Jung Et Al., 2023

Chemosphere 320 (2023) 138089
Contents lists available at ScienceDirect
Chemosphere
journal homepage: www.elsevier.com/locate/chemosphere
Review of polymer technologies for improving the recycling and upcycling

efficiency of plastic waste
Hyuni Jung a, 1, Giyoung Shin a, 1, Hojung Kwak a, 1, Lam Tan Hao a, b, Jonggeon Jegal a,
Hyo Jeong Kim a, Hyeonyeol Jeon a, b, **, Jeyoung Park a, c, ***, Dongyeop X. Oh a, b, *
a
Research Center for Bio-based Chemistry, Korea Research Institute of Chemical Technology (KRICT), Ulsan, 44429, Republic of Korea
b
Advanced Materials and Chemical Engineering, University of Science and Technology (UST), Daejeon, 34113, Republic of Korea
c
Department of Chemical and Biomolecular Engineering, Sogang University, Seoul, 04107, Republic of Korea
H I G H L I G H T S G R A P H I C A L A B S T R A C T
• Summarized recent advances for

increasing plastic recycling/upcycling
efficiency.
• Reviewed technologies for converting
plastic waste into other polymer
materials.
• Materials with higher performance than
the input plastic waste can be
manufactured.
A R T I C L E I N F O A B S T R A C T
Handling Editor: Y Yeomin Yoon Human society has become increasingly reliant on plastic because it allows for convenient and sanitary living.
However, recycling rates are currently low, which means that the majority of plastic waste ends up in landfills or
Keywords: the ocean. Increasing recycling and upcycling rates is a critical strategy for addressing the issues caused by plastic
Polymer technology pollution, but there are several technical limitations to overcome. This article reviews advancements in polymer
Recycling
technology that aim to improve the efficiency of recycling and upcycling plastic waste. In food packaging,
Upcycling
natural polymers with excellent gas barrier properties and self-cleaning abilities have been introduced as
Plastic waste management
Plastic sustainability environmentally friendly alternatives to existing materials and to reduce food-derived contamination. Upcycling
Abbreviations: APC, aliphatic polycarbonate; bio-PU, bio-based poly(amide urethane); CA, cellulose acetate; ChNC, chitin nanocrystal; ChNF, chitin nanofiber;
ChNW, chitin nanowhisker; CNC, cellulose nanocrystal; CNF, cellulose nanofiber; DMAP, N,N-dimethyl-4-aminopyridine; EVOH, ethylene vinyl alcohol; FDCA, 2,5-
furandicarboxylic acid; HAA, hydroxyalkanoyloxy alkanoate; HDPE, high-density polyethylene; LDPE, low-density polyethylene; MHET, mono-2-hydroxyethyl
terephthalate; MSA, methane sulfonic acid; OTR, oxygen transmission rate; PAA, polyacrylic acid; PC, polycarbonate; PCNS, porous carbon nanosheet; PET, poly
ethylene terephthalate; PHA, polyhydroxyalkanoate; PHB, polyhydroxybutyrate; PLA, polylactic acid; PP, polypropylene; PS, polystyrene; PVA, polyvinyl alcohol;
PVC, polyvinyl chloride; PVDC, polyvinylidene chloride; SLIPS, slippery liquid-infused porous surface; TBAB, tetrabutylammonium bromide; TBD, dec-5-ene; TPA,
terephthalic acid; TPC, thermoplastic copolyester.
* Corresponding author. Research Center for Bio-based Chemistry, Korea Research Institute of Chemical Technology (KRICT), Ulsan, 44429, Republic of Korea.
** Corresponding author. Research Center for Bio-based Chemistry, Korea Research Institute of Chemical Technology (KRICT), Ulsan, 44429, Republic of Korea.
*** Corresponding author. Department of Chemical and Biomolecular Engineering, Sogang University, Seoul, 04107, Republic of Korea.
E-mail addresses: hyjeon@krict.re.kr (H. Jeon), jeypark@sogang.ac.kr (J. Park), dongyeop@krict.re.kr (D.X. Oh).
1
These authors equally contributed to this work.
https://doi.org/10.1016/j.chemosphere.2023.138089
Received 7 November 2022; Received in revised form 2 February 2023; Accepted 5 February 2023
Available online 6 February 2023
0045-6535/© 2023 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
H. Jung et al. Chemosphere 320 (2023) 138089
and valorization approaches have emerged to transform plastic waste into high-value-added products. Recent
advancements in the development of recyclable high-performance plastics include the design of super engi
neering thermoplastics and engineering chemical bonds of thermosets to make them recyclable and biode
gradable. Further research is needed to develop more cost-effective and scalable technologies to address the
plastic pollution problem through sustainable recycling and upcycling.
1. Introduction physicochemical properties of plastics, issues related to contamination,

and the difficulty of reprocessing highly stable plastics like thermosets
The rapid increase in global plastics production is driven by the (Fig. 1). In Section 3, we examine the use of environmentally friendly
demand for inexpensive and durable materials that offer convenience coatings and their potential to increase the efficiency of recycling and
and enhanced functionality. Modern societies are highly dependent on upcycling by reducing surface contamination. Section 4 focuses on the
plastic, and plastics are widely used to produce many common items development of new polymer materials through the upcycling of plastic
such as clothing, car interiors, and packaging for goods and foods waste. Finally, in Section 5, we examine the potential of new
(Benson et al., 2021). Furthermore, the use of disposable plastic prod high-performance polymer materials that are easy to recycle and
ucts has increased rapidly owing to the SARS-CoV-2 (COVID-19) upcycle.
pandemic (Jang et al., 2020); in 2020, the global plastic consumption of
medical gloves and face masks reached approximately 69 billion units 2. Background on the difficulty of recycling/upcycling plastic
per month (Kalina and Tilley, 2020). Approximately 0.3–0.4 billion tons products
of plastics are produced annually worldwide, including an estimated 1.6
million tons per day due to COVID-19 (Benson et al., 2021), yet less than The lifecycle of polymer materials starts with raw materials, which
10% are recycled. Approximately 50% of all plastic waste ends up in are turned into a variety of products and components. At the end of life,
landfills, the most common method of disposal (Organization for Eco the products are discarded as plastic waste, which is collected by waste
nomic Co-operation and Development, 2022). The rest is incinerated or disposal companies either separately or with general waste. An effective
ends up in the ocean (Jang et al., 2020; Kumar et al., 2021b). There are option for reducing plastic waste is to recycle and upcycle these prod
currently over 150 million tons of plastic in the ocean, with an estimated ucts. Recycling can reduce the use of raw materials and reduce waste
8 million tons entering the oceans each year (Jambeck et al., 2015). through a closed loop system. Upcycling is the addition of value to
Instead of degrading in nature, plastics slowly disintegrate into micro plastic waste to obtain a product with higher value.
plastics and accumulate in soil and water (Bhatt et al., 2021). Therefore, The first factor hindering the recycling and upcycling of plastics is
sustainable plastic waste management strategies are required, particu the difficulty and cost associated with classification and separation ac
larly in countries with small terrains, such as South Korea, owing to the cording to plastic properties. This is particularly true for mechanical
limited space for landfill sites (Geyer et al., 2017). Incinerating plastic recycling (Pan et al., 2020). The basic premise of the chemical industry
waste is not an ideal solution, because it emits greenhouse gases, toxic is to produce pure chemical products through purification and separa
gases, and fine dust (Sharma et al., 2021). tion. The same applies to the recycling and upcycling of waste. Com
Increasing recycling and upcycling rates is the most effective solution modity plastics (Fig. 2) are polymer materials that maintain high
to global plastic problems. Nevertheless, it is often cheaper to produce mechanical strength up to 100 ◦ C, for example, low-density poly
new plastic products from virgin materials than to recycle and reuse ethylene (LDPE), high-density polyethylene (HDPE), polypropylene
existing materials (Hou et al., 2021). Researchers are developing new (PP), polystyrene (PS), and polyvinyl chloride (PVC) (Vieyra et al.,
technologies to improve recycling and upcycling efficiency, such as 2022). The largest portion of commodity plastics are olefin-based
thermomechanical processing, chemical recycling (glycolysis and py polymers, such as LDPE, HDPE, and PP. These polymers are inherently
rolysis), and biological depolymerization using catalysts, enzymes, and difficult to recycle or upcycle by chemical processes because their
microorganisms (Ellis et al., 2021). Despite these efforts, there are still polymer chains comprise C–C covalent bonds; therefore, their decom
challenges in terms of recycling technology, waste sorting, economics, position requires high temperatures and high-performance catalysts
and social behavior. Recycling plastic waste requires separating it, (Celik et al., 2019). Olefin-based polymers are typically produced from
which can be difficult and complex, particularly as many products shale gas at relatively low cost, while the value of recycled products
comprise several components and types of plastic (Thuy et al., 2021). from olefin polymers is relatively low. This has resulted in an
Mixed plastics and foreign substances significantly reduce the quality of olefin-based polymer recycling rate of less than 10% (Chaudhari et al.,
thermomechanically recycled plastics. Depolymerized products can be 2021; Thiounn and Smith, 2020). Engineering plastics (Fig. 2) are
upcycled to produce low-molecular-weight fine chemicals, such as fuels, polymer materials that maintain mechanical strength even at tempera
monomers, and surfactants (Hou et al., 2021), but there are few exam tures above 100 ◦ C, such as polyethylene terephthalate (PET), acrylo
ples of re-polymerization to form valuable polymeric materials from nitrile butadiene styrene, and nylon (Park et al., 2019). PET, a
recycled monomers owing to purity and yield problems. Additionally, condensation polymer with an ester-based polymer chain, can be
there is a need for more research on the physicochemical properties of decomposed relatively easily by hydrolysis. Thus, PET has relatively
polymers to improve the efficiency of recycling of plastic waste. high price competitiveness and is easy to upcycle and recycle by hy
In this review, we discuss the latest developments in technologies drolysis. Unfortunately, olefin-based plastics account for more than 50%
designed to improve the efficiency of recycling and upcycling plastic of all plastic waste, while PET accounts for less than 10% (Fig. 2). Thus,
waste from the perspective of polymer technology. Although there are advanced research is required to develop recycling and upcycling
many excellent reviews summarizing trends in catalytic chemical and technologies for olefin-based plastics. Recycling and upcycling methods
biological recycling/upcycling methods (Balu et al., 2022; Chen et al., vary for each type of plastic, making it possible to recycle and upcycle
2021; Ellis et al., 2021; Korley et al., 2021; Vieira et al., 2022; Zhao plastics by mechanical and thermal means only when they are classified
et al., 2022) and the production of value-added products through the into analogous or homogeneous polymer groups (Cafiero et al., 2015).
conversion of plastic waste (Hou et al., 2021), strategies of increasing Even for polymers whose chains comprise only C–C bonds, such as LDPE
the efficiency of recycling/upcycling plastic waste have not yet been and PP, the polymers are difficult to melt together to form a single
reviewed. In Section 2, we explore the technical challenges of plastic material, and difficult to separate when mixed (Aumnate et al., 2019).
recycling and upcycling, including the lack of knowledge on the This is further complicated by the fact that multiple types of plastic are
2
often combined within a single product (Roosen et al., 2020). Conse partially removed through caustic cleaning (Lange, 2021; Weber
quently, sorting mixtures of plastic waste is challenging and the sorting Macena et al., 2021). Thus, food packaging suffers from poor recycling
efficiency is low (Lange, 2021). and upcycling efficiency.
The second factor hindering the recycling and upcycling of plastics is The fourth challenge to plastic recycling and upcycling is the
the use of additives and coatings. Plastic products commonly contain inability to reprocess thermoset plastics. These materials do not melt or
coatings or additives such as reinforcing agents, antioxidants, plasti dissolve, making them theoretically impossible to recycle (Geueke et al.,
cizers, dyes, metals, and flame retardants, which are very difficult to 2018). Owing to their high coefficient of thermal expansion, thermo
remove from the base polymer owing to the low molecular diffusion rate plastics are unsuitable for applications that require dimensional stability
of polymers (Vogt et al., 2021; Wagner and Schlummer, 2020). at high temperatures such as substrates for electronics and heat-resistant
Furthermore, when the additive is an organic material, the polymer parts in aircraft and automobiles (Post et al., 2020). Therefore, ther
binds strongly to the additive via van der Waals forces. Coating layers moset plastics are commonly used, because their three-dimensional
must be removed for recycling, which requires significant energy and crosslinked structure provides high dimensional stability and resis
cost (Cherrington et al., 2022). Even if the substrate is recyclable, its tance to heat, chemicals, and applied loads. However, the increased use
recyclability is reduced if the coating is not. For example, a thermo of products such as personal computers and mobile phones has led to a
plastic material coated in a thermoset plastic cannot be re-molded 3–5% annual increase in e-waste (X. Ji et al., 2022) that contains
without separation to remove the coating layer. Dyes are used to precious metals such as Au, Ag, Cu, Pd, and Ta. To recover metals from
obtain colored plastics or to print text or pictures onto them. The color of e-waste such as printed circuit boards, the plastic must first be removed
the recycled material affects its commercial value (Ferreira et al., 2022). (Chen et al., 2019). Unfortunately, the use of thermoset plastics means
Black plastic, which is made by mixing plastic waste of various colors, that this cannot be achieved through simple heating and cooling cycles
has particularly low commercial value owing to its limited applications. (Post et al., 2020). As a result, the extraction and reuse of rare metals
Although decolorization is possible, such as by physical adsorption using from e-waste requires incineration or treatment with toxic solvents,
resins or activated carbon, there are costly issues associated with these which releases hazardous gases and strong chemicals (e.g., acid
methods, including the regeneration and disposal of adsorbents. Elec s/alkalis) that can cause serious environmental pollution (Chen et al.,
trochemical degradation methods have been developed, but they are 2019).
expensive and difficult to scale up because they use nanoparticle tech
nology and complex equipment (Huang et al., 2021). Therefore, the 3. Sustainable coating technologies for enhancing the recycling/
removal of additives and coatings is a major hurdle for plastic recycling. upcycling efficiency of plastic products
The third obstacle to plastic recycling is contamination. A significant
portion of plastic waste, including food packaging, which accounts for In Section 2, we discussed the various challenges that impede the
26% of all plastic waste (Drzyzga and Prieto, 2019), must be cleaned of recycling and upcycling of existing plastic products. One of the least
contaminants before it can be processed. This is crucial for mechanical efficient types of plastic product to recycle is food packaging. These
recycling but also applies to many chemical recycling methods. Cleaning materials frequently have coatings that are difficult to remove and are
is typically achieved using hot or cold water with corrosive chemicals or typically contaminated with food residue. In this section, we explore
detergents, but this can be costly owing to the need for drying and plastic film coating methods that have the potential to improve the
wastewater treatment. Moreover, it can be difficult to remove recycling and upcycling efficiency of food packaging materials.
food-derived pollutants; for example, odor components are only
Fig. 1. Summary of polymer technologies designed to improve the efficiency of recycling and upcycling plastic waste. (Top) Self-cleaning coatings reduce food
contamination and stains that otherwise downgrade the quality of recycled material, thereby enhancing the recyclability of plastic waste used as food packaging.
(Middle) By upcycling plastic waste to high-value-added materials instead of low-value chemicals such as fuel, the processing of plastic waste becomes more cost-
efficient. (Bottom) High-performance polymer materials that are easy to recycle and upcycle, such as recyclable thermoset resins, can circumvent the difficulties
associated with reprocessing highly stable plastics.
3
3.1. Film coatings made of sustainable and renewable polymers chemically accessible groups than cellulose because the amine group of
chitin is more chemically reactive than the hydroxyl group of cellulose;
One method to increase the efficiency of recycling and upcycling the amine groups generate a positive charge, resulting in gas barrier
food packaging materials is to use coatings made from sustainable and properties, odor barrier properties, antioxidant ability, and antibacterial
renewable polymers. PET and PP are the most commonly used plastics activity (Amorim et al., 2022; Priyadarshi and Rhim, 2020). Chitin and
for food packaging (Nisticò, 2020; Nuruddin et al., 2020); PET is chitosan are modified to have cations, whereas cellulose is modified to
transparent and lightweight, particularly compared with metal and have anions by oxidation of the hydroxyl groups.
glass, and PP is lightweight, inexpensive, and has excellent water-barrier Table 1 shows the OTRs of various polymer films used in food
properties owing to its hydrophobicity. However, both materials have packaging applications. Natural polymers exhibit relatively high OTRs
relatively high oxygen transmission rates (OTRs) of approximately 100 when used alone as bulk films. For example, bulk cellulose films have an
and 1000 cm3 m− 2 day− 1, respectively (T. Kim et al., 2019; Nakaya OTR of above 100 cm3 m− 2 day− 1 (Jang and Chang, 2008; Nguyen et al.,
et al., 2015), which is not suitable for food packaging purposes. To 2018; Zheng et al., 2019). In contrast, owing to their high crystallinity,
protect food from oxidation, packaging materials must have an OTR of cellulose nanofibers (CNFs) have an OTR of as low as 0.7 cm3 m− 2 day− 1
less than 1 cm3 m− 2 day− 1. Therefore, PET and PP are coated with gas at 50% relative humidity (Vartiainen et al., 2020), which satisfies the
barrier materials, such as metals (e.g., Al) or halogen-containing poly gas barrier requirements for food packaging materials.
mers (e.g., PVC and polyvinylidene chloride (PVDC)). These coatings are The oxygen permeability, which is calculated by normalizing the
difficult to remove, which makes food packaging hard to recycle OTR based on the film thickness, allows easier comparison of the gas
economically, leading to it being discarded in landfill or incinerated. barrier properties of different polymers. CNFs have a very low oxygen
This poses environmental hazards because chlorine-containing polymers permeability of as low as 0.256 cm3 μm m− 2 day− 1 kPa− 1 at 50% relative
emit polychlorinated dibenzodioxins (“dioxins”) during incineration, humidity (Vartiainen et al., 2020). This value is 100–1000 times lower
and metals that are not pyrolyzed can generate fine dust (Sharma et al., than that of representative substrate films used in food packaging, such
2021). To address this issue, research has been conducted on sustainable as polylactic acid (PLA), PET, and PP. In addition, it is lower than those
alternatives for halogen- and metal-based polymer coatings. One such of common polymer-based gas barrier materials, such as PVDC, PVC,
alternative is ethylene vinyl alcohol (EVOH), which is an environmen and EVOH (Wang et al., 2018). Unfortunately, a fatal disadvantage of
tally friendly gas barrier material that does not contain halogens or CNFs is that the oxygen permeability increases significantly under
metals. It has excellent gas barrier properties in low-humidity environ humid conditions. At 80% relative humidity, the oxygen permeability of
ments, but this is reduced at high humidities because the hydroxyl CNFs reaches 39.07 cm3 μm m− 2 day− 1 kPa− 1 (Vartiainen et al., 2020).
groups become hydrated. This large increase in oxygen permeability is due to the increased dis
Among natural polymers, chitosan (Cazón and Vázquez, 2019; tance between CNFs owing to hydration of the nanofiber surface (Y. Ji
Priyadarshi and Rhim, 2020), cellulose (Cazón et al., 2020; Qasim et al., et al., 2022).
2021), starch (García-Guzmán et al., 2022), whey protein (Kandasamy Natural polymer coatings can reduce the OTR of plastic films to a
et al., 2021), and gelatin (Noorbakhsh-Soltani et al., 2018) have been certain extent. For example, when a PP film was coated with chitin
widely studied for use in the food packaging industry. Cellulose and nanocrystals (ChNCs), the OTR decreased, but it was still above 150 cm3
chitin (or chitosan) are the most abundant biopolymers in nature and are m− 2 day− 1 (50% relative humidity) (Zhong et al., 2019). Similarly,
renewable and biodegradable. Crystalline nanofibers with excellent gas when a PLA film was coated with cellulose nanocrystals (CNCs) or chitin
barrier properties can be extracted from cellulose- and chitin-based nanofibers (ChNFs), the OTR was 270 cm3 m− 2 day− 1 (Satam et al.,
biomass by a top–down method (Jin et al., 2016). Chitosan has more 2018). When cellulose or chitin are used as single materials, the gas
Fig. 2. Classification, cost, recycling rate, and portion of total plastic waste of commercial plastics. (Left) Commodity plastics such as polyolefin polymers (e.g., PE
and PP). (Right) Engineering plastics such as polycondensation polymers (e.g., PET).
4
Table 1
Oxygen transmission rate (OTR) and oxygen permeability (OP) of various polymer films.
Materials Thickness Condition (RH, %) OTR (cm3 m− 2
OP (cm3 μm m− 2
day− 1
Ref.
(μm) day− 1) kPa− 1)
Single component film
Cellulose 30 – 239.4 70.88 Jang and Chang (2008)
CNF 37 50 0.7 0.256 Vartiainen et al. (2020)
80 107 39.07
PET 50 0 38.28 18.89 T. Kim et al. (2019)
12 0 129.23 15.30 Uysal Unalan et al.
30 120.67 14.29 (2016)
60 115.10 13.63
90 107.47 12.73
118.0 50 15.84 18.45 Idris et al. (2021)
PP 60 50 1117.51 661.74 Nguyen et al. (2021)
PLA 25.4 10–90 180–280 45–70 Satam et al. (2018)
CA 77 50 2043 1553 Y. Ji et al. (2022)
Coating
PET/CNF/ChNW 52.6 0 0.48 0.25 T. Kim et al. (2019)
52.6 submersion in water for 0.91 0.47
1h
57.1 0 1.61 0.91 Thuy et al. (2021)
30 1.63 0.92
60 4.12 2.32
90 9.77 5.51
PET/PVA 127.9 50 0.34 0.43 Idris et al. (2021)
PP/2,2,6,6-tetramethylpiperidine 1-oxyl oxidized 124.6 50 165.7 203.8 Zhong et al. (2019)
ChNC
PP/nanocellulose/nanochitin 60 50 13.10 7.76 Nguyen et al. (2021)
PLA/CNC 26.8 50 270 70 Satam et al. (2018)
PLA/ChNF 26.8 50 303 80
PLA/CNC/ChNF 26.4 50 70 20
CA/ChNW/CNC 83 50 50 41 Y. Ji et al. (2022)
barrier properties vary significantly depending on the experimental moisture via the formation of ionic or amide bonds and therefore
techniques, and are significantly reduced when exposed to moisture. expanding its application scope.
This is because cellulose and chitin have a negative or positive charge, Recently, considerable research has been conducted on biodegrad
and both become highly hydrated under humid conditions. Thus, they able polymer films. Polyvinyl alcohol (PVA) is an important water-
can be hydrated by hydrophilic groups or groups with the same charge, soluble synthetic polymer with excellent transparency in the visible
generating a repulsive force. region and excellent oxygen barrier properties (Lim et al., 2015). In
Compared to coatings containing only cellulose or chitin, coatings addition, PVA is a useful component of packaging films because of its
that combine these materials can have a synergistic effect (T. Kim et al., outstanding film-forming ability, high biodegradability, high crystal
2019). This is because the density of the coating structure is increased by modulus, and wide range of crystallinity (Szabo et al., 2020). Coating
the strong ionic bonds that form between cellulose and chitin owing to PVA on PET substrates and annealing at 160 ◦ C for 10 min increases the
their negative and positive charge, respectively (Thuy et al., 2021). crystallinity of the polymer matrix, resulting in a decrease in the OTR of
Layer-by-layer assembly enables the manufacture of structurally stable the film from 15.84 to 0.34 cm3 m− 2 day− 1. PVA is relatively biocom
multilayer thin films through electrostatic interactions, hydrogen patible and has been reported to be biodegradable to some extent
bonding, or covalent bonding between layers. A film in which nano (Chiellini et al., 2003). However, PVA is structurally similar to EVOH,
cellulose and nanochitin were alternately laminated on a PP substrate by and its gas barrier properties in humid environments remain unknown.
layer-by-layer assembly had an OTR of 13.10 cm3 m− 2 day− 1, and it was Thus, additional research is needed to determine the suitability of PVA
confirmed that the OTR was greatly reduced by 10–100 times compared for use in humid conditions and moisture-sensitive applications (Lim
to the uncoated and ChNC-coated films. In addition, when PLA was et al., 2015).
coated with CNCs and ChNFs by layer-by-layer assembly, the OTR was Cellulose acetate (CA) is a renewable and biodegradable compound
reduced by a factor of 3–4 (Satam et al., 2018). A film in which CNFs and formed by the acetylation of cellulose. Many possibilities exist for which
chitin nanowhiskers (ChNW) were alternately laminated on a PET sub CA may be commercially viable, but in general, its commercial use re
strate achieved a low OTR of ~0.5 cm3 m− 2 day− 1. A PET film coated quires its oxygen barrier properties to be improved. Y. Ji et al. (2022)
with 20 layers of CNFs and ChNWs maintained an OTR of 0.91 ± 0.33 applied CNCs and ChNWs as renewable barrier coatings to CA, resulting
cm3 m− 2 day− 1, even after immersion in water for 1 h, suggesting that in an OTR of approximately 50 cm3 m− 2 day− 1: a 40-fold decrease
peeling of the weakly bonded nanostructures marginally contributes to compared to that of uncoated CA (2043 cm3 m− 2 day− 1).
the gas barrier characteristics (T. Kim et al., 2019). This performance Almost half of all food packaging materials are derived from petro
meets the standards for food packaging that can prevent acidification. chemical polymers, which have a number of drawbacks, such as envi
Notably, Nguyen et al. (2021) demonstrated a PP film coated with ronmental challenges, nonbiodegradability, potential health hazards,
stacked cellulose and chitin layers that had excellent gas barrier prop and food quality (Sid et al., 2021). Therefore, research into plastic
erties and could be reprocessed into other forms by melting. This is a packaging and coating materials made of sustainable and renewable
particularly important advance, considering that conventional polymers is of great importance. However, it is challenging to replicate
metal-coated food packaging materials cannot be recycled by melting. the water-barrier and mechanical properties of petroleum-based plastic
The greatest advantages of CNFs and ChNFs are their biodegradability films (Abdullah et al., 2022; de Oliveira Filho et al., 2020). Additionally,
and renewability. Because nanocellulose can lose its oxygen barrier while film coating methods provide a cost-effective and straightforward
properties in humid environments, using nanocellulose in combination means of improving the water resistance and mechanical properties, the
with chitin is a promising avenue for increasing its resistance to resulting films are often difficult to recycle. Consequently, it is essential
5
to develop environmentally friendly film materials that possess both coatings that use bio-fibers and/or bio-oils. As presented in Fig. 3, Thuy
excellent water resistance and good mechanical properties, or to develop et al. (2021) developed a porous coating by spray-coating silica nano
coating materials that can be easily removed for recycling. particles and chitosan nanowhiskers on one side of a PET film by
layer-by-layer assembly. Subsequently, they injected a bio-based sun
flower oil into the porous coating. The coating was self-cleaning and
3.2. Development of self-cleaning plastic films
able to prevent food contamination when used as a packaging material.
Manabe et al. (2016) developed a film with SLIPS functionality by using
Another strategy being developed to solve the problems of recycling
a combination of polyacrylic acid (PAA), chitosan nanomaterials, and
plastic food packaging is to use a plastic film with self-cleaning ability to
paraffin oil. They also designed a fluid-infused film composed of
avoid food contamination. Per- and polyfluoroalkyl substances are
biodegradable materials and a biocompatible lubricant. The film was
widely used in stain-resistant and waterproof products owing to their
fabricated by constructing multiple layers of chitosan/alginate and
hydrophobicity and lipophobicity. However, they are highly persistent
covering the surface of the film with almond oil as the lubricant. This
synthetic chemicals that do not degrade easily, and are now known to
biodegradable and biocompatible SLIPS coating was low-cost and
accumulate in the human body and the environment. Moreover, they
environmentally friendly. Moreover, stains were repelled from the sur
have been linked to cancers, developmental toxicity, immunotoxicity,
face, and liquids flowed easily over it (Manabe et al., 2015). Table 2 lists
and other negative health effects (Schaider et al., 2017), making their
the characteristics of SLIPS films prepared from biodegradable
use less than ideal.
materials.
One promising method for producing self-cleaning plastics is the
Films with SLIPS coatings are advantageous because they can be used
slippery liquid-infused porous surface (SLIPS) technique, which was first
as packaging materials for non-Newtonian fluids such as ketchup and
reported by Aizenberg’s group (Wong et al., 2011). This technique
yogurt drinks while being easy to clean for recycling (Agarwal et al.,
prevents the adhesion of liquids from a surface via the use of a porous
2022). However, the porous coating and oil-impregnation steps intro
coating that is impregnated with a hydrophobic liquid such as an oil. The
duce engineering complexity compared to typical film coating processes
impregnated oil does not freely escape from the porous coating and
(without adding oil), which are straightforward and inexpensive. Ou
repels contaminants from the surface. Since the original study by Wong
et al. (2020) manufactured a self-cleaning coating film without an
et al. (2011), which used an inorganic porous coating and perfluorinated
oil-permeation process. They chemically bonded a fluorine-based poly
oil, several similar studies have been conducted on packaging materials
mer to chitin nanocrystals, which were then simply coated onto the
with self-cleaning functionality using the SLIPS technique.
plastic surface through spray or dip coating. This coating layer exhibited
Notably, some groups have reported relatively sustainable SLIPS
Fig. 3. Representative technologies designed to increase the recycling efficiency of food packaging materials. (1) Sustainable substitutes such as cellulose and chitin
can be used to form films with high gas barrier performance instead of halogen- and metal-based polymer coatings such as PVDC and Al. (2) Self-cleaning film
surfaces have been developed to remove food contamination. For example, SLIPS coatings have been designed by injecting oil into a porous coating of silica
nanoparticles and chitosan nanowhiskers. Reprinted from Ref (Thuy et al., 2021). With permission under the terms and conditions of the Creative Commons
Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
6
Table 2
Characteristics of SLIPS coatings prepared from biodegradable materials.
Material Lubricant liquid Coating Coating angle Property Ref.
Sliding angle
Silica nanoparticles, CNF, and chitosan nanowhisker Sunflower oil Spray 154◦ Sustainable Thuy et al. (2021)
<5◦ Self-cleaning
Transparent
Moisture barrier
Oxygen barrier
PAA and ChNF Paraffin oil Spray or dip <80◦ Transparent Manabe et al. (2016)
<10◦ Low adhesion
High transmittance
Chitosan and alginate Almond oil Dip <80◦ Biodegradable Manabe et al. (2015)
<15◦ Biocompatible
Anti-fouling
Anti-thrombogenicity
High transparency
Table 3
Different types of catalyst used for upcycling plastic wastes.
Starting material (plastic Final products (Bio-)catalyst Ref.
waste)
Biological
PET PHA, bio-PU Leaf-branch compost cutinase (LCC) and Pseudomonas umsongensis Tiso et al. (2021)
GO16
Catechol Bs2Est (chemo-enzymatic depolymerization) and Escherichia coli H.T. Kim et al. (2021)
(whole-cell biotransformation)
Vanillin Engineered Escherichia coli Sadler and Wallace
(2021)
PHB Yarrowia lipolytica Po1f and Pseudomonas stutzeri TPA3P Liu et al. (2021)
PS PHA Pseudomonas putida CA-3 Ward et al. (2005)
Goff et al. (2007)
PE PHA Pseudomonas aeruginosa PAO-1 Guzik et al. (2014)
Chemical
PE Long-chain alkylaromatics Pt/γ-Al2O3 Zhang et al. (2020)
High-quality liquid products (such as Pt/SrTiO3 Celik et al. (2019)
lubricants and waxes)
Amorphous carbon chips Li-ion battery H2SO4 Villagómez-Salas et al.
anodes (2018)
PC Aliphatic polycarbonates TBD:MSA, DMAP Saito et al. (2020)
Poly(aryl ether sulfone) M2CO3 Jones et al. (2016)
PET Poly(ester-amide)s TBD:MSA Demarteau et al. (2020)
Thermoplastic co-polyesters TBT/Mg(OAc)2 Karanastasis et al. (2022)
PVC Porous carbon spheres TBAB, NaOH J. Wang et al. (2020)
Microporous carbon materials KOH X. Liu et al. (2022)
Carbon materials ZnO or KOH Zhou et al. (2022)
PP Magnetic carbon materials Co(ac)2, Ferrocene, CuCl2 Feng et al. (2014)
PET, PE, PVC, PP, PS Graphene Ni foil Cui et al. (2017)
Mixed plastics (PP, PE, PS, Carbon nanosheets Montmorillonite, KOH Gong et al. (2014b)
PET, and PVC)
water and oil repellency with self-cleaning ability. technologies that convert inexpensive plastic waste with low intrinsic
Coatings with self-cleaning and anti-fouling functionality decrease value into high-value-added polymer materials (Table 3). The two main
the need for costly waste cleaning processes. Nevertheless, the problem methods for upcycling plastic waste, namely, biological and chemical
of separating the coating and substrate still exists, so it is crucial to processes, are discussed below.
develop upcycling technologies that can convert mixed plastic waste
into high-value-added materials.
4.1. Biological upcycling to form value-added products
4. Upcycling plastic waste into high value-added polymer
materials Studies on the biological treatment of plastic waste using microor
ganisms that decompose plastics have received increasing attention in
Extensive research is underway on the upcycling of plastic waste to recent years. Furthermore, several bio-upcycling studies are being con
form various chemicals, such as fuels, monomers, activated carbon, and ducted with the aim of converting plastics or depolymerized interme
surfactants, to build a circular plastic economy. Studies on the upcycling diate substances into high-value-added products using the metabolic
of plastic waste through catalytic or biochemical processes usually focus pathways of microorganisms. Some notable biological methods for
on producing low-molecular-weight chemicals, such as precursors of upcycling plastic waste are discussed below.
other materials, raw materials, and fuels; however, there is a desire to PET accounts for approximately 8% of all plastic waste; therefore,
find more direct applications of upcycled PET. Technologies for directly there is a critical need to develop cost-effective PET recycling/upcycling
converting plastic waste and degradation products into highly func methods. Owing to its condensation structure and ester-based polymer
tional polymer materials could further increase the economic feasibility chain, PET decomposes more easily than olefin-based plastics. It can be
of polymer upcycling. In this section, emphasis is placed on upcycling broken down into hydrolysates such as terephthalic acid (TPA), ethylene
glycol, and mono-2-hydroxyethyl terephthalate (MHET). The discovery
7
of Ideonella sakaiensis, a bacterium that can decompose PET, suggests the 4.2.1. High-performance plastic materials
possibility of biologically solving the PET waste problem (Yoshida et al., Millions of tons of polycarbonate (PC) are produced annually for use
2016). Two types of hydrolysate (PETase and MHETase) produced by in applications such as compact disks and automobile headlights. Un
bacteria during the degradation of PET are being studied to increase the fortunately, conventional methods of recycling PC have low efficiencies
degradation efficiency through structural analysis and genetic due to their low selectivity, difficult solvent systems, and safety issues
manipulation. (Antonakou and Achilias, 2013). Poly(aryl ether sulfone) is an
In recent years, several PET upcycling strategies have been devel ultrahigh-performance plastic with a high glass-transition temperature
oped to produce high-value-added products. Notably, PET-derived hy (Tg) of 180–230 ◦ C and excellent tensile strength. Jones et al. (2016)
drolysates can be converted into high-value-added chemicals. In developed a facile one-step process for the conversion of PC into poly
particular, the depolymerized monomers of PET (TPA and ethylene (aryl ether sulfone) by using carbonate and bis(aryl fluoride). They
glycol) can be converted into hydroxyalkanoyloxy alkanoates (HAAs), confirmed that carbonate plays two roles during this process: it de
catechol, gallic acid, vanillic acid, and muconic acid (Franden et al., composes PC by nucleophilic attack and promotes the reaction of the
2018; H.T. Kim et al., 2019; Pardo et al., 2020). One important example phenolate dimers and aryl fluoride formed thereafter. In another study,
is the production of HAA from TPA via microbial biosynthesis. Pseudo polymer electrolytes were produced from waste PC. Aliphatic poly
monas umsongensis GO16 can metabolize TPA as a carbon and energy carbonates (APCs) are promising solid electrolytes for the development
source. HAA biosynthesis was conducted using the evolved strain of safe and high-performance solid-state batteries. Saito et al. (2020)
P. umsongensis GO16 with enzymatic lysates of PET as feedstock. The reported the organocatalyzed depolymerization and polycondensation
evolved strain GO16 showed an improved ethylene glycol uptake rate by of bisphenol A polycarbonate to form APC. The depolymerization pro
adaptive laboratory evolution and was transformed with the HAA syn cess used aliphatic diols such as 1,3-propandediol and 1,5-pentanediol
thesis plasmid for extracellular HAA synthesis. The biotechnologically as nucleophiles and a mixture of 1,5,7-triazabiocyclo[4.4.0]dec-5-ene
produced HAA was then used to form bio-based poly(amide urethane) (TBD) and methane sulfonic acid (MSA) as a catalyst to mediate the
(bio-PU) through polymerization with diisocyanate and butanediol (Tiso transesterification depolymerization reaction. The target APC was syn
et al., 2021). In addition, biologically produced catechol, vanillic acid, thesized by polycondensation of the obtained carbonate-containing
and gallic acid can be used as functional coating materials (H.T. Kim diols with dimethyl carbonate and N,N-dimethyl-4-aminopyridine
et al., 2021). Catechol and gallic acid oxidize spontaneously in the at (DMAP).
mosphere and crosslink with other catechol/gallic acid molecules to Waste PET can be employed to create new polymer materials
form polymers. Moreover, they easily crosslink with amine or thiol through transesterification and ester-to-amide conversion reactions. The
groups and chemically adhere to substrate surfaces, regardless of their transesterification reaction involves the exchange of a covalent bond of
hydrophilicity. This means coating layers can be formed on various the ester group of PET with an ester group of another chemical in the
substrates when immersed in aqueous solutions of catechol and gallic presence of a catalyst. Notably, waste PET can be upcycled into plastics
acid. The coating layer exhibits chemical functionality such as anti with enhanced mechanical properties through transesterification re
bacterial properties and metal ion-reducing behavior. actions with bio-based diesters (Rorrer et al., 2019). The ester-to-amide
Polyhydroxyalkanoate (PHA) is a renewable plastic with excellent conversion reaction occurs when the ester group combines with an
biodegradability and biocompatibility. It is typically produced by amine group in the presence of a catalyst, which results in the loss of an
fermentation using sugar-based carbon sources, which is a costly alcohol group and the formation of an amide bond. This reaction enables
method. A more cost-effective alternative is to use plastic waste as a the production of polyamides or polyester-amides by heating a mixture
feedstock. Tiso et al. (2021) reported the production of PHA from of waste PET and bio- or petroleum-based diamine groups in the pres
enzymatically hydrolyzed PET using P. umsongensis GO16 KS3. The ence of a catalyst (Fukushima et al., 2013; Jamdar et al., 2018; Natar
medium-chain-length PHA comprised C10, C12, and C8 molecules (61, ajan et al., 2017; Tan et al., 2019). Introducing amide groups into the
24, and 15 mol%, respectively). Similarly, Liu et al. (2021) successfully polymer backbone typically reinforces the mechanical and thermal
demonstrated a bioconversion system for upcycling waste PET into properties of the polymer. Another study on PET upcycling used a
polyhydroxybutyrate (PHB) through the co-cultivation of two microor one-pot strategy for converting post-consumer PET into segmented
ganisms. To achieve PET degradation, the researchers engineered the thermoplastic copolyesters (TPCs) (Karanastasis et al., 2022). The re
yeast Yarrowia lipolytica to effectively express PETase from I. sakaiensis. searchers synthesized engineering-grade TPCs using a combination of
For PHB biosynthesis from enzymatic hydrolysates of PET, a PET and bio-derived dimer fatty acids with a titanate/magnesium ace
TPA-catabolizing Pseudomonas stutzeri strain was transformed with the tate (TBT/Mg(OAc)2) catalyst system. The mechanical properties of the
phbCAB operon from Ralstonia eutropha. Guzik et al. (2014) reported the TPCs were comparable to those of commercial TPC analogs.
synthesis of PHA from polyethylene through a two-step chemical–bio
logical process. PHA, corresponding to 25% of the dry bacteria, was 4.2.2. Carbon nanomaterials
produced from polyethylene pyrolysis products using the Pseudomonas Considering the high carbon content of plastic waste, it has the po
aeruginosa PAO-1 strain. These methods provide a way to convert tential to be used as a feedstock for the synthesis of carbon nano
nondegradable plastic waste into biodegradable plastics. materials (Jia et al., 2022; Zhuo and Levendis, 2014) and microporous
activated carbon (X. Liu et al., 2022; J. Wang et al., 2020; Yuan et al.,
2020). Carbon nanomaterials have excellent physicochemical properties
4.2. Chemical upcycling to form value-added products and are widely used in clinical, electrochemical, and environmental
applications (Aji et al., 2018; Dai et al., 2012; Deng et al., 2016; Sawant
Next, we introduce studies on the upcycling of plastic waste into new et al., 2014). Consequently, converting plastic waste into carbon nano
polymer materials using chemical methods. The chemical depolymer materials such as carbon nanotubes (Aboul-Enein and Awadallah, 2019;
ization of general industrial plastics has recently attracted considerable Liu et al., 2017, X. Liu et al., 2018; Yao et al., 2017), fullerenes (Elessawy
attention for treating environmental waste. To adequately repurpose et al., 2020a, 2020b), and graphene (Cui et al., 2017; Gong et al., 2014a;
waste plastic, new and price-competitive chemical processes that use Pandey et al., 2019) has garnered increasing attention in recent years.
waste polymers as the starting material need to be developed. To this Cui et al. (2017) produced high-quality graphene on Ni foil via
end, several studies are underway on the chemical upcycling of poly chemical vapor deposition by using several types of waste plastic as a
mers (Dennis et al., 2014; Fukushima et al., 2013).
8
carbon source, including PET, PE, PVC, PP, and PS. The graphene films Therefore, biological and chemical upcycling need to be developed for a
had a high electrical conductivity of up to 3824 S cm− 1 and high flexi cooperative effect to increase the efficiency of upcycling plastics.
bility. Gong et al. (2014b) synthesized porous carbon nanosheets
(PCNSs) from mixed plastic waste consisting of PP, PE, PS, PET, and PVC 5. Development of recyclable/upcyclable high-performance
on organically modified montmorillonite. The prepared PCNSs had a plastics
high specific surface area of 1734 m2 g− 1 and large pore volume of
2.441 cm3 g− 1. Moreover, the CO2 uptake and hydrogen adsorption Because thermoset plastics have high dimensional stability at high
capacities of the PCNSs increased at increased pressures; at 45 bar, temperatures, they are widely used as high-performance materials, such
values of 18 and 1.4 mmol g− 1 were achieved, respectively. Converting as in electronics and aerospace applications (Das et al., 2021). Most
mixed plastics into value-added materials is a significant approach for thermosetting resins, including epoxy resins, melamine resins, poly
sustainably harnessing “real world” plastic wastes. imides, and phenol resins, are difficult to recycling using traditional
methods because they do not melt or dissolve in organic solvents. While
4.2.3. Pollutant-removing materials polyimides are technically pseudo-thermoplastic resins, the majority are
Several research groups have developed methods for converting insoluble and unmeltable; therefore, they are often considered as ther
nondegradable plastic waste into sorbents for environmental pollutants mosetting plastics. Recent research has focused on developing recy
(Enyoh et al., 2021; Saleem et al., 2018). For example, carbon-based clable materials that have similar high-performance properties to
sorbents for the capture of CO2 have been synthesized from waste thermoset plastics, such as comparable coefficients of thermal expan
PVC. PVC has limited recyclability owing to its low thermostability and sion, and thermoset resins that can be recycled or decomposed at the end
high content of plasticizers and chlorides, which cause the formation of of their lifecycle (Fig. 4). These research areas are discussed in this
dioxins and chlorination. Therefore, green and sustainable methods are section.
required for consumer PVC upcycling. Converting PVC into porous
carbon-based materials is a promising strategy. X. Liu et al. (2022) 5.1. High-performance thermoplastic resins
synthesized microporous carbon materials from PVC pipes via a
water-acid washing procedure using KOH as the activating agent. The The first research area for developing high-performance plastics that
surface area and total pore volume of the samples were 504–2507 m2 can be recycled or upcycled involves the design of thermoplastic resins
g− 1 and 0.19–1.11 cm3 g− 1, respectively. At a CO2 partial pressure of with thermal and mechanical properties comparable to those of ther
100 kPa, CO2 adsorption capacities of up to 6.9 and 3.9 mmol g− 1 were moset resins. Thermoset resins have a relatively low coefficient of
achieved at 0 and 25 ◦ C, respectively. Wang et al. (2022) suggested a thermal expansion of <80 ppm K− 1 (Cheng et al., 2019; Wippl et al.,
strategy for directly transforming PVC into carbonaceous spheres for 2005), whereas those of thermoplastics range from 25 to 200 ppm K− 1
CO2 capture. Porous PVC-derived carbon spheres were prepared via (Irshad et al., 2021). Recently, researchers have synthesized recyclable
dehalogenation and oxidation crosslinking with tetrabutylammonium thermoplastics with have high heat resistance using bio-renewable
bromide (TBAB) and NaOH, followed by an activation–carbonization aliphatic heterocyclic monomers (Ali and Kaneko, 2022; Kim et al.,
step using KOH. With a specific surface area of up to 1738 m2 g− 1, the 2020; Zhu et al., 2016). The aromatic cyclic structure improves the
porous carbon spheres achieved CO2 adsorption capacities of up to 8.93 thermal and mechanical properties of plastics by limiting their molec
and 5.47 mmol g− 1 at 0 and 25 ◦ C, respectively. ular behavior compared to that of plastics with aromatic linear struc
Waste plastics have been investigated as a feedstock for aerogel tures. As shown in Fig. 4, a thermoplastic resin with a high Tg (212 ◦ C)
production. Aerogels are highly porous materials with large specific and very low coefficient of thermal expansion (23.8 ppm K− 1) was
surface areas, low densities, and excellent thermal insulation. They are developed using isosorbide, a sugar-based aliphatic cyclic monomer
applicable in various fields, including as filters for pollutants such as (Park et al., 2019). Because most thermoplastics melt at temperatures of
CO2 (Kong et al., 2016; Le et al., 2019; Wang and Okubayashi, 2019) and 200 ◦ C or higher, Shi et al. (2021) hybridized ε-caprolactone and
spilled oil (Le et al., 2020; Pawar et al., 2021). Le et al. (2019) prepared γ-butyrolactone to prepare a double-cyclic monomer and manufactured
waste PET-based aerogels coated with silicone ceramic and a polymer by opening only one ring through a ring-opening reaction.
amine-functionalized PET aerogels using (3-aminopropyl)triethox The resultant material had a high Tg of 135 ◦ C and melting temperature
ysilane, which achieved CO2 adsorption capacities of up to 0.15 and of 263 ◦ C. Furthermore, this material decomposed at a low temperature
0.44 mmol g− 1, respectively. Pawar et al. (2021) prepared hybrid aer of 135 ◦ C in the presence of a suitable catalyst, enabling it to be recycled.
ogels from PET, PVA, and glutaraldehyde, which had an adsorption Elastomers are important materials for the manufacture of flexible
capacity of 27.43 g g− 1 for pump oil, 39.30 g g− 1 for chloroform, and electronics (W.-C. Liu et al., 2018; Shin et al., 2019) and automobile tires
27.65 g g− 1 for soybean oil. Roy et al. (2021) developed a fabrication (Jeon et al., 2021; Qin et al., 2018). Although there are thermoplastic
approach for 3D electrospun PET aerogels from waste PET, and used the elastomers, they tend to have poor performance; therefore, thermoset
resultant aerogel for the removal of toxic chemicals and carcinogenic ting elastomers are far more commonly used for these applications. To
metal ions from contaminated water. The fluffy and flexible 3D PET utilize renewable materials, high-performance elastomers have been
aerogels exhibited Pb(II), Hg(II), and Zn(II) removal efficiencies of developed using lignin (Huang et al., 2019). This renewable elastomer
approximately 98.7%, 95.3%, and 92.7%, respectively. has higher mechanical performance than that of conventional thermo
Biological upcycling is possible to be used as various microorganisms plastic elastomers because it forms metal ionic bonds. Another group of
and enzymes under mild conditions without high temperatures and researchers created a thermoplastic polyurethane based on carbonate
pressures. The enzymatic hydrolysis of PET and PHA by a mixture of polyols (Hu et al., 2022). This elastomer had self-healing properties that
PETase and various enzymes results in a low yield rate and relatively compensated for the poor mechanical properties of thermoplastics;
slow degradation times for PET and PHA compared to chemical methods therefore, it was suitable for use as a tire material.
(H.T. Kim et al., 2021). Chemical methods, on the other hand, are
rapidly being developed by alternative methods such as 5.2. Recyclable crosslinked resins with dynamic or reversible bonds
high-performance plastic materials, carbon nanomaterials, and
pollutant-removing materials. It is possible to gain a high yield rate of The second method of creating high-performance plastics that can be
depolymerization and upcycling due to effective chemical reactions. recycled or upcycled is to develop recyclable crosslinked resins. While
However, there are significant drawbacks, including numerous envi traditional thermosetting resins have a crosslinked network structure
ronmental pollutant factors (e.g., consuming massive energies at high with irreversible covalent bonds, researchers have created a class of
temperatures and pressures) and a high cost (Carta et al., 2003). polymer material called vitrimers, which are crosslinked by dynamic or
9
Fig. 4. Overview of three major directions for the development of recyclable/upcyclable high-performance plastics as alternatives for thermoset resins toward
sustainable and circular e-waste or urban mining economies. (1) Super engineering thermoplastics: thermoplastics with similar high-performance properties to
thermoset plastics, such as comparable coefficients of thermal expansion. Reprinted from Ref (Park et al., 2019). With permission under the terms and conditions of
the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/). (2) Recyclable thermoset plastics: crosslinked resins with dy
namic or reversible bonds, to enable recycling at the end of the product lifetime. (3) Decomposable thermoset plastics: thermoset resins that decompose at the end of
their lifecycle.
reversible bonds. This approach was first proposed by Leibler’s group in can undergo imine–amine exchange and imine hydrolysis reactions.
2012 (Capelot et al., 2012). The crosslinking points are stable at low Zhao and Abu-Omar (2018) prepared a reprocessable imine-containing
temperatures; thus, at temperatures below 150–200 ◦ C, vitrimers exhibit thermoset epoxy resin. The thermoset epoxy resin with imine-embedded
the same behavior as thermosetting resins, such as high mechanical and bisphenol was recyclable and malleable. Malleability is characteristic of
thermal performance, while they adopt a moldable state above a certain self-healing materials, and it can occur in vitrimers due to the similarity
temperature (approximately 250–300 ◦ C), enabling them to be recycled of their bonding structures. Wang et al. (2019) and Zhao and Abu-Omar
by heating (Jin et al., 2019). It has been suggested that the reprocess (2018) synthesized recyclable high-performance epoxy vitrimers by
ability and recyclability of vitrimers will be instrumental to solving incorporating bio-based vanillin. An imine-containing hardener was
environmental problems (Trinh et al., 2022). The crosslinking points in synthesized from lignin-derived vanillin and isophorone diamine using
vitrimers are commonly hydrogen bonds (S. Wang et al., 2020). Disul ethanol as the solvent. The resulting epoxy vitrimer cured by the
fides, silyl ethers, and boronic esters are effective crosslinking agents for bio-based hardener exhibited impressive performance with a high Tg
vitrimers with reversible noncovalent bonds (Zheng et al., 2021). (>120 ◦ C), excellent tensile strength (>60 MPa), and high Young’s
Notably, biomonomer-based vitrimers are both recyclable and beneficial modulus (>2.5 GPa). Notably, the vanillin-based vitrimer had compa
for carbon neutrality (Wang et al., 2019). In this regard, citric acid is a rable thermal and mechanical properties to an epoxy cured by a
three-armed biomonomer that can be used as a potential crosslinking petroleum-based hardener, p-hydroxybenzaldehyde. Furthermore, the
agent in vitrimer biopolymers by transesterification (Chon et al., 2017; authors demonstrated that the epoxy vitrimers were degradable in an
Yoon et al., 2019). isophorone diamine solution and could be recycled to synthesize new
Dynamic bonding is a basic chemical property of self-healing mate epoxy vitrimers. The recycled resins exhibited similar mechanical and
rials. Therefore, self-healing materials and vitrimers are sister materials. thermal properties to the original resins.
Self-healing materials are linear polymers with dynamic covalent bonds, Diketoenamine bonds are efficient dynamic covalent bonds for
whereas vitrimers are crosslinked polymers with dynamic covalent developing recyclable thermoset plastics (Christensen et al., 2019).
bonds. Self-healing can be achieved using both dynamic covalent and Diketoenamine bonds are spontaneously formed from triketones and
noncovalent bonds (Cho et al., 2021; Lee et al., 2019). As a represen amines. At reaction equilibrium, triketones exchange different amine
tative example, structurally strong hydrogen bonding can induce water groups. Under acidic conditions, the diketoenamine bond is hydrolyzed
warping between molecules at a new interface. Therefore, self-healing to a triketone and ammonium salt, enabling the polymer to be recycled.
materials using hydrogen bonding have recently been developed. Ac
cording to the same principle, vitrimers can be made from 5.3. Decomposable thermoset resins
thiourea-based polymers via hydrogen bonding of the thiourea groups
(Feng et al., 2022). The third method of developing more environmentally friendly
Imine bonds are considered effective dynamic bonds because they thermoset resins is to achieve easy decomposition. Thermosetting resins
10
that are easily decomposed have a unique crosslinked structure that layers and anti-pollution materials instead of metals, halogen-based
decouples upon heating or specific chemical treatments (Fortman et al., polymers, and perfluoro compounds, the harmful gases and fine dust
2018; D.H. Kim et al., 2021; Y. Liu et al., 2022). These materials have that are produced during pyrolysis can be reduced. In the field of fine
high heat resistance as thermoset plastics before these decoupling re chemistry, researchers are actively working to develop low-molecular-
actions. After the decoupling reaction under external stimuli, the ma weight materials from plastic waste decomposed through catalytic
terial decomposes and returns to its monomer state. For example, a chemical or biochemical methods. However, the chemicals produced via
thermoset resin with silyl ester groups as the crosslinking points was these methods are effectively raw materials, and additional processes
found to hydrolyze in the presence of seawater and light (Xie et al., are required to use them. In contrast, technologies for upcycling plastic
2018). As another example, a thermosetting resin crosslinked with a waste or decomposition products into high-value-added materials or
hexahydro-1,3,5-triazine group was able to decompose in a relatively materials with additional characteristics, such as biodegradation, are
environmentally friendly phosphoric acid solution (Ma et al., 2020; Xu more cost-efficient and will therefore improve the efficiency of plastic
et al., 2020). Therefore, unlike conventional thermoset resins that must waste upcycling. Finally, research is actively underway to develop
be incinerated or treated with strong chemicals to decompose, these thermoset resins that can be reprocessed and decomposed beyond the
materials can decompose under relatively environmentally friendly limitations of existing thermosetting resins, along with thermoplastics
conditions. with high thermal and mechanical properties. By replacing existing
García et al. (2014) reported the synthesis and properties of poly thermosetting materials, such as those in electronic components, with
(hexahydrotriazine), a thermoset resin with a hemiaminal dynamic co high-performance materials that are easy to reprocess and decompose, e-
valent network. This thermoset resin had a high Young’s modulus of waste will be reduced and the efficiency of critical metal recycling will
14.0 GPa, yet could be degraded in a highly acidic environment (pH < 2) be improved.
to recover the monomers. Degradable phenolic resins have also been In conclusion, the development of sustainable polymer chemistry
reported. Li et al. (2020) prepared a phenolic polymer that was cross and engineering technologies is crucial for addressing the plastic waste
linked with asymmetric acetal groups. This thermoset plastic exhibited problem. To achieve highly efficient recycling and upcycling for a sus
excellent creep resistance even at 100 ◦ C. In addition, it could be effi tainable future, a multidisciplinary approach is needed that integrates
ciently decomposed to form soluble phenolic polymers via hydrolysis technological advances with a reconsideration of recycling and upcy
under mild acidic conditions. cling practices, strengthened policies and regulations, life-cycle assess
Biodegradable thermosetting resins made from bio-based resources ment, and social cohesion for expanding infrastructure alignment
can contribute to CO2 reduction. Epoxy resins have been synthesized (Kumar et al., 2021a). By optimizing social strategies and advanced
using 2,5-furandicarboxylic acid (FDCA), a representative bio-aromatic recycling and upcycling technologies, we can solve the plastic waste
ring monomer (Chen et al., 2020). FDCA does not have high chemical problem for current and future generations.
and thermal stability and can be used to induce the degradation of
FDCA-based epoxy resins. Ma et al. (2019) fabricated a Author contributions
high-performance thermoset resin using lignin-derived spiro diacetal.
The aromatic ring structure of lignin increased the heat resistance of the Hyuni Jung: Writing – original draft preparation; Giyoung Shin:
resin, and the diacetal group could be decomposed under relatively mild Writing – original draft preparation; Hojung Kwak: Data curation; Lam
conditions. Tan Hao: Data curation; Jonggeon Jegal: Supervision, Reviewing; Hyo
The sustainable thermosetting resins made using the three strategies Jeong Kim: Conceptualization, Reviewing; Hyeonyeol Jeon: Supervi
mentioned above can be used as raw materials for producing substrates sion, Reviewing, Funding acquisition; Jeyoung Park: Conceptualization,
of electronic components. Electronic substrates composed of sustainable Reviewing, Supervision; Dongyeop X. Oh: Conceptualization, Review
thermosetting resins are expected to exhibit high e-waste mining effi ing, Supervision, Funding acquisition.
ciencies (Guo et al., 2021). Notably, the expansion of these electronic
products promotes the reuse of critical metals.
Declaration of competing interest
6. Outlook and conclusions
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
Plastics are a vital part of modern life owing to their durability,
the work reported in this paper.
productivity, and affordability. However, the proliferation of plastic
waste is a growing concern, as plastics rapidly lose value after their
Data availability
intended use. In addition, plastic waste causes significant environmental
problems, as only ~9% of it is recycled as of 2015. Since the 1980s, 8300
No data was used for the research described in the article.
million metric tons of plastic waste have been generated (Geyer et al.,
2017). The global waste management market was valued at US$ 37
Acknowledgement
billion in 2021, and is projected to reach over US$ 59 billion by 2030,
with a compound annual growth rate of 5.4% (Shen et al., 2020). As a
This work was supported by the Bio-Industrial Technology Devel
result, it is crucial to improve the efficiency of recycling and upcycling
opment Program (20008628) funded by the Ministry of Trade, Industry,
plastic waste.
& Energy (MI, Korea), the Korea Research Institute of Chemical Tech
In this review, we summarized recent advances in sustainable poly
nology (KRICT) core project (KS2342-10), and the Basic Science
mer chemistry and engineering technologies for improving the effi
Research Program through the National Research Foundation of Korea
ciency of recycling and upcycling of plastic waste. Current recycling and
(NRF) funded by the Ministry of Science, ICT, & Future Planning
upcycling technologies are limited by the diversity of plastic types, the
(2020R1C1C1003665, 2022R1C1C1003468 and 2022M3H4A1A
use of additives, contamination, and the limitations of thermoset resins.
03076577).
To address these challenges, several approaches have been proposed.
One approach is to replace environmentally unfriendly additives with
eco-friendly ones, which can improve the recycling efficiency of plastic References
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Contents lists available at ScienceDirect

Review of polymer technologies for improving the recycling and upcycling

• Summarized recent advances for

1. Introduction physicochemical properties of plastics, issues related to contamination,

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