REVIEW PAPER

BIODEGRADABLE POLYMERS, CURRENT TRENDS OF

RESEARCH AND THEIR APPLICATIONS, A REVIEW

Maja Čolnik, Maša Knez Hrnčič, Mojca Škerget, Željko Knez

Laboratory for Separation Processes and Product Design, Faculty of Chemistry and Chemical
Engineering, University of Maribor, Smetanova 17, SI-2000 Maribor, Slovenia

Received 10.12.2019.

Revised 4.5.2020.

Accepted 6.5.2020.


zeljko.knez@um.si; Tel.: +386 2 2294 431; Fax.: +386 2 2527 774

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Abstract

Biodegradable polymers have been developed rapidly in the last years and are widely used
today in the fields of pharmacy, clinical biomedicine, cosmetic, medical, packing industries,
tissue engineering, agriculture and other areas. The interest in biodegradable polymers has been
increasing, mainly due to rising oil prices, which is the basic feedstock of plastic derived from
petroleum, and also due to the problem of the removal of waste plastics that accumulate in the
environment. Biodegradable polymers have many advantages in contrast to synthetic polymers
and can be decomposed in the environment to non-hazardous substances. Biodegradable
polymers are classified into two classes based on their synthesis i.e., synthetic and natural
polymers. They are derived either from petroleum resources or from biological resources. The
following review presents an overview of the different biodegradable polymers and their
properties, current scientific research, applications, global production of bioplastic and
replacement of conventional plastic.

Key words: biodegradable, polymers, natural origin, bioplastics

Highlights:

• An overview of the different biodegradable polymers and their properties

• The possibility of production of biodegradable plastics from renewable or non-renewable

sources

• Current scientific research, applications and global production of bioplastic has been
considered

• The properties of polymers obtained from biomass have been presented in details

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INTRODUCTION

Synthetic plastic was considered as the material of the future in the previous century, but today
it represents a major environmental problem [1]. The main disadvantages of synthetic polymers
are the lengthy decomposition process and the production based on non-renewable raw
materials. According to expert estimation, as much as 7 % of world oil and gas supplies are
used for polymers production [2]. An alternative possibility is presented by polymers that are
biodegradable or made from renewable sources. Thus, the production and use of bio-based and
biodegradable polymer materials significantly increase and consequently can contribute to
decrease of environmental problems concerning waste polymer materials [3]. Research on
renewable resources is focused on the use of corn, soy, sugarcane, potato, rice or wheat and
seeds rich in oil or fermentation products as raw materials to produce biopolymeric materials
[4]. The use of biomass to produce biopolymers has great advantage, since biomass-derived
polymers are biodegradable and relatively easy to recycle [3]. One of the main disadvantages
of biodegradable polymers obtained from renewable sources is fast degradation rate, due to
their dominant hydrophilic character and, in some cases, inadequate mechanical properties
particularly in wet environments [5]. Despite its disadvantages, biodegradable polymers offer
a wide range of advantages since many plant materials are used to make them. This means that
it is no longer necessary to use chemical fillers contained in synthetic plastic products.
Moreover, during the production cycle of biodegradable plastics, energy consumption is
reduced while the decomposition does not lead to unnecessary release of CO2 into the
environment. The use of biodegradable products could reduce dependence on fossil fuels and
thus contribute to a cleaner environment and more and more research is therefore being done
in the field of new biodegradable polymers and their improved properties.

The aim of this article is to review the recent research on the most used biodegradable
polymers, to examine their application possibilities, and the possibility to decrease or even
eliminate the usage of synthetic plastics, which have already caused major environmental
problems.

BIOPLASTIC - BIODEGRADABLE POLYMERS

Bioplastic materials are a family of materials with different properties and applications that can
be bio-based, biodegradable or both. Biodegradable plastics are made from renewable or non-
renewable sources, which are completely degraded in the environment through a

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thermochemical process into CO2, methane, water, biomass and inorganic compounds that
microorganisms can easily mineralize [6,7]. While bio-based polymers contain organic carbon
of renewable feedstock and are not necessarily biodegradable. Moreover, bio-based polymer
can be synthesized from naturally occurring materials as well as from natural substances that
have been polymerized into high molecular weight materials by chemical and/or biological
methods [8]. Bio-based materials have similar molecular structure to petrochemical polymers.
Above all, the biodegradability of a plastic materials depends on their chemical structure and
not the carbon source of the polymer [8]. According to the forecast [9,10] the global bioplastics
production capacity is set to increase from around 2 million tons in 2018 to approximately 2.6
million tons in 2023 (Figure 1) [9]. Currently, bioplastics represent about 1 % of 335 million
tons of plastic produced annually. Bioplastics are an increasing, innovative industry that offers
solutions for a sustainable plastics economy and that plays a key role in the transformation to
a bio-based circular economy [9,10]. Yet, despite these advantages, the data shows that the
overall growth of the global bioplastics industry is currently being slowed down by the low oil
prices and a lack of political support for the bio-based economy [9,10].

Figure 1:

Bio-based, non-biodegradable plastics, currently make up for around 48 % (1 million tonnes)

of the global bioplastics production capacities (Table 1) [9]. Just like for the bio-based
polymers, the global production of biodegradable polymers also increases (Table 1). The
production of PLA (polylactic acid) and PHA (polyhydroxyalkanoates) is currently growing.
Regarding to the global production capacities of bioplastic by material type, PLA share is
predicted to increase from 10.3 to 13.2 %, while the PHA share is projected to increase from
1.4 to 5.8 %. The production of other biodegradable polymers should remain the same or
decrease [10].

Table 1:

In the following, biodegradable polymers are classified as either bio-based or petrochemical-

based. The material is mostly biodegradable by nature and produced from biomass (plants,
animals or microorganisms) such as polysaccharides (e.g. starch, cellulose, lignin and chitin),
proteins (e.g. gelatine, casein, wheat gluten, silk and wool) and lipids (e.g. plant oils and animal
fats) [11,12]. The major natural polymers are starch, cellulose and soy protein. Natural rubber
as well as certain polyesters either produced by microorganism or plant (PHA) and poly-3-

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hydroxybutyrate (PHB) or synthesized from bio-derived monomers (PLA) fall into this
category [11,12]. Petrochemical-based biodegradable polymers such as aliphatic polyesters
(e.g. polyglycolic acid (PGA), polybutylene succinate (PBS) and polycaprolactone (PCL)),
aromatic copolyesters (e.g. polybutylene succinate terephthalate (PBAT)) and poly(vinyl
alcohol) (PVA) are produced by synthesis from monomers derived from petrochemical
refining, which possess certain degree of characteristic biodegradability (Figure 2) [11,12].
Particularly, PBS is already industrially produced from renewable resources by PTT MCC
Biochem Company and it is called BioPBSTM.

Figure 2:

Furthermore, the latest research on the most common biodegradable polymers, the addition of
copolymers, additives or fibers, which can improve the mechanical and physical properties of
polymers and possible applications of biodegradable polymers are shown in Table 2-9.
Thermoplastic starch (TPS) is still the most widely used material for the research and
production of biodegradable polymers. Namely, TPS has been the first biopolymer on the
market, but currently two groups of biodegradable polymers have the highest market potential.
The first is polylactic acid (PLA) produced by fermenting carbohydrates and the second
important group of biodegradable polymers are polyhydroxyalkanoates (PHA) synthesized
through bacterially guided fermentation processes. Their products are widely used in different
fields.

POLYMERS OBTAINED FROM BIOMASS

Starch
Starch is the major form of carbohydrate storage in green plants and is considered as the second
largest biomass produced on earth. Starch is a cheap and easily available raw material, which
is present in large quantities in potatoes, maize, rice and wheat [4,13]. In natural form, starch
is not meltable and cannot be processed as thermoplastic [14]. Starch granules can be
thermoplasticized through a gelatization process, where the granules are disrupted and the
ordered crystalline structure is lost under the influence of plasticizers, shears and heat [14]. The
resultant melt-processable starch is called thermoplastic starch (TPS) [15].
Bioplastics based on starch are suitable for the production of packaging, in agriculture, for
medical and cosmetic application [16-19]. Due to its low cost and high availability [20], starch

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attracts the increasing attention and interest of researchers and industries worldwide. Xie et al.
[21] studied a new completely biodegradable sisal fiber–starch packing composites, which
exhibited good biodegradability. This composites showed a promising replacement for
expandable polystyrene (EPS) as packing material, especially under large compression load
[21] (Table 2). In comparison to sisal fiber, which is the most used natural fiber on the world,
also cassava starch is usually used as matrix material. In addition, Medina-Jaramillo et al. [22]
investigated the active and smart biodegradable films from cassava starch and glycerol with
different natural extracts such as green tea and basil by casting. The high content of phenolic
compounds in the extracts significant antioxidant activity of the films. The films were
thermally stable up to 240 °C and degraded in soil in two weeks [22]. Other researcher the
cassava starch combined with biomass or biomass extract of microalgae Heterochlorella
luteoviridis and Dunaliella tertiolecta [18]. Incorporation of microalgae biomass resulted in
biodegradable and highly soluble films, making it difficult to apply in moist foods while the
films which contains 2.0% of H. luteoviridis extract were appropriate for application in foods
with high water content [18]. This prepared biodegradable films with antioxidant properties
can used for salmon packaging, as they provide protection against lipid oxidation [18]. Several
researchers investigated the use of starch and chitosan in the production of biofilms. Chitosan
is nontoxic, biodegradable and has antimicrobial activity [23]. Thus, chitosan as biopolymer
has a wide range application in drug delivery systems, in the areas of biomedicine, membranes,
hydrogels, adhesives, fuel cells, as a surface conditioner, for tissue engineering, etc. [24]. It has
also shown a great potential for removing pollutants from water and wastewater [25]. Besides,
chitosan is a promising material to produce food packaging materials and in comparison to
starch due to its more hydrophobic nature represents an attractive combination of price,
abundance and thermoplastic behavior [23]. Further, the researchers were successfully prepare
mixtures of corn starch (TPS) and chitosan (TPC) by extrusion and they produced more
thermally stable films with potential in the packaging industry [23].
Rice and maize are another widespread raw materials in the manufacture of biodegradable
films [26]. The biodegradable films from the hydroxypropylated rice starch (HPRS) provided
an increase in elongation at break, water vapor permeability, film solubility and transparency,
while the tensile strength value decreased when the propylene oxide proportion increased [26].
Lopez et al. [27] studied the mechanical properties, oxygen permeability and water vapor as
well thermo-sealing capacity of composite films from thermo-compressed films of TPS with
talc nanoparticles. By addition of talc (3% w/w) to TPC the water vapor and oxygen
permeability have reduced [27].

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Tacca leontopetaloides, also known as Polynesian arrowroot starch, is a wild perennial herb
[28]. This starch is an important food source for many Pacific Island cultures [28]. The potential
of T. leontopetaloides starch plasticized using glycerol and crude palm oil (CPO) were
investigated by Makhtar et al. [28]. The mixture becomes highly thermally resistant up to 430
°C when it is plasticized with CPO. The thermal behavior of glycerol TPS was quite similar to
the conventional bioplastic what supports the utilization of T. leontopetaloides starch for
bioplastic development [28]. In further study, starch was used also for other applications.
Namely, the disposed pressure-sensitive adhesive tape widely used in daily life has been
contaminating the environment and has produced the vastly non-degradable trash. Czech et al.
[29] studied the advanced biodegradable pressure-sensitive double-coated tape containing
starch carrier and water-soluble partially degradable modified pressure sensitive adhesive.
They observed the excellent tack and peel adhesion of these newly constructed biodegradable
self-adhesive tapes, and high thermal shear strength [29]. The complete biodegradability of
starch carrier and partial biodegradability of modified acrylic PSA were confirmed [29]. This
environmentally friendly technology based on the starch has great potentials for diverse
applications such as the paper industry for manufacturing of ecological biodegradable product,
the production of water-soluble biodegradable labels, medical tapes and biomedical electrodes
[29].
New research has confirmed that starch is a highly effective natural source and depending on
the starch source and processing conditions, a thermoplastic material with different properties
suitable for various applications and industries can be produced.

Table 2:

Cellulose
Cellulose is the most widespread natural organic polymer, representing about 1.5 × 1012 tonnes
of total annual biomass production and is considered an almost non-exhaustive source of raw
material for increased need for environmentally friendly products [30]. The primary source of
cellulose is the existing lignocellulosic source in forests [30]. Commercial cellulose production
is focused on sources such as wood and naturally very pure cotton source [30], [31]. Cellulose
fibers are used to produce biodegradable packaging materials, in cosmetic products without
synthetic polymers or strong composites together with biodegradable plastics [32]. Cellulose
derivate that have been used in bioplastic synthesis were cellulose nano crystals (CNC) [31],
nanofibrilated cellulose (NFC), cellulose acetate butyrate, cellulose acetate and bio-PE [32].

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Derivate of the cellulose was mixed with other biopolymers matrix in order to improve physical
properties or as a filler, such as starch and PLA [31]. NFC has an incredible potential as
reinforcement material in nanocomposites for many different uses, such as foams and
adhesives. Missoum et al. [33] prepared NFC and their derivatives with using three chemical
surface modification strategies. Antibacterial activities of all samples were investigated against
two kinds of Gram+ bacteria (Staphylococcus aureus) and Gram- bacteria (Klebsiella
pneumoniae) [33]. They also strongly enhanced the photo-catalytic antimicrobial effect of TiO2
additive (Table 3). This study shows that it is better to use grafted NFC either alone or
functionalized with TiO2 if anti-bacterial properties are desired [33].
The cellulose backbone is known to be easily biodegradable in different biodegradation
conditions and environments [33]. Also, biocomposites based on natural cellulose fibers (CF)
and hydroxyethyl cellulose (HEC) were produced in the form of green packaging films [34].
The effect of the different single-component plasticizers on the mechanical and dynamic
thermomechanical properties of the films was investigated. [34]. Moreover, the softening effect
of the two-component plasticizer based on deep eutectic solvents (DESs) was addressed. It was
found that DESs are a highly promising plasticizers for the cellulose-based biocomposites with
similar or even better plasticizing effect compared to conventional plasticizer [34].
In the following, cellulose was also used as material for new type of biodegradable cigarette
filters to accelerate their disappearance after disposal. About 4.5 trillion cigarette butts are
discarded every year. Joly et al. [35] compared the decomposition of cellulose and plastic
cigarettes filters, either intact or smoked, on the soil surface or within a composting bin over a
six-month field decomposition experiment [35]. It was found that conventional plastic filters
take 7.5-14 years to disappear, in the compost and on the soil surface, respectively in contrast
to cellulose filters, which take 2.3-13 years to disappear, in the compost and on the soil surface,
respectively. [35].
Sugarcane bagasse was fractionated to cellulose, hemicellulose and lignin by a proprietary
steam explosion process followed by downstream purifications [36]. The cellulose was
acetylated under heterogeneous conditions to obtain cellulose acetates. The novel feature of
this study was the utilization of the hemicellulose of bagasse as an internal plasticizer [36]. The
results show how lignocellulosic agricultural wastes can be utilized to produce high value
plastics [36].
Wu et al. [37] studied a facile way to prepare highly transparent antimicrobial films by grafting
chitosan as copolymer onto the oxidized cellulose matrix had a high transparent property of
above 80% transmittance, excellent antioxidant activity and antimicrobial properties against

8
Escherichia coli and Staphylococcus aureus [37]. Using a sausage model, it was shown that
the composites exhibited better performance than traditional polyethylene packaging material
and demonstrated good potential as food packaging materials [37].
Empty fruit bunch (EFB) is available abundantly in Indonesia as side product of CPO
production [38]. Potential cellulose amount from EFB is 11.50 million tons [38]. For that
reason, Isroi et al. [38] investigated bioplastic production based on cellulose from EFB.
Cellulose was isolated by sodium hydroxide methods and bleached using sodium hypochlorite.
Purity of obtained cellulose was 97 %. For bioplastic synthesis glycerol as plasticizer and
cassava starch as matrix were used. In this research bioplastic sheets were successfully
produced by casting method. In future prospects, bioplastic from EFB cellulose can be used
for plastic bags and food packaging [38].

Table 3:

Soy proteins
Soy is cheap, and renewable source of biopolymers, which has a great potential to replace
petrochemical polymers in many applications. Soy protein (SP) is commercially available in
three various SP concentrations: soy flour (54 %), soy concentrate (65-72 %) and soy isolate
(90 %) [39].
Molecules of SP include 20 different amino acids with strong inter and intramolecular
interactions. Such interactions make SP unmeltable and therefore it is impossible to process SP
in the form of a thermoplastic polymer, unless a sufficient amount of plasticizer is used [40,41].
The use of a significant amount of plasticizers results in low mechanical properties of SP
plastics. On the other hand, when the plasticizers migrate away from the SP plastics during
storage or service, the materials become very brittle [40,41]. Moreover, the hydrophilicity of
SP and the plasticizers leads to low moisture resistance of SP plastics. Blending of SP polymers
with biodegradable polymers is a natural choice to overcome the said lack of SP-based
polymers. The polymers used for mixing with SP are hydrophobic and therefore cannot
establish a strong bond with SP and a compatibilizer such as maleic anhydride is required in
the mixture [40,41]. By adding it in a smaller amount, it is possible to improve the mechanical
properties, the resistance to moisture and the viability due to the increased interactions within
their compounds [40,41].
Many reports have been published about biomedical applications of pure SP or blending with
other polymers or macromolecules [42–49]. SP also is used in infant formulas and in baked,

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meat, and dairy products [50]. The use of SP as a film-forming agent can add value to soybeans
by creating new channels for marketing SP [51].
Tulamandi et al. [52] found that with the addition of gelatin to the papaya puree, the films have
shown significant increase in color properties, tensile strength and seal strength [52].Whereas,
with the addition of defatted SP along with gelatin to the papaya puree, the films have shown
significant increase in elongation, water permeability, water contact angle and decrease in
water solubility (Table 4).
Non-biodegradable polyvinyl alcohol (PVA) derived from petroleum is the primary sizing
agent due to its excellent sizing performance on polyester-containing yarns, especially in
increasingly prevailing high-speed weaving [53]. However, due to the poor biodegradability,
PVA causes serious environmental pollution, and thus, should be substituted with more
environmentally friendly polymers [53]. Because of reason, Yang et al. [53] developed soy
sizes from SP treated with glycerol and the biodegradable triol that was also obtained from soy.
It was observed that the soy sizes had good film properties, adhesion to polyester and abrasion
resistance close to PVA. In summary, the fully biodegradable soy sizes have potential to
substitute PVA for sustainable textile processing [53]. Also Zhao et al. [54] grafted soy protein
with acrylic acid and cast into biodegradable films as substitutes of non-biodegradable PVA
films. Acrylic acid grafting provided SP films with biodegradability, flexibility, and adhesion
to yarns substantially higher than PVA, while water solubility and abrasion resistance similar
to PVA, leading to high potential applications of the grafted SP in the fields of water soluble
packaging films and slashing to substitute PVA [54].
Reddy et al. [55] developed completely biodegradable SP composites reinforced with jute
fibers with used water without any chemicals as plasticizer. It was found that the SP composites
developed have excellent flexural strength, tensile strength and tensile modulus, much higher
than polypropylene (PP) composites even at high relative humidity (90 %) [55].
Soy protein isolate (SPI) seems to be an adequate resource for the manufacture of natural-based
superabsorbent materials due to its hydrophilic character and excellent processability when
combined with a plasticizer [56]. Yu et al. [57] studied SP-based films incorporated with CNCs
and Cedrus deodara pine needle extract (PNE) for potential food packaging material. When a
high content of PNE was incorporated in the films, the water vapor permeability was decreased
due to the reduction of hydrophilic domains in the film matrix. Moreover, the PNE-added films
contained phenolic compounds and displayed strong antioxidant activities [57]. In the
following, Carpiné et al. [58] presented an alternative by incorporating virgin coconut oil
(VCO) (hydrophobic component with good oxidative stability) into SPI films. In addition, as

10
natural surfactant, the Yucca schidigera (YS) saponin was applied. Morphological analyses
indicated that the incorporation of VCO or Yucca extract caused notable changes in the
structure of the SPI films. Therefore, these data should help to better understand the role of
lipids and surfactants in protein-based films for future industrial purposes [58]. Jiménez-
Rosado et al. [56] studied the SP-based bioplastic matrices which were loaded with zinc
sulphate monohydrate for potential applications in horticulture. It was confirmed that
significant amounts of an essential micronutrient for a plant (Zn) can be incorporated into
bioplastic matrices, modifying water absorption, mechanical and microstructural properties
[56].
For medical purposes Tansaz et al. [59] investigated the fabrication of SP isolate/nanoscale
bioactive glass composite films by solvent casting method as a matrix for wound-dressing
applications. The effect of the addition of bioactive glass nanoparticles on blood clotting was
assessed [59]. The composite films could meet the essential requirements for an appropriate
wound dressing with additional favorable properties such as hemostatic capability, mechanical
properties and significant cell cytocompatibility [59].
Table 4:

BIODEGRADABLE POLYMERS OBTAINED VIA MICROBIAL PRODUCTION

Polyhydroxyalkanoates (PHAs)
PHAs are classified as a natural aliphatic biopolyesters, synthesized by many different bacteria
as intracellular carbon and energy storage materials.
PHAs have the ability to combine more than 150 monomers to produce materials with very
different properties and functionalities [60,61]. Mechanical and biological compatibility can
be altered by mixing, altering the surface, or by combining PHA with other polymers, enzymes
or inorganic materials, allowing them a wider spectrum of use [60]. The main areas of PHA
use include packaging (containers and films), coatings, pharmaceutical and medical
applications (wound dressings, medical devices, orthopedic pins, stents, nerve guides and bone
marrow scaffolds). Besides, PHAs are used as hardeners in cosmetic products, hygiene
products, toners and adhesives, electronic issues and golf balls [62]. PHA plastics are in
contrast to other types of bioplastics (eg. PLA), UV stable, can withstand temperatures up to
180 °C and are poorly water-permeable [60].

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Some specific forms of PHA are not present only in microorganisms, but are also found in
plants, animals, and even in humans as a component of membrane tissues in the form of
polyhydroxybutyrate (PHB), which is the most representative member of this family [63]. PHB
is a rare example of a hydrophobic polymer that is biocompatible and biodegradable. It has a
high melting point (170-180 °C) and a crystalline degree close to 80%. PHB is rigid and brittle,
the degree of fragility being dependent on recrystallization, the glass transition temperature,
and the microstructure of the polymer. The longer the time of its storage, the more fragile it
becomes. Thermal instability during continuous polymer processing at high temperatures and
the tendency to crack and fracture limits its wider use. The combination of high crystallinity
and low density of nucleation sites is reflected in the formation of large spherulitic crystals that
influence the spread of cracks and the fragility of the material. In order to improve mechanical
and thermal properties, different nucleation agents are added. Among the most common
procedures for the modification of the original properties of PHB, it is certainly the mixing of
the basic polymer component with other polymers or with additives. PHB can be processed
using conventional technological processes for the processing of plastics, which makes its use
widely available [64,65].
PHAs have emerged as highly promising biomaterials both for bulk and biomedical
applications (Table 5) [66]. Wound management, coronary angioplasty, nerve regeneration,
bone tissue engineering, cardiac tissue engineering and drug delivery are some examples of
biomedical applications where PHA-based materials have been explored [67]. PHB has been
found to have low toxicity, since it degrades in vivo to d3- hydroxybutyric acid, a normal
constituent of human blood. Applications of these polymers previously tested or in phase of
development include controlled drug release, artificial skin, and heart valves as well as such
industrial applications as paramedical disposables [68,69]. Subsequent applications in the
packaging and cosmetic industries included the production of a wide variety of bottles, tubs,
bags and wrappings.
Progress in tissue engineering is dependent on the availability of suitable biomaterials. To
overcome the brittleness of poly(3-hydroxybutyrate) P(3HB), and widen its biomedical
applications, plasticizing of P(3HB) with oligomeric substances of related structure was
investigated by Lukasiewicz et al. [66]. A biosynthesized medium-chain-length
polyhydroxyalkanoate (mcl-PHA) copolymer, the plasticizer precursor, was obtained using
vegetable waste frying oil as a sole carbon source [66]. Addition of oligomeric mcl-PHA to
P(3HB) resulted in softer and more flexible materials based entirely on PHAs. The proposed
approach for P(3HB) plasticization has the potential for the generation of more pliable

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biomaterials based on P(3HB) which can find application in unique soft tissue engineering
applications where a balance between stiffness, tensile strength and ductility is required [66].
The biodegradability, mechanical properties and fabrication of three-dimensional (3D) printing
filaments of composite materials made from maleic anhydride-grafted polyhydroxyalkanoate
(PHA-g-MA) and coupling agent-treated palm fiber (TPF) were studied by Wu et al. [70]. TPF
was successfully combined with PHA-g-MA by an esterification procedure and 3D printing
filaments were fabricated from the composites [70]. The strong interaction of the PF with the
PHA matrix in the PHA-g-MA/TPF composites led to improved tensile properties and had
lower water absorption than the corresponding PHA/PF membranes, and the aqueous release
solutions had good cell viability [70]. When incubated in soil, the biodegradation rate of PHA-
g-MA/TPF was lower than that of PHA/ PF, while still higher than that of pure PHA. Due to
their low cost and excellent characteristics the prepared composites can be used as the
biodegradable material of 3D printing filaments [70]. In order to improve properties and cost
reduction Godbole et al. [71] studied the compatibility of PHB with starch. The results revealed
that blend films had a single glass transition temperature for all the proportions of PHB and
starch tested [71]. The nature of all combinations was found to be crystalline. This blend films
might also be used as a coating material on paper or cardboard used for food packaging [71].
Garcia-Garcia et al. [72] explores the potential of vegetable oil‐derived plasticizers (maleinized
linseed oil) and an epoxidized fatty acid ester as environmentally friendly solutions for P3HB
industrial formulations with improved toughness [72]. The optimum balance between ductile
properties is achieved with low plasticizer content for both plasticizer types [72].
Andler et al. [73] studied the biosynthesis of PHA utilizing poly(cis-1,4-isoprene) as sole
carbon source in order to find recycling methods for rubber waste materials and alternative
carbon sources for the synthesis of PHA [73]. Costa et al. [74] demonstrated that the methods
used for extracting PHAs from the cyanobacterium Spirulina sp. LEB-18 show different
efficiencies in the extraction of the polymers. The use of sodium hypochlorite in the
initial extraction stage increases polymer accumulation, while the use of methanol at the end
of the process is important for obtaining higher purity PHAs [74]. The extraction methods
significantly influenced the molecular mass, degree of crystallinity, and monomeric
composition of PHAs, showing that the extraction method is critical in obtaining polymers with
desired characteristics for industrial applications [74]. The PHAs extracted from
the Spirulina sp. were composed largely of the 11-hydroxyhexadecanoate monomers and
hydroxytetradecanoate, which is a scientific novelty because these building blocks are
constituents of completely new polymers [74]. Further, in the study of Soon et al. [75] the

13
nanocellulose and chitosan were incorporated into the PHA composite with use of Pickering
emulsion-electospining method and the material was then tested as adsorbent for removal of
dye from industrial wastewater. The results showed that dye (Congo red) removal percentage
in the case of nanocellulose addition was much better (30.9%) than in the case of chitosan
addition (10.5%) [75]. In the work of Perez-Arauz et al. [76] for the first time peanut oil as a
carbon source for production of PHA films was used. The novel PHA films showed positive
mechanical, physical and barrier properties so the material could be suitable for food packaging
applications and in the biotechnology industry [76]. Xu et al. [77] created the well-designed
multifunctional and robust PHA/ GO-g-LAQ (long alkyl chain quaternary salt functionalized
graphene oxide) nanocomposites with superior gas barrier, heat resistant inherent antibacterial
performances, which could be ideal for eco-friendly food packaging [77].
The influence of the coconut fiber used as reinforcement in PHB composites was studied by
da Silva Moura et al. [78]. The microstructure showed a good interfacial adhesion between the
PHB and coconut fiber [78].

Table 5:

BIODEGRADBLE POLYMERS CHEMICALLY SYNTHESIZED USING

MONOMERS OBTAINED FROM AGRO-RESOURCES

Polylactic acid (PLA)

PLA is a synthetic biodegradable polyester with monomer, lactic acid (LA), derived from
natural resource. The most used raw material is maize or other industrial plants with high starch
content. In the fermentation processes of hydrocarbons Lactobacillus lactic acid bacteria or
fungi Rhizopus oryzae are used. The fermentation process requires the presence of bacterial
strains and sufficient amounts of carbon (glucose, sucrose or lactose), nitrogen (yeast extract,
peptides), and mineral elements for their active functioning. The final product of bacterial
synthesis is an optical isomer of lactic acid L- (+), which can be converted to polymeric form
of poly (L-lactic acid) (PLLA) of low molecular weight in subsequent polycondensation
reactions. The properties of the PLA depend on its molecular structure, crystallinity, the size
of the spherulitic crystals, the morphology, and the level of arrangement of the polymer chains.
The stereochemical structure of PLA determines its crystalline arrangement. Depending on the
selected synthesis polymerization processes, the final form of the PLA can be completely
amorphous (with 50-93% content of L-lactic acid) or semicrystalline (with > 93% content of

14
L-lactic acid) [79,80]. The glass transition temperature of the PLA homopolymer is 55 °C and
the melting temperature is about 175 °C. Under controlled composting conditions, the material
is completely biodegradable and can be processed using standard plastics processing
techniques. To improve process properties, lactide is often copolymerized with an enantiomer
of the opposite configuration. This represents a copolymerised form of PLA, referred to poly
(DL-lactide) (PDLLA) [4,81].
The use of PLA polymers has great potential for automotive and packaging industry and
medicine. It can be used in the production of flexible and waterproof films, bottles, labels and
cups, bakery packaging and disposable dishes. In biomedicine it is used as a binding material
in tissue engineering [81]. However, its poor thermal stability, rigidity, intrinsic brittleness,
low crystallization rate and high cost, limits its large-scale applications [82]. The introduction
of Boron Nitride (BN) as a reinforcement inorganic material in PLA may significantly improve
their properties, making them more suitable for packaging electronic products. Namely, BN
has superior thermal conductivity and mechanical properties. The prepared PLA/BN composite
material has improved mechanical properties and it is suitable for packaging in industries
(Table 6) [83]. D'Amico et al. [84] prepared biodegradable polymeric blends based on poly(3-
hydroxybutyrate) (PHB) and PLA by melt mixing. They concluded that plasticized PHB/PLA
(30/70) and PHB/PLA (40/60) blends, may be considered a sustainable alternative to current
non-natural and non-biodegradable materials for food packaging films considering their
flexibility, transparency, possibilities for processing at the industrial level and compostability
in terms of their final disposition [84]. The composite film by embedding nanochitosan in a
PLA matrix using polyethylene glycol (PEG) as a cross linking agent and PVA as plasticizer
were developed by Fathima et al. [85]. The interactions between the PLA/NCS and PEG had a
significant effect on the tensile strength and the heat-sealing properties. Antimicrobial
properties of PLA/NCS films have been confirmed against aerobic microorganisms and
consequently the PLA/NCS composite films can be used for packing of fresh prawn to increase
its shelf life [85]. Arrieta et al. [86] prepared a flexible electrospun PLA-PHB biocomposites
with chitosan or catechin as active film materials. Due to well-known antioxidant activity of
both loaded components and good qualities of PLA-PHB biocomposites, this are promising
materials for biodegradable film applications (agricultural mulch films, films for food
packaging) [86]. In a brand new invitro study, Abasian et al. [87] have successfully
incorporated the NaX/Fe3O4 nanoparticles and doxorubicin (DOX) into the PLA/chitosan
nanofibers. These prepared nanofibers show excellent potential in the local chemotherapy of

15
carcinoma tumors. Namely, invitro studies have shown that the maximum killing percentage
of the human carcinoma cells was 82% after 7 days [87].
Swaroop et al. [88] produced the biofilms by reinforcement of magnesium oxide (MgO)
nanoparticles in PLA biopolymer using the solvent casting method. PLA/MgO films exhibited
superior antibacterial efficacy and they caused progressive damage and death of nearly 46% of
E. coli bacterial culture after 12 h treatment [88]. The produced films are transparent, capable
of screening UV radiations and exhibit superior antibacterial efficacy what makes them an
excellent food packaging material [88].
Moreover, the researchers investigated the effect of cardanol-based compatibilizers, which can
react by reactive extrusion with PLA and ABS (acrylonitrilebutadiene-styrene). The modified
chains of both PLA and ABS with cardanol derivatives during reactive extrusion would
intersperse between PLA and ABS, reducing the interfacial tension and improving the
interfacial adhesion, leading to the outstanding compatibilization of the blend [89]. For medical
application Zheng et al. [90] co-encapsulated verapamil and DOX in methoxy poly (ethylene
glycol)-poly (l-lactic acid) (MPEG-PLA) nanoparticles to reverse the drug resistance in ovarian
cancer [90]. These MPEG-PLA nanoparticles reveal high biocompatibility and superior safety.
They also demonstrated the enhanced anticancer effects of verapamil and DOX loaded
nanoparticles, with a sufficient evaluation of safety in vivo [90].

Table 6:

BIODEGRADABLE POLYMERS DERIVED FROM PETROLEUM

Polycaprolactone (PCL)
PCL is a semi crystalline aliphatic polyester, which is well known for its slow biodegradation
rate and high biocompatibility. PCL is produced by ring-opening polymerization of ε-
caprolactone in the presence of various anionic and cationic catalysts [91]. Due to its slow
biodegradation, it is suitable for production of prolonged-release delivery systems. The
decommissioning takes place over two phases. First, the hydrolytic cleavage of the ester bond
is carried out, and in the second phase, intracellular degradation occurs into the non-toxic
metabolites that are excreted directly from the body or after the metabolic change in the Krebs
cycle [91]. Unlike most other biodegradable polyesters, PCL locally does not lower the pH in
the area of its degradation [91].

16
The main problem is its hydrophobicity, which can be solved by combining it with other natural
or synthetic polymers, thus improving its mechanical properties and biocompatibility [92].
Besides, PCL has low glass transition (− 60 °C) temperature and low melting (60 °C) point but
presents an ideal biodegradable matrix for natural antimicrobial agents as it can be processed
at low temperature. Moreover, the toughness of PCL is superior to than most biodegradable
polymers. On the other hand, lower modulus and rigidity of PCL limit its many applications
[93]. High molecular weight PCL is not suitable as an oxygen barrier material. Despite many
attractive properties (slow degradation rate, high permeability, easy availability and good
mechanical properties), the applications of PCL have also been limited by its relatively high
cost [94,95].
Nevertheless, PCL is very common in the production of food packaging and because of its
excellent biocompatibility it is explored as a structural material in tissue engineering (eg.
microstatic PCL foams are used for tissue regeneration and stem cell transplantation) [96].
PCL has been repeatedly and successfully used for the production of nanofibers [97]. Choi et
al. [98] was among the first that produced nanofibers from PCL/collagen for cell regeneration
of skeletal muscles [98] (Table 7). Zamani et al. [99] successfully incorporated metronidazole
benzoate (MET) in PCL nanofibers for periodontal diseases [99]. In the work of Potrč et al.
[100], PCL nanofibers were incorporated in water-poorly soluble agents such as resveratrol,
carvedilol and ibuprofen, thereby enabling prolonged release from the delivery form [100].
Zupančič et al. [101] produced PCL nanofibers with built resveratrol in order to treat
periodontal disease [101]. Sessini et al. [102] studied the influence of the addition of polyester-
grafted-cellulose nanocrystals on the shape memory properties of biodegradable PLA/PCL
nanocomposites [102]. Joo et al. [103], biocompatible biodegradable PU/PCL blends were
obtained by blending. Such polymer blends with suitable mechanical properties and shape-
memory behavior can be used in surgical sutures or other medical devices [103]. Xu et al. [104]
studied the feasibility of utilizing PCL as biocompatible and biodegradable binding agent to
fabricate electrospun three-dimensional (3D) scaffolds. The obtained 3D scaffolds are soft
while elastic, and they possess interconnected and hierarchically structured pores with sizes in
the range from sub-microns to hundreds of microns; hence, they are morphologically similar
to natural extracellular matrices (ECMs) thus well suited for cell functions and tissue formation
[104]. These various thermoplastic polymers could be fabricated into 3D nanofibrous
scaffolds/structures by first making blend nanofibers with PCL followed by processing via the
thermally induced (nanofiber) self-agglomeration (TISA) method and finally being thermally
stabilized [104].

17
Table 7:

Poly (butylene) succinate (PBS)

PBS is synthesized by the polycondensation reaction between succinic acid and butanediol.
The reaction takes place in two steps. In the first part of sintering the esterification takes place
between the diacids and the diols. Then, polycondensation takes place under high temperature
conditions to form high molecular weight PBS [105].
PBS has a relatively low biodegradation rate due to its high crystallization rate and high
crystallinity. It has good thermal stability and mechanical properties. Furthermore, PBS
naturally decomposes to nontoxic and into harmless products such as water and CO2 [106]. To
promote the physical properties, to extend the application field, and to increase the
biodegradability of PBS, numerous approaches have been used, such as physical blending,
copolymerization, or formation of composites. Owing to the excellent processability of PBS,
it can be processed using conventional polyolefin equipment in the range 160-200 ºC. Injection,
extrusion or blow molding are suitable for processing of PBS [107].
The applications of PBS are still increasing in many areas. In the field of packaging, PBS can
be processed into foils, bags or food and cosmetic packaging. In agriculture, PBS is used to
produce mulching foils or delayed release materials for pesticides and fertilizers. PBS is also
increasingly used in fishing materials, forestry, construction, or other areas where processing
and recycling of materials is problematic [106]. In the medical field, PBS can be used as a
biodegradable drug for encapsulation systems and is also investigated for implants [108].
Production of PBS is more expensive than of synthetic polymers hence it can be mixed with
cheap natural fibers or fillings (wood). Jiang et al. [109] prepared wood plastic composite,
where were the CaCO3 as a reinforcing component, and aluminum hypophosphite,
ammonium polyphosphate and calcium hypophosphite as a flame-retardant component were
separately incorporated into PBS matrix. The investigation of mechanical and thermal
properties of PBS composite, can present a foundation for development of various application
of PBS composite in different fields [109] (Table 8). Shi et al. [110] studied the preparation,
characterization, and biodegradation of PBS/cellulose triacetate (CT) blends. PBS and CT were
blended with different ratios using chloroform as a solvent. This finding indicated good
hydrophilicity [110]. The weight loss became close to 90% after 16 h of degradation for
PBS/CT10 [110]. Therefore, the blend economized the PBS material, was environment
friendly, and showed preferable solid-state properties [110].

18
Sun et al. [111] investigated non-isothermal crystallization of biopolyesters of PBS formed via
in-situ polymerization in presence of poly(vinyl butyral) (PVB). The effects of the PVB content
and molecular weights on non-isothermal crystallization and mechanical properties were
examined in detail [111]. Adding PVB greatly reduced spherulitic sizes and increased the peak
temperature of crystallization [111]. An optimal content was observed for a minimal size of
spherulites, and the PVB with a low molecular weight led to a smaller spherulitic size than did
its counterpart of a high molecular weight [111]. A molecular model was proposed to explain
accelerated nucleation and spherical growth from PVB's structural perspective. The nucleated
PBS exhibited a considerable improvement in mechanical properties [111]. The design and
synthesis of a new PBS ionomer containing a novel bisfunctional phosphinate monomer named
kalium salt of 10H-phenoxaphosphine-2,8- dicarboxylic acid,10-hydroxy-,2,8-dihydroxyethyl
ester,10-oxide (DHPPO-K) was studied by Xu et al. [112]. PBS ionomers contain aromatic
cationic groups content was synthesized by condensation polymerization of succinic acid and
1,4-butanediol in the presence of DHPPO-K [112]. The crystallization properties, rheological
properties, dynamic mechanical properties, oxygen permeability, thermal conductivity and
physical properties were thoroughly investigated considering their structure-property
relationships [112].
PTT Public Company Limited (PTT) and Mitsubishi Chemical Corporation (MCC) produce
not only petro-based PBS but also bio-based PBS (BioPBSTM). Both plastics have the same
properties and processability, only difference is their source material. BioPBSTM is produced
from succinic acid derived from natural resources (sugarcane, cassava and corn) and the 1,4-
butanediol. BioPBSTM products have high heat deflection temperature point and high seal
strength in heat sealing. The polymer is highly compatible with PLA. Bio-based PBSA contains
higher percentage of amorphous structure, is stickier and has higher adhesion strength, than
standard PBS. Properties of BioPBSTM are similar to those of LDPE. Possible commercial
application for BioPBSTM are paper lamination, multi-layer bags, films (plastic bags, mulch
films) [113].
Qahtani et al. [114] used this BioPBS and PLA for making more sustainable 3D printed
PLA/BioPBS blends. It was found that with the blending ratio 90/10 of PLA and BioPBS
higher tensile and impact strength were achieved than by the neat PLA, while further addition
of BioPBS lead to improved toughness of the 3D blends and increased the viscosity [114].
Furthermore, BioPBS was combined by varying contents of apple pomace (AP) [115] and
grape pomace (GP) [116], byproducts from the vine and apple juice industries, and
biocomposites were fabricated by melt extrusion-injection. Both byproducts can be utilized as

19
fillers and to decrease the amount of polymer in a bio-based composite blend. The results
indicated that high levels of GP and AP can be successfully incorporated into polymer matrix
and improved its mechanical and thermo-mechanical properties. So prepared BioPBS-based
composites could be used for production of disposable or single use and sustainable
biodegradable applications [115,116]. Platnieks et al. [117] prepared BioPBS/micro cellulose
(MCC) woody-like composites, by using a melt blending of 70 wt% of MCC processed from
bleached softwood. Besides, in order to enhance dispersion and compatibility, MCC was
modified by using carbodiimide (CDI), polyhydroxy amides (PHA), alkyl ester (EST), (3-
Aminopropyl) trimethoxysilane (APTMS), maleic acid anhydride (MAH), and polymeric
diphenylmethane diisocyanate (PMDI). The chemically modified MCC composites lead to
very enhanced mechanical, thermo-mechanical, and thermal properties of the PBS/MCC
composites. This composite material can be suitable for various construction applications
including profiles, decks and housing appliances [117]. Unlike the others, Cooper et al. [118]
created highly porous electrospun fibers, where BioPBS were dissolved in three different
solutions: chloroform, chloroform/N,N-dimethylformamide (DMF), or chloroform/dimethyl
sulfoxide (DMSO). Thus prepared electrospun BioPBS fibers have high porosity at the micro-
and nanoscale and consequently have suitable mechanical properties for potential in wound
healing and soft tissue engineering [118]. In the work of Seggiani et al. [119] bio-based PBSA
and raw hydrolysed collagen (HC), by-products of the tannery industry were used, to produce
thermoplastic blends. Different PBSA/HC blends with 5-20 wt% of HC were processed by
extrusion, film blowing and injection molding. The PBSA/HC based blends with higher content
of HC (10-20wt%) showed good mechanical properties and present promising candidates to
produce biodegradable products for agriculture applications [119].

Table 8:

Poly (butylene-adipate-co-terephthalate) (PBAT)

PBAT is an aliphatic aromatic copolyester that can be fully degraded in few weeks [120]. It
has good mechanical properties, such as adequate toughness and tear resistance, but it has a
low barrier character to water vapor, oxygen and carbon dioxide [120].
PBAT can be used to produce fibers, textile, films and packaging materials. It has also been
used for the preparation of antimicrobial films that could be used in food packaging to inhibit
bacterial growth, helping to preserve food products safely [121]. In such films, PBAT serves
as the bulk of the film with the antimicrobial agent being incorporated during processing.

20
Sangroniz et al. [120] studied PBAT/PHAE blends for packaging applications. It was found
that immiscible blends are obtained with very good compatibility. The mechanical performance
and the permeability to water vapour, limonene and carbon dioxide was measured to assess the
suitability of these blends for packaging applications [120] (Table 9). Tavares et al. [122]
studied the PBAT-kraft lignin (KL) blend films, which were obtained by extrusion. Multilayer
composites were obtained by lamination, in which PBAT-KL blend films were bonded to a
polyethylene layer using polyurethane adhesive [122]. PBAT-KL could be a synergetic
solution for food packaging that can integrate the reuse of industrial waste, mechanical
properties, flexibility, peeling resistance, and the well-known biodegradability of PBAT [122].
In the work of Wei et al. [123], the non-leaching antimicrobial biodegradable PBAT was
prepared through reactive extrusion with PBAT and the antimicrobial thermoplastic starch
(ATPS) in the presence of the coupling agent, 2,2′-(1,3-phenylene)-bis (2-oxazoline) (PBO).
The antimicrobial PBAT films with the excellent and rapid antimicrobial activity were obtained
by using a blown film extrusion system. PBAT films have a great potential to be used in the
prevention of disease infections in the hospitals and in some fields requiring rapid and highly
efficient antimicrobial activity [123].

Table 9:

BIODEGRADABLE ALTERNATIVES TO CONVENTIONAL PLASTICS

Many bioplastics have mechanical properties equivalent to that of their conventional
counterparts (e.g. PP, PS and PE) and can be processed using technologies widely used in the
polymer industry (e.g. compounding, film processing and moulding) [10]. Their use has been
found in many short service life applications where biodegradability is a key advantageous
feature including consumer packaging (e.g. trays, pots, films and bottles in food packaging),
convenience food disposables (e.g. cutlery/tableware), bags (shopping, garden or domestic
waste), agriculture mulch films, personal-care disposals (e.g. nappies) and even golf tees [10].
Bioplastic polymers have also been used in more durable applications such as in textiles,
consumer goods, automotive parts and building and construction where the focus is on the use
of renewable (bio)resources and any inherent biodegradability properties need to be suppressed
or controlled by careful design [124].
PLA is eco-friendly, it is 100 % bio-based and biodegradable but only under certain conditions
and it is industrially compostable [125]. PLA is also a biocompatible material and should not
produce carcinogenic or toxic effects in local tissue treatment. Compared to the other

21
biopolymers such as PCL it has a better thermal processibility [125]. PLA is also relatively
hydrophobic and has a slow degradation rate. Table 10 shows that PLA has similar mechanical
properties to PET polymer. Elastic modules and tensile strength are comparable to PET [125].
High molecular weight PCL polymer has mechanical properties similar to PE (HDPE and
LDPE), processing a tensile strength of 12-30 MPa and a break extension of 400-900 %
[3,105]. Disadvantages of PCL are very low glass transition (-60 °C) and low melting point;
60-65 °C, which prohibits its application at elevated temperatures [3,105]. Therefore, PCL is
often blended with other polymers, such as PP, PC, polyethylene oxide (PEO), and starch, to
produce composites with desired properties [89].
Due to the plastic-like properties and biodegradability of PHAs these polymers present a
potential replacement for non-degradable PE, PP [126]. The homopolymers PHB possess
several physical properties, e.g., Tg (15 °C), crystallinity (80 %), and tensile strength (40 MPa),
similar to those of PP. However, PHB is significantly more brittle than PP (strain at break 6 vs.
400 %) [123]. PBS is biodegradable and currently mostly fossil-based but could in theory be
100 % bio-based. His mechanical properties resemble to those of PE and PP, while its melting
point is between 90-120 °C, glass transition temperature is around -45 °C to -10 °C [3,127,128].
PBS has good processability, better than that of PLA [105]. Furthermore, the properties of
BioPBSTM are similar to those of LDPE [113]. PBAT is also currently mostly fossil-based. Its
commercial name is Ecoflex®, prepared by BASF (Germany). Ecoflex® F Blend C1200 has
properties similar to PE-LD because of its high molecular weight and its long chain branched
molecular structure [105].
Cellulose and starch are an alternative for PP and PS. Cellulose acetate (CA), which is the most
important cellulose derivate has tensile strength comparable to PS [129]. Starch blends are
completely biodegradable and 25-100 % bio-based, when starch added to one or several
biodegradable polymers [129].

Table 10:

22
CONCLUSION
More than the origin, the chemical structure of the biopolymer is a key factor that determines
its biodegradability. Indeed, the future outlook for development in the field of biopolymer
materials is promising, the future of each polymer is dependent on its competitiveness but also
the social ability to pay for it. Biodegradable plastics made from renewable resources can retain
all the benefits of petroleum-based plastic without the negative environmental impact. The
discovery and implementation of plastic made from natural resources is an enormous leap into
the future for different branches of industry. In order to successfully replace biodegradable
polymers with current plastics, cooperation is needed not only with industry and academics,
but also with various disciplines such as chemistry, engineering, material science,
biogeochemistry and climate science. This will require a plenty of time and a key
multidisciplinary development will be needed.

Acknowledgments

The authors would like to acknowledge Slovenian Research Agency (ARRS) for financing
research in frame of Programme P2-0046.

REFERENCES

[1] M. Raja, A. Murali, J. Mater. Sci. Eng. B 1 (2011) 86–89.

[2] T. Helmer Pedersen, F. Conti, Waste Manage. 68 (2017) 24–31.
[3] I. Vroman, L. Tighzert, Materials 2 (2009) 307–44.
[4] M.B. Kannan, in Surface Modification of Magnesium and its Alloys for Biomedical
Applications, T.S.N.S. Narayanan, I.S. Park, M.H. Lee Ed., Woodhead Publishing,
United Kingdom (2015), p. 355.

23
[5] L. Yu, K. Dean, L. Li, Prog. Polym. Sci. 31 (2006) 576–602.
[6] S. Lambert, M. Wagner, Chem. Soc. Rev. 46 (2017) 6855–6871.
[7] J.P. Greene, in Sustainable Plastics: Environmental Assessments of Biobased,
Biodegradable, and Recycled Plastics, John Wiley & Sons (2014), p. 336.
[8] K. Sudesh, T. Iwata, Clean – Soil Air Water 36 (2008) 433–442.
[9] H. Rosenheim, I. De, S. Hyvedemm, Bioplastics market data 2018,
https://www.european-bioplastics.org/wp-content/uploads/2016/02/Report_
Bioplastics-Market-Data_2018.pdf, [accessed 9 June 2019].
[10] H. Rosenheim, I. De, S. Hyvedemm, Bioplastics market data 2017,
https://docs.european-bioplastics.org/publications/market_data/2017/Report_
Bioplastics_Market_Data_2017.pdf, [accessed 9 June 2019].
[11] R. Smith, Biodegradable polymers for industrial applications, Woodhead Publishing,
United Kingdom (2005), p. 552.
[12] M.A. Elsawy, K.-H. Kim, J.-W. Park, A. Deep, Renew. Sustain. Energy Rev. 79
(2017) 1346–1352.
[13] A.B. Balaji, H. Pakalapati, M. Khalid, R. Walvekar, H. Siddiqui, in Biodegradable and
Biocompatible Polymer Composites: Processing, Properties and Applications, N.G.
Shimpi Ed., Woodhead Publishing, Duxford (2017), p. 3.
[14] P. Lescher, Starch/Staerke 61 (2009) 43–45.
[15] J. Rydz, M. Musioł, B. Zawidlak-Węgrzyńska, W. Sikorska, in Biopolymers for Food
Design, A.M. Grumezescu, A.M. Holban (Eds.), Elservier (2018), p. 431.
[16] J. Jane, J. Macromol. Sci., Part A: Pure Appl.Chem. 32 (1995) 751–757.
[17] A.J. Gunorubon, Res. J. Eng. Appl. Sci. 1 (2012) 219–214.
[18] M. Carissimi, S. Flôres, R. Rech, Algal Res. 32 (2018) 201–209.
[19] R.V. Gadhave, A. Das, P.A. Mahanwar, P.T. Gadekar, Open J. Polym. Chem. 8 (2018)
21-33.
[20] K. Petersen, P. Nielsen, G. Bertelsen, M. Lawther, M. B. Olsen, N. Nilsson, G.
Mortensen, Trends Food Sci. Technol. 10 (1999) 52–68.
[21] Q. Xie, F. Li, J. Li, L. Wang, Y. Li, C. Zhang, J. Xu, S. Chen, Carbohydr. Polym. 189
(2018) 56–64.
[22] C. Medina-Jaramillo, O. Ochoa-Yepes, C. Bernal, L. Famá, Carbohydr. Polym. 176
(2017) 187–94.
[23] J.F. Mendes, R.T. Paschoalin, V.B. Carmona, A.R. Sena Neto, A.C.P. Marques, J.M.
Marconcini, L.H.C. Mattoso, E.S. Medeiros, J.E. Oliveira, Carbohydr. Polym. 137
(2016) 452–458.
[24] S. Kumar, A. Mukherjee, J. Dutta, Trends Food Sci. Technol. 97 (2020) 196–209.
[25] H. Honarkar, M. Barikani, Monatsh. Chem. 140 (2009) 1-18.
[26] T. Woggum, P. Sirivongpaisal, T. Wittaya, Food Hydrocolloids 50 (2015) 54–64.
[27] O.V. López, L.A. Castillo, M.A. García, M.A. Villar, S.E. Barbosa, Food
Hydrocolloids 43 (2015) 18–24.
[28] N.S.M. Makhtar, M.F.M. Rais, M.N.M. Rodhi, N. Bujang, M. Musa, K.H.K. Hamid,
Procedia Eng. 68 (2013) 385–391.
[29] Z. Czech, K. Wilpiszewska, B. Tyliszczak, X. Jiang, Y. Bai, L. Shao, Int. J. Adhes.
Adhes. 44 (2013) 195–199.
[30] H.P.S. Abdul Khalil, A.H. Bhat, A.F. Ireana Yusra, Carbohydr. Polym. 87 (2012) 963–
979.
[31] M.P. Arrieta, E. Fortunati, F. Dominici, J. López, J.M. Kenny, Carbohydr. Polym. 121
(2015) 265–275.
[32] L. Shen, E. Worrell, M. Patel, Biofuels Bioprod. Biorefining 4 (2010) 25–40.

24
[33] K. Missoum, P. Sadocco, J. Causio, M.N. Belgacem, J. Bras, Mater. Sci. Eng. C 45
(2014) 477–483.
[34] J. Sirviö, M. Visanko, J. Ukkola, H. Liimatainen, Ind. Crops Prod. 122 (2018) 513–
521.
[35] F.-X. Joly, M. Coulis, Waste Manag. 72 (2018) 349–353.
[36] H.M. Shaikh, K.V. Pandare, G. Nair, A.J. Varma, Carbohydr. Polym. 76 (2009) 23–29.
[37] Y. Wu, X. Luo, W. Li, R. Song, J. Li, Y. Li, B. Li, S. Liu, Food Chem. 197 (2016)
250–256.
[38] A. Isroi, T. Cifriadi, N.A. Panji, K. Wibowo, K. Syamsu, IOP Conf. Ser.: Earth
Environ. Sci. 65 (2017) 012011.
[39] J. Zhang, P. Mungara, J. Jane, Polymer 42 (2001) 2569–2578.
[40] J. John, M. Bhattacharya, Polym. Int. 48 (1999) 1165–1172.
[41] W. Liu, A.K. Mohanty, P. Askeland, L.T. Drzal, M. Misra, Polymer 45 (2004) 7589–
7596.
[42] S. Tansaz, A.R. Boccaccini, J. Biomed. Mater. Res. A 104 (2016) 553–569.
[43] S. Tansaz, L. Liverani, L. Vester, A.R. Boccaccini, Mater. Lett. C 199 (2017) 143–
146.
[44] M. Santin, C. Morris, G. Standen, L. Nicolais, L. Ambrosio, Biomacromolecules 8
(2007) 2706–2711.
[45] C. Morris, J. Thorpe, L. Ambrosio, M. Santin, J. Nutr. 136 (2006) 1166–1170.
[46] A. Merolli, L. Nicolais, L. Ambrosio, M. Santin, Biomed. Mater. 5 (2010) 015008.
[47] G.A. Silva, C.M. Vaz, O.P. Coutinho, A.M. Cunha, R.L. Reis, J. Mater. Sci.: Mater.
Med. 14 (2003) 1055–1066.
[48] Z. Peles, M. Zilberman, Acta Biomater. 8 (2012) 209–217.
[49] S. Tansaz, A.K. Durmann, R. Detsch, A.R. Boccaccini, J. Appl. Polym. Sci. 134
(2017) 1-9.
[50] S.A. Witherly, Am. J. Clin. Nutr. 51 (1990) 705–706.
[51] N. Cao, Y. Fu, J. He, Food Hydrocolloids 21 (2007) 1153–1162.
[52] S. Tulamandi, V. Rangaraju, S. Rizvi, R. S. Singhal, S. Kr. Chattopadhyay, N.
Chandra Saha, Food Packag. Shelf Life 10 (2016) 60–71.
[53] M. Yang, H. Xu, X. Hou, J. Zhang, Y. Yang, J. Environ. Manage. 188 (2017) 26–31.
[54] Y. Zhao, H. Xu, B. Mu, L. Xu, Y. Yang, Polym. Degrad. Stab. 133 (2016) 75–84.
[55] N. Reddy, Y. Yang, Ind. Crops Prod. 33 (2011) 35–41.
[56] M. Jiménez-Rosado, V. Pérez-Puyana, F. Cordobés, A. Romero, A. Guerrero, Ind.
Crops Prod. 121 (2018) 345–351.
[57] Z. Yu, L. Sun, W. Wang, W. Zeng, A. Mustapha, M. Lin, Ind. Crops Prod. 112 (2018)
412–419.
[58] D. Carpiné, J.L.A. Dagostin E.F. de Andrade, L.C. Bertan, M.R. Mafra, Ind. Crops
Prod. C 83 (2016) 364–371.
[59] S. Tansaz, M. Schulte, U. Kneser, D. Mohn, W. Stark, J.A. Roether, I. Cicha, A.R.
Boccaccini, Eur. Polym. J. 106 (2018) 232–41.
[60] S. Chanprateep, J. Biosci. Bioeng. 110 (2010) 621–632.
[61] Z. Li, J. Yang, X.J. Loh, NPG Asia Mater. 8 (2016) e265. R.
[62] R. Tarrahi, Z. Fathi, M.Ö. Seydibeyoğlu, E. Doustkhah, A. Khataee, Int. J. Biol.
Macromol. 146 (2020) 596–619.
[63] A. Shrivastav, H.Y. Kim, Y.R. Kim, BioMed Res. Int. 2013 (2013) 1-12.
[64] S.Y. Lee, Biotechnol. Bioeng. 49 (1996) 1–14.
[65] M. Avella, E. Martuscelli, M. Raimo, J. Mater. Sci. 35 (2000) 523–545.
[66] B. Lukasiewicz, P. Basnett, R. Nigmatullin, R. Matharu, J.C. Knowles, I. Roy, Acta
Biomater. 71 (2018) 225–234.

25
[67] G.Q. Chen, Chem. Soc. Rev. 38 (2009) 2434–2446.
[68] Y. Doi, Y. Kanesawa, M. Kunioka, T. Saito, Macromolecules 23 (1990) 26–31.
[69] R. Sodian, S.P. Hoerstrup, J.S. Sperling, D.P. Martin, S. Daebritz, J.E.J. Mayer, J.P.
Vacanti, ASAIO J. 46 (2000) 107-110.
[70] C.S. Wu, H.-T. Liao, Y.-X. Cai, Polym. Degrad. Stab. C 140 (2017) 55–63.
[71] S. Godbole, S. Gote, M. Latkar, T. Chakrabarti, Bioresour. Technol. 86 (2003) 33–37.
[72] D. Garcia‐Garcia, O. Fenollar, V. Fombuena, J. Lopez‐Martinez, R. Balart, Macromol.
Mater. Eng. 302 (2017) 1-12.
[73] R. Andler, R. Vivod, A. Steinbüchel, J. Biosci. Bioeng. 127 (2019) 360–365.
[74] S.S. Costa, A.L. Miranda, D. de J. Assis, C.O. Souza, M.G. de Morais, J.A.V. Costa,
J.I. Druzian, Algal Res. 33 (2018) 231–238.
[75] C.Y. Soon, N.A. Rahman, Y.B. Tee, R.A. Talib, C.H. Tan, K. Abdan, E.W.C. Chan, J.
Mater. Res. Technol. 8 (2019) 5091–5102.
[76] A.O. Pérez-Arauz, A.E. Aguilar-Rabiela, A. Vargas-Torres, A.-I. Rodríguez-
Hernández, N. Chavarría-Hernández, B. Vergara-Porras, M.R. López-Cuellar, Food
Packag. Shelf Life 20 (2019) 1-8.
[77] P. Xu, W. Yang, D. Niu, M. Yu, M. Du, W. Dong, M. Chen, P. Jan Lemstra, P. Ma,
Chem. Eng. J. 382 (2020) 1-11.
[78] A. da Silva Moura, R. Demori, R.M. Leão, C.L. Crescente Frankenberg, R.M.
Campomanes Santana, Mater. Today Commun. 18 (2019) 191–198.
[79] L. Jiang, M.P. Wolcott, J. Zhang, Biomacromolecules 7 (2006) 199–207.
[80] M. Yasuniwa, S. Tsubakihara, Y. Sugimoto, C. Nakafuku, J. Polym. Sci. Part B
Polym. Phys. 42 (2004) 25–32.
[81] K. Madhavan Nampoothiri, N.R. Nair, R.P. John, Bioresour. Technol. 101 (2010)
8493–8501.
[82] A.K. Abay, M.B. Gebeyehu, H.K. Lin, P.C. Lin, J.Y. Lee, C.M. Wu, R.I. Murakami,
T.C. Chiang, J. Polym. Res. 23 (2016) 1-12.
[83] B. Bindhu, R. Renisha, L. Roberts, T.O. Varghese, Polym. Test. 66 (2018) 172–177.
[84] D.A. D’Amico, M.L. Iglesias Montes, L.B. Manfredi, V.P. Cyras, Polym. Test. 49
(2016) 22–28.
[85] P.E. Fathima, S.K. Panda, P.M. Ashraf, T.O. Varghese, J. Bindu, Int. J. Biol.
Macromol. 117 (2018) 1002–1010.
[86] M.P. Arrieta, J. López, D. López, J.M. Kenny, L. Peponi, Polym. Degrad. Stab. 132
(2016) 145–156.
[87] P. Abasian, M. Radmansouri, M. Habibi Jouybari, M.V. Ghasemi, A. Mohammadi, M.
Irani, F.S. Jazi, Int. J. Biol. Macromol. 121 (2019) 398–406.
[88] C. Swaroop, M. Shukla, Int. J. Biol. Macromol. 113 (2018) 729–736.
[89] A. Rigoussen, J.M. Raquez, P. Dubois, P. Verge, Eur. Polym. J. 114 (2019) 118-126.
[90] W. Zheng, M. Li, Y. Lin, X. Zhan, Biomed. Pharmacother. 108 (2018) 565–573.
[91] M.A. Woodruff, D.W. Hutmacher, Prog. Polym. Sci. 35 (2010) 1217–1256.
[92] M. Abedalwafa, F. Wang, L. Wang, C. Li, Rev. Adv. Mater. Sci. 34 (2013) 123-140.
[93] S. Khalid, L. Yu, M. Feng, L. Meng, Y. Bai, A. Ali, H. Liu, L. Chen, Food Packag.
Shelf Life 18 (2018) 71–79.
[94] K.K. Sadasivuni, J.J. Cabibihan, D. Ponnamma, M.A. AlMaadeed, J. Kim, in
Biopolymer Composites in Electronics, Elsevier (2016), p. 544.
[95] V. Sessini, I. Navarro-Baena, M.P. Arrieta, F. Dominici, D. López, L. Torre, J.M.
Kenny, P. Dubois, J.-M. Raquez, L. Peponi, Polym. Degrad. Stab. 152 (2018) 126–
138.
[96] B. Dariš, Acta Medico-Biotech. 9 (2016) 42-48.
[97] Z. McEachin, K. Lozano, J. Appl. Polym. Sci. 126 (2012) 473–479.

26
[98] J.S. Choi, S.J. Lee, G.J. Christ, A. Atala, J.J. Yoo, Biomaterials 29 (2008) 2899–2906.
[99] M. Zamani, M. Morshed, J. Varshosaz, M. Jannesari, Eur. J. Pharm. Biopharm. 75
(2010) 179–185.
[100] T. Potrč, S. Baumgartner, R. Roškar, O. Planinšek, Z. Lavrič, J. Kristl, P. Kocbek, Eur.
J. Pharm. Sci. 75 (2015) 101–113.
[101] Š. Zupančič, S. Baumgartner, Z. Lavrič, M. Petelin, J. Kristl, J. Drug Deliv. Sci.
Technol. 30 (2015) 408–416.
[102] V. Sessini, I. Navarro-Baena, M.P. Arrieta, F. Dominici D. López, L. Torre, J.M.
Kenny, P. Dubois, J.M. Raquez, L. Peponi, Polym. Degrad. Stabil. 152 (2018) 126-
138.
[103] Y.S. Joo, J.R. Cha, M.S. Gong, Mater. Sci. Eng. C 91 (2018) 426–435.
[104] T. Xu, Z. Liang, B. Ding, Q. Feng, H. Fong, Polymer 151 (2018) 299–306.
[105] L. Jiang, J. Zhang, in Applied Plastics Engineering Handbook (Second Edition), M.
Kutz Ed., William Andrew Publishing, (2017), p. 127.
[106] J. Xu, B.-H. Guo, in Plastics from Bacteria: Natural Functions and Applications, G.
G.Q. Chen Ed., Springer Berlin Heidelberg, Berlin, (2010), p. 347.
[107] Y. Tokiwa, B. Calabia, C. Ugwu, S. Aiba, Y. Tokiwa, B.P. Calabia, C.U. Ugwu, S.
Aiba, Int. J. Mol. Sci. 10 (2009) 3722–3742.
[108] C. Brunner, E. Baran, E. Duarte Pinho, R.L. Reis, N. Neves, Colloids Surf. B
Biointerfaces 84 (2011) 498–507.
[109] S. Jiang, Y. Yang, S. Ge, Z. Zhang, W. Peng, Arab. J. Chem. 11 (2018) 844–857.
[110] K. Shi, Y. Liu, X. Hu, T. Su, P. Li, Z. Wang, Int. J. Biol. Macromol. 114 (2018) 373–
380.
[111] H. Sun, Y. Luo, B. Yang, H. Zhang, J. Huang, Polymer 153 (2018) 378–390.
[112] Y. Xu, S. Zhang, P. Wang, J. Wang, Polymer 154 (2018) 258–271.
[113] BioPBS, http://www.pttmcc.com/new/faq.php, [accessed, 15 March 2020].
[114] M. Qahtani, F. Wu, M. Misra, S. Gregori, D. Mielewski, A. Mohanty, ACS Sustain.
Chem. Eng. 7 (2019) 14460-14470.
[115] M.C. Picard, A. Rodriguez-Uribe, M. Thimmanagari, M. Misra, A.K. Mohanty, Waste
Biomass Valor. (2019) 1-13.
[116] A. Gowman, T. Wang, A. Rodriguez-Uribe, A.K. Mohanty, M. Misra, ACS Omega 3
(2018) 15205–15216.
[117] O. Platnieks, S. Gaidukovs, A. Barkane, G. Gaidukova, L. Grase, V.K. Thakur, I.
Filipova, V. Fridrihsone, M. Skute, M. Laka, Molecules 25 (2020) 1-18.
[118] C.J. Cooper, A.K. Mohanty, M. Misra, ACS Omega 3 (2018) 5547–5557.
[119] M. Seggiani, V. Gigante, P. Cinelli, M.-B. Coltelli, M. Sandroni, I. Anguillesi, A.
Lazzeri, Polym. Test. 77 (2019) 1-10.
[120] A. Sangroniz, L. Sangroniz, N. Aranburu, M. Fernández, A. Santamaria, M. Iriarte, A.
Etxeberria, Eur. Polym. J. 105 (2018) 348–358.
[121 L. Bastarrachea, S. Dhawan, S.S. Sablani, J.H. Mah, D.H. Kang, J. Zhang, J. Tang, J.
Food Sci. 75 (2010) 215–224.
[122] L.B. Tavares, N.M. Ito, M.C. Salvadori, D.J. dos Santos, D.S. Rosa, Polym. Test. 67
(2018) 169–176.
[123] D. Wei, H. Wang, Z. Ziaee, F. Chibante, A. Zheg, H. Xiao, Mater. Sci. Eng. C 58
(2016) 986–991.
[124] J.H. Song, R.J. Murphy, R. Narayan, G.B.H. Davies, Philos. Trans. R. Soc. B Biol.
Sci. 364 (2009) 2127–2139.
[125] S. Farah, D.G. Anderson, R. Langer, Adv. Drug Deliv. Rev. 107 (2016) 367–392.

27
[126] M. L. Ortiz-Hernandez, E. Sanchez-Salinas, E. Dantan-Gonzalez, and M. L. Castrejon-
Godınez, in Biodegradation: Life of Science, R. Chamy and F. Rosenkranz Eds.,
Intech, Rijeka (2013), p. 380.
[127] X. Wang, J. Zhou, L. Li, Eur. Polym. J. 43 (2007) 3163–3170.
[128] G. Z. Papageorgiou, D.S. Achilias, D.N. Bikiaris, Macromol. Chem. Phys. 208 (2007)
1250-1264.
[129] F. Aeschelmann, M. Carus, Ind. Biotechnol. 11 (2015) 154–159.

[130] T.R. Crompton, Physical Testing of Plastics, Smithers Rapra Technology, (2012).
[131] B. Demirel, A. Yaraş, H. Elçiçek, BAÜ Fen Bil. Enst. Dergisi Cilt. 13 (2016) 26–35.
[132] G. Kfoury, J.M. Raquez, F. Hassouna, J. Odent, V. Toniazzo, D. Ruch, P. Dubois,
Front Chem. 1 (2013) 1-46.
[133] Properties of Polystyrene,
https://polymerdatabase.com/polymer%20classes/Polystyrene%20type.html, [accessed,
5 May 2019].

28
Figure captions:

Figure 1: Global production capacities of bioplastics [10].

Figure 2: Classifications of biodegradable polymers [12].

29
 Table 1: Global production capacities of bioplastic by material type in 2018 and 2023 [10].

MATERIAL TYPE 2018 (%) 2023 (%)

Biodegradable 43.2 44.5
PBAT 7.2 4.2
PBS 4.6 4.1
PLA 10.3 13.2
PHA 1.4 5.8
Starch blends 18.2 15.8
Other (biodegradable) 1.5 1.4
Bio-based/non-degradable 56.8 55.5
PET 26.6 20.5
PA 11.6 11.0
PEF1 0.0 2.9
PE 9.5 11.3
PP1 0.0 2.0
Other (biobased/non- 10.1 7.8
biodegradable)

1
Bio-based PP and PEF are currently in development and predicted to be available in
commercial scale in 2023.

30
Table 2: Starch as biodegradable polymers, addition of copolymers, additives/fibers and their
potential applications.
Biodegradable Material Co-polymer Additives/fibers Application Ref.
polymer
Starch Corn starch / Sisal fiber Packing [21]
material
Starch Cassava / Glycerol, natural Food [22]
starch extracts such as packaging
green tea
Starch Cassava Biomass / Salmon [18]
starch extract of packaging
microalgae
Starch Corn starch Chitosan / Packaging [23]
Starch Native rice / Propylene oxide Packaging [26]
starch
Starch Corn starch / Talc Packaging [27]
nanoparticles bags
Starch Polynesian / Glycerol and Bioplastic [28]
arrowroot crude palm oil development
starch
Starch Potato starch / Glycerol, Medical [29]
monohydrate tapes and
citric acid biomedical
electrodes

31
Table 3: Cellulose as biodegradable polymers, addition of copolymers, additives/fibers and
their potential applications.
Biodegradable Material Co- Additives/fibers Application Ref.
polymer polymer
Cellulose Wood / Tio2 Paper, packaging [33]
pulp and composites
Cellulose Softwood / Natural cellulose Green packaging [34]
kraft pulp fibers, films
Glycerol,
propylene
carbonate and
ethylene
carbonate
Cellulose Cellulose / / Cigarette filters [35]
Cellulose Sugarcane / Hemicellulose High value plastics [36]
bagasse (5%) of bagasse
Cellulose Native Chitosan / Food packaging [37]
cellulose
(cotton
linter)
Cellulose Empty Cassava Glycerol Plastic bags and [38]
fruit starch food packaging
bunch

32
Table 4: SP as biodegradable polymers, addition of copolymers, additives/fibers and their
potential applications.
Biodegradable Material Co- Additives/fibers Application Ref.
polymer polymer
SP Defatted Gelatin, Glycerol Packaging [52]
soy papaya
protein puree
(Shakthi
soyas)
SP Soy / Glycerol Textile processing [53]
proteins
SP Soy / Acrylic acid Packaging [54]
proteins
SP Soy / Jute fiber Various [55]
proteins applications
SP Soy Cellulose Glycerol Active food [57]
protein nanocrystals packaging material
isolate (cncs) and
Cedrus
deodara
pine needle
extract
SP Soy / Virgin coconut Industrial purposes [58]
protein oil,
isolate Glycerol
SP Soy / Zinc sulphate Horticultural crop [56]
protein monohydrate, applications
isolate glycerol
SP Soy / Nanosized Wound-dressing [59]
protein bioactive glass, applications
isolate Glycerol

33
Table 5: PHA as biodegradable polymers, addition of copolymers, additives/fibers and their
potential applications.
Biodegradable Material Co- Additives/fibers Application Ref.
polymer polymer
PHA Bacillus subtilis P(3HB) Acetic acid Soft tissue [66]
OK2 and engineering
Pseudomonas applications
mendocina CH50
PHA/ PHA / Treated palm 3D printing [70]
PHA-g- fibre filaments
MA/TPF Maleic
anhydride
PHB PHB Starch / A coating [71]
material on
paper or
cardboard
used for food
packaging
P3HB Commercial P3HB / Maleinized Packaging [72]
linseed oil
(MLO) and an
epoxidized fatty
acid ester
(EFAE)
PHA Gordonia / Poly(cis-1,4- Recycling [73]
polyisoprenivorans isoprene) method for
VH2, Ralstonia rubber waste
eutropha,
Pseudomonas
aeruginosa
PHA Spirulina sp. LEB- / Sodium Industrial [74]
18 hypochlorite,
Microalgae Methanol

34
PHA Commercial PHA NCC, Tween 80 Industrial [75]
chitosan wastewater
PHA Peanut oil and / sodium Food [76]
Cupriavidus hypochlorite packaging,
necator H16 solution biotechnology
industry
PHA Bacterially / GO, LAQ Food [77]
synthesized packaging
applications
PHB PHB industrial Coconut / Packaging [78]
fiber in
nature
and
coconut
fiber
treated

35
Table 6: PLA as biodegradable polymers, addition of copolymers, additives/fibers and their
potential applications.
Biodegradable Material Co-polymer Additives/fibers Application Ref.
polymer
PLA, PLA/BN PLA resin / Boron nitride Packaging in [83]
industries
PLA Industrial PHB Tributyrin Food [84]
PLA (TBL) packaging
PLA PLA resin Nanochitosan Polyethylene Packing of [85]
glycol, fresh prawn
polyvinyl
alcohol
PLA Industrial PHB Chitosan, Agricultural, [86]
PLA catechin, acetyl- food
tri-n-butyl packaging
citrate (ATBC)
PLA Industrial chitosan DOX Local [87]
PLA Triflouroacetic chemotherapy
acid
PLA Commercially / MgO Food [88]
available nanoparticles packaging
PLA
PLA Industrial ABS Cardanol 3D printing [89]
PLA
MPEG-PLA Industrial / Verapamil Ovarian [90]
MPEG-PLA and doxorubicin cancer

36
Table 7: PCL as biodegradable polymers, addition of copolymers, additives/fibers and their
potential applications.
Biodegradable Material Co- Additives/fibers Application Ref.
polymer polymer
PCL Industrial Collagen / Cell regeneration [98]
PLC of skeletal muscles
PCL Industrial / Metronidazole Periodontal [99]
PLC benzoate (MET) diseases
PCL Industrial / Resveratrol, Different fields [100]
PLC carvedilol and
ibuprofen
PCL Industrial / Resveratrol Periodontal [101]
PLC disease
PCL Industrial PLA CNC Biomedicine, food [102]
PLC packaging
PCL Industrial PU / Medical devices [103]
PLC
PCL Industrial Cellulose / Tissue engineering [104]
PLC acetate
(CA)

37
Table 8: Research PBS as biodegradable polymers, addition of copolymers, additives/fibers
and their potential applications.
Biodegradable Material Co- Additives/fibers Application Ref.
polymer polymer
PBS Industrial PBS Decayed CaCO3 Different fields [109]
wood AHP, APP and
CaHP
PBS Industrial PBS Cellulose / Different fields [110]
triacetate
PBS Synthesized Poly Tetrabutyl titanate Biochemical [111]
PBS with the (vinyl engineering
content of butyral)
butyral group (PVB)

PBS ionomer Synthesized / / Package [112]

PBS ionomer material, such
by as film, foams
condensation
polymerization
of succinic
acid, 1,4-
butanediol and
DHPPO-K
BioPBS BioPBSTM PLA / Different [114]
industries and
applications
BioPBS BioPBSTM / Apple pomace Packaging [115]
BioPBS BioPBSTM / Grape pomace Food [116]
packaging
BioPBS BioPBSTM cellulose CDI, PHA, EST, Construction [117]
(FZ71PB) APTMS, MAH, applications
PMDI

38
BioPBS BioPBSTM / CHCl3 Biomedical or [118]
(FZ91PM) DMSO tissue
DMF engineering
application.
PBSA BioPBS™ collagen / Agriculture [119]
(FD92PM) applications

39
Table 9: Research of PBAT as biodegradable polymers, addition of copolymers,
additives/fibers and their potential applications.

Biodegradable Material Co- Additives/fibers Application Ref.

polymer polymer
PBAT Industrial PHAE / Packaging [104]
PBAT applications
PBAT Industrial Kraft lignin / Food packaging [107]
PBAT
PBAT Industrial ATPS, PBO Prevention of [105]
PBAT PHGH disease infection in
the hospital

40
Table 10: Comparison of the properties of biodegradable and synthetic polymers.
Polymers Glass Melting Tensile Strain at Flexural
transition temperature strength break (%) modulus
(°C) Tg (°C) Tm (MPa) (MPa)

PHB [105] 15 175 40 6 3500-4000

PLA [89,125] 55 165 59 7 5000

BioPBS [113] -22 115 30 170 630

PBS [105,109] -32 114 57 700 656
LDPE [105] -120 110 35 176 400
HDPE [105] -120 129 29 1070 650
PP [105] 5 163 44 1370 800
PBAT (Ecoflex) [105] - 110-115 32-36 580-800 -
PVC [130] 82 100-260 20-76 150-400 1300-4690
PET [131,132] 73,5 250 80 36 2410
PCL [3,105] -60 60-65 23 400-900 -
PS [133] 100 240 30-60 1.5-2.3 3200

41
 Global production capacities of bioplastic
3000
2616
2500 2357
2194 2216 2205
2060 2112
2000 1328
in 1000 tonnes

1244
1200 1190 1179
1500 1175 1200

1000

1288
500 994 1026 1026 1113
885 912

0
2017 2018 2019 2020 2021 2022 2023

Biodegradable Bio-based/non-biodegradable Total capacity

Figure 1: Global production capacities of bioplastics [10].

42
Figure 2: Classifications of biodegradable polymers [12]

43