PERSPECTIVE
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Toward Sustainable Fiber-Reinforced Polymer Composites

Iris Elser* and Michael R. Buchmeiser*

Dedicated to Prof. Dr. Rolf Mülhaupt on the occasion of his 70th birthday

Fiber-reinforced polymer composites (FRPCs) are versatile materials with
applications in diverse fields such as transportation, construction, and
electronics. With the composites market expected to reach 15.5 Mt by 2026,
increasing the sustainability of FRPCs is imperative. The main factors driving
the sustainability of FRPCs, namely end-of-life management and recyclability,
the use of natural, bio-based, and sustainable materials, as well as
biodegradability and product simplification are presented and discussed.

1. Introduction

Fiber-reinforced polymer composites (FRPCs), consisting of a
polymer matrix reinforced with fibers, find wide-spread appli-
cation. The main industries using FRPCs are the transporta-
tion (28%), construction (20%), electronic/electrical (16%), and
pipelines/tanks (15%) sectors (Figure 1).[1] Glass fibers (GFs), fol-
lowed by natural fibers and carbon fibers (CFs) are the most com-
mon reinforcement materials, while thermoset matrices domi-
nate over thermoplastic matrices (Figure 1).

In 2021, the global composites market was estimated at 12 Mt
and 37 B$. By 2026, the market is forecast to reach 15.5 Mt.[1]

Future growth is expected to come from markets where compos-
ites are already well established, but also from the penetration
of new sectors made possible by technological breakthroughs.
The associated increase in resource consumption (water, en-
ergy, chemicals) and waste streams (greenhouse gases GHG,
wastewater, and chemicals) raises the question of sustainability.
Efforts for more sustainability are also driven by new national
and international regulations and policies such as the European
Union´s Green Deal[2] or the Circular Economy Action Plan[3]

and by rising public concerns on topics like climate change or

I. Elser, M. R. Buchmeiser
Deutsche Institute für Textil- und Faserforschung (DITF)
Körschtalstrasse 26, D-73770 Denkendorf, Germany
E-mail: iris.elser@ditf.de; michael.buchmeiser@ipoc.uni-stuttgart.de
M. R. Buchmeiser
Institute of Polymer Chemistry
University of Stuttgart
Pfaffenwaldring 55, D-70569 Stuttgart, Germany

The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/mame.202400013

© 2024 The Authors. Macromolecular Materials and Engineering
published by Wiley-VCH GmbH. This is an open access article under the
terms of the Creative Commons Attribution License, which permits use,
distribution and reproduction in any medium, provided the original work
is properly cited.

DOI: 10.1002/mame.202400013

microplastics. The latter are defined as poly-
mer particles <5 mm in size.[4] Key parame-
ters for achieving sustainability in compos-
ites are end-of-life management and recy-
clability, the use of natural, bio-based, and
sustainable materials (fiber/matrix), as well
as biodegradability and product simplifica-
tion. At the moment, the majority of FR-
PCs are landfilled at their end-of-life, as re-
cycling is costly and energy-intensive.[5] As
an example, 35% of CF-reinforced polymer

composites (CFRPCs) and 67% of GF-reinforced polymer com-
posites (GFRPCs) were landfilled in the UK in 2020, while only
20% of CFRPCs and 13% of GFRPCs were recycled and a negligi-
ble amount of 2% of CFRPCs and 6% of GFRPCs were reused.[6]

Recycling of FRPCs is complicated by the complexity of the waste
(material mix), impurities in post-consumer products, and un-
derdeveloped infrastructures for waste collection. Additionally,
material properties typically deteriorate as a result of the harsh
recycling conditions and either the matrix or fibers are retrieved,
but seldom both.[7] Consequently, costs for existing technologies
are high and the market for recycled materials is limited. Nev-
ertheless, an increase in recycling of FRPCs is mandatory to in-
crease the sustainability and circularity of the FRPC market. For
example, WindEurope, a consortium of over 500 companies, pub-
lished a position paper committing to reuse, recycle, or recover
100% of decommissioned blades by 2025, with blade waste ex-
pected to reach about 25 000 tons per year by 2025.[8]

Generally, any meaningful recycling may not be ars gratia ar-
tis and should therefore require less energy and resources, in-
cluding air and water, than are necessary to produce new ma-
terial. The replacement of fossil-based feedstocks with natu-
ral or bio-based feedstocks is an important step in increasing
the sustainability of FRPCs. Even better is the production of
FRPCs from bio-based and bio-degradable plastics. Bio-based
plastics are plastics made from renewable resources (biomass,
waste), while biodegradable plastics are plastics that can be
assimilated by bacteria or fungi to give environmentally be-
nign products (Figure 5).[9] Not all bio-based materials are
biodegradable. Nevertheless, some petrochemistry-based poly-
mers like poly(butylene adipate terephthalate) PBAT can also be
biodegradable.[9] Biodegradability is especially important in the
context of long-term macro- and microplastics pollution. Plastic
pollution is impressively illustrated by the Great Pacific Garbage
Patch located in the north pacific, covering an area of 1.6 million
km2 of ocean surface.[10,11]

In addition, microplastics contribute to pollution. The top ten
major contributors to microplastics pollution are wear and tear of
tires, emissions during waste disposal, abrasion of asphalt, pel-
let losses, drifts from playgrounds and sports fields, release at

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Figure 1. Composite use expressed in numbers: Main applications and commonly used fiber and matrix materials.[1]

construction sites, abrasion of shoe soles, plastic packaging, road
markings and abrasion of textiles during washing (Figure 2A).[12]

The complexity of plastic waste in general is a major obstacle
to its recycling. In 2020 plastic waste recycling rates for single-
variety plastics were 13 times higher for separate compared to
mixed waste collection schemes in Europe (Figure 2B).[13]

With composites and multilayer packaging made of var-
ious interwoven materials, separation becomes increas-
ingly difficult.[14,15] Consequently, there is a trend toward
mono-material solutions, albeit often at the cost of material
performance.[15]

2. Current Recycling Strategies

Overall, CF-based composites are recycled more often than GF-
based composites, as the higher market value of carbon (≈20 $
kg−1) versus GFs (≈2 $ kg−1 for E-glass) makes recycling more
economically viable.[16,17] Contrastingly, GFs account for 88% of
fibers used in FRPCs, while CFs account for only 1%.[1,18] Exist-
ing recycling technologies include thermal recycling (pyrolysis),
mechanical recycling (grinding/shredding), and chemical recy-
cling (solvolysis) (Figure 3).[16,19]

In mechanical recycling, multiple steps of size reduction in-
cluding shredding and grinding lead to resin- and fiber-rich

fractions.[18,20] The different fractions are separated with the aid
of cyclones, sieves, zig-zag air classifiers, flotation separators,
or electrostatic separators.[5] While resin-rich fractions are of-
ten used as fillers, fibrous fractions find new applications as
reinforcements in the form of short fibers. Mechanical recy-
cling is mainly used for GFRPCs, as, in contrast to other re-
cycling techniques, the fibers are not retrieved in “pure” form
and the products have a rather low value. In contrast, thermal
and chemical recycling lead to higher-value fibers while using
more energy and are therefore more often used for CFRPCs.[5]

Recently, electrodynamical fragmentation and high-voltage frag-
mentation (HVF), respectively, found application in the size re-
duction of CFRPC and GFRPC wastes.[20–25] Both methods utilize
high voltage pulses (≈50–200 kV) to break down the composites.
A study comparing conventional mechanical recycling to HVF
for GFRPC waste found that HVF of GFRPC produced cleaner
fibers and a broader fiber length distribution with a higher per-
centage of fibers at the mean fiber length.[22] In addition, the re-
tained resin content for HVF was lower than that observed for
mechanical recycling, thereby increasing the value of the recy-
cled GFs. The main thermal recycling methods are pyrolysis and
fluidized beds.[6] In thermal recycling, fibers are recovered from
the (thermoset) matrix by a high temperature treatment ranging
between 450 and 700 °C.[18] During pyrolysis, FRPCs are heated

Figure 2. A) Top ten contributors to microplastic pollution.[12] B) Fate of plastic waste from mixed and separate waste collection schemes in Europe in
2022.[13]

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Figure 3. Main recycling methodologies for FRPCs.

to 450–700 °C under inert gas in the absence of oxygen. Pyrol-
ysis of GFRPCs at 500 °C afforded recovered GFs with tensile
strengths of 65% of the initial value.[19] In contrast, pyrolysis
of CFRPCs below 600 °C led to recovered CFs with mechani-
cal properties (80–95% of tensile strength of virgin fibers) and
surface properties similar to the virgin fibers.[19] Pyrolysis has
also been performed using microwaves.[17] Microwave-assisted
pyrolysis has the advantages of fast heat transfer deep into the
FRPC core and minimum heat loss to the environment.[19] The
fluidized bed method involves burning the matrix in a hot (450–
550 °C) and oxygen-rich air-stream. The fibers are recovered by
a cyclone while the matrix is used for energy recovery in an af-
terburner. For both GFRPCs and CFRPCs, a reduction in the
recovered fiber length as well as an unstructured or fluffy fiber
architecture were observed.[17] Additionally, fiber strengths de-
creased to 25−50% of the initial value.[5] In general, thermal
recycling allows both fiber and energy recovery from the ma-
trix. The degree of fiber degradation differs for GFs and CFs.[20]

Both, the high thermal stability and the high cost of CFs, make
CFRPCs more suitable for thermal recycling. As a result of the
higher thermal stability, CFRPCs often retain their mechani-
cal properties better after thermal recycling than GFRPCs.[6,26]

To counteract the reduced mechanical properties of GFs re-
sulting from thermal recycling, several post-treatment methods
have been developed. Chemical etching and post-silanization re-
stored 30–70% of the lost mechanical properties, while the so-
called short-hot sodium hydroxide solution treatment restored
75% of the suffered strength-loss.[27–29] Furthermore, metal ox-
ide catalysts have been introduced to facilitate resin decompo-
sition during thermal recycling of GF-reinforced epoxy, result-
ing in shorter processing times and significantly reduced energy
consumption.[30,31] The strength of the recovered GFs was in-
creased when catalysts were used. In addition, varying the at-
mosphere in the pyrolysis chamber from vacuum to nitrogen
and to superheated steam, respectively, allowed the process to be
fine-tuned for specific FRPCs.[6] Chemical FRPC recycling com-
monly involves solvolysis of the matrix resin with reactive media
at temperatures around 350 °C while the fibers remain. Com-
pared to thermal recycling, chemical recycling recovers longer,
cleaner, and less damaged fibers[20] with reasonable mechan-
ical properties compared to the virgin fibers.[17,32] While low-
temperature solvolysis is usually conducted at ≈200 °C in the
presence of catalysts and an acid or nucleophilic solvent, high
temperature solvolysis applies supercritical fluids (mostly water
or alcohols).[33,34] Fluids previously used in the solvolysis of CFR-
PCs include acetone, methanol, ethanol, propanol, and water.[16]

The energy demand is highest for chemical recycling (21–91 MJ
kg−1), followed by thermal recycling (24–30 MJ kg−1), and the
least energy-intensive mechanical recycling (0.1–4.8 MJ kg−1)
(Figure 4).[17]

Figure 4. Average energy demand in MJ kg−1 for virgin fibers compared
to common recycling methods for FRPCs.[17]

All described recycling methods except mechanical recycling
require high amounts of energy, associated with high costs. How-
ever, the scale-up of recycling methodologies is expected to in-
crease energy efficiency, which can make recycled fibers compet-
itive to virgin fibers (CF: 183–286 MJ kg−1, GF: 13–32 MJ kg−1),
especially in the case of CFs (Figure 4).[5] Of note, all the above-
mentioned recycling processes focus on fiber recycling, while the
matrix is used for energy recovery only.

3. Sustainable Fiber and Matrix Materials

Both, matrices and reinforcement fibers, can be bio-based or
bio-degradable (Figure 5). Conventional petrochemical polymers
from alternative bio-based or recycling-derived monomers, so-
called drop-ins, or completely novel bio-based polymers can be
employed.[9] Additionally, in terms of reinforcement, natural
fibers can be used.[35–38]

Indeed, after GFs (88%), natural fibers (11%) are the second
most employed reinforcements in composites (Figure 1).[1] The
production of 1 ton of continuous filament GF products from
raw materials emits between 1.4 and 2.2 tons of CO2 equiva-
lents. In comparison, natural fibers only emit between 0.3 and
0.7 tons of CO2 equivalents.[39] Natural fibers can be of plant, an-
imal, or mineral origin.[40] While animal-derived fibers mostly
consist of proteins, plant-based fibers mainly consist of cellu-
lose, hemicellulose, lignin, and negligible amounts of waxes
and pectin.[40] Cellulose is mainly responsible for fiber tensile
strength, and hemi-cellulose is responsible for moisture ab-
sorption, thereby enhancing degradability. Lignin links cellu-
lose and hemi-cellulose and provides rigidity to the plant cell
wall.[40] Plant-based cellulosic fibers are usually classified as seed
fibers (coir, kapok, palm), bast fibers (jute, flax, ramie, hemp, ke-
naf), leaf fibers (sisal, pineapple leaf fiber, banana fiber, bam-
boo fiber), or agricultural waste fibers (bagasse, corn stalk, rice
straw).[7] Most cellulose fibers in natural fiber-reinforced com-
posites (NFRPCs) are bast fibers like flax, hemp, and kenaf, as

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Figure 5. Options for sustainable fiber and matrix materials.

well as recycled cotton.[41,42] Their abundance, light weight, high
sustainability, low costs, and lower abrasive characteristics com-
pared to GFs make natural fibers excellent candidates for FRPCs
(Figure 6).[7,35,37] Compared to synthetic fibers, natural fibers have
a low density. For example, the average natural fiber has a den-
sity of ≈1.5 g cm−3 while GFs have a density of ≈2.5 g cm−3.[43]

A large number of NFRPCs has been synthesized and used com-
mercially. In fact, NFRPCs found numerous commercial appli-
cations in the automotive sector, mainly in door and headliner
panels, seats and carpets.[38] Additionally, flax and hemp com-
posites found application in sports equipment and acoustic pan-
els as their vibration damping is at least 2.5 times higher than
for CFRPCs.[44–46] Despite their many advantages, NFRPCs often
suffer from inferior mechanical properties compared to GFs and
CFs (Figure 6), incompatibility between the hydrophilic fibers
and the hydrophobic matrices as well as high moisture absorp-
tion (swelling) resulting in low durability.[7,47] Additionally, the
variability of the feedstock, (i.e., length and diameter) as well
as competition with agricultural land pose challenges to their
application.[7]

To overcome the often-inferior mechanical properties of nat-
ural fibers compared to synthetic fiber-reinforced composites,
various fiber treatments are applied (Figure 7).[47–51] As cellulose
is largely responsible for the good mechanical and thermal prop-
erties of plant-based natural fibers it is not surprising that many
chemical surface treatments aim to increase the cellulose con-
tent by removing excess amorphous constituents (hemicellulose,
lignin, wax).[40] Additionally, chemical surface treatment changes
the morphological properties of natural fibers and is used to im-
prove fiber–matrix bonding. Care must be taken to avoid cellulose
degradation in the process.[51] Morphological properties (fiber
roughness) were also improved by physical methods. Popular
chemical treatment methods include alkaline treatment (mercer-
ization), bleaching, acetylation, and the use of coupling agents

Figure 6. Comparison of specific properties of glass fibers, carbon fibers,
and natural fibers.[35]

(silane, maleates).[48] Examples of physical methods are corona
or plasma treatment.[48] Mercerization, the treatment of natural
fibers with aqueous sodium hydroxide solution, often leads
to increased surface roughness resulting in better mechanical
interlocking and cellulose exposure to the surface.[47,49,51] Bleach-
ing aims at the removal of surface lignin after mercerization
by treatment with, for example, hydrogen peroxide and sodium
hydroxide.[48] Acetylation after a preceding alkaline or bleaching
step by reaction with acetic acid and acetic anhydride leads to an
improvement in fiber–matrix adhesion by reducing hydrophilic-
ity and moisture adsorption.[48] Coupling agents like silanes or
maleates provide covalent linkages between fibers and matrix.[48]

Treatment with plasma increases fiber roughness.[48] Overall,
surface treatments often require large amounts (often excess) of
hazardous chemicals, result in large waste (water) streams, or
need a lot of energy, thereby counteracting the inherent sustain-
ability of natural fibers.[43] In an effort to increase the sustain-
ability of fiber treatments, an ionic liquid (IL) has been used as a
green alternative to modify cellulosic fiber surfaces, resulting in
improved surface hydrophobicity but also a decrease in thermal
stability.[52]

In addition to chemical and physical treatments, raw natural
fibers often have to be processed into a continuous fiber product
to obtain high quality reinforcement.[53] Hence, the production of
so-called man-made cellulosic fibers (MMCFs) was pursued.[54]

Cellulose is non-meltable, consequently, melt-spinning is not an
option. Instead, wet spinning approaches must be considered.
As cellulose is insoluble in water and most organic solvents,[55]

the emergence of cellulosic fibers is closely related to the de-
velopment of solubilizing methods or suitable solvents. The
frequently used viscose process for cellulose fiber production is
an example of a solubilizing method (Figure 8).[55–58] Initially,
the pulp is activated in aqueous alkaline medium followed by
solubilization through reaction with CS2. The resulting cellulose
xanthate solution is spun into a sulfuric acid bath to afford vis-
cose fibers. To overcome usage of highly toxic CS2 and corrosive
sulfuric acid, the more step-efficient Lyocell process has been de-
veloped (Figure 8).[59] In the Lyocell process, cellulose is directly
dissolved in N-methyl morpholine-N-oxide (NMMO) without
a previous solubilizing step and spun by air gap spinning.[60]

The spinning dope must be stabilized by additives like isopropyl
gallate to prevent side reactions.[61] In the pursuit of more
environmentally friendly solvents for cellulose, Swatloski et al.
established ILs that successfully break the inter- and intramolec-
ular bonds in cellulose.[62] ILs offer low vapor pressures, low
flammability, and good recyclability. The efficiency of an IL to
dissolve cellulose has been shown to depend on both, the struc-

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Figure 7. Chemical and physical surface treatment for natural fibers.[47–51]

ture of the anion and the cation and the DP of the cellulose.[55]

The solubility of cellulose is highly dependent on the structure
of the IL. While good solubility was correlated with anions
having a high propensity to form hydrogen bonds (chloride,
carboxylate, phosphate), anions with a low ability to form hy-
drogen bonds were described as non-solvents (tetrafluoroborate,
hexafluorophosphate, bis(trifluormethylsulfonyl)imide).[63–68]

Some non-solvents (e.g., 1-butyl imidazolium hydrogen sulfate)
were able to exclusively dissolve hemicellulose and lignin, which
is of considerable interest for the pretreatment of lignocellulosic
biomass.[69–71] Similarly, the cation structure affects the disso-
lution of cellulose in ILs.[72] Long chain N-alkyl substituents
on imidazolium cations and high cation symmetry have been
proposed to negatively impact solubility of cellulose due to
decreased C─H bond acidity and/or increased viscosity.[66,72,73]

Electron-withdrawing substituents appear to increase the
solubility of cellulose.[72] Other cations include pyridinium,
ammonium, phosphonium, and protonated superbases (1,5-
diazabicyclo(4.3.0)non-5-ene DBN, 1,8-diazabicyclo(5.4.0)undec-
7-ene DBU).[66,67] In addition, ILs may be non-innocent or
derivatizing solvents for cellulose, causing depolymerization
or other side reactions.[74–79] In contrast to the Lyocell process,
usage of IL-based solvents for cellulose spinning requires

no stabilizers and uses a water-based coagulation bath for
spinning.

IL-based spinning dopes can be processed by wet spinning
and dry jet wet spinning.[80] Notably, ILs are almost entirely re-
covered (>99.5%) and reused after processing.[56] The cellulose
content in 1-butyl-3-methylimidazolium chloride [C4C1im][Cl]-IL
based spinning dopes was successfully increased to 16.5 wt%
(maximum for viscose process: 8.10 wt%).[61] In addition
to the plethora of imidazolium-based ILs with differing N-
substitution and anion, Sixta et al. developed a process based on
1,5-diazabicyclo[4.3.0]non-5-ene acetate ([DBNH][Ace]) (Ioncell
process).[55,81–85] Cellulose fibers derived from the different pro-
cesses show promising mechanical properties when compared to
“natural” cellulose fibers like hemp or flax (Table 1, Figure 8). The
choice of IL in combination with the spinning process has been
shown to impact fiber properties.[67] When comparing cellulose
dry jet wet spinning from imidazolium-based ILs, lower viscosi-
ties were observed for dopes based on ILs with acetate anions and
higher tenacities for the fibers obtained from spinning solutions
of chloride anion containing ILs.[86] Notably, all observed tenac-
ities were higher than those observed for the Lyocell process. A
dry jet wet spinning process with the IL 1-ethyl-3-methyl imida-
zolium diethyl phosphate ([C2C1im][DEP]) produced fibers with

Figure 8. Different processes for the production of cellulosic fibers.

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Table 1. Mechanical properties (tensile strength 𝜎, Young´s modulus E, elongation at break 𝜖b) of MMCFs from different processes compared to "natural"
cellulosic fibers.[55]

Process Solvent 𝜎 [cN tex−1] 𝜎 [MPa] E [GPa] 𝜖b [%] Reference

IL-based [C4C1im][Cl] 53 – – 13 [86]

IL-based [C4C1im][Ace] 44–49 – – 13–16 [86]

IL-based [C2C1im][Ace] – 198 13 3 [91]

IL-based (Ioncell) [DBNH][Ace] 28–48 354–784 9.5–33 9–21 [81, 82, 84, 92]

Lyocell NMMO 40–44 – – 13–17 [86]

Viscose Cellulose derivatization 20–25 – 7 18–23 [55]

Flax fiber 345–1035 27.6 2.7–3.2 [48]

Hemp fiber 690 70 1.6 [48]

high crystallinity, while fibers from the wet-spinning process
afforded lower crystallinities.[87] In another study, a comparison
of dry jet wet spinning of dissolving pulp from [C4C1im][Cl],
[C2C1im][DEP], and NMMO·H2O, respectively, showed a
decreasing fibrillation resistance for [C4C1im][Cl] >

[C2C1im][DEP] > NMMO·H2O.[88] The densest fiber struc-
ture and the highest tensile and knot strength were observed for
[C4C1im][Cl], followed by fibers spun with [C2C1im][DEP] and
NMMO·H2O. Dry-jet wet spinning from the non-imidazolium
IL [DBNH][Ace] (Ioncell process) allows for low processing
temperatures and viscosities, resulting in reduced cellulose and
solvent degradation and high cellulose concentrations, as well as
properties better than or comparable to Lyocell fibers.[67,84] Other
fibrous biopolymers like chitin or silk with equally striking
mechanical and functional properties require similar smart
solution processing approaches to allow competition with syn-
thetic fibers.[89] Indeed, the IL spinning technology was also
successfully applied to the spinning of cellulose/polymer blends
like cellulose/chitin,[90] cellulose/chitosan, cellulose/lignin and
cellulose/poly(acrylonitrile) (PAN).[55,57]

CF production makes up for most of the environmental im-
pact in CFRPCs.[93] In that regard, CF production from natural
sources such as lignin or cellulose may reduce the carbon foot-
print substantially.[94] While most commercial carbon-fibers are
made from petrochemical PAN or, less frequently, from pitch pre-
cursors, more sustainable and low-cost options such as fibrous
biopolymer precursors like lignin[95–100] or MMCFs[94,101–103] find
increasing interest.[104–107] However, as of now, their mechani-
cal properties are still slightly inferior to the petrochemical al-
ternatives and are therefore unsuitable for high-performance
aerospace applications.[108]

Apart from natural fibers and biopolymer fibers (MMCFs,
lignin, chitin, silk, …), bio-based (drop-in/novel) fibers and ma-
trix polymers can find applications in FRPCs. Examples of drop-
in plastics are bio-polyethylene (PE), bio-polypropylene (PP),
bio-polyethylene terephthalate (PET), and bio-polyamides (PAs,
PA 6. PA 6.6).[9,109–111] Common examples of thermoplastic
bio-based polymers are polylactic acid (PLA),[112,113] polyglycolic
acid,[114] polybutylene succinate[112,115,116] and polyhydroxyalka-
noates (PHAs, especially the butyrate PHB),[117–121] polycaprolac-
tone and PBAT, which can find application as fiber-reinforcement
and as matrix polymer.[122–124] PHA is unique in that it is pro-
duced by fermentation from renewables (agricultural/industrial
waste) through microorganisms and does not lead to the deple-

tion of finite resources.[125] Additionally, the availability and de-
velopment of novel bio-based polymers (polyesters, polycarbon-
ates (PCs), PAs, polyurethanes) steadily increase (Figure 9).[126]

Common bio-based monomers that are directly extractable from
biomass or immediately accessible by biomass deconstruction
are fatty acids, amino acids, furans, monomeric sugars, ter-
penes/terpenoids, and lignin monomers (Figure 9).[126]

These monomers can either be transformed directly into poly-
mers or chemically altered to give further bio-based monomers
like lactones, lactames, diacids, epoxides, anhydrides, diols,
or diamines (Figure 9).[111,126] A specific novel bio-based poly-
mer, close to commercialization is poly(ethylene furanoate)
(PEF, Figure 10).[127–130] PEF is a bio-based, recyclable plastic,
which is seen as a more sustainable alternative to PET.[131] In
fact, PEF production reduces energy consumption and GHG
emissions by 40–45% compared to PET production.[127,129]

Additionally, PEF shows better barrier performance as well
as better mechanical and thermal properties than PET.[128,132]

PEF is synthesized from furan-2,5-dicarboxylic acid (FDCA)
and monoethylene glycol (MEG) or furan-2,5-dicarboxylic acid
dimethyl ester (FDME) and MEG (Figure 10). In terms of in-
dustrialization, the latter pathway is less favorable due to the
incompatibility of most current PET plants with the by-product
methanol. FDCA is accessible by oxidation of the bio-based
platform chemical 5-hydroxymethylfurfural (5-HMF), which is
derived from sugars.[127] Bio-MEG was synthesized by several
bio-based synthetic pathways like glycerol hydrogenolysis or
by dehydration/oxidation of bioethanol to ethylene, followed
by ethylene hydration.[127] High purity of the FDCA/FDME
monomer is crucial to achieve PEF with high intrinsic vis-
cosity for technical applications. PEF with intrinsic viscosities
suitable for melt-spinning (up to 0.85 dLg−1) was achieved by
catalyst optimization and solid state polycondensation.[130] The
derived melt-spun multifilament yarns reached tensile strengths
of 65 cN tex−1 with an elongation of 6% and a modulus of
1370 cN tex−1. The application of PEF in FRPCs so far remains
underexplored.[133]

Other sustainable monomers are recycling-derived monomers
and CO2.[134] Recycling-derived monomers are obtained from ter-
tiary recycling of polymers, allowing complete circularity and
providing a solution to the end-of-life issue.[135–138] Further-
more, usage of recycling monomers decouples polymer prices
from oil prices.[139] Chemical recycling of the commodity poly-
mer PET already allowed recovery of the monomers MEG,

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Figure 9. Bio-based monomers and derived bio-based polymers.[111,126 ]

terephthalic acid, dimethyl terephthalate, or bis(hydroxyethyl)
terephthalate.[139,140] However, many chemical recycling meth-
ods require large amounts of energy. For both, economic via-
bility and sustainability, the development of mild depolymeriza-
tion methods is of high importance.[135,141,142] One promising
emerging method is enzymatic depolymerization.[141,143,144] In-
deed, the biotechnology company Carbios recently announced
the launch of the first plant for enzymatic PET depolymeriza-
tion with a processing capacity of 50.000 tons of PET waste
for 2025.[145,146] The upcycling of industrial waste CO2 into
monomers or the usage of CO2 as comonomer leads to sus-
tainable polymers that can find applications in FRPCs.[147,148]

Among other approaches, CO2 can be transformed into sus-
tainable poly(carbonates) by copolymerization with bio-based ter-
pene oxides for multiple potential applications in foams, coat-
ings, and adhesives.[149–153] As a proof of concept, waste CO2
from a coal-fired power station was successfully employed in
copolymerization with cyclohexene oxide.[154] CO2-derived five-
membered cyclic carbonates further find application in the syn-
thesis of polyhydroxyurethanes (PHUs). PHUs have the addi-
tional advantage of isocyanate-free polyurethane synthesis (non-
isocyanate polyurethanes, NIPUs).[148,155,156] Apart from thermo-
plastic materials, thermosets find application as matrix polymers
in FRPCs.

Figure 10. Synthesis of poly(ethylene furanoate) (PEF) from furan-2,5-dicarboxylic acid (FDCA) or furan-2,5-dicarboxylic acid dimethyl ester (FDME) and
MEG via (trans)esterification and polycondensation.[127,130]

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Figure 11. Vitrimers combine the advantageous properties of thermosets and thermoplasts through associative exchange reactions and a fixed crosslink
density.[204,206,207,212–214]

Thermoplastic matrices are generally considered more
sustainable than thermosets because of their better
recyclability.[18,157] Nonetheless, in 2019, thermoset matrices
still accounted for 61% of matrices employed in compos-
ites, while thermoplastic matrices only accounted for 38%
(Figure 1).[1] As thermoset composites have performance
advantages compared to thermoplastic composites in some
applications (chemical resistance, less prone to creep),[158] the
development of sustainable thermoset matrix systems is still
of high interest.[159] Similar to thermoplastic polymers, the
use of renewable raw materials can increase the sustainability
of thermoset matrices (Figure 9).[160–162] Available thermosets
from renewables include benzoxazine resins, epoxy resins,
and unsaturated polyester resins.[159,162–170] Among the most
commonly used resins for FRPCs are epoxy thermosets.[171]

Their low shrinkage, high crosslinking density, high rigidity,
and high chemical and thermal stability make them excellent
candidates for high-performance applications.[172] Sustainable
epoxy resins include resins derived from epoxidized plant oils
like epoxidized linseed oil, epoxidized soybean oil, or epoxi-
dized canola oil.[167,168] Furthermore, saccharide-based resins
like furan-based epoxy resins,[163,166,173] or isosorbide derived
epoxies[174,175] were developed. Additionally, epoxidized natural
polyphenols (catechin, tannic acid)[176–179] and phenols (resor-
cinol, vanillin, cardanol, eugenol)[180–185] as well as epoxidized
terpenes[186–188] and rosin[189,190] found applications in epoxy
resins.[168,191] Bio-based epoxy hardeners include amines (furan-
based, aminated grape seed oil AGSO, Priamine),[192–196] phenols
and polyols (humins, lignin, tannic acid)[170,197–199] as well as
(amino)[200] acids (citric/tartaric/maleic/oxalic acid)[178,201] and
bio-based anhydrides.[187,168,195,202,203] Apart from the bio-based
approach, a novel promising concept for sustainable thermoset
matrices was developed: vitrimers.[204–207] Vitrimers, a term
coined by Leibler and co-workers,[208] belong to the group of
covalent adaptable networks.[209–211] More specifically, vitrimers
consist of an organic network of covalently bound chains that
can change its topology by thermally triggered associative
exchange reactions (Figure 11).[204,206,207,212–214] The exchange
reactions can be catalyzed or uncatalyzed. The viscoelastic
behavior of vitrimers is best described by their glass transition
temperature Tg and their topology freezing transition temper-
ature Tv.

[204,213] At Tg, the polymer transfers from the glassy
to the rubbery state due to long-range coordinated molecular
motions. At Tv, the network transforms from a viscoelastic
solid to a viscoelastic liquid because the timescale of bond

exchange reactions is shorter than the timescale of material
deformation. Hence, when the temperature is increased above
Tv, exchange reactions become fast enough to allow the network
to flow and rearrange, despite a constant crosslink density.
The rearrangement is controlled by the cross-link exchange
kinetics. Tg and Tv can be controlled by the density of cross-links
and exchangeable groups, the exchange reactions kinetics,
and the inherent rigidity of the monomers.[204] Sustainability
of vitrimers has been further improved by using bio-based
resources.[205,215]

Like traditional thermosets, vitrimers merely swell in the
presence of solvents and show low creep in a large tem-
perature window and are therefore excellent candidates for
composites.[204] Furthermore, vitrimer composites, like tradi-
tional thermoplastic composites, can be reprocessed after curing
by heating and remolding. Additionally, vitrimers possess self-
healing properties.[212,216–218] Vitrimer-based composites were
even recycled in a solution of their resin precursors, regain-
ing both fiber and matrix with excellent properties.[212,219]

Systems based on retro-Diels-Alder reactions,[220–226]

transesterification,[227,228] imine exchange,[229,230] viny-
logous urethanes,[231–234] disulfide metathesis,[235,236]

transcarbamoylation[237] and siloxane exchange[238,239] were
applied in vitrimer composites.[214,216,217,240–242]

4. Self-Reinforced Composites

The energy-intensive sorting process can be omitted for self-
reinforced composites (SRPCs) from a single polymeric material
serving both as matrix and reinforcement. SRPCs hence
present an opportunity to recycle otherwise complex composite
materials.[243] SRPCs were pioneered by Capiati and Porter in
1975 using high density PE.[244] Since then, more PE-based
SRPCs have been developed.[243,245,246] Further SRPCs are based
on polypropylene,[247–249] polyethylene terephthalate,[250–252]

PLA,[112,253] polyamides (PA6,[254–256] PA12[257,258]).[243] Com-
mercial PP-based SRPCs are Curv (BP Amoco/Propex Fabrics),
PURE (Lankhorst Pure Composites), Tegris (Milliken and Com-
pany) and Armordon/Torodon (Don and Low), Torodon.[259]

Fabrics of comingled PET fibers for SR-PET production were
commercialized by Comfil.[260] Though not bio-degradable
all-PE, all-PP, and all-PET SRPCs are of great interest since
commercial capacities for the recycling of the respective base
polymer already exist. In particular, separate waste collection
schemes (deposit return schemes, DRS) for PET bottles are in

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Figure 12. Preparation of all-cellulose composites by partial dissolution of cellulosic fibers or impregnation of cellulosic fibers with a cellulosic matrix
solution.

place in many countries, with collection rates reaching up to
96% (Denmark, 2020).[261] The single-component architecture of
SRPCs ensures excellent fiber–matrix interfaces but also poses
challenges in their production, since the reinforcement fibers
can be damaged during matrix infusion.[259] Too high processing
temperatures can lead to relaxation and ultimately melting of the
reinforcement fibers, resulting in both, loss of mechanical prop-
erties and reinforcement volume fraction. Similarly, too high
applied pressures can cause flow accompanied by disruption of
molecular alignment and mechanical properties. Conversely, if
the applied temperatures and pressures are too low, composite
consolidation may be insufficient.[259] Additionally, a low-melting
matrix translates into a very low upper service temperature for
the final composite. In consequence, a variety of techniques to
overcome fiber degradation during matrix melting including
powder impregnation, fiber and film stacking, solution impreg-
nation, fiber intermingling,[262] exploitation of polymorphism,
fiber surface melting, coextruded tape, partial fiber dissolution,
nanofibrillation,[250] hot pressing of PET non-wovens made
of high and low melting fibers[251] and hot consolidation of
bicomponent yarns were developed.[259] The environmental
impact of SRPCs can be further reduced if bio-based and
biodegradable polymers are employed. Also, if biopolymer
fibers are embedded in “themselves” the problem of inferior
fiber–matrix adhesion with “conventional” matrices due to the

polarity difference is mitigated and fiber treatment becomes
obsolete.

Apart from biodegradable PLA-based SRPCs,[112,243,253,263–267]

cellulose-based SRPCs, or all-cellulose composites (ACCs), are
of particular interest since they are comparably cheap[50] and
their mechanical properties are often superior to classical
biocomposites.[41,268,269] Fiber-based ACCs are mainly prepared
by two different pathways (Figure 12):[270] Either (i) by surface-
selective partial dissolution of cellulosic reinforcing materi-
als and in situ regeneration of the dissolved portion to form
the matrix[271–279] or (ii) by separate production of cellulosic
fibers and cellulosic matrix and combination into a composite
material.[41,269,280–282]

For the matrix, the non-meltable cellulose is processed from
solution and regenerated in a subsequent coagulation step. While
the direct dissolution pathway readily achieves high volume frac-
tions of the reinforcing phase and formally is a one-step pro-
cess, the second approach is more modular as matrix and re-
inforcement fibers can consist of cellulose from different raw
materials or processes. Furthermore, the high-quality reinforc-
ing fiber is weakened by the partial dissolution and downgraded
to a less oriented bulk material.[269] Solvent systems for ma-
trix preparation include DMAc/LiCl,[271,272,275–278,280,281] NaOH-
urea[282] and, based on the Lyocell process, NMMO.[41] Addition-
ally, ILs were proven as potent environmentally friendly, and re-

Figure 13. Preparation of ACCs in a two-step process utilizing ILs as solvents. Reproduced (adapted) with permission. Copyright 2018, Springer
Nature.[42]

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Table 2. Mechanical properties of original and recycled ACCs.[42]

Tensile strength [MPa] Young´s modulus [GPa] Elongation [%] Flexural modulus [GPa] Charpy impact strength [kJ m−2]

Composite 53 ± 3 2.0 ± 0.04 12.7 ± 0.9 5.3 ± 1.8 70 ± 15

Composite first rec. 41 ± 5 2.0 ± 0.15 14.7 ± 3.7 6.0 ± 0.4 64 ± 2

Composite second rec. 57 ± 3 1.7 ± 0.10 13.9 ± 2.4 6.3 ± 0.7 65 ± 3

Composite third rec. 50 ± 2 2.4 ± 0.10 6.9 ± 0.8 7.8 ± 0.1 66 ± 3

5 layers of fabric with 90° relative orientation. Concentration of matrix precursor: 6%. Dwell time: 60 min. Tensile properties were measured in fiber direction of the 3 layers.

cyclable solvents for ACC preparation by both pathways.[269,279]

In the two-step process with IL, first a pulp cellulose solu-
tion in an IL ([C2C1im][Ace]) is prepared as a matrix precursor
(Figure 13).[42,55,269] Next, high strength rayon fibers/fabrics are
embedded in the matrix precursor solution. Subsequent removal
of the IL by coagulation and washing in a water bath provides the
wet prepreg. In the last step, consolidation by hot pressing (6 bar,
110 °C) affords the ACC.

The prepared ACCs reached mechanical properties compa-
rable to thermoplastic glass-fiber reinforced plastics. Tensile
strengths from 45–75 MPa, Young´s modulus from 1.5 to
2.3 GPa as well as elongations from 4% to 17% were achieved.
The flexural modulus was in the range of 5.3 to 7.6 GPa and the
Charpy impact strength ranged from 50 to 115 KJ m−2. For recy-
cling, the ACC was milled, dissolved in IL, and reused as ma-
trix material for composite preparation. Three recycling cycles
were realized with the mechanical properties remaining constant
over all three steps (Table 2). Furthermore, ACCs have been car-
bonized and infiltrated with silicon to give C/C-SiC composites
that retain the shape of their ACC precursors.[283]

5. Conclusion

Tailoring sustainability approaches to specific applications is crit-
ical. The best approach considers all safe-and-sustainable-by-
design (SSbD) factors, carbon and water footprints and is sup-
ported by life cycle assessment. For example, the design of FRPCs
for prosthetics may involve biodegradable and bio-based mate-
rials, while those for aircraft may prioritize traditional CFRPCs
and their recycling, with an emphasis on light weight and me-
chanical properties during the use-phase. Advances in sensing
and separation techniques will allow a more tailored approach
to FRPC recycling. In addition, thermal recycling of FRPCs (py-
rolysis, fluidized bed) is expected to benefit from the optimiza-
tion of existing recycling technologies based on thorough studies
correlating fiber properties with process parameters. Newer tech-
niques such as high-voltage fragmentation or post-treatment of
GFs will increase the economic value of recyclates and broaden
their applicability. Chemical recycling can complement the other
recycling techniques by providing access to resources of the same
quality as primary resources. Enzymatic recycling, supported by
high-throughput testing, may allow selective depolymerization
of one component in complex composite wastes. In addition,
(biotechnological) research into the valorization of biomass is ex-
pected to increase feedstock diversity and lead to the development
of new polymer structures with performance-advantaged proper-
ties. While the development of new sustainable materials with

tailored properties for FRPCs is important, their impact depends
on reaching industrial maturity. Well-studied, sustainable mate-
rials like vitrimers, or bio-based polymers such as PEF, as well as
sustainable concepts such as self-reinforced composites need to
bridge the gap between research and industry. The applicability of
new polymers for fiber spinning or matrix materials needs to be
demonstrated in real-world applications. Therefore, application-
oriented research is essential for practical implementation and
to ensure a significant impact in the near future. In order to fur-
ther promote the application of sustainable FRPCs, it is essential
not only to focus on research but also to introduce incentives for
industry. In addition, increased consumer awareness plays a key
role in promoting the adoption of these sustainable materials in
various applications.

Acknowledgements
Open access funding enabled and organized by Projekt DEAL.

Conflict of Interest
The authors declare no conflict of interest.

Keywords
bio-based, composites, fibers, polymers, recycling, vitrimers

Received: January 13, 2024
Revised: February 8, 2024

Published online: February 25, 2024

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Iris Elser received her doctoral degree from the University of Stuttgart (Germany) in 2018 under the
supervision of Prof. M. R. Buchmeiser. After a short postdoctoral stay at the University of Stuttgart,
she worked as a DFG-funded postdoc in the group of Prof. Douglas W. Stephan at the University of
Toronto, Canada. In 2022 she returned to Germany for a 1-year stay in the group of Prof. Matthias Wag-
ner at the University of Frankfurt, Germany. Since July 2023, she has been the head of the Competence
Center Polymers & Fiber Composites at the German Institutes of Textile and Fiber Research Denk-
endorf in Germany.

Michael R. Buchmeiser received his doctoral degree from the University of Innsbruck, Austria. He then
spent 1 year at MIT in the group of Prof. Richard R. Schrock. In 1995, he became an assistant professor
at the University of Innsbruck, where he finished his “Habilitation” in Macromolecular Chemistry and
then became an associate professor. From 2000 to 2001, he was a visiting professor at the Graz Uni-
versity of Technology, Austria; from 2004 to 2009, he was a full professor at the University of Leipzig,
Germany. In 2009, he accepted a full professorship in Macromolecular Chemistry at the University of
Stuttgart, Germany.

Macromol. Mater. Eng. 2024, 309, 2400013 2400013 (15 of 15) © 2024 The Authors. Macromolecular Materials and Engineering published by Wiley-VCH GmbH

http://www.advancedsciencenews.com
http://www.mame-journal.de

	Toward Sustainable Fiber-Reinforced Polymer Composites
	1. Introduction
	2. Current Recycling Strategies
	3. Sustainable Fiber and Matrix Materials
	4. Self-Reinforced Composites
	5. Conclusion
	Acknowledgements
	Conflict of Interest
	Keywords