Review

Advanced Thermoplastic Composite Manufacturing

by In-Situ Consolidation: A Review
Isabel Martin 1 , Diego Saenz del Castillo 1 , Antonio Fernandez 2 and Alfredo Güemes 2, *
1 FIDAMC, Foundation for the Research, Development and Application of Composite Materials,
Avda. Rita Levi Montalcini 29, Tecnogetafe, Getafe, 28906 Madrid, Spain;
Maria-Isabel.Martin@fidamc.es (I.M.); Diego.Saenz@fidamc.es (D.S.d.C.)
2 E.T.S.I. Aeronáutica y del Espacio, Universidad Politécnica de Madrid, Pza. de Cardenal Cisneros 3,
28040 Madrid, Spain; antonio.fernandez.lopez@upm.es
* Correspondence: alfredo.guemes@upm.es




Received: 23 August 2020; Accepted: 10 October 2020; Published: 13 October 2020


Abstract: This article provides an overview of the evolution of the in-situ consolidation (ISC) process
over time. This evolution is intimately linked with the advancements in each of the steps of the ISC
manufacturing process, is additive in nature, and is limited by the orthotropic nature of composite
materials and the physicochemical behavior of the thermoplastic matrix. This review covers four key
topics: (a) Thermal models—simulation tools are critical to understand a process with such large
spatial gradients and fast changes. Heating systems once marked a turning point in the development
of industrial ISC systems. Today, lasers are the most recent trend, and there are three key issues being
studied: The absorption of energy of light by the material, the laser profile, and the laser focusing.
Several approaches have been proposed for the distributed temperature measurements, given the
strong temperature gradients. (b) Adhesion—this refers to two subsequent mechanisms. In the first
place, the process of intimate contact is one by which two surfaces of thermoplastic pre-impregnated
composite materials are brought into contact under pressure and temperature. This enables closure of
the existing gaps between the two microscopic irregular surfaces. This process is then followed by the
healing or diffusion of polymer molecules across the interface. (c) Crystallinity—mostly influenced
by the cooling rate, and strongly affects the mechanical properties. (d) Degradation—this refers to the
potential irreversible changes in the polymer structure caused by the high temperatures required
for the process. Degradation can be avoided through adequate control of the process parameters.
The end goal of the ISC manufacturing process is to achieve a high product quality with a high
deposition rate through an industrial process competitive with the current manufacturing process for
thermoset composites.

Keywords: thermoplastic composites; automatic lamination; in-situ consolidation; aircraft structures;

laser assisted tape placement

1. Introduction
The key properties that justify the wide use of composite materials in the aeronautical industry
were described in [1] including weight savings due to the increase of specific resistance and stiffness,
which leads to reductions in fuel consumption and, consequently, allows an increase in aircraft
payload. Furthermore, the specific properties are not the only driver for material selection for
aerospace applications—costs are also important. It is necessary to demonstrate how affordable it
is to manufacture and use materials during operation. Any selected material must also have the
ability to withstand stresses in the presence of typical damages, durability, resistance to fatigue,
and environmental degradation.

J. Compos. Sci. 2020, 4, 149; doi:10.3390/jcs4040149 www.mdpi.com/journal/jcs

J. Compos. Sci. 2020, 4, 149 2 of 36

The carbon–thermoset matrix composite materials meet the vast majority of the requirements
described above, improving the performances over typical light metal alloys. Despite its potential,
the application of these materials to aeronautical parts has been very progressive until full confidence
on the in-service behavior has been demonstrated, and the strict certification process required for the
composite structures is fulfilled.
The application of thermoplastic polymeric matrix materials has not currently reached the same
levels of development as those already attained with thermosets. The high process temperature
requirements and the lower productivity achieved with thermoplastics are among the possible reasons
for this delay. In thermoplastic composite reinforced materials, at room temperatures the material
is in solid state and has no tackiness, a crucial property for the thermoset automatic layup process.
Additionally, at temperatures above the melting point, the viscosity values are still very high, as the
matrix is already in a polymerized state. This makes higher temperatures and pressures necessary and,
therefore, the processes have higher costs than thermosets.
Positive properties for the development of thermoplastic material include the possibility of
manufacturing structures with high levels of integration, avoiding the need for subsequent assembly
processes, and practically unlimited life without the need for refrigeration and low risk of contamination
or toxicity in human manipulation as the polymer has already been polymerized [2]. Currently, aspects
such as sustainability and environmental conservation are also important [3]; thermoplastic materials
have the capability to be recycled. The possibility of making a future where the parts of retired aircrafts
can be reused represents a point in favor of the incorporation of this type of material.
To achieve similar application levels to thermosets in the aeronautical industry, it is necessary
to develop new processes for thermoplastics that simplify or reduce costs with respect to current
manufacturing processes. Currently, for the manufacturing of large structures with thermoset material,
automated layup is used, with layup speeds of the order of 50 m/min. As the material is partially cured,
it preserves its adhesiveness, making it possible to join the different plies. After layup, stacks require
shaping and/or vacuum bags for a subsequent autoclave curing step. For their part, thermoplastic
reinforced materials have not been able to undergo the same sequence due to the important differences
that automatic layup processes have between them.
Shorter cycles are a clear advantage of thermoplastic composite materials compared to conventional
ones with thermosets. The lack of tackiness among layers at room temperatures requires an increase in
their temperatures to values over their melting point (semi-crystalline) or glass transition (amorphous).
However, it also allows the lay-up to be done and simultaneously creates high-quality bonding among
layers, suppressing the next curing stages in the oven or autoclave.
Using this idea, the developments that led to the automatic layup process and in-situ consolidation
were established, where a heating source heats surfaces of thermoplastic material, subsequently
contacting them under the action of a compacting element. This process involves multiple physical
parameters that take place simultaneously and whose control is essential to enable the application
of improvements in the product. In order to apply this process in a profitable way for the industry,
it is necessary to ensure that it is possible to achieve high degrees of consolidation without the need
for a second cycle of re-consolidation in the stove or autoclave; references such as [2] report degrees
of consolidation around 80–90%; however, current results from the Automated Dynamics company
confirm the possibility of reaching compaction levels comparable to those obtained in stove and
autoclave cycles with speeds suitable for industrial production. In the application of the reinforced
thermoplastics to aeronautical parts, Ref. [4] points out the need to use them in applications where
the temperature limits are close to their glass transition minus 30 K, since over this temperature the
softening of the material occurs, modifying its mechanical properties.
The use of thermoplastic composites for long size composite structures requires the development
of in-situ consolidation, as it is considered the most promising manufacturing process capable of
reducing manufacturing time and cost. The first patent referring to this process dates from 1986,
associated with DuPont [5] (layup method and equipment patent), where the outstanding point is the
J. Compos. Sci. 2020, 4, 149 3 of 36

approach of applying the automatic layup to a thermoplastic material using a secondary pre-heating
source on the substrate and a main source that acts between said substrate and the material being
supplied, with an energy distribution between the substrate and incoming tape of 20–80%. Northrop
Corporation, the American aircraft manufacturer, issued a patent on this topic in 1991 [6]. Among the
particularities of its proposal, it presents the use of a heated roller, a cooling system just at the exit
of the roller (compactor foot), and the interposition of a sheet of material between the roller and the
material to be taped to avoid adhesion between them. The patent also presents a working system for
the first layer layup based on the use of a perforated tool from which a vacuum will be applied to the
taped material, between the tool and the piece a layer of insulating glass and a film of Kapton.
In 1997, the Boeing Company was the assignee of a patent on a multi-wick wrapping machine
(at least two wicks of material). A detailed description of each of the components of the equipment
was reported in the patent, giving specific details about the compaction roller. The proposed system
consisted of cavities with air circulating for cooling, equipped with a component that allowed it to
be tilted (axis of rotation in the direction of the layup) to enable the application of pressure on all
the tows in non-flat layup conditions. The Boeing Company in 2002 also protected its work on the
heating method and the heating control system in the process of layup of composite materials, without
specifying the type [7]. In the previous patent, the heating system used was a group of diode lasers
that allowed control of the energy supplied in the longitudinal and transverse directions of the layup,
favoring concave–convex tapes and with different inclinations of the substrate. As a control system
they used a thermography measurement system.
Aerospatiale, the French aerospace company which would later become part of the European
business conglomerate, Airbus, filed a patent in 2003 which protected the development of a layup with
integration, with a technology known as co-consolidation [8]. The patent considers the lamination
of a skin on the stiffeners the consolidated skin and the stiffeners joined by diffusion/conduction
welding, indicating a preferred application of this system in the manufacture of fuselage segments or
engine covers.
The already-formed Airbus patented another methodology for thermoplastic layup in 2011 [9],
in which a part of the layup tool was made of porous material. The proposal included the use of a
microporous aluminum positioned on the surface of a larger non-porous tool. The size of the cavities
was small enough so that, together with the high viscosity of the polymer, they cannot block or affect
the surface quality of the part. This system can also help in the de-molding stage, if the change from
negative to positive pressure on the part is carried out.
Machine manufacturers have also protected their advances with patents. Cincinnati Milacron,
Inc. protected heating control in the thermoplastic layup process [10], and Automated Dynamics
protected their technology with various patents [11–15], related to the layup equipment, layup material,
and manufacturing technology for the incorporation of lightning protection systems. For its part,
in 2008 Accudyne Systems, Inc. launched a patent for equipment and processes for the layup of
thermoplastic composite material [16] highlighting the proposal for the use of a flexible compaction
system consisting of segments that apply pressure independently. The company that produces robotic
cells for the layup of composite materials, Coriolis Composites, patented in 2016 [17] an innovative
solution for the compaction roller, in line with the solution proposed by Accudyne. The solution was
based on the fact that each of the segments that make up the roller are in turn cylinders with an interior
made up of elements with curvatures that give it greater flexibility.
Concerning the scientific production, Figure 1 gives the evolution of the number of documents
found at the Scopus database with the words “thermoplastic composite manufacturing” appearing
either in the title, keywords, or abstract. About half of these documents were journal articles, while
the other half were mainly papers submitted to scientific conferences (ICCM, Sampe, and similar).
By adding the word “consolidation” to the search, the number of documents was reduced to 10–20%.
We may conclude that the number of publications per year was consistently maintained, but not very
J. Compos. Sci. 2020, 4, x 5 of 45

reduced
J. Compos. Sci.to 10–20%.
2020, 4, 149 We may conclude that the number of publications per year 4was of 36

consistently maintained, but not very high compared to other topics in Composites.
Most of thesetopapers
high compared have
other topics been reviewed
in Composites. forthese
Most of thispapers
work,have
and roughly
been half
reviewed for of
thisthem
work,
and roughly half of them are
are included in the reference list. included in the reference list.

(a)

(b)
Figure 1. Documents
Figure 1. Documents in
inthe
theScopus
Scopusdatabase
database under
under “thermoplastic
“thermoplastic composite
composite manufacturing”
manufacturing” (a)
(a) and
and “thermoplastic composite manufacturing consolidation”
“thermoplastic composite manufacturing consolidation” (b). (b).

This article
This article is organized
is organized as follows:
as follows: After theAfter the Introduction,
Introduction, Section
Section 2 details 2 details
of the ISC of
machines,
its evolution over time, and the reasons for it. Section 3 is called “Thermal
the ISC machines, its evolution over time, and the reasons for it. Section 3 is called Models”, because it was
recognized early that a process with such a large spatial gradients and very fast changes (the material
“Thermal Models”, because it was recognized early that a process with such a large
melts and cool within seconds in a small region of the laminate) could not be understood without
spatial
the help gradients
of simulation and very
tools. fast changes
A point of interest (the material
was the heatingmelts and
systems, andcool within seconds
the absorption of light
in a small region of the laminate) could not be understood without
energy by the material, as lasers are a recent trend, driven by the need of focusing the power input.the help of
simulation tools.have
Different solutions A point of interest
been proposed was
for the the heating
distributed systems,
temperature and the absorption
measurements, of
because of the
localized large gradients. Next, Section 4 is a review on the “Adhesion”,
light energy by the material, as lasers are a recent trend, driven by the need of or mechanisms by which
two surfaces of thermoplastic composite materials brought into contact, by the application of pressure
J. Compos. Sci. 2020, 4, 149 5 of 36

and temperature, are able to close the existing gaps due to the inherent irregularity of the surfaces of
the material before its manufacturing process. Two other quite important related topics are Sections 5
and 6, respectively: (5) Crystallization, a characteristic of some thermoplastic materials that benefits its
mechanical properties, particularly toughness, and solvent resistance; the percentage of crystallinity
and morphology is linked to the thermal profile. (6) Degradation, when a polymer is exposed to very
high temperatures over the melting point, even for seconds.
This article has been extracted from the Doctoral Thesis of the first author, written in Spanish and
available in Ref. [18]. This survey has been kept opened to every fiber/thermoplastic matrix system,
even though carbon fiber/PEEK is the system that has received more attention. Poly-ether-ether-ketone,
commonly referred to as PEEK, is a semi-crystalline polymer with a glass transition temperature of
143 ◦ C, and a melting point of 343 ◦ C. Worthy to remember that processing temperature needs to be
higher than melting point, while Tg is the maximum service temperature as a composite material,
because the drop of stiffness in the matrix for temperatures higher than this value implies a drop of
longitudinal compressive strength of the laminate.

2. Automatic Lamination and In-Situ Consolidation (ISC)

The automatic lamination and in-situ consolidation process with thermoplastic reinforced material
has been studied since the 1980s [19]. Most of the initial references based on this process refer to the
development of laminates where it is not possible to obtain a total degree of bonding between the
parts, making a second consolidation stage necessary [20]. It was estimated that the speeds required to
obtain a real in-situ consolidation were about 0.5 m/s.
The reasons that lead to consideration of this manufacturing process as advantageous are the
reduction of costs due to a limited amount of scrap or excess material in the tapes, improvements in
the positioning of the material, repetitive results, and lower labor costs. It is also an essential step for
the development of large structures [21].
The basic outline of this process is included in Figure 2. Plies of reinforced thermoplastic material
adhere to each other after increasing their temperature due to the heating generated by a thermal
source (laser or any other type) and by bringing them into contact with the application of pressure by
J. Compos. Sci. 2020, 4, x 7 of 45
means of a compacting roller.

Figure 2. In-situ
Figure 2. In-situ consolidation
consolidation equipment
equipment inin FIDAMC
FIDAMC (Foundation
(Foundation for
for the
the Research,
Research, Development
Development
and Application of Composite Materials) (left); and a schematic diagram of the manufacturing
and Application of Composite Materials) (left); and a schematic diagram of the manufacturing process
including manufacturing tooling, compaction roller, a diode laser, and an infrared
process including manufacturing tooling, compaction roller, a diode laser, and an infrared thermographic
camera (right). camera (right).
thermographic

Although semi-crystalline thermoplastic materials are used in most of the references on automatic
Although semi-crystalline thermoplastic materials are used in most of the
lamination and in-situ consolidation, because these materials offer the highest performances, the process
references
does onany
not present automatic
restriction tolamination
the layup withand in-situthermoplastic
amorphous consolidation, because
materials. these
Dai described
materials offer the highest performances, the process does not present any
restriction to the layup with amorphous thermoplastic materials. Dai described in
[22] the application of this process to the layup of carbon fiber and polyetherimide
with revolution geometry.
In 2016, the first study where the application of this manufacturing process to
J. Compos. Sci. 2020, 4, 149 6 of 36

in [22] the application of this process to the layup of carbon fiber and polyetherimide with
revolution geometry.
In 2016, the first study where the application of this manufacturing process to the layup of
flax fibers with polypropylene polymer was conducted [23]. A little later [24], results on flax
fiber-reinforced polyamide layup were published. Such articles demonstrate the possible application
of this manufacturing process to materials reinforced with natural fibers.
The critical aspect of productivity, a need for transfer of this process to an industrial scale, has
been considered by different authors addressing different aspects. Among them, the reduction of the
prohibitively high prices of materials [25] and of the auxiliary elements has helped to promote it as an
alternative to consider in its application to the production of aeronautical parts.
Regarding the characteristics and the physics of the process of the layup, Khan et al. did a quite
complete analysis on how different conditions/aspects of layup affect the level of porosity and the
degree of joining between the layers and the relationship with the processing speed [26]. The following
list contains its main conclusions. It can be seen that the improvements of some of the conditions
normally have a negative impact on others, wherein the special complexity of this manufacturing
process lies.

• Tooling temperature. The trend in void volume to decrease with lower layup speed is reversed
when tool temperatures approach the melting temperature of the polymer included in the tape.
When the temperature is low, the tool usually acts as a heat sink, leading to a high viscosity
that prevents good movement of the chains and impacting a low degree of bonding, making it
necessary to decrease the wrapping speed. In contrast, when the tool is at a high temperature
(around 573 K for PEEK), good degrees of bonding are obtained even close to 10 m/min.
• Compaction force. The degree of bonding increases with higher contact forces, as should be
expected, and the void content also declines. Its effect being more marked with the increase in
the speed of the layup (the more speed, the more force required). Regarding the layup speed,
the level of porosity should decrease with increasing force and increase in speed. On the other
hand, the degree of bonding, despite increasing with force, decreases with speed.
• Number of layers. When the number of layers of a laminate is high, a double effect occurs;
the lower ones receive more consolidation stages (reconsolidation) but the upper ones are more
isolated from the heat sink-tooling. This causes them to experience greater heating and therefore
it contributes to increasing the size of the pores.
• Heating length. Longer heating lengths contribute to increasing the level of porosity. On the
other hand, the degree of bonding is improved, and the process can be carried out at higher
speeds. Heating length is directly related to the heating time as both are related through the speed
of lamination.
• The use of several rollers contributes to improving the degree of bonding, which can go from
varying between 20–95% to a range between 70–95%. Despite the advantage of having several
rollers over compaction, increasing their number has a detrimental effect on the layup machine,
making it necessary to have more components (more occupied volume) and making layup of
complex geometries nearly impossible.

Despite all the problems present in this manufacturing system, parts of relative complexity have
already been executed using this technology. Some of them are: Helicopter landing gear [27,28], tail
cone of a helicopter [29], rocket engine covers [30], cryogenic space tanks [31], and wingboxes [32,33].
In the manufacture of the wingbox, stiffeners designed with a closed omega geometry have also
been implemented with automatic lamination and in-situ consolidation. To facilitate this development,
tools made of metal alloys were used, whose melting point is 75 ◦ C under the glass transition
temperature of PEEK, thus facilitating their extraction by fusion once the layup has been completed.
J. Compos. Sci. 2020, 4, 149 7 of 36

Improvements to the ISC Process

There are several sources of process distortion that are localized and whose improvement/resolution
would imply, among other aspects, improving productivity. The layup and fastening of the first layer
is one of them. Bibliographic solutions include tapes on unreinforced polymer sheets [34], tools with
vacuum application or fixation adhesives [25,35], or employment of microporous tools [9].
The improvements to the process are not limited to physical components of the machine, control
systems, or considerations of the layup; the material object of the lamination also has a dominant role
in the results [36]. Based on the aforementioned statement, many works conclude that the results
could be better with improvements on the quality of the taped material [22]. Other characteristics to be
evaluated are [37]: Surface roughness, viscosity, and distribution of fiber and resin.
Another problem that is also extensible to any manufacturing process with composite material
is the appearance of residual stresses [38–40]. Its development is inherent in the differences in the
coefficients of thermal expansion between fiber and resin, but also the large thermal excursions of this
process pose a greater problem. The layup process has another associated penalizing element, the
sequential increase of layers of the material, leaving the material in an unfavorable state from the point
of view of stresses. The residual stresses are not the same if the laminate cools evenly, as happens in
autoclave, instead of a consolidation layer-by-layer. The residual stresses can become large enough to
cause micro-cracks in the resin, and annealing over Tg may lower the residual stress gradients through
the thickness of the laminate. An analysis was done by Sonmez et al. [41], where they propose certain
ideas to reduce these thermal residual stresses:

• Pre-heating the incoming tape, in order to achieve a progressive drop in temperature when the
tape and substrate come into contact, resulting in more progressive cooling and therefore reducing
residual stresses.
• Working with a higher wrapping speed increases the residual stresses. The cause is the existence
of point zones that are experiencing higher thermal gradients.
• The size of the heated surface also influences the residual stresses. The smaller the heated surface,
the sharper the heating–cooling profiles. Better results are observed when the heated surface of
the substrate is larger than that of the contribution.

August et al. [42] indicated that the need to use low layup speeds comes from a misinterpretation
of De Gennes’ theory of reptation; as the material enters the region of shear thinning the viscosity is
reduced and therefore the time for chain relaxation is lower. In fact, Automatic Dynamics, producer of
machines associated with the work of the cited reference, indicates that there is a real the possibility
of producing pieces with this technology, indicating that they produce parts equivalent to 5000 kg of
material each year using this technology.
From the work of Hoang [35], it was deduced how the effect of interlayer porosities is eliminated
by the successive passes of the machine in the placement of the subsequent material. However, the last
three layers are the most affected, indicating that three passes on the material are not sufficient to
achieve the perfect bonding, with a wrapping speed of 1.5 m/min and with heating provided by a hot
gas torch. Furthermore, in that work it is argued that, according to the layup sequence, the need for
reconsolidation passes is different, with different requirements for panels where all the layers are 0◦
or +/−45◦ . The problem is solved with reconsolidation passes without the input of material from a
different number of layers depending on the sequence being taped. In some laminates, cooling systems
are used when their thickness is such that the entire bottom laminate can act as an insulator with
respect to the tool surface and generate an overheating effect. The above improvement is meaningless
when active control systems are capable of acting on the power supplied by the heating source.
The compaction roller is also presented as an element of improvement for the process. Some authors
are in favor of working with heated rollers (mainly proposed when they are metallic), while others
propose solutions in which the roller requires cooling systems that avoid excessive deterioration of the
constituent rubber (elastomers or silicones). The proposals for roller cooling systems are usually based
J. Compos. Sci. 2020, 4, 149 8 of 36

on the fact that compaction must coincide with the solidification stage of the material to avoid the
development of porosity in the laminates. The roller also plays a relevant role in the surface finishing
of the part. In [30] the surface finishing results obtained with different cooling solutions for the roller
were presented (by external air jet, by thermal contact against a cooled roller, or by flow of internal
water) with cooling by internal water being the preferred solution.

3. Thermal Transfer and Temperature Measurements

In the processing of polymeric composite materials, either thermosets or thermoplastics, the applied
thermal profile strongly influences the results for the obtained part. In the particular case of
thermoplastic materials, by exhibiting a behavior that is dependent and not stable with temperature,
it is of great interest to know precisely the thermal history to which the material is subjected.
More particularly, for the automatic layup and in-situ consolidation process, the applied thermal
profile will determine the development of changes in the material such as melting, chain diffusion,
crystallization, the possible thermal degradation and the development of residual stresses.

3.1. Heating Systems

The heating system in the wrapping machines is one of the most questioned elements in the
references, as reported [43–46]. Initially, the system was based on the use of hot gas torches, later
evolving to the use of lasers, starting with CO2 lasers, going through the Nd:YAGs, and reaching the
laser diode as the best alternative. This diversity of solutions for heating have been implemented with
different results: Infrared sources have not reached the high intensity demanded by the heating to the
nip point, while the hot gas torch manifests a low energetic efficiency and slowness in its response
time, despite its low cost and design flexibility. The laser has turned out to be the first option based on
its good energy efficiency and speed of response. Furthermore, in the case of lasers, for deciding on the
use of one source or another it is vital to know the interaction with the material, especially the ability
of the material to absorb radiation. In the case of CO2 type lasers (λ = 10,600 nm), the resin shows a
high absorbance; on the other hand, in the Nd:YAG and diode lasers (λ = 1064 and 805–940–980 nm
respectively), the resin is transparent to radiation, transmitting and reflecting all energy.
Regarding heating, in certain references the possibility using two sources of heating instead of a
single one is alluded to. Tierney and Gillespie [47] indicates that the existence of a pre-heating system
does not seek consolidation but a first effect of adhesion between the parts, helping to avoid harmful
effects derived from cutting the material (lack of tension in the positioned tape, misalignment of fibers,
etc.). The possibility of achieving this improvement is also reported in [48,49], with a machine structure
where there is only one laser-type thermal source and two roller-type compaction systems.
Many machines carry lasers with two groups of laser diodes at wavelengths λ = 975 ± 10 nm and
two others with λ = 1025 ± 10 nm [50–52]. The incorporation of the diode laser type NIR (near-infrared)
has allowed working with greater focal lengths than the carbon dioxide laser sources, from 127 mm to
250 mm.
The diode laser is the most commonly used solution; Köhler et al. [53] mentioned a possible
disadvantage of using this type of system, the lack of a homogeneous intensity distribution. The use
of homogenizers can mitigate this effect, carrying out the homogenization by means of different
alternatives. One of them is the superposition of beams of the laser itself; another system consists of
incorporating a waveguide equipment. This can also be done by using a set of micro-optical lenses [54].
The use of CO2 lasers is shown as an alternative for heating uncolored surfaces as polymers
without reinforcement or with glass fiber reinforcement [55]. The proposed solution has a direct
application to fixing first layer problems or the use of sheets as functionalized surfaces, as well as in
the development of hybrid components.
Currently, there are also machines where alternative heating systems are being tested, such
as an ultrasonic heating source [56,57]. Ultrasonic heating consists of excitation and friction of the
polymer molecules due to the low amplitude and high frequency of vibration of the ultrasonic waves.
J. Compos. Sci. 2020, 4, 149 9 of 36

The advantages of using ultrasound heating sources are the focused heating, reducing the amount
of energy required, allowing the increase of the welding speed. Its use has allowed automatic layup
with polyethylene materials and glass fiber and polyethylene terephthalate with carbon fiber, but gives
lower results than those obtained by press processing of the same material.
Lichtinger [58] reported the use of a different heating system, quartz lamps that apply infrared
heating, developed by Heraeus Noblelight. The main disadvantage of this system is the need to be
located almost in contact with the substrate and newly incoming tape.
Another alternative system referenced in several studies is the vertical-cavity surface-emitting
laser (VCSEL) [59]. This system, made up of an array of microlenses, allows control of independent
lines of the laser emission power. Among the advantages of using systems of this type are possible
differential heating to join surfaces of different materials, compensation of areas with heat loss/areas
with heat accumulation (homogenize the heating footprint), control of temperature distributions in
complex tapes (curvatures) or control of the cooling profiles. Considering complex areas such as
changes in curvatures or ramps, the effects that occur usually correspond to overheating, related to
the laser position with respect to the laminate, where irradiation results from a relationship between
the power supplied and the surface being irradiated. The decrease in the surface generates a higher
irradiation for the same applied power level.
The advantages of VCSELs also have direct applications to the effects of under-heating at the
laser inputs or possible overheating experienced at the outputs. In contrast, this system does not
homogenize the laser beam, making it necessary to position it very close to the layup area and hindering
the positioning of temperature reading and control systems.

3.2. Heat Transfer Models

With the aim of being able to control the automatic lamination and in-situ consolidation process,
many research groups have tried to simulate the evolution of the thermal profiles in the heated material
under the action of various thermal sources [60–80].
The first studies in this regard date from the 1980s, with the work of Grove [60] that uses the finite
element method to solve the thermal transfer problem in APC2 with a two-dimensional simplification
of geometry of the heating process using a laser source. However, experimental validation of the
obtained results was not reported.
Some of the works also show the coupling of the thermal model with others, such as consolidation
or degradation, in order to determine the optimal processing conditions, such as [64,66]. Sonmez [64]
highlight the benefits of pre-heating the substrate and not the incoming tape to optimize the degree of
bonding. The distribution between percent of heating in incoming tape and substrate is also discussed
in [46], determining a high and stable value of peel strength between layers when the distribution of
the area of heating is 60—incoming tape/40—substrate; they also recognize the need to run the tapes of
the last layers at a lower speed to compensate for the reduction in consolidation times.
Toso [66] solved the problem of heating with a hot gas torch on laminate to obtain a geometry of
revolution. He used a cylindrical coordinate system in the substrate material and a Cartesian system in
the incoming tape. In this study, the contribution of heat flows from the crystallization exotherm and the
fusion endotherm were neglected based on experimental results obtained by calorimetry. Their analysis
determine that an over-estimate of the temperature values occurred when considering these effects, an
over-estimate that was increased with the real cooling profiles of the manufacturing process.
Contrary to what was hypothesized previously by [66], in the case of modeling a similar thermal
problem in thermoset materials, Hassan [80] takes into account the curing of the exotherm in the model
as an added heat source. In his work, he modeled the added plies by adding new elements to the
meshing at each iteration step. Nicodeau [81] carried out the modeling of the thermal problem with
APC2 including in the equations the terms related to the melting and crystallization of the material.
The problem is solved numerically with a two-dimensional geometric simplification. In order to
account for the effect of depositing new layers of material, the elements of the interfaces are acted
J. Compos. Sci. 2020, 4, 149 10 of 36

upon, modifying their boundary conditions: Before the actuation of the roller they will be isolated
elements from each other and after the passage of the roller, equal temperatures will be imposed
between these elements but not equal heat flow. It is worth noting in this reference the simplification
of the tooling, which will be taken into account in the simulation as a boundary condition and not as
a physical element, thus impacting calculation times. This simplification is also carried out in other
references and hence different values for tooling are incorporated, which are also used in cases where
it is estimated that there is no perfect material-tooling contact.
Ghasemi Nejhad et al. [62] performed an inter-comparison for solving the thermal problem using
a numerical solution based on finite elements and also applying an analytical solution by means of a
development based on variable separation. In his work it was shown that there is a good agreement in
the solutions reported by both calculation methodologies.
On the other hand, Pitchumani et al. [63], proposed to execute the layup process by using two
heating sources. The first one is a system for preheating the material. Among the hypotheses elaborated
in this work, the following stand out: The heat flow of the crystallization is neglected as it is much
lower than the others involved in the process and the first source of heating exerts its effect on the
upper surface of the incoming tape. The work uses the thermal model to feed its study on the degree
of consolidation and the evolution of porosity in the laminate. It reported improvements in the degree
of bonding with increases in the compaction force, with increases in the air temperature of the heating
torch, with the incorporation of a compaction system between both heat sources and with subsequent
forced cooling (by reducing porosity when compacting during solidification).
Belonging to the same research group as the authors mentioned in the previous paragraph, Tierney
and Gillespie [47] developed a work in which the numerical simulation of the thermal model in an
automatic lamination process and the mathematical model that applies to dynamics in the formation
of voids are presented together. The formulation of its thermal model considers a simplification in a
single dimension and under a steady state.
As shown above, several groups worked on dual heating sources to improve consolidation.
With a similar purpose but a different architecture, Li et al. [82] alludes to the use of an infrared
preheating system of the material fed by the machine. They proposed a simplified thermal model for
this pre-heating effect, which allows estimation of the diminution in layup time due to pre-heating,
related to the tape speed. Experimental validation was not done.
Regarding the heating system, Lee [44] presents the differences to be imposed in the thermal
transfer equation in the analysis of a layup process with composite material, depending on what type
of heating source is being used, such as heating with a hot gas, hot air, and with a solid element.
In the case of heating with a hot fluid/liquid, it is estimated that the coefficient of thermal convection
should be at least twice that considered when using a hot gas source. When heating with a solid
element, the convection contour condition is replaced by a constant temperature condition in the
interface between the element and part, this being the system that allows the shortest response times
and also the one that offers the least risk to possible degradation effects on the material. The only
disadvantage linked to this type of system is the need to generate them as heated rollers with a
temperature control system.
Thermal simulations are run by using the FlexPDE software in [83,84], including for the output
heat losses of the material due to radiation. Thermal simulation allows explanations for variations in
the mechanical properties of the fracture between test specimens manufactured with different holding
times on the melting temperature of the polymer.
Other methodologies used in solving the thermal problem can be found in [48,49,85–87], with the
use of the numerical method called proper generalized decomposition (PGD), which solves the heat
equation by variables separation and with a methodology based on the application of the principle of
virtual works. Likewise, in these works the effect of the thermal resistance between layers (also used
by Grouve, [71]) is accounted for. Taking into account that there is no perfect contact between the
layers for heat transmission, it generates more precise results of the temperature profile experienced by
J. Compos. Sci. 2020, 4, 149 11 of 36

the material, especially improving the precision of the adjustment in the cooling phase. The resistivity
condition between the layers acts in such a way that it considers that there is a blockage to the heat
transmission to the lower layers and therefore the cooling is more impeded and is therefore more
progressive. In other studies, by contrast, this effect is considered negligible for simulation [88].
In some works [48], a correlation between heat transmission and the mechanisms of diffusion
and degradation by cross-linking in the material is also presented (without considering the effect of
intimate contact, assuming perfect contact), reporting a beneficial effect by keeping the tool heated at
a temperature of 473 K, a condition in which 100% adhesion is obtained with a minimum cross-link
value. Normally, the tooling temperature should be kept at a value between the glass transition
and crystallization peak of the material. In the case of a material such as PEEK, PEKK, or LMPAEK
(well-known as high performance thermoplastics), 473 K is a conventional temperature that has proven
to improve the quality of the final part.
Appling a layup process with an electromagnetic inductor-type heating source, Duhovic et al. [72]
presented a resolution of the thermal model using the finite element method. His study highlights
the possibility of executing hybrid metal–carbon composite or –carbon fiber composite joints against
another counterpart using an intermediate susceptor. The special feature of this simulation was the
need to add cooling on the upper surface to avoid its excessive heating, because the objective was to
join an interface far away from this surface area. The simulation has also made it possible to reach
conclusions regarding the correct adhesion of the elements, indicating that to achieve a correct joint,
the compaction step must take place in the temperature range of 653 K to 553 K, since it corresponds to
the interval in which the re-crystallization/solidification of the polymer takes place.
In the model of Li et al. [74] the novelty lies in the methodology used to simulate the sequential
addition of layers to the laminate in a layup with a hot gas torch. The strategy is based on the
programming of an algorithm in ANSYS that gradually activates the elements with the evolution of
the layup. It does not mean that the elements of the model appear and disappear, but rather they
are multiplied by certain factors so that during the layup of layer 1, the highest layers do not have
influence on the model; their contribution appears upon reaching the layup to them and so on. Among
his hypotheses, it is worth highlighting they ignore the effect of heat dissipation towards the roller, a
simplification not carried out by most of the works consulted. In one of his conclusions it was indicated
that increasing the layup speed decreases the temperature in the nip point, presenting a trend that is
not linear between both parameters.
Contrary to neglecting the roller as a participant in the simulation, Kergomard, [76], proposes
the development of a mechanical simulation that allows calculation of the deformation of the roller
under the state of loads to which it is subjected, then evaluation of the thermal model. In this way,
less uncertainty is generated about the area of the roller’s action in the thermal model.
The thermal study carried out by Stokes-Griffin et al. [51,89,90] alludes to an effect penalizing
heating in automatic lamination compared to heating obtained by filament winding; the shadow of
the roller is an effect to be included in simulations. Due to the positions that each of the elements
must occupy in the machine head and the deformation of the elastomeric rollers, a reduced area
is generated where the laser is not capable of heating, a few millimeters before the contact of the
incoming tape with the substrate (nip point). The experimental validations as well as the models show
a temperature drop in this shadowed region, greater for the substrate than for the incoming tape due
to the greater heat losses at the substrate. The author of the work indicates that said shadow effect
affects the subsequent consolidation area (started from the nip point) and therefore, each machine will
be subjected to very different results only due to differences in this simple element of the machine.
In its development, the roller is counted as a physical body, including its geometry in the finite element
model applied to solve the heat equation, unlike the vast majority of previous references where the
roller is considered a boundary condition. The condition that applies between roller and laminate is a
thermal conduction condition which includes the possibility of considering a thermal resistance effect;
the higher this thermal resistance, the less the heat sink effect of the roller. The value that best adjusts
J. Compos. Sci. 2020, 4, 149 12 of 36

the roller–laminate thermal resistance in this investigation corresponds to: 1–2 [m2 K/kW], a typical
value in stainless steel–silicone interactions.
In the thermal model proposal of the previous reference, velocity terms are included in the
left-hand side of the heat equation, which is not normally considered, to include the effect of mass
transport of heat due to moving elements, proposing Equation (1).

∂T ∂T ∂T ∂ ∂T ∂ ∂T
! ! !
..
ρc + vx + vy = q+ Kx + Ky (1)
∂t ∂x ∂y ∂x ∂x ∂y ∂y

Furthermore, this study analyzes the need for mesh reinforcement for the validity of the simulation.
To do this, it reports thermal diffusivity values of the different components of the modeled geometry,
using this parameter to calculate the Peclet number, which establishes the limit of the size of the mesh
elements. Because of the results, a greater number of elements are required in the area of the roller
directly in contact with the laminated material.
In [69,89] the effect of the multiple passes experienced by a layer of material on the final result
of the laminates is considered. Ref. [69] considers that approximately two layers below the layup
area the material is still melted, while several more layers experience temperatures between the glass
transition and the melting (considering layup speeds of 1.2 to 4.8 m/min). This effect implies, according
to the authors, an increase in the degree of contact between the parts that evolve from 0.75 to 0.9 in the
joint line after only three layup passes, thus making it necessary to re-consolidate the upper layers to
obtain a homogeneous laminate. Ref. [89] reports that at speeds of 6 and 24 m/min with AS4/PEEK150.
Only the layer that is being laminated with the 673 K set point undergoes fusion, the bonding processes
being conditioned by these thermal profiles.
The same author of the previous article published a study [91] with a new methodology that seeks
to obtain the requirements of heat flow on the laminate by imposing the temperature that is desired to
govern the interface region. In this way, the power that would be required for that specific result can
be estimated. The work highlights the statements made on the “heat soak”, which is described by the
author as the time the material is kept at the set temperature; when the “heat soak” value is reduced,
the material spends less time at the maximum temperature and the cooling profiles are slower, which
positively affects crystallization.
Pignon et al. [92] couples the contribution of the heat flow generated by the crystallization of the
material in an injection molding process to the thermal model. They apply the Nakamura model for
the crystallization process.
Di Francesco et al. [34], proposed an analytical and a semi-empirical approach of the thermal
problem, applied to a machine able to tape thermoplastic and dry fiber prepreg. An equation is
presented in his work to estimate the temperature of the nip point, as a function of the layup speed
(V), the power (P), material parameters (K), and the machine set-up (K) (heating footprint), showing a
linear trend with the variation of power (Equation (2)). Some deviations from linearity happen due to
the dependency of the material properties and the temperature, but experimental errors are lower than
10%, so its validity is demonstrated. Its development has allowed establishment of an open control
loop to adjust the parameters of power–speed–temperature of lamination.

TVNP = KV −0.5 P + T0 (2)

Weiler et al. [77] proposed an analytical resolution of the thermal Equation (1) considering that
it is the most effective/fastest method to establish online control of the automatic layup and in-situ
consolidation. Numerical solutions used to be more accurate, but less flexible and more time consuming
than analytical solutions, which require some simplifications in the problem statement, in order to be
solved. Among the novel hypotheses and considerations that appear in this work are those listed below:

• The thermal resistance to heating of the laser source is determined to be of infinitely small value,
hence the advantage of this type of heating over others.
J. Compos. Sci. 2020, 4, 149 13 of 36

• The temperature-dependent properties of the material are simplified using its average value in
the temperature range considered.
• Even executing an analysis of the layup process of a curved geometry, the author proposes to
simplify the material as a plate geometry.
• The depth of penetration of the laser is considered to be less than the depth of penetration of the
heat flux.

The validity of these hypotheses has been proven by comparison of the analytical predictions
with the numerical results for eight different cases. The article proposes two control models for the
process, one based on an open loop system (a system that is not based on any external reading but on
previously calculated solutions) and another a closed-loop system (using readings on the back of the
fed material obtained with pyrometers).
The power supplied by the source will be included in the models as a heat flow estimated from
the value of the power in (W) and its application area.
For the correct operation of the simulations presented by the different authors, feeding with
the values of the different thermal properties of the material is required, properties that in the case
of composite materials are anisotropic and in many cases are also dependent on the temperature.
To shed more light in this regard, Table 1 contains a compilation of the bibliographic values of different
parameters required for thermal modeling together with the information provided on the material
under study.

Table 1. Thermal properties of the poly-ether-ether-ketone (PEEK)–carbon fiber (CF) composite.

J W W kg
[Ref.] Material cp ( kgK ) k11 ( mK ) k22 ( mK ) ρ( m3 )
(Grove, 1988) [60] APC2 ICI a a a -
(GhasemiNejhad et al., 1991) [62] APC2 10 b 6 b 0.72 b 1560 b
(Phillips et al., 1994) [75] APC2 1700 5.9 0.7 b 1600
(Kim et al., 1996) [64] APC2 ICI - 10 k22 a a -
(Shih, 1997) [93] APC2/AS4 1425 6.0 0.72 1562
969.32
(Toso, 2003) [66] CF/PEEK +5.0244 T 0.55 0.41 1640
−0.009794 T2
(Tierney and Gillespie, 2003) [47] APC2 1370 - 0.34 1584
(Lamèthe et al., 2005) [84] APC2 1300 c - 0.7 c 1575 c
(Tierney, Gillespie,2006) [69] APC2 1370 3.5 0.34 1584
(Barasinski et al., 2011) [48] APC2 1700 5 0.5 1560
(Li et al., 2015) [74] APC2 ICI 1124 d 7.5 d 0.75 c 1562
5.54 0.813
886 (298 K)
(Maurer and Mitschang, 2015) [50] APC2 (298 K) (298 K) 1540
1803 (573 K)
9.36 (573 K) 1.188 (573 K)
(Stokes-Griffin et al., 2015) [51] AS4-PEEK150 1300 e 5.9 e 0.7 e 1575 e
(Lionetto et al., 2016) [94] CF/PEEK 1088 5.4 0.5 1532
(Weiler et al., 2018) [77] CF/PEEK 1425 - 0.72 1560
aNumerical values reported by graphs; b Different values for process window were used based on bibliography;
cValues for 473 K, check reference for 523, 573, 623, 673 K; d Values for 453 K, check reference for others; e Values for
473 K, check reference for others.

It is also possible to locate some work [95] where the thermal properties of the fiber and the resin
are presented independently, allowing estimation of the validity of the law of mixtures, useful for
other fiber/resin systems when laminate properties are not available. The reported values for PEEK
and carbon fiber (T300) are, respectively, conductivity of 0.25 W/(mK) and 50 W/(mK). Densities of
1.32 g/cm3 and 1.85 g/cm3 and specific heat 320 J/(kg K) and 710 J/(kg K). The law of mixtures may
work for the density, but fails for the anisotropic thermal conductivities.
In the simulation, not only will the material’s own parameters intervene, but also the transmission
of heat to the environment, by the tooling or by the compaction roller; this requires feeding the model
J. Compos. Sci. 2020, 4, 149 14 of 36

with a set of numerical values. In the case of the tooling used for lamination, it is possible to find a
variety of parameters according to the references; Table 2 includes some of them.

Table 2. Thermal properties for the tooling.

J W kg
[Ref.] Tooling Material cp ( kgK ) k( mK ) ρ ( m3 )
(Ghasemi Nejhad, 1991) [62] Steel 473 43 7800
(Stokes-Griffin et al., 2015) [51] Aluminum 951 237.5 2689

The remaining thermal transfers will be modeled based on boundary conditions. The parameters
that apply have been reported by references and are compiled in Table 3.

Table 3. Thermal properties for boundary conditions.

[Ref.] Roller Material hRoller ( mW

2K ) hAir ( mW
2K )

(Grove, 1988) [60] - 500 7

(Nicodeau, 2005) [81] Metal 1000 13
(Stokes-Griffin et al., 2015) [51] Elastomer 1000 5–17.1

In the simulations, the results are totally linked to the layup speed considered (which will condition
the heating time, among others), hence it is of interest to know the values reported in the different
works, which have been collected in Table 4.

Table 4. Layup speeds for PEEK–carbon fiber and other thermoplastics in in-situ lamination and
consolidation processes.

[Ref.] Lamination Speed (m/min)

(Grove, 1988) [60] 6
(Ghasemi Nejhad et al., 1991) [62] 0.6−6
(Kim et al., 1996) [64] 2.4−3.6−4.8
(Sonmez y Hahn, 1997) [65] 1.8
(Pistor et al., 1999) [79] 0.9
(Tumkor et al., 2001) [67] 2.4
(Toso, 2003) [66] 6
(Tierney y Gillespie, 2003) [47] 2.4
(Nicodeau, 2005) [81] 1.2−2.28−4.2 a
(Grouve, 2012) [71] 4.5−6−7.5 b
(Han et al., 2014) [73] 0.3−1.5 c
(Maurer y Mitschang, 2015) [50] 3−6−12
(Stokes-Griffin et al., 2015) [51] 8
(Stokes-Griffin y Compston, 2015) [89] 6−24
(Weiler et al., 2016b) [78] 12
(Lionetto et al., 2016) [94] 0,06−0,24 d
(Di Francesco et al., 2017) [34] 6−12−24−48
(Weiler et al., 2018) [77] 0 to 30
(Murray et al., 2017) [31] 12
a Considering the intermediate value the nominal condition and the other two extreme conditions, lower and upper.
b Unidirectional PPS/CF lamination on PPS/CF 5HS fabric laminate. c PEI/CF lamination. d Layup process with
induction heating and IM7/PEEK from Suprem.

Recent simulations, based on systems with laser heating sources, take into account the optical
behavior of the material for the calculations. In the above cases, it is key to know the optical properties
of the materials, which are compiled in Table 5. To obtain the reflectance and transmittance of
a thin material, experimental measurements can be carried out using a spectrophotometer; later,
J. Compos. Sci. 2020, 4, 149 15 of 36

by using mathematical expressions, the reflection index value (real and complex components) can be
obtained [96].

Table 5. Optical properties of the PEEK–CF composite material.

Refraction Refraction
[Ref.] Reflectance Absorbance Emissivity Index Index
(n)—Material (n)—Roller
(Grove, 1988) [60] 0.28 - - - -
(Grouve, 2012) [71] - - 0.9 1.8 -
(Stokes-Griffin and
- - - 1.95–2.30 a 1.42
Compston, 2015) [51]
(DiFrancesco et al.,
- 0.6 b 0.8 c - -
2017) [34]
(Weiler et al., 2018) [77] - 1 0.9 - -
(Reichardt et al., 2018) [97] - - - - 1.4
aThe value depends on the simulation run, such as specular surface or half a cylinder of microns in diameter. b
Measurement with laser incidence angle of 80◦ . c The reference indicates that said value has been calculated in
an experimental process without taking into account the possible reflections of the incoming tape; using a higher
emissivity value could compensate for this.

Some of the works that take into account the optical behavior of the material in their simulations
are [51,71] with a two-dimensional or 3D ray tracing approximation, respectively. In these works,
it is stated that the use of the ray tracing approach to describe the behavior of the material is justified
because the diameter of the carbon fibers is an order of magnitude greater than the working wavelength
of the laser.
Ref. [51] performs thermo-optical modeling based on the result of the optical model under the
hypothesis of a micro half cylinder (MHC), a divergent emitting source and a spatial emittance function.
In the work, he performs intercomparisons with different methodologies of representation both of
the surface of the material (specular, non-specular, or MHC) and of the irradiation system. He also
incorporates an analysis of the variations in the thermal profiles caused by the differences in the
orientation of the fiber of the substrate material, observing that its effect can be considered negligible.
Schaefer et al. [88] uses a thermo-optical model in the layup with carbon fiber reinforced polyamide
(CF/PA-6); they establish a laser source term depending on the absorbance of the material which is in
turn dependent on the angle of incidence of the laser. Reichardt et al. [97] developed a three-dimensional
model considering non-specular reflection.
The references agree on the identification of the PEEK polymer as a material where the main
behavior against laser radiation is transmission (both in an amorphous and semi-crystalline state).
For its part, the carbon fiber acts as a highly absorbent element in which the reflected radiation depends
on the orientation of the fibers in relation to the radiant focus.
When a laser irradiates a material, the energy is absorbed, transmitted, or reflected, and the
percentage for each of these contributions directly affects the properties of the material, and also
affects its crystalline or amorphous state. Due to the participation of the properties of the material,
some studies are dedicated to its determination and the estimation of its dependencies with respect
to different factors, for example the temperature (Ref. [71] for the CF/PPS, Ref. [51] for the CF/PEEK,
and Ref. [88] for CF/PA-6). Among the results obtained for the CF/PEEK the following conclusions
stand out.

• The crystalline phases scatter light by local variations of the refractive index. The detection of
higher absorbance in a semicrystalline material compared to an amorphous one is associated with
the subsequent reception of the reflected rays. In the case of the composite material, the limited
thickness of the surface resin layer and the small size of the spherulites formed make these points
of reflection limited and can be considered negligible.
• The behavior of reflection of the PEEK in the NIR (near-infrared) can be considered representative
of that presented by this material under laser radiation.
J. Compos. Sci. 2020, 4, 149 16 of 36

• The refractive index of the resin is estimated to be dependent on temperature inversely to the
dependence of the coefficient of thermal expansion.
• The optical properties of the carbon fiber can be considered constant in the range of temperatures
experienced during the in-situ consolidation and lamination process.
• Radiance is considered to be proportional to the irradiance in this material.
• The transmittance can be considered negligible for the CF/PEEK. The polymer, which in the
amorphous state would have a high transmittance of laser energy, being reinforced by the fiber,
would have a negligible effect on the whole. Transmittance can be neglected in calculations.
• In the composite material, the reflection depends on the orientation of the fiber with respect to the
emitting focus, showing special reflection patterns.
• Knowing the angle of incidence of the laser, it is possible to estimate the angle of reflection by
applying Snell’s law.
• It can be estimated that most of the incident light is both absorbed and reflected by the first carbon
fiber layer of the surface and this allows the analysis to be simplified to a surface to run models of
macroscopic behavior.
• It is possible to consider the refractive index in the composite material only for its real part as
there is practically no absorption.
• In radiation simulation, choosing a collimated beam with the geometry of a hat-shaped profile is
not appropriate when working with NIR lasers with the inclinations required by the ISC process;
it is essential to consider the beam divergence.
• After two beam reflections, the irradiation intensity becomes negligible. To realistically model
heat transfer, the laser incidence profile should also account for these first two reflections.

Once the optical model is developed, the next step is to perform its coupling with the thermal model.
In the bibliography, the importance of elaborating these thermo-optical simulations is highlighted
due to the underestimation that conventional thermal models make of the real energy required by the
material for heating, since they do not take into account the reflectance of the material. Weiler et al. [78]
compiled information from different works where the previous statement is supported, but also from
others, where it is indicated that the laser radiation impacts on the substrate and incoming tape, which
are reflected from each other and, therefore, leave a final balance in which there is no loss or energy gain.
The author presents a variation in absorbance and reflectance depending on the angle of incidence
of the heating source where it can be seen that once the incidence angles of 60◦ have been exceeded,
the reflectance begins to be important, estimating that its impact on radiant exposure (integration in
time of radiation exposure) is approximately 16%.
Referring to the thermo-optical coupling, Grouve [71] did his model under the assumption
that the speed of heat conduction in the forward direction of the layup is much lower than the
displacement of the machine. Under these conditions, the process is governed by conduction through
thickness, proposing a methodology for solving the energy balance based on a pseudospectral or
placement method. Also, Reichardt et al. [97] coupled their optical and thermal models, with the special
characteristic of describing the reaction of the material to radiation with a micro-model, the reflections
obtained from its application are extrapolated to the macro- model.
To take into account the orientations of the reflected rays, Reichardt et al. [97] uses a bidirectional
reflectance distribution function, solving the thermo-optical problem numerically. It is also the first
work we identified where the problem was solved in an analytical way, comparing the results of the
application of both methodologies. The numerical and analytical results are very similar when specular
reflection of light is taken into account in the numerical solution.
Weiler et al. [78] proposed an optical model for a VCSEL heating source. The work carries out
a first view on the generalities of laser heating and the requirements to simulate it by considering
the distribution of angular intensity, irradiance, and absorbed intensity, but leaving the depth of
penetration of the laser out of the study. In the simulation, a calculation is carried out to consider the
J. Compos. Sci. 2020, 4, 149 17 of 36

superposition of the effect of the independent lamps constituting the VCSEL, demonstrating that the
irradiation decays towards the nip point in the substrate and increases towards the nip point in the
incoming tape.
A model with simpler optical considerations is the one proposed by Maurer and Mitschang [50],
the first document in which COMSOL Multiphysics software was used. This model in turn uses two
sub-routines programmed in MATLAB for the heating source and for the roller. The laser model
estimates the power applied to the substrate and input material. Since the system is focused, it is
modeled considering the height of the focal point and the focal distance to the nip point. In addition,
the laser beam has its own coordinate system that allows it to vary its position in the model, then
change the substrate-incoming tape temperature distributions. The incident heat flow in the material
comes from a calculation that takes into account absorption and reflection (considering the same angle
for incidence and reflection).
For its part, the roller model is used to approximate the contact length by simplifying its geometry
by means of a rectangular area (contact with the substrate) and another trapezoidal area (drop area of
the incoming tape). The simulated roller takes into account the cooling system built with the roller.
Lionetto et al. [94] also uses COMSOL Multiphysics to run a thermal model of a process with
heating with an ultrasound source. Moving mesh is used for simulation, an element made possible by
the characteristics of the software. The heat equation to be solved incorporates a term that accounts
for the endotherm corresponding to the heat absorbed during the melting process of the material
polypropylene/E-glass. The same research group also developed a work where heating was carried
out using a source of induction on CF/PEEK [98], re-accounting the melt heat flow (Equation (3)) and
incorporating a term corresponding to crystallization (Equation (4)). This last term was obtained
by means of the Ozawa equation, with Cr being the relative crystallinity, whose relationship with
temperature and time is described as indicated by Equation (5). The Ozawa equation is not the most
suitable representation to describe crystallization in PEEK under dynamic conditions, because it does
not take into account the secondary crystallization, but still may be used to estimate the enthalpic effects.
1
Xm (T ) = [1 + (d − 1) exp(kmb (T − TC ))] 1−d (3)
" #
dT
XC = Cr 0.42 − 0.03 ln ( ) (4)
dt
dT
log[− ln (1 − Cr )] = log (exp[−0.037·T + 11.3]) + nlog(
) (5)
dt
Besides those works where only the heat transfer model is analyzed, there are other works where
multi-model couplings with all the possible physics involved in this process are analyzed together
(thermal-bonding–crystallization–degradation) [71,81].

3.3. Experimental Determination of Temperature

As this manufacturing process is carried out, it is necessary to know the laminate temperatures in
real time to act operatively by varying the intensity supplied by the heating source based on those
readings. The equipment used for this purpose usually reports temperature values by non-contact
measurements on the area under action of the heating source. The roller pressure application area is
hidden from the non-contact reading, thus losing all the information on the cooling profile. Speed
for the cooling profiles and the successive stages of reheating in the environment at 200 K/s are
reported [60]. This is one of the motivations for carrying out the simulations. Likewise, executing
experimental measures with various systems contributes to extracting this information and evaluating
whether the simulations developed are close to the actual results.
The methodologies used to monitor the temperature and analyze the validity of the
simulation results are different depending on the document consulted. They are usually based
J. Compos. Sci. 2020, 4, 149 18 of 36

on thermocouple-type temperature probe readings as reported in [48,51,61,64,70,80,81,88,93],

pyrometers [63], or thermal imaging cameras [71].
In verifying the thermocouple readings of the thermal profiles, there are several references that
discard the results of the first tapes on the thermocouple. The ruling out of these measures is based on
the unfavorable effects of direct laser irradiation on the thermocouple [88], which can be surrounded
by air after the first tapes on it. As the layup evolves, the thermocouple embedding improves, making
the data more rigorous. The simulations may later serve to complement the information of those
measurements that were considered unreliable.
Seeking to correct this negative effect of the measurement, [51] analyzed the temperature recorded
by the thermocouple at a location. Taking a point at the same distance from the nip point as the
thermocouple, the differences between the thermography and thermocouple reading were estimated.
These differences were used to propose a correction of the temperature value of the thermocouple,
which was applied to understanding what happens in areas where thermography cannot be used as a
measurement system.
In relation to the control through a thermography camera, the former authors [89] established the
polluting effect of the reflections of the material being taped on the thermal reading in the substrate
material. This causes the readings on the thermal imager to be higher than the real values presented by
the laminate.
Taking into account the positions of the incoming tape and substrate, the bibliography indicates
the impossibility of monitoring the temperature for both in the same way. The substrate may support
thermocouple monitoring; however, the incoming tape is limited to thermography measurements.
Oromiehie and Saenz del Castillo [98,99] demonstrated a system to monitor temperatures in
manufacturing systems with thermoplastic composite materials by the use of Fiber Bragg Grating
sensors (FBG). The basic principle of FBGs lies in engraving a small section of an optical fiber in such
a way that the core refractive index is periodically modulated using an optical interference pattern,
allowing it to receive a response in reflection. Under certain conditions, the response obtained presents
a peak centered on a different wavelength from the initial one recorded on the sensor. This effect is
related to an external effect such as the application of a mechanical load or a thermal load.
Saenz del Castillo et al. have compiled in [100] the equations for thermal analysis, and the results
for predicted and measured temperatures are presented in Figures 3 and 4, compared with a real
experiment monitored by FBG with good agreement.
J. Compos. Sci. 2020, 4, x 25 of 45

Figure 3. Wavelength
Figure 3. Wavelengthshiftshift
monitored
monitoredby by
sensors UPM,
sensors UPM,ZEUSZEUSand Fiber
and Bragg
Fiber BraggGrating
Gratingsensors
sensors(FBGs)
(FBGs)
during the during
in-situ the in-situ consolidation
consolidation of a singleof CF/PEEK
a single CF/PEEK layer. different
layer. Three Three different
stagesstages
can becan be
identified:
identified:
Heating-up byHeating-up by the
the laser (a), laser
effect of (a),
theeffect of the compaction
compaction roller (b),roller (b), and cooling
and cooling down (c).
down (c).
 Figure 3. Wavelength shift monitored by sensors UPM, ZEUS and Fiber Bragg Grating sensors
J. Compos. Sci. during
(FBGs) 2020, 4, 149
the in-situ consolidation of a single CF/PEEK layer. Three different stages can be19 of 36
identified: Heating-up by the laser (a), effect of the compaction roller (b), and cooling down (c).

Figure
Figure 4.4.Comparison of thermal
Comparison profiles
of thermal provided
profiles by FBG
provided by process monitoring
FBG process and thermal
monitoring model
and thermal
simulation.
model simulation.

3.4. Control
3.4. ControlSystems
Systems
Thermal models determine the temperatures experienced by any point of the laminate during
Thermal models determine the temperatures experienced by any point of the
the layup process. Another objective for the development of the model is to enable control over the
laminate during the layup process. Another objective for the development of the
wrapping equipment, seeking that it can autonomously carry out modifications to the power signal
model
sent by theis laser
to enable
and that itcontrol over the
is simultaneously wrapping
capable equipment,
of extracting informationseeking
about thethat it can
consolidation
autonomously
states, crystallinity,carry outstress,
residual modifications to the
or degradation power signal sent by the laser and that
effects.
Obtaining information on what happens
it is simultaneously capable of extracting information in lower layers than the positioned
about one allows
the consolidation
establishment
states, of a possible
crystallinity, qualitystress,
residual status in
orthe piece; however,
degradation for active control it seems logical that
effects.
the system uses a fundamental criterion for the control the adhesion requirements of the layer to be
Obtaining information on what happens in lower layers than the positioned one
taped at that specific moment. Khan [101] highlights the problem of applying a control by means of a
allows establishment of a possible
PID (proportional–integral–derivative quality
system) due to status
the slowin the piece;
response of thishowever, for active
system to changes in the
control it seems
profile, with logical
deviations of upthat
to 15the system
K from uses
the set pointa temperature.
fundamental criterion for
To compensate forthe
this control
problem,
he proposed two solutions based on two different methodologies within control theory: The optimal
quadratic control strategy and the predictive control model (MPC).
In the optimal quadratic control system, the determination of a law for a control vector is pursued;
a linear quadratic regulator (LQR) is used, which receives measurements from external sources such as
pyrometers, accompanied by a linear quadratic estimator (LQE), a Kalman filter, to predict uncertainties
in areas where it is not possible to extract values of measurements. The combination of both is carried
out by means of a Gaussian quadratic linear control (LQG). The strong point of the predictive control
model (MPC) is the combination of control algorithms together with the modeling of the process for
predicting the response. The responses by both control systems (LQG and MPC) are similar except
when certain restrictions are taken into account in the MPC. These restrictions can be limitations of the
types: Maximum value of power that the heating system can supply or maximum value of temperature
that can be reached during the process.
Heider et al. [68], on the other hand, based its control system on the use of a neural network.
The system is used to control the values of the machine parameters, looking for those that lead to the
most optimal manufacturing solution. According to the authors, this control system shows the best
response capabilities as compared to a traditional proportional–integral–derivative (PID) system.
J. Compos. Sci. 2020, 4, 149 20 of 36

4. Adhesion
In the analysis of the adhesion mechanism between the layers of the composite material, the process
must be described taking into account two factors: On one hand, the elimination of surface roughness
in the incoming material to allow the displacement of the polymer chains and, on the other hand,
the mechanism that controls this movement of chains.

4.1. Intimate Contact Theory

Between two surfaces of thermoplastic pre-impregnated composite materials brought into contact,
without the application of pressure or temperature, there are gaps due to the inherent irregularity of
the surfaces of the material. The high viscosity values of thermoplastic resins mean that they have a
limited ability to cover these areas only by natural flow of the polymer, making it necessary to force the
contact of both surfaces by physical means (application of pressure). In order to account for the effect
of this contact and the evolution of the destruction of the irregularities, models of “intimate contact”
emerge, the starting point of which is to characterize the surface state of the material.
It should be pointed out that the time required to achieve contact between the surfaces will
increase the greater the irregularity carried by the material, hence the importance of characterizing and
controlling this effect, whose impact on the productivity of the process is decisive.

4.1.1. Representation of the Material Surfaces

The starting point for modeling the removal of roughness in the material is to know its initial
state. In the bibliography, it is possible to locate different references where models of representation of
the material are included, taking into account different geometric approximations of its surface. Woo Il
Lee and Springer [19] proposed to model the surface of these materials as a succession of identical
rectangles. On the other hand, Loos and Dara [102] used a histogram of heights measured on the
surface of the material to represent its irregularity using a Weibull-type distribution function.
Pitchumani et al. [63] used a surface model of rectangles. In this work, the temperature and
pressure profiles developed in the automatic layup process were used to evaluate the evolution of the
roughness state of the material, unlike values used by other works where average estimated values in
temperature were used.
Yang and Pitchumani [103–106] proposed a representation using fractal surfaces, a model also used
in [107,108] that lead to Equation (6). This approach is based on proposing that the surface irregularity
exists on different scales. In [107] the need for re-consolidation passes on the material to achieve high
values of intimate contact is analyzed. The work concluded that at least three reconsolidation passes
are required without material input to achieve 100% degree of contact.

!2 2nD 1/5
f 2−D +n+4 t Papp
Z
1 5 hr
Dnic (t) = n[ dt + 1] (6)
f 4 Lr ( f + 1] 2 tn+1 µm f

Equation (6) is the one used for the evolution of the degree of intimate contact. D is the fractal
dimension, f the scaling factor, n the number of irregularities, Lr the total length to establish the Cantor
set, Papp the applied pressure, t the duration of pressure of the roller, ηmf the viscosity of the compound,
and hr the depth break of the first generation of irregularities found. A summary of the mentioned
surface representation methodologies is presented in [109]. The authors carry out the application of
the models of identical rectangles and fractal surfaces for the analysis of the degree of intimate contact
in polyamide (PA6) reinforced with carbon fiber. Regarding the application of fractal models, it is
indicated that with them it is possible to obtain the parameters required by the model by means of
simple profilometric measurements, an important fact compared to models that use rectangles as they
are supported by approximations with mathematical adjustments. In return, these models are not
J. Compos. Sci. 2020, 4, 149 21 of 36

always applicable to any material and after their use they show an underestimation of the degree of
real intimate contact between the two parts.
In [52] the experimental determination of the degree of contact was obtained from the analysis
of the areas with and without deconsolidation in the interfaces of the different layers of the material.
Levy et al. [110] used an optimization algorithm to extract the roughness parameters based on the
results under specific processing conditions.
In Perez et al. [111] the surface of the material is represented by means of multi-level elements.
The authors carry out a comparison of the evolution of the degree of intimate contact over time in
the automatic layup and in-situ consolidation starting from different surface finishes of the material
and under the action of different laser powers. In all the results, the material with the most stable
roughness is presented as the one that requires the shortest time to reach 100% of the degree of contact.
Similar developments were also applied to thermoset material [112]. In the case of these materials,
as it happened with thermoplastics, the temperature, the viscosity, the compaction force, and the layup
speed are the parameters that impact the result.

4.1.2. Evolution of the Surface Irregularity

Considering an initial distribution of identical rectangles on the surface of the material, with height
a0 , width b0 , and separation between them w0 , [19] uses the volume conservation equation, Equation
(7), as tool to analyze the evolution of intimate contact on the surfaces of the material once the crushing
takes place.
V0 = a0 b0 = ab (7)

As a definition for the degree of intimate contact between two surfaces, the relationship between
the final width of the irregularity or rectangle (b) over the sum of the initial width (b0 ) plus the initial
rectangle spacing is established (w0 ). In addition, taking into account the conservation of volume,
we reach Equation (8).
a0
b a
Dic = = b
(8)
w0 + b 0 1+ 0 w0

By applying the conservation of mass equations to a control volume, assuming laminar flow,
executing algebraic simplifications and estimating the force to be exerted in the unit area, the equation
that predicts the evolution of the degree of intimate contact as a function of time, temperature, pressure,
and surface finish of the material is Equation (9).

!2 1/5
5Papp
!
1 b0 a0
Dic = [1 + 1+ t] (9)
w0 + b0 µm f w0 b0

Considering that the total degree of contact is reached when Dic = 1, it is possible to calculate the
time needed to attain it as shown in Equation (10):

µm f
!2 !5
1 b0 w
tic = w0 [ 1+ 0 − 1] (10)
5Papp 1 + a0 b0
b
0

When the process conditions are non-isothermal, the integral expression to analyze the evolution
of the degree of intimate contact is given by Equation (11) [66].
!2 Z t Papp
!
1 b0 a0
Dic = w0 [1 + 5 1 + dt] (11)
1+ b w 0 b0 0 µm f
0
J. Compos. Sci. 2020, 4, 149 22 of 36

The expression shown in [63] appears simplified as Equation (12).

tb 1/5
Papp
Z
Dic = a∗ [ dt] (12)
0 µm f

Adopting a a* value of 0.29 in the case of APC2/AS4.

As can be inferred from the previous equations, the calculation requires knowledge of the viscosity
of the fiber–resin composite material. The surface of this material is primarily polymer. The viscosity
is determined as the value obtained from the zero shear rate at different temperatures, assuming that
the cutting speed does not intervene in the automatic layup process.
In the case of APC2/AS4 material, Table 6 shows the equations from different bibliography
sources. The matrix-fiber viscosities were obtained by measuring the thickness change of samples
when compressed at different temperatures in the interval of interest (340–400 ◦ C for PEEK), for a
given compaction force and time (details are given in [107]) then adjusting the values to an Arrhenius
kinetics. Significant differences happen among these equations, suggesting a strong dependence on
the tape characteristics.

Table 6. Definition of bibliographic parameters for the intimate contact degree equations.

[Ref.] µm [Pa.s] µmf [Pa.s]

h  i
Woo Il Lee, Springer 1987 [19] 1.13 ·10−10 exp 19100 h  i
T 1.14 ·10−12 exp 26300T
(Marchello, Messier, 1996) [113] PEEKh 150P
 i h  i
(Mantell, Springer, 1992) [114] 1.13 ·10−10 exp 19100
T 132.95 exp 2969 T
h  i
(Sonmez, Hahn, 1997) [65] - 132.95 exp 2969
h  T i
(Khan, Schledjewski, 2009) [107] - 643 exp 4367 T

4.2. Polymeric Chain Movement Theories of Self-Adherence

When two polymeric surfaces come into contact with each other, their temperature over their
glass transition, a diffusion of the polymer chains occurs in the interface, commonly known as healing,
diffusion, or self-adhesion. In the development of a resistant joint, a correct diffusion of the chains
must be developed so that the interface can become indistinguishable.
The basic theory for explaining the mechanism of chain diffusion at the interface is De Gennes’
theory of reptation [115,116]. A description of this theory is beyond the scope of this article; it can be
found elsewhere [117].
Moving now towards the adhesion mechanism between two surfaces of material during automatic
layup and considering chain reptation, it is necessary to take into account the movement of the
well-known minor chains [118]. Initially, a chain is surrounded entirely by a tube (topological
restrictions). For a time t1, the chain begins to leave the tube, mainly at the ends, and those initial
portions that have evacuated the tube are called minor chains. The length of the chain leaving the
tube l(t) is an increasing function over time; this magnitude will be the main control mechanism in the
development of the binding resistance.
Depending on the capacity of interpenetration of the polymer chain in the face of the material,
it is possible to develop a more or less resistant bonding, which is a direct cause of the mechanical
behavior of the joint.
The relationship of diffusion/healing is directly alluded to the mechanical properties developed
by the interface of the material, presenting the following dependencies for resistance and energy of
fracture with time [104,118] (Equation (13)) and the estimation of the value of the degree of diffusion
(Equation (14)).
σ t 1/4 G t 1/4
= ( ) ; Ic = ( ) (13)
σ∞ tr GIc∞ tr
J. Compos. Sci. 2020, 4, 149 23 of 36

σ χ l 1/2
Dh = = =( ) (14)
σ∞ χ∞ L
Likewise, those references establish a relationship between the lengths (minor chain and fully
evacuated chain) with the temperature holding times, only in isothermal conditions, with the
relationship represented by Equation (15).

l t 1/2
=( ) (15)
L tr

Combining the above equations, for the case of isothermal conditions the degree of healing can be
expressed as indicated in Equation (16), as a function of the holding time of the process conditions and
the polymer reptation time.
t 1/4
Dh = ( ) (16)
tr
The equation may be reformulated by dividing the thermal history into infinite intervals to take
into account the possible non-isothermal conditions of the process [65]. In this way Equation (17) is
obtained. The integration of the previous expression leads to Equation (18) for calculating the degree
of self-adherence.
dl dt
= p (17)
L 2 ηtr (η)
Z t 1/2
S dη
Dh = Dau = =( ) (18)
S∞ 2 ηtr (η)
p
0

An experimental verification of the healing value achieved in APC2/AS4 is carried out using a
mechanical tensile test between two parts joined under different thermal cycles in a press [19]. After the
temperature stabilization, the specimens are quenched in cold water. Based on the degree of healing
obtained, the authors are able to provide a relationship of dependency with time and temperature,
as shown in Equation (19). Note that the higher the temperature, the less time required to reach 100%
of the degree of self-adhesion. It is important to note here that the models used by the reference are
valid in the case of amorphous materials, hence the quenching of the samples.

3810 1/4
Dh = 44.1· exp ( )ta (19)
T
Pitchumani et al. [63] on the other hand, did use the models proposed by Bastien and Gillespie [118]
for the PEEK-based composite materials, estimating the degree of healing achieved by Equation (20)
when the process takes place in non-isothermal conditions.
τh
τ j 1/4 − τ j−1 1/4
1 ∆τ
1 4 X
Dh (τh ) = ( ∗ ) (20)
tr
j=1 aT T1/4
j

With: !
Ea 1 1
 
aT = exp ( − ) (21)
R T Tre f
The parameters of the equation adopt the following numerical values in the reference cited:
Ea = 57.3 kJ/mol and (tr ) = 0.11 s for the reference temperature 673 K.
More recent works [26,107] use the mathematical integral relation of Equation (23) to extract the
degree of healing through its dependence on the welding time. This equation had already been used
by Yang and Pitchumani [104,106] in their statistical analysis. Welding time is extracted for the greatest
molecular relaxation of the molten polymer and at a specific test temperature. The greatest relaxation
is found in the change from the linear to the non-linear regime in the curves obtained from a dynamic
J. Compos. Sci. 2020, 4, 149 24 of 36

rheology test. Likewise, they propose a solution for the evolution of that time with temperature based
on an Arrhenius-type dependency relationship with PEEK 150 PF (Equation (22)).

43000
 
−5
tw (T ) = 2·10 exp (22)
RT
Z t 1/4
1
Dh = ( ) (23)
0 tw

4.3. Bonding Theory

Once the degrees of intimate contact and diffusion have been obtained, it is possible to combine
their results to obtain information on the general degree of bonding.
In the work of Pitchumani et al., 1996, it is indicated that during automatic layup with thermoplastic
reinforced material, the available times for intimate contact are much shorter than those of chain
reptation or diffusion (since this mechanism it does not need an associated pressure to take place),
therefore it can evolve as long as the temperature does not freeze the movement of the chains and allows
the following simplification to be made for the degree of bonding (Equation (24)). Experimentally,
there seems to be a good correlation between the obtained degree of bonding values and the resistance
values of the test specimens to “short beam shear” (SBS).

Db (τb ) ≈ Dh (τh )·Dic (τic ) (24)

Sonmez and Akbulut [119] presented a complete algorithm to locate the best parameters in the
layup with thermoplastic material and to do it they analyzed the degree of bonding by means of
Equation (25), which is a convolution of the degrees of contact and diffusion.
Z tb Z tb −τ 1/2
dη dDic
Db ( t b ) = [ ] · dτ (25)
ηtr (η) dτ
p
0 0

Nicodeau [81] compiled models by various authors and clarified that the application of some of
them is restricted to amorphous thermoplastic polymers. In the case of semi-crystalline polymers,
not only does it present a different behavior, but it also clarifies that not reaching a perfect fusion in
the material generates a crystal remnant in the set that prevents free movement of the chains. It also
incorporates one more element into the study that gives an idea of the complexity of the process
with semi-crystalline materials, the adhesion and formation of a crystalline interface, and the effect of
co-crystallization, which makes the fracture mechanism very complex. The experimental determination
of the relaxation times is carried out using rheology tests and attending to different criteria: With the
time provided by the Carreau model in the change of tenure between the Newtonian regime and shear
thinning, with the time of the crossing of the slopes of G0 and G00 when the frequency of the dynamic
test tends to zero, and with the longest time of the relaxation spectrum.
Tierney and Gillespie [69] analyzed the development of intimate contact as a function of the layup
passes and the lamination speed. Their results show that with very high layup speeds, increasing the
consolidation passes does not impact the degree of contact but, on the other hand, it increases with the
passes when the speed decreases. They also detect that approximating the distance between the hot
gas torch and the laminate increases the value obtained from the degree of intimate contact.
In a recent study [57], which performed the layup with glass fiber reinforced polypropylene,
the equations previously exposed were also used to analyze the degree of self-injury and intimate
contact. Its purpose is to determine the minimum times necessary to reach the total degree of bonding,
highlighting the importance of the viscosity of the material in estimating this time.
Among the limitations of these models are, on the one hand, the analysis of the consolidation in
the first stage between two layers of material, which is the evolutionary process, and the involvement
J. Compos. Sci. 2020, 4, 149 25 of 36

of the bond of multiple layers impacting time after time on the lower ones. Zhao et al. [120] presents a
work that tries to cover this problem, presenting an equation for the analysis of the pressure on the nth
layer and the relationship of the degree of contact with the evolution of the layup. The work is carried
out under the assumption that viscosity of the composite material can be approximated by that of the
resin, since this is the most superficial component of the ply.
The times described above for both intimate contact and diffusion or healing can be high if
extrapolated to the industrial application of the automatic layup and consolidation process in situ,
as they result in very high conservative values.

5. Crystallization
Crystallization is probably one of the most important topics for polymer science. It is out of the
scope of this review to attempt to summarize the state-of-the-art methods. We just included some
works dealing with specific aspects of crystallization during ISC and its consequences on mechanical
properties. It is worth mentioning that, when cooled from melt, some thermoplastic polymers such as
PEEK can arrange in a partially ordered crystalline structure, called lamellae, about 10–20 nm thick
and formed by folding the polymer chain. In a bulk polymer these lamellae grow radially from a
nucleation point, creating spherical crystalline regions called spherulites. In the presence of fibers, new
phenomena appear.

5.1. Transcrystallization
Transcrystallization consists of a process of crystal growth affected by restricted space. Interfacial
crystallization, or transcrystallization, offers a new possibility to improve the interaction between
the polymer and the reinforcement in a composite material. The reinforcement acts as a nucleus that
induces crystal growth, as occurs with PEEK on carbon fiber reinforcements. The presence of the
reinforcement forces growth to take place in a direction perpendicular to the surface of the fibers, until
the crystals collide with those generated in the bulk [121].
This crystalline formation has a fundamental impact on the mechanical behavior of the material.
In the case of longitudinal properties, an improvement is reported with the interaction of the
trans-crystalline layer, since the matrix in the direction of the fiber has greater strength and stiffness
and its thermal expansion is reduced, which directly impacts on the residual stresses. Transversally,
an example is reported for glass fiber reinforced polyamide, where there is a maximum in the tensile
strength and in the modulus for cases where slow cooling leads to better transcrystalline layers.
More information regarding the effect of this layer on mechanical properties is included in the section
on the relationship between mechanical properties and crystallization.
There are several studies that analyze the crystallization phenomenon in the PEEK polymer and
in the PEEK thermoplastic matrix composite materials, for the particular process of automatic layup
and in-situ consolidation [122,123].

5.2. Crystallization and Mechanical Properties

Despite the fact that there are numerous effects conditioning the final mechanical behavior of parts
manufactured with composite materials of thermoplastic matrixes (porosity, residual stresses, etc.),
crystallization is one of the most highlighted factors in the references consulted as a key element in
the development of some mechanical or other properties [124–127]. Its findings are linked to the
thermal profiles to which the part was subjected. The references analyze the impact of the crystallinity
percentage, such as the impact of the crystal morphology and the mechanical property under analysis.
The impact of the crystallinity of the polymer on the mechanical properties requires independent
presentation for the net and reinforced polymer. In the composite material, the contribution of the
fiber as a nucleating agent and the impact of the transcrystalline layer on the result under different
mechanical stresses must be considered.
J. Compos. Sci. 2020, 4, 149 26 of 36

5.2.1. Crystallization and Mechanical Properties in PEEK

Cebe et al. [128] analyzed the mechanical behavior affected by crystallinity for the net PEEK
polymer, using tensile tests on samples that were, respectively: Abruptly cooled to obtain an amorphous
state, crystallized from the amorphous state, and crystallized at fast and slow speeds from the melt.
In addition, the tests were run at three different temperatures below the glass transition. The samples
crystallized in the conditions of slow cooling from the melt, and in all test cases a zone of plastic
behavior with the lowest values of deformation at break and resistance to final failure was present.

5.2.2. Crystallization and Mechanical Properties in Composite Material

Lee et al. [129] analyzed glass fiber and polypropylene composite materials under different cooling
profiles, drawing conclusions against different states of mechanical stress. In unidirectional traction,
the highest value is obtained in the case of lower cooling speed due to the good adhesion achieved
between resin and fiber. On the other hand, in a fracture (mode I, mode II and mixed), interlaminar
shear (ILSS), and impact, the behavior improves at a higher cooling rate. However, it should be
emphasized here that the tests were carried out with cooling programs at 1, 10, and 20 K/min, with
ranges very close to each other and not very representative of the large values observed in automatic
lamination and consolidation in-situ.
One of the causes for the variations in mechanical properties is the correct or incorrect development
of the transcrystalline layer during cooling of the material [130]. This work draws different conclusions
about the effects of applying different “annealing” conditions on samples with polyamide 6 and
polyamide 6 with continuous reinforcements of carbon fiber. Among their conclusions, they mentioned
an increased thermal conductivity with crystallization since it is a property that depends on the
vibration of the structure of the crystalline lattice.
Gao and Kim [130,131] show a correlation between crystallinity and properties such as interfacial
shear strength (IFSS) or short beam shear (SBS). According to their analysis, there is a marked difference
between specimens that have undergone cooling at 1 K/min over those that have undergone cooling at
600 K/min, reflecting a decrease both in mechanical properties and in the measured value of crystallinity
by calorimetry. The study of the fracture gap also shows a cohesive behavior when cooling was
slow and a cohesive–adhesive (matrix-open) behavior when cooling was abrupt. These same authors
extended their investigations to the analysis of the effect of crystallinity on the interlaminar fracture
toughness in laminates with PEEK and carbon fiber [132]. In mode I, the conclusions were that the
crack propagation is more stable as the cooling rate increases, as a cause of the plastic behavior of
the resin in the peel gap. Likewise, for greater cooling speeds, the crack length is also shorter for
a given opening displacement. In both failure modes, I and II, the energy decays with increasing
crystallinity, which is equivalent to increases in energy with increasing cooling speed; however, these
increases are not as high as when the net resin was subjected to these cooling profiles. Possible causes
for differences in toughness with the resin are associated with the non-plastic behavior of the fiber
and also the weak fiber-resin interface generated in rapid cooling. A third extension of the work [133]
analyzes the relationship between crystallinity and impact damage behavior in samples crystallized
in the range of 1 to 80 K/min. According to the tests carried out, laminates with a lower crystalline
percentage (higher cooling speed and smaller spherulite size) are characterized by being more ductile
and having a greater capacity to resist the onset of delamination and absorption of impact energy.
These findings were in agreement with those presented by D. Ray et al. [134]. They found that
mode I fracture toughness is 60–80% higher for the LATP (laser assisted tape placement) processed
specimens than for the autoclave processed specimens. The higher fracture toughness of the LATP
processed specimens is partially due to significant plastic deformation in the interior of plies during
the DCB (Duble Cantilever Beam) test, because of the lower crystallinity.
Not every mechanical property was improved. Regarding the tensile and flexural behavior and
the effect of crystallinity on these properties, Gao et al. published a study [135] where the results for
transverse and longitudinal specimens were shown. Except for the longitudinal traction, influenced by
J. Compos. Sci. 2020, 4, 149 27 of 36

the fiber, the other tests showed a decreasing trend with the decrease in crystallinity, and the flexural
properties were much more affected. The samples that underwent rapid cooling contained a matrix
rich in amorphous phase, unable to bear the bending load, particularly the compression component.
Furthermore, the authors reported a limit value on the cooling rate of 600 K/min, above which there
were no variations in the results.
El Kadi and Denault [136] proposed to analyze the variation of mechanical properties, both static
and fatigue, in laminates where the presence and absence of spherulites was confirmed. In this
work they alluded to other bibliographic references where it was indicated that the variation in
mechanical properties with rapid cooling is more associated with an increase in residual stresses
than with the modifications of crystalline structure, as well as the possibility of obtaining similar
crystallinity percentages with totally different crystal morphologies. In fatigue, there does not seem to
be a significant effect of the characteristics of the matrix, but, on the other hand, in static conditions it
does not occur in this way and the important effect of the fiber–matrix interface is again mentioned.
In line with the effect on the mechanical properties of crystallization, there is also an effect
of crystallinity on the glass transition and on the enthalpic relationship, as proposed by Toft [137].
The crystal–amorphous interface is indicated to have a remarkable role in the response to thermal
aging in the vicinity of the glass transition, detectable through enthalpic relaxation. Higher degrees
of crystallinity imply a greater number of chains with restriction and therefore the need for higher
temperatures to get those chains to move.

6. Thermal Degradation
The impact of thermal degradation on the consolidation of the material in its application to
the automatic wrapping and in situ consolidation process was analyzed in [138], one of the first
works to deal with this issue. The degradation analysis was carried out by analyzing the results of
interlaminar shear strength (ILSS) in test specimens manufactured under different heating conditions.
They concluded that there are two competing mechanisms governing laminate ILSS: Bonding among
layers and degradation. At very high temperatures (laminates of PEKK were exposed for a short
time to a gas torch with temperatures ranging 700–900 ◦ C) a degradation effect is induced in the
polymer, creating voids at the surface, that cannot be compensated for in the successive passes and
causing the strength values to drop. Microscopic examinations were also done. A higher void content
was found at the two extremes of the temperature interval: At low temperatures because of poor
bonding, and at high temperatures and long dwell times because of degradation. The former reference
is purely empirical, and more insight was needed to address this issue; it can be found in the next set
of references.
By definition, the thermal degradation of a polymer consists of a process such that, due to the
action of heat or high temperature, an irreversible loss of physical, mechanical, or electrical properties
occurs [139].
In the degradation process of a polymeric material, the long molecules are usually broken down
into smaller segments capable of volatilization. The lighter the fragments, the greater their capacity
to evaporate as soon as they are generated; meanwhile, the rest of the molecules will remain in the
condensed phase (liquid or solid) and will continue to undergo decomposition until the fragments are
appropriately sized. Some of the waste generated may remain in the form of carbonaceous residue,
not volatilizing. The atmosphere in which the process takes place has an important role; when oxygen
intervenes (oxidative atmosphere) it can produce changes both in the reaction rate and in the order of
the reaction. It can also decrease the minimum temperature required for degradation.
The mechanisms that apply in the thermal decomposition of a polymer are:

• Random excision of chains. Breakage occurs at apparently random positions on the chain.
• Excision at the end of the chain. Individual monomer units are successively removed from the
end of the chain.
J. Compos. Sci. 2020, 4, 149 28 of 36

• Stripped from the chain. Atoms or groups thereof are broken which are not part of the backbone
of the polymer.
• Crosslinking. Links between chains of the polymer are formed.

For manufacturing processes where it is required to raise the temperature of the polymers
approaching their degradation, it is important to analyze their thermal resistance. Hancox [140] did
a review on the main decomposition mechanisms of polymeric materials. In the particular case of
PEEK, the reference indicates that for a material with an aromatic structure, its reaction to thermal
degradation is more stable than other polymers. The work indicates that the degradation of the first
1–2% in the material takes place by means of an autocatalytic mechanism.
The works of Nicodeau [81] and Patel et al. [141] analyze the possible products obtained in
the degradation process in PEEK. The first of the works make hypotheses about the two possible
routes in which material degradation is expected to occur in an oxidative atmosphere. In the first
hypothesis, degradation is considered to take place by breaking the constituent bonds of the polymer
chain (breaking in ether or ketone bonds) and a second hypothesis is that the radicals that initiate the
reaction come from peroxides that can exist in the polymer structure (possibly generated during the
impregnation process of the material). Starting from the polymer, oxygen can act by removing the
hydrogens from the CH aromatic bonds, leaving a structure with a free position to react, generating
crosslinking and attraction between the different positions that have been left free in the chain.
The second of the works [141] studied the PEEK response to fire. In this work, the analysis carried
out on how chain linkage breaks and recombines is highlighted. In the process, both in oxidative
and inert atmospheres, there are two fundamental mechanisms where the presence of reinforcements
such as carbon fiber provide stability by slowing down the degradation process. Contrary to what
was reported by other works, the authors indicate that the process begins with the breaking of the
carbonyl–ketone bond and continues with the breaking of the carbonyl–ether bond.
The previously referenced working group also presents a PEEK decomposition analysis using
thermogravimetry [141]. The document alludes to the existence of two stages of degradation in the
decomposition process of the polymer in an oxidative atmosphere. The first stage is based on the
cleavage of the ether and ketone bonds and the second stage is associated with the oxidation of the
carbonaceous residue. In the work, calorimetry tests were developed at different speeds. With these
tests it is possible to observe that the first of the processes is not affected by speed, the same with the
second, which has a marked dependence on speed. Furthermore, in the intercomparison between the
oxidative and inert atmospheres they carry out, the behavior of the polymer reflects an early start
of degradation for the oxidative case with a difference of about 100 K compared to the inert case;
however, in the first stage of degradation in inert conditions there is a drop 10% higher than that of the
oxidative case.
In line with these observations made on the thermogravimetry curves in PEEK, Ref. [142] shows
the short temperature interval between the degradation of 5% by mass and the maximum degradation
peak of the material (this interval being the equivalent of about 10 K). This result shows that, despite
this material having a high temperature of degradation, the speed at which it occurs is very high and
once the appearance of volatiles has been generated, the evolution of polymer degradation is rapid.
The effects of degradation on samples subjected to short heating cycles are analyzed in the
works of Bayerl et al. [143] and Tsotra et al. [144]. Ref. [143] conducted a study on the possible
thermal degradation experienced by carbon fiber reinforced PEEK under the action of a laser-type
heating source (wavelength 980 nm) and temperature maintenance times of the millisecond order.
The experimental techniques used for the analysis were differential scanning calorimetry, electron
microscopy, and infrared spectroscopy by Fourier transform. Infrared spectroscopy lead to the
conclusion that decomposition begins with the breakdown of the phenyl bond, the ether bond, and
the aromatic hydrogen, with new peaks appearing that are the result of new associations of the
cleaved chains.
J. Compos. Sci. 2020, 4, 149 29 of 36

The behavior of GF/PP laminates manufactured by ISC consolidated with a CO2 laser is described
in [145]. A good mechanical and micrographic characterization is given. Thermal degradation kinetics
models and experimental characterization techniques are detailed in [146]. The analysis was applied
to a carbon fiber/PEEK composite, and a good agreement among the predictions done by the kinetics
analysis and degradation measured on samples submitted to laser irradiation was found. This paper
is a good demonstration on how to combine experimental measurements and kinetic simulation to
define the optimal processing conditions.

7. Conclusions
The in-situ consolidation process for manufacturing thermoplastic composites is a delicate balance
among the high temperatures required for local melting and healing of the surfaces of the substrate and
incoming tape, but avoiding the thermal degradation of the material. A compaction pressure is needed
to ensure an intimate contact. The roughness of the tape has a strong influence on the final quality.
The whole heating–cooling process takes a quite short time, about 10 s, over a small, moving area.
Higher taping speeds means shorter times and more difficulties. It is then understandable that, in spite
of the potential benefits of these materials, the application of this process to large serial production is
still under discussion. This article compiles the relevant literature, identifying some of the existing
issues to be addressed and models being used.

Author Contributions: Conceptualization, A.G. and I.M.; methodology, A.G.; investigation, I.M.; resources, I.M.,
A.F., D.S.d.C.; writing—original draft preparation, I.M.; writing—review and editing, A.G.; visualization, A.F.;
supervision, A.G. All authors have read and agreed to the published version of the manuscript.
Funding: This research is funded by the Institutions of the authors.
Conflicts of Interest: The authors declare no conflict of interest.

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