print;6,80 MFI values close to 10 g per 10 min print
ABS materials. To further improve the properties of the mate-
well for FFF80
rials, the prints beneted greatly from annealing. The dual ABS/
To reduce warpage or delamination in E3DP
PC laments aer annealing experienced ductile failure instead
B Add a brim to the printed sample
of brittle failure like the un-annealed 3D printed samples.180
B Change printing parameters like layer height, nozzle
4.6.2 Selective laser sintering of binary and ternary blends.
temperature
One of the challenges to implementing engineering thermo-
B Print samples with a bed temperature close to the glass
plastic blends in SLS pertains to the commercial availability of
transition temperature
powdered materials.181 Most oen in research, the powder must
B Maintain a heated environment during printing: add
be made in small batches via cryomilling, or is subjected to
heated chamber if needed
other size-reducing technologies. If more polymers were
commercially available in powder form, it would offer more
research potential for all and make the process more time-
efficient. This has challenges and would decrease the ability
of the materials to be implemented commercially. Dechet
et al.181 wanted to study the combination of PBT and PC but
there were no powder precursors. The authors then suggested
the implementation of a co-grinding process to overcome this
limitation. Co-grinding is the process of placing pellets from
both polymers into a ball-mill to produce powdered samples.
The co-grinding strategy showed promise but does require some
further investigation on the resulting chemical and physical
nature of each blend.
Polyamide blends have also been investigated via SLS with
a CO2 laser. Samples were printed with a 20 W laser, at a scan-
ning speed of 44 mm s1, chamber temperature of 120 C, and
a layer thickness of 150 mm. PA 12 and PA 6 blends were found
to have greater absorption during sintering.162 One of the key
ndings in this work was that the porosity and crystalline
structures were dependent on the compositions of the samples,
rather than the printing conditions. Based on PA 12, the blends
were heterogeneous with a mixture of co-continuous and
dispersed phases. The success of the printed materials meant Fig. 15 Interconnectedness of all aspects of printing for product
that there was a new powder feedstock material that could be development.
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B Improve the crystallinity of samples6,183 and has an extremely high melting temperature,168 implying
- If a smaller crystal size is desired, add compatibilizer, that more energy input is required to produce samples. This
impact modier or both highlights the current challenge within the 3D printing mate-
- If a large crystal size is needed, anneal the parts aer rials market, where exceptional performance can come with
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printing a high cost. Challenges with performance at the expense of the
To improve mechanical performance economic viability of 3D printing materials have led researchers
B Blend polymers that are miscible or that can form a co- to focus on the optimization of printing parameters, polymer
continuous phase162 blends, or even fabricating composite materials.2,188,189 Some
B Add ller or bers that have good ber surface interface work may be required to make all engineering thermoplastics
To improve weight-bearing/impact strength cost-competitive.
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B Print long ber composites with ber perpendicular to 6.1.1 3D printing in industry. The costs of equipment,
the desired weight direction136 labour and resources are important aspects for the industry
To increase the renewability content when adopting 3D printing technologies such as E3DP or SLS as
B In SLS, blend the used and virgin polymers at approxi- a replacement for other polymer processing methods.190 A
mately 20 wt% to maintain the properties but reuse the powders comparison of 3D printing and injection molding has been
B Use biobased polymers like biobased PAs or PTT6 studied through life cycle costing, which is discussed more
B Fabricate composites with natural/biobased llers or below.191 Other strategies include determining the break-even
composites184 cost point for each production method versus the number of
To improve thermal and electrical properties products required. As a reference, Franchetti and Kress
B Fabricate composites with electrically conductive or compared the injection and FFF processes to nd that 187 parts
thermally conductive materials. For example, y ash spheres, was their break even. If producing less than 187 parts, the
carbon bre, graphite140,141 equipment, labour and resources are more economically
B Blend with ame retardant to improve ame retardancy149 feasible via 3D printing.190 This supports the idea that 3D
To improve surface nish/print resolution printing is best used for intricate, complex or custom parts not
B SLS required in mass-quantities.
- Size the powder between 25–75 mm for reduced porosity
B E3DP
- Rene nozzle diameter185 6.2 Viability of composites
To improve biocompatibility To date, the addition of brous materials has addressed some
B Optimize the surface porosity to improve cell adhesion concerns with a lack of strength and the inability of many 3D
B Use biocompatible polymers like PEEK155,157,186 printed parts to function in load-bearing applications.136 In
B Perform surface modications to traditionally non- some cases, the improved mechanical properties have been
biocompatible polymers such as photo-induced gra attributed to bre alignment, uniform particle distribution and
polymerization105 layer interactions.192 However, the adaptation of engineering
To improve the ller matrix interface thermoplastic composites into commercially available printing
B Chemically modify ller surface via treatments materials requires the composites to be cost-effective or have
B Add a compatibilizing agent superior mechanical performance as compared to the current
B Use polymers, such as PAs, with functional groups, which market options. Not only are there challenges with the materials
are more conducive to binding with the ller187 cost and performance, but some experimental materials are not
able to perform successfully due to a lack of interfacial adhesion
between the polymer and ller.192 The lack of adherence
6. Feasibility, viability and between the bre and the matrix materials is noted by pull-outs
sustainability dened at point 3 in Fig. 16. Like other 3D printed parts, voids
(point 2, Fig. 16) and air bubbles (point 1, Fig. 16) can also be
6.1 Economic feasibility present and reduce the mechanical performance134 of the
Although many works were completed on engineering thermo- composite materials. This is important to understand the
plastics, such as ABS, polyamides, PMMA, and PEEK,168 the potential challenges with printing composites. To overcome
implementation of the materials for consumer products is this, there is oen the need for compatibilizing agents or
dependent on commercialization and the mass product of surface modications for the ller. This has an associated
research materials. It is well understood that product develop- increase in cost, but would increase the performance of the
ment is highly impacted by the cost, such that additional costs product.
or high-cost materials must be balanced with exceptional To date, there are many successful uses of composites
performance or benets to prove feasible. Some polymers far implemented in industries to produce viable 3D printed prod-
exceed others in performance, but the cost is too large, such as ucts. Composites produced from FFF or SLS (Table 4) are used
with PEEK. As an example, PEEK was able to out-perform other in biomedical, electrical, automotive and other industries.193
engineering thermoplastics by 120% with respect to tensile Most oen, composites are implemented for improved
strength (Table 3).168 However, this polymer is very expensive mechanical performances, enhanced electrical characteristics,
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be studied to determine the potential human health impacts.
For SLS of PA 12, the major emissions were carbon dioxide and
VOCs.204 One of the greater concerns with emission in the
addition of VOCs is the release of ultra-ne particles.205 To
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mitigate some of these concerns, small desktop printers should
be operated under fume hoods or well-ventilated areas. This is
far easier to implement in industry and research laboratories as
compared to home print set-ups. Thus, it is suggested that
consumers take special precautions when printing with their
desktop printers to reduce health-related concerns. The addi-
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tion of proper ventilation205 and personal protective equipment
Fig. 16 SEM analysis of the fracture surface of FFF samples.134 can further reduce the risks associated with printing.
Reprinted with permission from Elsevier: Composites Part B: Engi-
neering, Copyright 2019, License: 4694210938408.
6.4 Sustainability
increased thermal properties, or better environmental friendli- The success of 3D printing in a great number of industries has
ness. The major concept here is that composites can be used to given rise to the design and fabrication of materials or parts that
address the limitations mentioned throughout this paper. The are sustainable.198 Sustainable materials are those that address
distributive phase in composites can dissipate forces more the societal, environmental and economic aspects of product
evenly though samples to improve their impact strength.95,96 If development, which have reduced impacts on natural resource
continuous bres are used, the bres can be oriented normal to depletion, reduced emissions206 and energy consumption.207
the force and allow 3D printed parts to be used in weight- This would help to address concerns about the future environ-
bearing applications.136 mental impacts of the technology. There are some concerns for
3D printing, which are associated with the accumulation of
waste materials, substantial energy consumption and the end of
6.3 Safety life applicability of equipment and prints. Currently, some 3D
More recently, there has been signicant research interest in printing technologies result in the accumulation of waste
the safety hazards associated with SLS and E3DP. For example, materials. Waste is most oen generated by FFF/BAAM, due to
the E3DP can result in the release of nanoparticles into the the required support material that is needed to fabricate the
surrounding environment. This is of particular concern for part, but is removed aer the print. Some of the prints can also
home desktop-sized printers200 where some of the emitted take a long time, which requires greater energy input.208
materials include volatile organic compounds (VOCs) that need One way to compact the environmental concerns for 3D
to be assessed to ensure safe operation and no long-term health printing is to generate a design of experiments that focuses on
effects. the materials and energy consumption, as well as production
Recently, 216 VOCs have been attributed to the FFF printing and the weight of scrap materials.56 Reductions in energy
process.201 In addition to nozzle temperature,201 emissions are consumption and waste can contribute to sustainable longer-
dependent on the lament brand and material.202 The emis- term product development.209
sions for PA were 1660 mg per hour as compared to 147 mg per Less work has been completed with natural llers or bres
hour for polyvinyl chloride (PVA).201 When it comes to printing with SLS. This may be due to concerns regarding the degrada-
engineering thermoplastics, the common VOCs associated with tion of the materials. Most natural bres have relatively low
ABS and PAs are styrene and caprolactam, respectively.203 Both thermal stability210 as compared to carbon-based materials.
styrene and caprolactam possess the potential for carcinogenic However, biocarbon (also known as biochar) is a sustainable
impacts.203 Likewise, SLS also produces emissions that need to and cost-effective alternative to carbon black.211 One challenge
Table 4 3D printed composites implemented in industry
Matrix Filler Application General industry Method Ref.
ABS Bakelite–SiC–Al2O3 Suggested for automotive Thermal FFF 194
PEEK HA Scaffolds Biomedical SLS 165
ABS OMMT Suggested electronics or automotive Thermal FFF 114
ABS Carbon black Sensors and conductive materials Electrical FFF 195
PA 11 Glass beads Medical clamps and scaffolds Biomedical SLS 196
PA 12 CF Structural parts Mechanical SLS 197
PET Biochar Automotive parts and engineering Thermal, non-structural FFF 47
applications
PA 12 Limestone Manufacturing Thermal, structural SLS 198
ABS Bismuth telluride Effective energy harvesting materials Thermoelectric FFF 199
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with the use of natural bres is the loss in the recyclability of the the largest emissions producers, impacting climate change,
material at the end of life.93 fossil fuel depletion, eutrophication, land use, ozone depletion
The circular economic approach of 3D printing can be found and others.218 These impacts have been suggested for consid-
in Table 4. A reminder that the circular economic approach eration by both industry and government, prior to the imple-
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focuses on recycling, reuse/redistribution, and maintenance, mentation of AM technologies, as well as a comparison to other
remanufacturing/refurbishing.212 The other concepts include technologies like CNC machining as mentioned previously.
resource conservation, regeneration and the optimization of There is still some interest focusing in the energy
processes to increase yields and reduce the leakage of wastes consumption during the 3D printing process in regards to
and harmful environmental impacts (Table 5).213 sustainable product development.115 In understanding the
energy consumption of FFF, the global warming impacts can be
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6.5 Life cycle assessment assessed and used to suggest improvements to the technology.
A life cycle assessment (LCA) is used to analyze a product from In some cases, reduced energy consumption could reduce
the development stages to the end of life stage, which includes operating costs, which also offers an additional benet to
raw materials extraction, manufacturing of the product, industry.115 One of the largest energy-consuming steps during
implementation and disposal.215 This type of analysis is printing for FFF is the warming up, where the nozzle is heated
commonly referred to as either cradle-to-cradle (if repurposed) to the print temperature. It has been suggested that this be an
or cradle-to-grave if there is no further use for the product.216 A area of improvement for the printing process.
completed LCA comparing a computer numerical control (CNC) In addition to printing process modication, a solely
milling machine to FFF was completed by Faludi et al.,217 where economic assessment of AM was proven to be the most
they analyzed the impacts per job in relation to their specic important for industries. Such assessments could be imple-
hazards. There were benets and disadvantages discussed for mented when adapting AM technologies to industry. For
both processes. For example, for solid parts, the CNC example, FFF and other AM processes oen require limited to
machining produces substantially more waste as compared to no tooling, which reduces energy consumption219 as compared
FFF processes under maximal utilization. As far as the ecolog- to processes like CNC machining. There is also less material
ical impacts for each production step, that is manufacturing, consumption, which not only saves cost but is less resource
electricity consumption waste, transport and disposal, both demanding and therefore more sustainable.219
processes produce the largest impacts during the energy There have also been some works on LCA of SLS. Researchers
consumption stage during manufacturing. As a result, the have shown that the largest environmental impacts for the
largest resulting impacts are on fossil fuel depletion and process were associated with the waste materials, and subsequent
climate change with respect to human health.217 From this electricity consumption.59 For E3DP, there are also environmental
work, it can be noted that potential reductions in energy concerns with waste materials and energy consumption. However,
consumption for both processes could reduce the environ- waste materials have been suggested to be reduced based on the
mental impacts of the nal products. optimal parameter selection for a print.220
To further improve the reliability of LCA, Ma et al.218 sug-
gested that the strategic analysis and design of a sustainability- 6.6 The future of this technology
based LCA could foster the adaptation of AM technologies by For both SLS and E3DP, there is the increasing demand for
both business and industry.218 The authors suggested that LCA versatile and sustainable materials. Substantial efforts have
could focus on both an economic assessment as well as been made regarding research into this technology to serve end-
consider the social and environmental sustainability of the use parts, whether automotive parts, medical parts or devices,
prints on a case-by-case basis.218 The processes were broken consumer goods or aerospace.221 However, two of the greatest
down into economic, environmental and social considerations. challenges for this technology are the commercialization of
The service and production stages of 3D printed products are materials and the scalability of the printing process. As noted
Table 5 Sustainability aspects of 3D printing
Sustainability factor Description Ref.
Recycle The implementation of locally recycled materials for 3D printing without 212
the need for additional transportation or logistics
Recycling of used polymers from one process to the next in SLS printing 48
Maintenance Repairs for the broken parts of a 3D print can be printed from a device 212
in a faster and cheaper manner
Reuse/remanufacture Redesign parts for 3D printing due to high customizability 212
Manufacturing Less waste from 3D printing for designs that need no post-printing modications. 212
Less transport and logistics to nd complex parts since they can be made via 3D
computer-aided designs and printed
Resource conservation The use of natural llers or other wastes in composite applications since there is 184 and 214
valorisation and reduction of waste entering the environment
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from the discussed literature, there are many materials with CF Carbon bre
diverse properties to address current industry concerns. DOE Design of experiments
However, the feasibility of the materials needs to be studied E3DP Extrusion 3D printing
regarding cost, ease of implementation and materials avail- EBA– Poly(ethylene-n-butylene-acrylate-co-glycidyl
This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence.
ability. Other lesser concerns include improving the reproduc- GMA methacrylate)
ibility of products, as well as uniformity222 and dimensional FDM Fused deposition modelling
accuracy,42 and focusing on sustainability56 and resource (such FEA Finite element analysis
as time or energy) management.223 Such considerations seem at FFF Fused lament fabrication
this point to be the major set-back for this technology. To GMA Glycidyl methacrylate
address these challenges and concerns, there is a need for HA Hydroxyapatite
Open Access Article. Published on 01 October 2020. Downloaded on 10/6/2020 11:47:43 PM.
further study, as well as possible technology modications. HDPE High-density polyethylene
There are two strategies that may be investigated to improve HT-SLS High-temperature SLS
these processes. The rst is process intensication technolo- i.e. That is
gies. Process intensication technologies are those that reduce LCA Life cycle assessment
capital investment, reduce raw materials cost and energy use, L-CNC Lignin-coated cellulose nanocrystals
increase environmental performance and safety, as well as MA Maleic anhydride
MWCNT Multiwalled carbon nanotubes
improve quality.207 The second method for improving this
OMMT Organic modied montmorillonite
technology is through LCA and interpretation, which was dis-
PA Polyamide
cussed in the paragraphs above.
PBT Poly(butylene terephthalate)
Some of the challenges experienced through E3DP and SLS
PC Polycarbonate
may be addressed through the implementation of process
PE-c- Poly(ethylene-co-glycidyl methacrylate)
intensication technologies.224 Such technologies may modify GMA
the printers structurally or functionally to better address PEEK Polyetheretherketone
concerns relating to dimensional stability, warpage, delamina- PEI Polyetherimide
tion, as well as waste and energy consumption. PEK Polyether ketone
PET Poly(ethylene terephthalate)
7. Conclusions PETG Glycol-modied PET
PHR Parts per hundred rubber
Although engineering thermoplastics are known for their PI Polyimide
excellent mechanical performances, thermal stability, resiliency PLA Poly(lactic acid)
and relative chemical inertness over commodify plastics, they PMDI Polymeric methylene diphenyl diisocyanate
do experience some major pitfalls when implemented in addi- PMMA Poly(methyl methacrylate)
tive manufacturing. A general lack of biocompatibility, anisot- PTT Poly(trimethylene terephthalate)
ropy and limited electrical conductivity have halted the SMA Styrene maleic anhydride
progression of 3D printing into more industries. Currently, SEBS Styrene–ethylene–butylene–styrene
selective laser sintering and extrusion 3D printing serve SLA Stereolithography
a limited number of functions within the automotive, electrical, SLS Selective laser sintering
aerospace and biomedical industries. Strategic materials SMA Polystyrene–maleic-anhydride
modication in addition to process and print optimization has TNPP Tris(nonylphenol) phosphite
TPU Thermoplastic polyurethane
evolved polymers, blends and composites to exhibit novel traits
UHNWPE Ultra-high molecular weight polyethylene
to fulll the desired traits for 3D printed products that are
UL Underwriters laboratory
comparable to, or outperform traditional products. Exciting
VOC Volatile organic compounds
advances have led to the development of 3D printed ceramic
wt% Weight percent
foams for automotive applications, electrically conductive
3D Three-dimensional
customized sensors, surface modied novel biocompatible
printing materials, and many more. Each work outline in this
review offers vital information on materials, which could
diversify the use of E3DP and SLS in industry and boost the
growth of AM technologies to unforeseen potential.
Conflicts of interest
Authors hereby conrm that this manuscript has not been
List of abbreviations published and is not under consideration elsewhere. Authors
declare no conict of interest.
ABS Acrylonitrile butadiene styrene
AM Additive manufacturing
Acknowledgements
BAAM Big area additive manufacturing The authors are thankful for the nancial support from: (i) the
CNC Computer numerical control Ontario Research Fund, Research Excellence Program (ORF-
36084 | RSC Adv., 2020, 10, 36058–36089 This journal is © The Royal Society of Chemistry 2020
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RE09-078) from the Ontario Ministry of Economic Develop- 19 N. Dangseeyun, P. Supaphol and M. Nithitanakul, Polym.
ment, Job Creation and Trade, Canada (Project #053970 and Test., 2004, 23, 187–194.
054345); (ii) the Ontario Ministry of Agriculture, Food and Rural 20 M. Zaverl, O. Valerio, M. Misra and A. Mohanty, J. Appl.
Affairs (OMAFRA), Canada University of Guelph, Bioeconomy Polym. Sci., 2015, 132, 1–11.
This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence.
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Research Council (NSERC) Canada Discovery Grants Project 22 G. Cicala, G. Ognibene, S. Portuesi, I. Blanco, M. Rapisarda,
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to the Bioproducts Discovery and Development Centre, 23 B. P. Chang, A. K. Mohanty and M. Misra, RSC Adv., 2018, 8,
University of Guelph supported by FedDev Ontario, Canada; 27709–27724.
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