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Biodegradable Synthetic Polymers in Textiles– What Lies Beyond PLA and

Medical Applications? A Review.

Article  in  Tekstilec · January 2021

DOI: 10.14502/Tekstilec2021.64.32-46

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 Tekstilec, 2021, Vol. 64(1), 33–47  |  DOI: 10.14502/Tekstilec2021.64.33-47 33

Thomas Grethe
FTB, Hochschule Niederrhein - University of Applied Sciences,
Webschulstrasse 31, 41065 Moenchengladbach, Germany

Biodegradable Synthetic Polymers in Textiles – What Lies

Beyond PLA and Medical Applications? A Review.
Biorazgradljivi sintetični polimeri v tekstilstvu – kaj sledi PLA in
medicinskim načinom uporabe? Pregled.
Original scientific article/Izvirni znanstveni članek
Received/Prispelo 9-2020 • Accepted/Sprejeto 10-2020

Corresponding author/Korespondenčni avtor:

Dr. Dipl.-Chem. Thomas Grethe
E-mail: [email protected]

Abstract
Biodegradable polymers are currently discussed for applications in different fields and are becoming of
increasing interest in textile research. While a plethora of work has been done for PLA in medical textiles,
other biodegradable polymers and their textile application fields are studied less often, presumably due
to higher costs and fewer market opportunities. However, some are emerging from research to pilot scale,
and are already utilized commercially in packaging and other sectors but not, unfortunately, in textiles. The
commercialisation of such polymers is fuelled by improved biotechnological production processes, show-
ing that textile applications are increasingly conceivable for the future. Additionally, commonly accepted
definitions for biodegradability are probably misleading, if they are used to estimate the environmental
burden of waste management or recycling of such materials. In this review, the current state of research in
the field of biodegradable polymers for the application in textile materials is presented to identify emerging
developments for new textile applications. It was clearly seen that PLA is most dominant in that field, while
others facilitate new options in the future. The production costs of raw materials and the current patent
situation are also evaluated. A special focus is placed on fibre raw materials, coatings, and additives for
clothing and technical textiles. Fibre-reinforced composites are excluded, since polymers applied for the
matrix component require very different properties compared to the textile materials. This represents a
topic to be discussed separately. As a result, these new biodegradable polymers might serve as interesting
coating materials for textiles that seem to sneak on to the textile market, as the patent search for such
coating formulations suggests. Moreover, new biodegradable fibrous materials for clothing applications can
be suggested, but some material properties must be addressed to render them processable on common
textile machines.
Keywords: biodegradable polymers, recycling, biodegradability, PLA, textile coatings

Izvleček
Danes so biorazgradljivi polimeri predmet razprav za rabo na različnih področjih in postajajo čedalje bolj pri-
ljubljeni v raziskavah na področju tekstilstva. Medtem ko je raziskav rabe PLA za medicinske tekstilije veliko, pa
se drugi biološko razgradljivi polimeri in njihova raba v tekstilstvu verjetno zaradi večjih stroškov in manjših
tržnih možnosti proučujejo manj pogosto. Nekateri od njih so že na stopnji pilotskih raziskav in jih že tržijo za
embalažo in v drugih sektorjih, na področju tekstilij pa žal še ne. Trženje takšnih polimerov spodbujajo izboljšani
biotehnološki proizvodni procesi, kar kaže, da bo v prihodnosti njihova raba za tekstilije bolj razširjena. Poleg
34 Tekstilec, 2021, Vol. 64(1), 33–47

tega splošno sprejete opredelitve biorazgradljivosti verjetno vodijo do zavajajočih sklepov, če se upoštevajo le
ocene obremenitve okolja z ravnanjem z odpadki ali recikliranjem takšnih materialov. V tem pregledu je podano
trenutno stanje raziskav na področju biološko razgradljivih polimerov za rabo na področju tekstilij z namenom,
da bi identificirali nastajajoči razvoj novih tekstilnih aplikacij. Ugotovljeno je bilo, da na področju tekstilne rabe
prevladuje PLA, medtem ko drugi polimeri odpirajo nove možnosti v prihodnosti. Ocenjeni so tudi proizvodni stroški
surovin in trenutno stanje patentov. Poseben poudarek je na tekstilnih surovinah, premazih in aditivih za tekstilije
za oblačila in tehnične namene. Kompoziti, ojačeni z vlakni, niso zajeti, ker so zahtevane lastnosti za polimerne
matrice drugačne kot za tekstilije in bi to področje moralo biti obravnavano posebej. Novi biološko razgradljivi
polimeri bi se lahko uporabljali kot funkcionalni premazi na tekstilijah, saj jih, kot je mogoče razbrati iz poizvedb
za tovrstne patentirane formulacije premazov, že tržijo tudi za področje tekstilij. Predlagati je mogoče tudi nova
biološko razgradljiva vlakna za oblačila, vendar je treba nekatere njihove lastnosti prilagoditi, da jih bo mogoče
predelovati na standardnih tekstilnih strojih.
Ključne besede: biorazgradljivi polimeri, recikliranje, biorazgradljivost, PLA, tekstilni premazi

1 Introduction 2 Definitions
Current legislation and increasing public aware- The term biodegradability needs to be defined first,
ness about polymer waste call for new options in since every material will degrade in the environment
the recycling of such materials. While everyday over a sufficient amount of time and/or under appro-
products such as bags, nettings or packaging mate- priate environmental conditions. To narrow down the
rials are already manufactured from biodegradable temporal and environmental conditions, considera-
plastics to some extent, the development of textile tion of the field of application looks promising. For the
products appears to be more challenging. In this medical sector, the timeframe should be in the range
overview, only synthetic polymers are discussed, of the targeted duration of therapy, which may be in
since natural polymers like cellulose or proteins are the order of several weeks or less, while environmen-
already well-known and utilized in the textile sec- tal conditions are physiological (nearly neutral pH,
tor. Therefore, this report will focus on manmade 37 °C, water-based surrounding, etc.). For technical
polymers for textile purposes. In this narrowed textiles, the definition will obviously be different,
field, primarily three applications can be considered: since degradation is meant to be fulfilled by micro-
fibre-reinforced composites, fibrous substrates and organisms. In this context, the OECD (Organisation
coatings/finishings. The first field has been already for Economic Co-operation and Development) gives
widely addressed and thus will not be discussed four classifications of biodegradability [1]:
here. However, interesting options emerge in the • primary biodegradation
latter two sectors of fibrous substrates and textile It is understood as the loss of certain properties of a
coating materials. The majority of publications for material; consequently no complete decomposition
biodegradable fibrous substrates address the medi- has to occur.
cal sector and, to a lesser extent, technical textiles. • ultimate biodegradation
Thus, a systematic literature review was conducted Here the material hast to be decomposed c­ ompletely
to identify previously evaluated materials and de- into carbon dioxide, water, minerals, and poten-
velopments, as well as new opportunities in these tial biomass (of the microorganism involved in the
fields. Biodegradable textile coatings are even less degradation).
prominent in the literature, so a patent search was • readily biodegradable
also conducted. Materials screened by strict tests on ultimate biodeg-
Moreover, commonly accepted definitions for the radability that assume a rapid and complete biodeg-
term “Biodegradability” do not address environ- radation in aquatic environments.
mental requirements sufficiently, since degradation • inherently biodegradable
products are either defined too strictly or are left Materials in this class exhibit unambiguous biodeg-
completely vague. An extended definition may serve radation behaviour in any tests.
to characterize possible future products more mean- These definitions and the associated test methods
ingfully instead. all address degradation in natural environments
 Biodegradable Synthetic Polymers in Textiles – What Lies Beyond PLA and Medical Applications? A Review. 35

and asses material degradation by direct or indirect

measures of organic carbon, usually after 28 days.
However, the transformation products of the degra-
dation process and possible non-degradable residues
are not taken into account by these definitions and
tests, but must be assessed for a complete picture. If
those residues exist and are bio-accumulative, the Figure 1: Concept of bioneutral degradability
continuous emission of small amounts may lead to
future issues, as seen in fluorinated compounds to- Therefore, literature for this overview qualifies if it is
day. For this reason, such tests only deliver useful about a manmade polymer and meets at least one of
results if the material is completely degraded into the three following criteria:
carbon dioxide, biomass and water. • biodegradable under physiological conditions;
In a practical example, the biodegradability of min- • biodegradable or bioneutral degradable in natu-
eral oils was investigated and found to be up to 70% ral environments with respect to [1], or materials
in some cases by using a test method where the time- assumed to fit in that category; and
frame was 20 weeks (CEC-L-33 A-93). Testing was • biodegradable in industrial composting similar
done by extracting the oil soluble phase and sub- to EN 13432, or materials assumed to fit in that
sequent infrared spectroscopy using the 2950 cm-1 category.
band of CH-vibrations. It remained unclear what Materials that are not tested explicitly but can be as-
kind of residues are present in the extract and also sumed to fit in these categories are not excluded to
which metabolites remained in the aqueous phase ensure the widest overview on current substances.
[2]. Although some sources consider this method as
outdated, [3] other actual sources such as OECD 301
and the above-mentioned OECD definitions also do 3 Materials
not evaluate residues.
For the context of this report, the OECD definitions Most synthetic biodegradable polymers can be cate-
above, except primary biodegradability, and an ex- gorized either as plant-based, microorganism-based
tended degradation time of up to one year, will serve or animal-based. The latter consists mainly of chitin
valid criteria for review. and its derivatives and gelatine, which is rarely used
While this definition addresses only natural envi- to produce fibrous materials. However, chitosan is of-
ronmental conditions, industrial composting is also ten utilized in antibacterial textile finishing. Polymer
considered a form of biodegradation in the context of materials produced by microorganisms can be al-
this report. Several standards do exist to characterize ginate-based materials, but also polymeric esters,
the industrial compostability of materials, usually de- proteins and other biological macro molecules, since
manding a 90 % decomposition in 180 days, [4] where such organisms can be easily genetically modified
the EN 13432 is probably the most common standard. to produce a wide variety of materials. Plant-based
An additional classification to biodegradable must polymers are mostly based on carbohydrates and
be introduced for this review, which will be named can be obtained from starchy or cellulosic biomass.
bioneutral degradation (see Figure 1 for a summa- Polymers of greater interest in the field of biodegrad-
ry of its definition). While biodegradability requires able polymers are polylactic acid (PLA), and polyhy-
the complete breakdown into water, carbon dioxide droxy alkanoates (polyhydroxy fatty acids). PLA is a
and biomass, bioneutral degradability will include very common thermoplastic for many applications
every substance that will break down into naturally including melt spinning into fibres, mainly for med-
occurring substances in the respective eco system. ical applications. It is also used for the 3D-printing
For practical application, it can be assumed that of structures on textile materials [5].
these reaction products will blend into the natural In general terms, most biodegradable polymers are
substance cycles, without significant environmental esters, since hydrolytic cleavage of esters by enzymes
impacts. This is obviously a question of quantity as is a common reaction in nature (see Figure 2). It is
for the definition of biodegradability as well. It can further assumed that aliphatic esters are of better
be assumed that such residues will be degraded into degradability than aromatic ones, since the former
carbon dioxide and water after some time. may fit better in enzymatic active sites [6].
36 Tekstilec, 2021, Vol. 64(1), 33–47

O
H3C OH
H3C OH
H3C O CH3 + H2O +
O
aliphatic Ester aliphatic Alcohol aliphatic Carboxylic Acid

O OH
H3C OH
O CH3 + H2O +
O
aromatic Ester aromatic Alcohol aliphatic Carboxylic Acid

Figure 2: Hydrolytic cleavage of aliphatic and aromatic esters; hydrolysis is greatly accelerated by catalysts such
as strong acids and bases, but also enzymes. Aromatic esters contain at least one aromatic carbon ring system,
either in the alcohol or in the acid part.

Figure 3: Stages of hydrolysis for polymeric esters, according to new and old definitions

Polyhydroxy alkanoates (PHA) are a class of poly- allows for the production of block-copolymers [9].
mers formally consisting of a fatty acid chain, with Variations of chemically modified substrates can
an additional hydroxyl group that can be used to also be used to produce modified polymers [10]. In
form ester linkages between monomers, which places such cases, however, the environmental impact and
them in the class of bio-polyesters. The degradation corresponding biodegradability must be assessed
of polymeric esters by hydrolysis can reach different individually.
endpoints as shown in Figure 3, while ultimate deg- The main drawback of these polymer types is the
radation will lead to carbon dioxide and water. high cost. Although new developments led to a high
PHAs can be synthesized by different bacteria, which yield of polymer output in bio reactors, production
lead to the different types of esters [7]. Bacteria use costs are governed by the raw materials, namely fatty
these structures for energy storage and internally acids. Production efficiency can possibly be increased
depolymerize these molecules for energy production. through the bioengineering of the corresponding
Since most PHA polymers also depolymerize under microorganisms, while the optimization of the fer-
human physiological conditions, they also are used mentation process may lead to lower production costs
in the medical field in non-textile areas like implants, [11]. Moreover, PHA polymers may be suitable for
etc. [8]. The decomposition products will be hydroxyl specialized applications, where low costs are not the
alkanoates, i.e. fatty acids, which will be easily degra- main requirement.
dable by most natural organisms. Another natural carboxylic acid is hexanoic acid, or
Beside the inherent bioneutral degradation capability capronic acid. The cyclic form ε-capro lactone can
of such polymers, it is interesting to note that ho- be polymerized into poly-ε-caprolactone (PCL). The
mopolymers as well as copolymers can be synthe- material can thus be understood as related to PHA.
sized by using different substrates for the bacteria. Monomeric raw material is usually produced indus-
Furthermore, changing the substrates over time also trially through the oxidation of cyclohexanone that
 Biodegradable Synthetic Polymers in Textiles – What Lies Beyond PLA and Medical Applications? A Review. 37

was derived from benzene in the first place. Most of Other polymers, copolymerized from the building
the PCL available on the market is therefore of fossil blocks of non-biodegradable and biodegradable pol-
origin, although biodegradable. Recent developments ymers, sometimes show a significant biodegradabil-
show processes for synthesizing capronic acid from ity. However, this property is highly dependent on
corn stover and also discuss market opportunities for the ratio of the different monomer types involved.
this approach [12], potentially rendering the polymer If decomposition products occur that are made of
bio-based and biodegradable. the initial building blocks or even of more complex
Polylactic acid (PLA) and polybutylene succinate nature, the sweeping claim of a bioneutral degrada-
(PBS) are also polymers built from natural mon- bility cannot be made as in the aforementioned cases.
omers, so that their decomposition products will In fact, it must be determined whether an ultimate
be lactic acid, succinic acid and a diol component. degradation eventually takes place or an assessment
Because these building blocks are available on large of the residues on the environment is necessary.
industrial scales, a significant cost advantage can be In particular, numerous studies have been conducted
achieved compared to PHA. with the aim of determining whether microorgan-
PLA can be manufactured in three different ways: the isms and/or enzymes are capable of decomposing
direct condensation of lactic acid, azeotropic conden- such copolymers [19−21], sometimes evaluating de-
sation, and ring opening polymerization after prior composition by the weight loss of the polymer [22] or
lactide formation (cyclic lactic acid dimers), where solubility [23]. Although remarkable efforts consider-
the last two methods are the most common ones [13]. ing the amount of polymer types covered were made,
The raw material for all processes is lactic acid, which these works give no insight into biodegradability or
can be produced either by chemical synthesis or the bioneutral degradability as long as xenobiotic mon-
fermentation of carbohydrates. The last process is omer building blocks were involved.
widely investigated and optimized, so that most of Thus, copolymers involving, for example, tereph-
the lactic acid for technical applications is produced thalic acid or 1,4-butandiol may be decomposable by
in that manner [14]. Current processes utilize starchy microorganisms, but the residues must be assessed.
biomass for fermentation, but recent developments Since both substances are xenobiotics, the bioneutral
applying metabolic engineering methods open op- degradability of such polymers cannot be generally
portunities to metabolize lignocellulosic substrates, assumed.
which leads to a further reduction in costs [15]. For Although not biodegradable by any means, it is in-
chemical synthesis, a multi-step approach involving teresting to look at the relatively new substance pol-
the addition of HCN to acetaldehyde forming lac- yethylene furanoate (PEF), which is discussed as a
tonitrile is followed. While the chemical synthesis potential alternative to polyethylene terephthalate
delivers racemic products, stereo-chemically pure (PET). It is partially manufactured from biomass
substances can be obtained through fermentation and, although its production appears to be quite
[16]. Thus, homo- and copolymers of L- and D- forms ambitious, it finds itself at the brink of becoming
can be obtained exhibiting different thermal and me- commercially relevant, which demonstrates that such
chanical properties. processes can possibly be implemented successful-
To obtain PBS, succinic acid is used as a commodity ly. It is obtained through the polycondensation of
that is produced mainly through fermentation [17]. polyethylene 2,5-furandicarboxylate (FDCA) and
Substrates can vary along different types of carbo- ethylene glycol. Publications discussing technical
hydrates, depending on the chosen microorganism. production from lignocellulose [24] and investigating
As a rule, succinic acid is only one single product material properties in depth [25] date back only five
among others in the metabolic cycle of a bacterium. years. The chemical synthesis of furan derivatives as
Accordingly, metabolic engineering is used here too, a precursor is reported by using starch [26] and cel-
to delete pathways for the production of unwanted lulose [27]. An interesting approach for ­synthesizing
by-products [18]. Succinic acid is then directly po- 2,5-­f urandicarboxylate using supported noble met-
lymerized with butane diol to form PBS. al catalysts was reported recently [28]. Industrial
The above-mentioned materials can be classified, at pilot plants started up in 2011 to produce 40 t/a of
a minimum, as bioneutral degradable, since decom- 2,5-furandicarboxylate. In the years that followed,
position will lead to monomeric building blocks that different major chemical companies developed new
all have natural origins. processes, and partially joined forces to increase the
38 Tekstilec, 2021, Vol. 64(1), 33–47

production of FDCA [29]. In 2016, AVA Biochem as bacteria or fungi. For degradation in natural en-
announced its objective to achieve a production ca- vironments, the biodiversity of such organisms is
pacity of 30,000 tonnes/year, increasing to 120,000 crucial for ultimate biodegradability. Testing should
tonnes/year [30]. Textile applications have not yet therefore be done using organisms of ubiquitous oc-
been reported in patent or scientific literature. The currence in the targeted eco system and under re-
material thus seems to be new and interesting as a spective test conditions. For industrial composting,
replacement for PET-based polyesters. This may serve the conditions can be adjusted, so a wider range of
as a promising model for some of the above-men- polymers may be utilized, if such a recycling meth-
tioned processes, which are not yet commercialized. od is targeted. Actually, commonly accepted test
methods do not focus on that issue, which addresses
3.1 Thermal properties a regulatory gap, should these substances gain wider
For technical applications, the thermal properties market relevance.
of the materials are of crucial interest. In Table 1, Bioneutral degradation can hypothetically occur
glass transition temperatures and melting ranges are chemically, since most of the mentioned polymers
shown for different homopolymers. Specific require- will eventually be hydrolysed. However, the rapid
ments will evolve from targeted applications, and environmental ability to hydrolyse and lifetime dura-
polymers can be adapted through either copolymer- bility frame a solid conflict of interest, which may be
ization or blending. As long as bioneutral degradable solved best only for single-use products or materials
components are utilized, degradability should not for indoor applications.
expect to be altered. However, secondary reactions Degradation by microorganisms can take place intra
are possible and should be assessed before larger or extra cellular. In the latter case, enzymes are se-
commercialisation efforts. creted in the substrate which catalyse the degradation
reactions. In every case, the physical properties of the
Table 1: Thermal properties of selected biodegradable polymer also contribute to the degradation proper-
polymers and PA, PP for comparison [31−34] ties. Besides the molecular weight, the crystallinity
of the polymer also influences the degradation rate,
Biodegradable Tg (°C) Tm (°C)
since amorphous phases are generally more prone to
polymer
the enzymatic attack [35, 36]. Also, higher melting
PLA 45–60 150–162 temperatures are usually linked to the reduced ability
PLLA (L isomer of 55–65 170–200 to achieve enzymatic hydrolysis [37].
PLA)
PCL −60–−65 58–65 5 Costs
PHB 5–15 168–182
PH-octanoate −32.6 162 Many promising chemical efforts have been made
PBS −28.5 116.4 to develop polymers with their respective produc-
tion process to potentially produce biodegradable
PA 50 265
products. The issue of costs nevertheless remains a
PP −15 176 drawback. In 2000, the costs of PLA were estimated
to be approx. five times that of PP, and PHA noted
A wide window of technical opportunities can be even more. A comparison with other commodity
utilized by copolymerization, blending and the ad- plastics do not show other major differences [38].
dition of plasticizers. Such additives need to be bio- Ten years later, prices were reported to USD 3.5 to
degradable too, so a wide range of materials can be 4.5/kg for PHB and GBP 1.5 to 2.5/kg for PLA, while
considered, which is not covered here, but maybe in a prognosis for PHA cited that price could reach as
a future overview. low as EUR 1 to 2/kg [39]. In late 2017, prices for com-
modity polymers (US export) are as follows: USD
2.7/kg for PET, USD 8.4/kg for LDPE (low density
4 Degradation pathways polyethylene), USD 9.2/kg for PA and USD 1.9/kg for
PLA [40] However, a wide range of prices was found
The molecular biodegradation of organic substances depending on the exporting country. This shows that
is usually conducted using microorganisms, such at least PLA prices are similar to those of c­ ommodity
 Biodegradable Synthetic Polymers in Textiles – What Lies Beyond PLA and Medical Applications? A Review. 39

­ olymers. Since lactic acid for the production of PLA

p Since the initial manual overview showed a high
is mostly synthesized through fermentation and PLA number of papers dealing with electrospun PLA na-
is gaining market share, the reduction in price may nofibres mostly for medical applications, both results
be a scaling effect. From this, it can be estimated that were filtered in JabRef using abstract!=PLA and ti-
prices of other polymers such as PHA/B and PBS will tle!=PLA and abstract!=nanofib and title!=nanofib
also be competitive, if scaling markets will allow for and abstract!=electrospun and title!=electrospun
that. Available data for the commodity pricing of and title!=lacti, which excludes publications with the
PHB is rare, but Mudliar et al. published an evalua- respective substrings in the title leaving 95 results
tion of production costs for a hypothetical produc- that were manually evaluated by title and abstract,
tion plant, and determined a value of USD 5.38/kg delivering 47 results.
for the best investigated case [41]. A similar approach was applied for PLA and electro-
spun nanofibres, delivering 45 and 15 results, respec-
tively, regarding these topics alone.
6 Textile applications For the topic of biodegradable coatings, Clarivate’s
Web of Science was queried using ts=(biodegradable
Synthetic polymers in textiles can be considered coating$) AND (ts=textile$ or ts=fibre$ or ts=fabric$)
in three fields: the fibrous material itself, coatings AND ti=biodegradable.
and finishings, and fibre-reinforced composites. A patent search was conducted exclusively for
The latter has already been widely investigated for the coating topic using ti=biodegradable UND
example using natural fibres and bio-based or bio- PUB>1.1.2000 UND AB=coating UND (AB=textile?
degradable polymer matrices. Since matrix devel- ODER AB=f ibre? ODER AB=f ibre? ODER
opment is a broad field and is also closely linked to AB=fabric?) NICHT ti=wound NICHT ti=medical,
the used fibres, this topic is not further discussed delivering 132 results which were manually revised,
here. However, interesting opportunities are given leaving 25 hits for further evaluation. Ti searches
in the field of coating and finishing, and in the field in the title, PUB defines the publication time, AB
of fibrous raw materials. searches within the abstract and the question mark
acts as wildcard for one or more characters. Since the
Research method search engine is German, the operator UND stands
To assess the current situation regarding the use of for and, ODER for or, and NICHT for not. However,
biodegradable polymers in these fields, a systemat- international patents from the world patent office
ic literature and patent review was conducted. For (WPO) were also delivered by these queries.
this, the academic search engines Google Scholar,
Microsoft Academic, Crossref, and Clarivate’s Web Results for PLA and electrospun fibres for
of Science were consulted, while the patent research medical applications
was conducted using a search engine provided by the As expected, PLA and its derivatives are the most
German patent office. common biodegradable polymers for fibre fabrica-
The first three databases were queried using the key- tion. A wide field of application is given in medical
words “biodegradable polymers” and a search peri- contexts. For example, stents made from PLA and
od of the last 30 years if applicable. This delivered coated by a layer-by-layer technique with chitosan
approx. 2,000 results. The results were exported to have been investigated [43]. Scaffolds for tissue
the open source literature database JabRef [42] and engineering are another field where physiological
filtered by the regular expression title=”fibre” or ti- biodegradation is useful. The degradation of PLA
tle=”fabric” or title=”textile”, resulting in 83 hits. in vivo may lead to local decrease of pH due to
Clarivate’s Web of science was queried using the reg- the produced lactic acid, while medium molecu-
ular expression ts=(biodegradable polymer$) AND lar weight oligomer degradation products can also
(Ti=textile$ or ti=fibre$ or ti=fabric$) to search with- potentially initiate immune responses in some pa-
in the category of biodegradable polymer(s) for pub- tients. It is therefore crucial to understand the influ-
lications with textile(s), fibre(s) or fabric(s) in their ences or fabrication parameters on the d ­ egradation
titles. The results were then refined using the Web rate, since extrusion speed and twist of the spun
of Science category Materials science, subcategory PLA fibres is reported to have an impact on those,
textiles, delivering 81 results. besides the chemical composition of the polymer
40 Tekstilec, 2021, Vol. 64(1), 33–47

[44]. Further research in that direction was done by incorporating additional substances, such as phar-
studying the influence of plasma treatment on the maceuticals, make these materials interesting can-
moisture wicking behaviour of PLA fabrics [45]. didates for drug delivery [56, 57]. A material spun
Shape memory textiles are interesting materials from polyethylene oxide and poly vinyl alcohol was
in the medical field, for example for self-adjusting investigated for the use as a scaffold for potential tis-
implants, scaffolds or anchor systems for grafts. sue engineering [58]. In addition, blends of PLA and
Nonwoven materials fabricated using melt blown PCL with added hydroxyl apatite were investigated as
PLA-PHB blends have shown shape memory prop- electrospun nanofibre mats [59]. Additional insights
erties while being biodegradable [46]. Biodegradable on electrospun biodegradable scaffolds are given by
ligament replacements can be considered to be made Sun et al. [60]. A further detailed review on biode-
of PLA-PCL copolymers, so their creep and stress-re- gradable polymers for tissue engineering is also given
laxation properties have been investigated [47]. by Xing et al. [61].
The rheological properties of PLLA and PLDA (L
and D isomers of PLA) have been studied to produce Summary of medical applications of PLA
physiological degradable fibres having a potential A wide range of ambitious applications can be seen
drug delivering property [48]. Hollow PLA fibres ob- for the utilization of PLA fibres in the medical sector.
tained by melt spinning can serve as platforms for the Electrospun nano fibres made from physiologically
delivery of drugs in the medical field, but also for the degradable polymers are promising substrates for
retarded release of pesticides in agricultural settings. tissue engineering and drug delivery.
Melt spun PLA 9 fibres have been investigated for that It is therefore obvious that lots of effort is currently
purpose based on different physical properties [49]. directed to that area. It is furthermore known that
Sutures are another field where PLA is a useful pol- commercial feasibility is crucial for the widely ac-
ymer. The stiffness of pure PLLA was reported to be cepted clinical use of medical products. One pathway
reduced by blending with PLA-co-caprolactone co- is keeping the investment burden low by addressing
polymer [50]. regulatory issues in the early stages of research. This
In addition, potentially implantable sensors made is especially necessary for the development of new
from PLA components have been reported, with the textile products in that field, since they mostly ad-
advantage of not requiring explantation after therapy dress market fields with modest profit opportunities.
[51]. A special composite made from PLA and CNTs
was produced using a melt blown process to produce Results beyond PLA and medical applications
sensory fibres [52]. Research in biodegradable polymers in the textile
The antibacterial properties of PLA fibres coated with context, excluding PLA and medical textiles, has
titanium oxide have been investigated. However, the been reported in fewer publications.
use of such material in medical applications requires A drawback of PHBV (poly hydroxy butyrate valer-
a thorough assessment of possible side effects and ate) lies in its low crystallization rate, which challeng-
cytotoxicity [53]. es melt spinning. Hufenus et al. investigated a core
It can often be seen that lots of effort is put into devel- shell structure with PLA in different configurations,
oping new medical materials or devices, but regulato- together with a special spinneret, to overcome this
ry issues are not addressed in the early stages of such issue [62]. As early as 2000, Schmack et al. investigat-
research. This can lead to obstacles in the subsequent ed the melt spinning of PHB and the dependency of
development to commercialized medical products drawing speed on the resulting crystal structures us-
[54]. Commercially available melt spun PLA fibres ing wide‐angle X‐ray scattering [63] for use in textile
often contain finishings from secondary spinning, applications. PHB and PHBV have limitations in the
which may hinder medical uses. Jozwicka et al. stud- melt processing, since at higher temperatures (above
ied different PLA fibre types and found glycerol as a 160 °C as reported), cis-elimination leads to random
suitable finish for medical appliances [55]. chain breaks. Moreover, bacterially produced PHB is
Electrospinning is a process capable of delivering strongly isotactic; together with its glass transition
nanofibre fabrics exhibiting a high surface area and temperature of 5−15 °C, the material shows significant
small pore sizes, but can only be utilized in small brittleness. The underlying cause of high crystallinity
scales. This issue renders the process suitable for only lowers its degradation rate under physiological con-
specialized applications. However, the possibility of ditions [64]. The authors also summarized different
 Biodegradable Synthetic Polymers in Textiles – What Lies Beyond PLA and Medical Applications? A Review. 41

works dealing with spinning conditions to control the Results of biodegradable textile coatings
crystallisation behaviour of the spun fibres, including During the review of literature, it became evident
the use of cyclodextrins as nucleation agents. that almost no scientific publications exist that ad-
Bicomponent fibres were also studied based on the dress the coating of textiles using biodegradable
poly butylene terephthalate/poly butylene succinate polymers, with some exceptions in the medical field
lactate system. The drawing speed influenced the core utilizing chitosan. Consequently, an additional liter-
shell ratio, while the range between 65% and 35% ature search was conducted, together with a patent
delivered the maximum fibre strength [65]. Also, here search on that topic.
the ultimate biodegradability can be questioned due Some authors have reported the development of a
to the terephtalic acid monomer. Although less toxic, super hydrophobic coating made from soya bean oil,
the substance can be considered a xenobiotic. stearic acid and ZnO [68]. This approach will proba-
Twarowska-Schmidt evaluated two commercially bly lack an ultimate biodegradability because of the
available PBS derived polyesters (poly butylene succi- ZnO particles. A similar approach was established
nate adipate (PBSA) and poly butylene adipate tereph- using poly dopamine [69]. Yarn sizing using nano
thalate) in terms of their fibre forming capability in a cellulose and soy protein has been investigated [70].
melt spin process, as well as their degradability. For the Antibacterial coatings achieved by silicone contain-
latter, only the weight loss of the fibres was recorded, ing cations have also been reported [71], but the ul-
so it is highly likely that at least terephtalic acid or po- timate biodegradability can be questioned, at least
tentially oligomers will be found in the substrate. As because the ultimate degradation of silicones is not
expected, the aromatic ester was degraded to a higher defined. As a result, the most meaningful definition
extent, but this only remains true for higher degrada- may state silicon oxide as end product.
tion temperatures. Thus, the general rule for the ali- The patent search delivered even fewer results, ex-
phatic esters is only partially valid here. Although the cluding medical applications. Glycerol together with
low glass transition temperatures of the materials (-33 gelatine for coating of natural fibres is described in
°C and -44 °C) can be an issue for apparel, technical KR000100647872B1 (2006). A coating for a biode-
applications such as those in the medial or agricultural gradable textile is described in FR000002879224A1
sector are considered to be feasible [66]. (2004) using natural rubber latex, and proteins. The
The cost issue of PHA is addressed by a recent pub- coating of sheet substrates and fabrics is consid-
lication regarding the production of PHB in cyano- ered in US020050031882A1 (2005) by PHA copol-
bacteria [67]. However, commodity prices for PHAs, ymers. An aqueous dispersion of PHB is described
PBS or similar polymers are not available, since the in EP000001566409A1 and in JP002004099883A
materials are not yet commercialized. (2003) for PVA, which can potentially be applied as
a coating. JP002003221786A (2002) utilizes PVA to-
Summary beyond PLA and medical gether with sulfonic acid polymers for polyester fibre
applications finishings. However, the sulfonic acid polymer may
The remaining field, after excluding medical applica- not be ultimately biodegraded. The Canadian appli-
tions, composites and PLA materials, spans mostly cation CA000002410457C (2010) deals with different
across PBS and different types of PHA. The produc- PHA copolymers for the coating of fabrics, threads or
tion of fibrous materials out of these polymers re- yarns. In JP002002121288A (2002), the use of more or
mains challenging, when mechanical requirements less degradable plasticizers for formulating an aque-
set higher stakes. While the degradation over time ous dispersion of a biodegradable resin is claimed.
is the key feature in drug delivery systems, technical
applications require specific tensile stiffness, elonga- Summary of biodegradable textile coatings
tion behaviour, brittleness, etc. together with textile Scientific literature only discusses textile, biodegrad-
haptics in the final fibrous product. Furthermore, the able coatings for non-medical applications to a lesser
processing properties of the polymer must be met, extent. However, patent literature shows some evi-
e.g. processing temperatures, viscosities and crys- dence for commercial attention in that area, although
tallization rate, to successfully melt spin them into this is also limited. The patents found likely address
these fibres. Subsequently, the produced fibres must textile coatings more as an additional option. But
be spun secondarily to yarns and woven, knitted or aqueous coating dispersions are also discussed there,
fabricated otherwise into textiles. which is valuable, since the discussed polymers in
42 Tekstilec, 2021, Vol. 64(1), 33–47

this study are thermoplastics and one would con- The direct utilization of fibrous materials in apparel
sider extrusion coating in the first place. However, a can be considered. For this, however, different issues
water-based coating is a common textile technique, must be addressed: Again, the material properties
and the associated patents allow for conceiving such must be designed so that production on conventional
an application onto textiles too. machinery for all intermediate semi-finished prod-
PVC (polyvinyl chloride) is a cheap and widely uti- ucts is realizable. Secondly, the degradation rate must
lized coating substrate for textiles, but acrylates and be tailored so that it will not take place at significant
polyurethanes are also applied. Thus, it is somehow rates during the normal product life. Thus, hydrolyz-
surprising, that nearly no biodegradable alternatives ability issues might need to be addressed. PHAs, in
are discussed in recent literature. particular, may release fatty acids during hydrolyza-
tion, which can lead to olfactory discomfort, even in
lower amounts that do not affect the substrate’s me-
7 Future opportunities chanical stability. Furthermore, such new products
should exhibit comfortable textile haptics. However,
Younes classified different biopolymers regarding synthetic materials offer numerous opportunities to
their commercialization in a review in 2017. Classes fine tune these kinds of properties.
ranged from research, pilot plant, commercial, large The literature and patent search resulted in a sig-
scale, to mature [72] Maturity was assigned only to nificant gap in the field of textile coatings. A few
cellulosic materials, which is not surprising. PLA was research bodies are already aware of this gap [73].
noted as the only one in the large scale group. PHA/B It is therefore a highly interesting field for research
was classified between pilot plant and commercial, and new developments. It is also interesting for re-
and PBS in the research state. It can be assumed that cycling purposes to develop materials composed
cost effects play a major role here, since petrol-based of similar chemical substances, since no material
and non-biodegradable polymers are usually more separation is necessary. The variety of synthetic
cost efficient. Congruent with his findings is that PLA biodegradable polymers due to the abundance of
is narrowing its price gap to petrol-based commod- raw materials, and the ability to form blends, co-
ity polymers. In the medical sector, physiological polymers and introduce additives can pave a way to
biodegradability represents an additional function coated textiles, where the fibrous substrate and the
that justifies higher costs. However, public pressure coating are made at least of similar biodegradable
and/or regulatory issues may shift parts of the textile chemistry. Biodegradable fibres, either natural or
economy to biodegradable materials. manmade, are gaining market share in the technical
In the sub field of geo textiles, biodegradability can textiles sector, while biodegradable coatings seem to
be conceived as an additional function, making it an lie inevitably on the way.
interesting application sector. The need for develop- Coatings can be applied on textiles through the ex-
ment is given by the tailoring of the degradation rate, trusion of thermoplastics or by applying aqueous dis-
depending on operational conditions. It would also persions of polymers, e.g. by knife coating or other
be a great advantage if such geo textiles could be fab- means. One research target is therefore the manu-
ricated with a defined lifetime and if the degradation facturing of such stable and applicable dispersions
rate over time could be engineered. But as discussed with the new polymers, which includes issues such as
previously, manufacturing requirements must also viscosity tailoring, degradation and storage stability,
be met by such new materials. Meeting both chal- and drying properties of the applied wet film.
lenges may lead to new products, which could result In addition, crosslinking offers the opportunity to
in higher market prices. It should be noted that dif- develop possibly biodegradable duromers, which
ferent semi-finished products can be found on the may also help to enhance the mechanical stability of
path from polymer, over fibres, yarns, possibly textile such coatings. It is thus additionally of fundamental
surfaces or nets to the finally confectioned product. research interest to study the degradation pathway
Thus, many production steps must be covered. and decomposition products of such crosslinked
Other fields in technical or apparel textiles will most polymers.
probably not make use of the biodegradation func- Further general fields of research are the develop-
tion directly. That function may, however, be benefi- ment of biodegradable plasticizers, flame retardants,
cial in the recycling of these products. crosslinkers, and other additives.
 Biodegradable Synthetic Polymers in Textiles – What Lies Beyond PLA and Medical Applications? A Review. 43

8 Potential textile products it a promising field of further development, given

that textile base substrates will be replaced by more
Many textile products can be conceived assuming eco-friendly substances in the future.
the successful outcome of the above-described re-
search and development efforts. To start with, blend-
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