Conversion of Waste Plastics Into Value Added Carbon Materials

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Environmental Chemistry Letters (2023) 21:3127–3158

https://doi.org/10.1007/s10311-023-01638-7

REVIEW ARTICLE

Conversion of waste plastics into value‑added carbon materials


Yueyue Luo1 · Xiao Lin1 · Eric Lichtfouse2 · Hongru Jiang3 · Chongqing Wang1

Received: 18 May 2023 / Accepted: 24 July 2023 / Published online: 19 August 2023
© The Author(s), under exclusive licence to Springer Nature Switzerland AG 2023

Abstract
Plastic pollution is a major environmental issue worldwide, calling for advanced methods to recycle waste plastics in the
context of the circular economy. Here we review methods and strategies to convert waste plastics into value-added carbon
materials, with focus on sources, properties, pretreatment of waste plastics, and on preparation of carbon materials. Pretreat-
ment techniques include mechanical crushing, plastic stabilization and electrospinning. Carbon materials such as carbon
nanotubes, graphene, carbon nanosheets, carbon spheres and porous carbon are prepared by oxygen-limited carbonization,
catalytic carbonization, the template-based method, and pressure carbonization. We emphasize the conversion of polyethene
terephthalate, polyethylene, polypropylene, polystyrene, halogenated plastics, polyurethane and mixed plastics.

Keywords Carbon materials · Circular economy · Environmental pollution · Waste management · Waste valorization

Introduction valuable land resources, but also causes environmental pol-


lution (Islam 2018; Nanda and Berruti 2021a; Wang et al.
Due to low cost, durability, hygiene, and formability, plastics 2022e). During the slow degradation process of waste plas-
are widely used in various fields such as building materials, tics in landfill sites, toxic leachate streams and microplas-
electronic equipment, automotive manufacturing, medical tics are continuously released, causing significant pollution
devices, and packaging materials. According to Plastics of the environment (Naqash et al. 2020; Chia et al. 2021;
Europe 2023, global plastic production in 2021 was 390.7 Jiang et al. 2023). Additionally, direct incineration of waste
million tons. However, the rapid growth of plastic produc- plastics will release a large number of organic compounds
tion combined with short shelf life results in a large amount and volatile gases, causing serious air pollution. Moreover,
of waste plastics (Zhang et al. 2023). By 2050, the total heavy metals such as lead, mercury, and cadmium may be
amount of waste plastics may reach 850–950 metric tons, released into the environment along with ash and gas during
causing great harm to natural ecosystems and public health the incineration process (Islam 2018; Padervand et al. 2020;
(Degnan and Shinde 2019; Singh et al. 2022). Currently, Zhang et al. 2021a). The analysis of current incineration
the major methods for disposing waste plastics are land- practice shows that the efficiency of energy recovery through
fill and incineration. Due to the chemical stability and low incineration is usually very low (Degnan and Shinde 2019).
bio-degradability, traditional landfilling not only consumes In recent years, nano-carbon materials and carbon-based
composites have broad application prospects in catalysis,
separation, environment, energy, and fuel due to their excel-
* Chongqing Wang lent properties. Waste plastics contain a large amount of car-
[email protected] bon, especially in polyolefins (85.7%). Therefore, converting
Eric Lichtfouse waste plastics into high value-added carbon materials is a
[email protected] promising method for management of waste plastics, favor-
1
School of Chemical Engineering, Zhengzhou University,
ing the reduction of environment pollution and the resource
Zhengzhou 450001, China recycling (Chen et al. 2020; Gong et al. 2019; Sun et al.
2
State Key Laboratory of Multiphase Flow in Power
2022; Huang et al. 2022). Waste plastics, such as polyvinyl
Engineering, Xi’an Jiaotong University, Xi’an 710049, chloride, polystyrene, polyethylene terephthalate, polyethyl-
Shaanxi, People’s Republic of China ene, and polypropylene, has been studied for fabricating car-
3
College of Chemistry and Chemical Engineering, Central bon materials, such as graphene, carbon nanosheets, carbon
South University, Changsha 410083, Hunan, China

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Vol.:(0123456789)
3128 Environmental Chemistry Letters (2023) 21:3127–3158

nanotubes, and porous carbon (Chen et al. 2022; Hou et al. different types of carbon materials derived from waste plas-
2021). Waste plastics can undergo different carbonization tics in batteries, supercapacitors, water electrolysis, pollut-
methods to obtain carbon materials with different proper- ant removal, solar evaporation, and carbon dioxide capture
ties. Carbon materials with high porosity, large surface area, in recent years. This work gives a better understanding of
abundant surface groups, and good conductivity have been carbonization methods, carbonization mechanism, and the
widely used in batteries, supercapacitors, water electroly- properties and application of carbon materials derived from
sis, pollutant removal, solar energy evaporation, and carbon waste plastics.
dioxide capture (Al-Enizi et al. 2020b; Deka et al. 2020;
Gim et al. 2021; Kaur et al. 2019b; Kumari et al. 2022; Luo
et al. 2023). Sources and properties of waste plastics
The conversion of waste plastics valuable carbon mate-
rials through thermochemical processes has many benefits Waste plastics originates from different sources, mainly
from both social and industrial aspects. This strategy reduces involving daily plastics such as packaging materials and
environmental pollution resulted from waste plastics, pro- disposable plastic products, industrial wastes such as lefto-
moting the sustainable of our society. As to industrial aspect, vers and defective products, agricultural materials such as
recycling waste plastics can decline the consumption of fos- plastic films and irrigation pipes, as well as building materi-
sil feedstocks, and the functional carbon derived waste plas- als, electrical equipment, and automobiles. Waste plastics
tics can be applied in various industries such as energy, envi- are difficult to handle due to its complex composition and
ronment, and fuel. Due to increasing attention and extensive large quantity, and the recycling of waste plastics in green
studies on carbon materials derived waste plastics, review methods gains global attention (Nanda and Berruti 2021b;
papers have been published to summary carbonization meth- Nandhini et al. 2022). The polymers are different for dif-
ods (Dai et al. 2023; Jiang et al. 2022a), graphene-based ferent plastics. Waste plastics can be divided into oxygen-
materials (Vieira et al. 2022), carbon nanomaterials (Ren containing plastics and oxygen-free plastics based on the
et al. 2022), and energy and environmental applications presence of oxygen atoms in the polymers. Herein, oxygen-
(Chen et al. 2022). Currently, this is still no comprehensive containing plastics means the presence of oxygen atoms in
summary of the sources and properties of waste plastics, main chains of polymers such as polyethylene terephthalate.
the carbonization methods, and the application of carbon Plastics such as polyacrylonitrile, polypropylene, polysty-
materials derived from waste plastics. Here we survey the rene, and polyvinyl chloride are oxygen-free plastics due to
plastic sources, synthesis methods, and various applications the absence of oxygen atoms in polymers. The main chains
of carbon materials derived from waste plastics (Fig. 1). The of oxygen-containing plastics do not decompose during car-
properties, pre-treatment methods, carbonization methods, bonization, but form carbon materials through cyclization,
and factors affecting the morphology of carbon materials aromatization and cross-linking. During carbonization of
are described. The review discusses the applications of oxygen-free plastics, the main chain of these plastics breaks,

Fig. 1  Waste plastics from


different industries can be
converted into carbon materials
by different synthesis meth-
ods, then applyed for different
applications such as batteries,
solar evaporation, and pollutant
degradation

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Environmental Chemistry Letters (2023) 21:3127–3158 3129

and small molecules such as propylene, methane, and ben- 26 million tons and generating approximately 62.8 bil-
zene are generated through dehydrogenation, cyclization, lion plastic bottles (Sang et al. 2020). How to dispose
and aromatization, resulting in low yield of carbon prod- waste polyethylene terephthalate has become one of the
uct. In order to improve carbon yield, pre-treatment of these most urgent problems (Hu et al. 2014a; Kaur et al. 2019a;
plastics can be conducted to stabilize the carbon chain, and Dhaka et al. 2022).
catalysts or templates can be added during carbonization For waste plastics that do not contain oxygen in the
to promote the generation of carbon materials from small main chain of polymer, they can be classified based on the
molecules (Chen et al. 2020). The information of common heteroatoms such as Cl, N, and S in the polymers. Poly-
plastics is summarized in Table 1, including chemical for- ethylene, polypropylene, and polystyrene have no heter-
mula, source, and properties. Waste plastics are derived from oatoms in their polymer molecules, only containing C and
various industries, and show different properties. Except H atoms. The carbon content of these plastics higher than
Polyurethane, most plastics have high carbon content and 80% makes them suitable for producing carbon materials.
are potential precursor for fabricating carbon materials. Polypropylene is a thermoplastic plastic commonly used
Polyethylene terephthalate is a thermoplastic polymer in packaging, textiles, and automotive, while polystyrene
that is chemically and physically stable, lightweight, and and polypropylene are thermoplastic plastic commonly
transparent. Coupled with high availability and low cost, used as single-use food packing and disposable masks.
polyethylene terephthalate is widely used as packaging Carbonization of waste polyethylene, polypropylene and
materials, with an annual production of approximately polystyrene with high carbon content to obtain functional

Table 1  Common plastics used for preparing carbon materials


Polymer Structural formula Carbon Sources of waste plastics Properties
content
(wt%)

Polyethylene 85.6 Household, industrial packag- Excellent low-temperature resist-


ing plastics, and agricultural ance, chemical stability, and
plastics electrical insulation
Polypropylene 85.6 Household, industrial packaging, Chemical resistance, heat resist-
and automotive ance, good electrical insulation,
and high mechanical strength
Polystyrene 92.2 Household, industrial packaging Good electrical performance,
plastics, building, demolition, easy processing, good thermal
waste of electric and electronic insulation, and excellent optical
equipment performance
Polyethylene terephthalate 67.9 Household packaging plastics Chemical and physical stability,
light weight and transparency,
high availability, low cost
Polyacrylonitrile 67.9 Products of everyday use Good stability and construction,

Polyurethane 20.3 Building, demolition, automotive High C and N content, good ther-
mosetting and flexible structure

Polyvinyl chloride 38.4 Building Good chemical stability and ther-


mal stability, easy to discharge
harmful by-products
Polyphenylene sulfide 66.7 Electronics, machinery, automo- High mechanical strength, good
tive, and chemical stability, and good electrical
performance
Polycarbonate 75.6 Glass, automotive, and electronics Good mechanical properties, heat
aging resistance, solvent resist-
ance, and excellent insulation
Polymethyl methacrylate 60.0 Building and sanitary ware High transparency and easy to
machine

Polyamide 63.7 Parts and chemical Tough, soft, wear-resistant, and


highly absorbent

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3130 Environmental Chemistry Letters (2023) 21:3127–3158

carbon materials is recognized as a convenient and attrac- improve the yield, components, structure, or morphology of
tive option for treating wastes plastics (Ma et al. 2020). carbon products.
Polyurethane, polyacrylonitrile and polyphenylene sulfide
with N, S atoms in the polymer chain can also be potential Mechanical crushing
carbon sources for fabricating functional carbon materials.
Self-doped N and S heteroatoms can enhance the chemical Waste plastics derived from real plastic products are often
properties of carbon materials, improving the conductivity, large in size, and reducing the size of waste plastic is often
surface wettability, and pseudo-capacitance. In addition, het- necessary for sufficient carbonization. Mechanical crushing
eroatom doping can increase the active sites on the surface of waste plastics results in uniform particles or fragment
of carbon materials and improve the adsorption performance of plastics with small size, and this is favorable for mixing
for pollutants (Xiang et al. 2017; Yuan et al. 2020a). The with additional substances and subsequent carbonization.
main component of packaging materials, sponges, uphol- The modes of mechanical crushing are different for plastics,
stered furniture, and car seats is polyurethane, and approxi- mainly involving ball milling, grinding, and shearing. Shear
mately 19 million tons of waste polyurethane is generated milling is suitable for reducing plastic size due to the good
annually (Deka et al. 2020; Schneidermann et al. 2019). Pol- flexibility of waste plastics, for example flexible polyethyl-
yacrylonitrile is mainly used to manufacture synthetic fibers ene terephthalate and polyvinyl chloride (Liu et al. 2020,
that are mainly used in daily clothing and woolen fabrics. 2022b). Waste polyethylene bags were not easy to cut and
The production of high-performance carbon materials using grind, and ball milling was used to evenly mix them with
the high melting point of polyacrylonitrile has been reported other substances before carbonization (Lian et al. 2019b).
(Yin et al. 2022). Polyphenylene sulfide is widely used due Moreover, a ball mill tank was used to reduce the size of
to its high mechanical strength, good thermal stability, and polyurethane plastic, and then it was thoroughly mixed with
excellent electrochemical performance, and a large amount potassium carbonate as activator and urea for N-doping in
of waste polyphenylene sulfide is generated and accumu- the ball mill tank for sufficient mixing, and finally carboni-
lated in the environment (Guo et al. 2018a). Therefore, using zation was conducted to obtain carbon material (Schneider-
waste polyurethane, polyacrylonitrile, and polyphenylene mann et al. 2019).
sulfide plastics as carbon sources to prepare multifunctional
carbon materials will be a promising method for sustainable Plastic stabilization
treatment of waste plastics.
For waste plastics containing halogens such as fluorine The carbon chain of oxygen-free plastics will decompose
and chlorine, polyvinylidene chloride and polyvinyl chloride into gases such as ­CO2, ­H2O, and ­H2 during the carboni-
are also used to synthesize carbon materials. Polyvinyl chlo- zation process, resulting in low carbon yield. Introducing
ride is widely used in healthcare, packaging, and building oxygen-containing groups or chemical treatments to obtain
materials. Polyvinyl chloride has very good chemical stabil- cross-linked or trapezoidal structures is essential to stabilize
ity and thermal stability. A large amount of waste polyvinyl the carbon chain of oxygen-free plastics. Direct injection of
chloride causes significant problems. During the process of oxygen into the carbonization process of waste plastics is
incineration or landfill, extremely harmful by-products of the most commonly used stabilization method. When poly-
­Cl2, HCl, and organochlorinated compounds are emitted, acrylonitrile was carbonized in air, the oxygen atoms helped
which will lead to serious environmental pollution (Chang to improve its stability, reduced the exothermic rate, and
et al. 2018). improved the final carbon yield (Duan et al. 2019). Com-
pared to polyacrylonitrile, it is relatively difficult to stabilize
polyolefins and polystyrene chains through simple thermal
Pretreatment of waste plastics oxidation. After chemical stabilization, polyethylene and
polystyrene can also be further carbonized and converted
Commonly, waste plastics need to be pretreated before into carbon materials at high temperatures. Chemical treat-
carbonization. Mechanical crushing is the most used pre- ment typically utilizes sulfuric acid to introduce sulfonic
treatment for sufficient carbonization or uniformly mixing acid groups and stabilize polymer carbon chains (Chen
materials with waste plastics. Pretreatment of oxygen-free et al. 2020). Intermolecular or intramolecular crosslinking
plastics is essential to increase the yield of carbon prod- inhibits the decomposition of macromolecular chains dur-
ucts. Moreover, pretreatment of waste plastics is conducted ing the carbonization process, promotes the carbonization
to obtain carbon products with special morphology and of polymers, and greatly improves the carbon yield. For
properties, such as electrospinning for carbon microfiber polyethylene, the carbon chain was chemically stabilized
and metal–organic framework for porous carbon loaded by sulfonation with Oleum (Hu et al. 2019). The chemical
with metals. Pretreatment of waste plastics is examined to stability of polystyrene can be achieved not only through

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Environmental Chemistry Letters (2023) 21:3127–3158 3131

sulfonation, but also through Friedel Crafts reaction with the framework (Al-Enizi et al. 2020a). N-doped mesoporous
phenyl group of polystyrene. Through Friedel Crafts reac- carbon with high surface area was prepared by carbonizing
tion, the high-density carbonyl cross-linked bridge formed the metal–organic framework-5 structure (Ubaidullah et al.
between polystyrene chains contains an appropriate amount 2021). In addition, the metal oxide nanoparticles were
of oxygen atoms, which has good carbonization performance embedded in the metal–organic framework by chemical
(Zou et al. 2010). methods to obtain the pristine metal–organic framework-5
and Co-metal–organic framework. Subsequently, the car-
Electrospinning bonization of metal–organic frameworks produces metal
oxides containing carbon networks, which promotes the
Electrospinning is considered to be an ideal method for enhancement of surface area, conductivity, and stability.
manufacturing nanofibers with adjustable pore size. Electro- Metal–organic framework improves the surface area and
spinning can be used to fabricate carbon fibers using waste porosity of carbon materials, and metal oxide nanoparti-
plastics, and dissolution of plastics using organic solvents is cles improve the electrochemical performance and stabil-
imperative to prepare polymer solution for electrospinning. ity of carbon materials. Therefore, it is economically feasi-
The fiber density and size distribution can be controlled by ble to convert waste plastics into metal–organic framework
changing the feed rate and humidity of electrospinning, and (Al-Enizi et al. 2020a, 2020b).
the fiber structure before carbonization can be maintained Pretreatment of waste plastics prior to carbonization
even after high temperature carbonization (Mirjalili et al. can change the physical and chemical properties of plas-
2020). Benefiting from the versatility of electrospinning, tics. Reducing the size of waste plastics and stabilizing the
metal coordination compounds and polymer solutions can carbon chains of oxygen-free plastics are the main strate-
be encapsulated in the electrospinning precursor (Jin et al. gies, while using electrospinning technology and convert-
2017). For N-doping of carbon fibers, electrospinning of ing waste plastics into metal–organic framework can help
the solution of dicyandiamide, polyacrylonitrile and nickel prepare carbon materials with the desired morphology and
acetophenone was conducted to prepare carbon fibers, and functionality through carbonization.
porous carbon nanofiber loaded with NiO was obtained after
carbonization (Fig. 2) (Li et al. 2018b). Nickel oxide par-
ticles were uniformly distributed on the surface of porous Preparation of carbon materials
carbon nanofibers, providing many electroactive sites for
high carbon dioxide absorption. Waste plastics usually need to be converted into carbon
materials through high-temperature carbonization under
Metal–organic framework materials different atmospheres, catalysts, templates, and pressure
conditions. By changing the conditions during the carboni-
Recently, metal–organic frameworks have attracted much zation process, carbon products with different structures
attention due to the high surface area and excellent poros- and properties can be obtained, such as activated carbon,
ity. Polyethylene terephthalate derived from plastic bottles carbon fibers, carbon spheres, carbon nanotubes, and gra-
was depolymerized with ethylene glycol to form benzene- phene (Hou et al. 2021; Hussin et al. 2021; Kumari et al.
1,4-dicarboxylic acid as the precursor of the metal–organic 2022). This section introduces the carbonization methods,

Fig. 2  N-doped porous carbon


nanofiber loaded with NiO
using electrospinning and
carbonization methods. Dicy-
andiamide, polyacrylonitrile
and nickel acetophenone were
electrospun and carbonized
to fabricate carbon nanofiber
loaded with NiO. Reprinted
with permission of Wiley from
Li et al. (2018b)

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3132 Environmental Chemistry Letters (2023) 21:3127–3158

Fig. 3  The commonly used carbonization methods of waste plastics. the presence of catalysts. c Template-based method: carbonization of
a Oxygen-limited carbonization: carbonization of waste plastics into waste plastics into carbon materials assisted by templates. d Pressure
carbon materials under oxygen limiting conditions. b Catalytic car- carbonization: two ways of pressure carbonization to carbonize waste
bonization: carbonization of waste plastics into carbon materials in plastics into carbon materials

and Fig. 3 shows the commonly used methods, including Oxygen‑depleted carbonization
oxygen-limited carbonization, catalytic carbonization,
template-based method, and pressure carbonization. The For oxygen-containing plastics, oxygen-limited carboni-
general features of carbonization methods are summarized zation is a commonly used carbonization method. Usu-
in Table 2, including carbonization conditions, obtained ally, inert gases N
­ 2 or Ar are introduced in a tube furnace
carbon materials, and advantages and disadvantages. for high-temperature carbonization of waste plastic. The

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Table 2  Carbonization methods for synthesizing carbon materials from waste plastics
Methods Conditions Typical plastics Carbon materials Advantages Disadvantages

Oxygen-limited carbonization Inert atmosphere or in molten Polyethylene terephthalate, Activated carbon, mesoporous Simple, low equipment Low carbon yield relatively
salt, 500–1000 °C stabiliza- polyacrylonitrile, polyvinyl carbon, carbon fibers requirements, relatively, low high energy consumption
tion if needed, activation if chloride, polyethylene, cost, applicable for most
needed polystyrene, polyolefin plastics
Catalytic carbonization Inert atmosphere 400–900 °C, Polyethylene, polypropylene, Carbon nanotubes, graphene, Applicable for most plastics, Needs catalysts, relatively high
Environmental Chemistry Letters (2023) 21:3127–3158

catalysts polystyrene, polyvinyl carbon spheres, carbon generation of graphitic energy consumption
chloride, polyvinylidene nanofibers carbons
fluoride, polytetrafluoro-
ethene, polyvinyl alcohol,
polyethylene terephthalate
Template-based method Hard template ­(SiO2, Zn), Polystyrene, polyacrylonitrile, Carbon spheres, carbon Low cost, easy to purify, Acid or alkali pollutes the
soft template (MgO, organic polytetrafluoroethene, poly- nanosheets, porous carbon adjustable, easy to control environment, the production
modified montmorillonite, ethylene, polyvinyl chloride, the parameters of carbon process becomes complex
­Fe2O3), 600–900 °C, under polypropylene, polyethylene materials and improve the
inert atmosphere terephthalate carbonization yield
Pressure carbonization Sealed reactor at 600–850 °C Polypropylene, polyethyl- Activated carbon, carbon dots, Sophisticated techniques, high High equipment, requirements,
or hydrothermal reaction at ene, polyvinyl chloride, carbon spheres carbon yields relatively high energy con-
150–300 °C polystyrene, polyethylene sumption
terephthalate
Flash Joule heating Vacuum reactors, at high cur- Polyethylene terephthalate, Graphene Simple, low energy consump- Difficult management of
rent density in a short time polyethylene, polyvinyl tion, fast preparation, appli- volatile products, high current
chloride, polypropylene, cable for most plastics involved, needs conductive
polystyrene substances
Microwave conversion Microwave reactors, micro- Polyethylene, polypropylene, Carbon nanotubes, char Simple, fast preparation, Relatively high energy con-
wave irradiation, catalysts if polystyrene ensure control of reaction sumption, limited carbon
needed conditions, such as tempera- yields, expensive, not suitable
ture and reaction time for mass production

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3134 Environmental Chemistry Letters (2023) 21:3127–3158

physical and chemical properties of carbon materials, such Catalytic carbonization


as carbon structure, morphology, composition, and surface
groups, can be regulated by changing carbonization tem- Catalytic carbonization is an effective strategy to converting
perature. Carbonization temperatures higher than 700 °C can waste plastics into liquid or gas products. In the process of
improve the porosity and conductivity of carbon materials, catalytic carbonization, the decomposition products can be
but reduce oxygen-containing functional groups. Carbon converted into carbon materials on the surface of catalysts.
materials formed by carbonization at a lower temperature Catalysts play a dual role in promoting polymer decompo-
of around 500 °C retain relatively more surface groups, mak- sition at the beginning and catalyzing the formation of car-
ing them more suitable as adsorbents of pollutants. Adding bon materials later (Li et al. 2017a). Catalysts containing
activators can adjust the porosity of carbon materials and Ni, Co, Al and Fe can be used in the catalytic process to
improve the adsorption capacity, and the common activa- convert waste plastics into carbon materials such as carbon
tors are NaOH, KOH, or Z ­ nCl2. For KOH, the activation nanotubes (Ribeiro et al. 2022), carbon nanoflakes (Liu et al.
reactions can be shown as Eqs. 1–4 (Yuan et al. 2020c). The 2021b), and layered porous carbon (Ma et al. 2020). During
thermal decomposition of plastics generates volatile com- the catalytic carbonization of plastics, the surface of Fe–Ni
pounds such as ­CO2 and CO, which react with KOH. KOH bimetallic catalyst showed high hydrogen and carbon deposi-
also reacts with carbon to release CO, ­H2, and vaporized tion yield, which was attributed to the enhanced reducibil-
metal potassium, while the formed ­K2CO3 and ­K2O can react ity and synergistic effect of Fe–Ni species (Yao and Wang
with carbon to release more CO and regulate the porosity 2020). Cup-shaped carbon nanotubes were synthesized
of carbon materials. Physical activation of O ­ 2 or air is an through the combined catalysis of different halogenated
alternative activation method. The reaction process between compounds and nickel oxide (Gong et al. 2014d). During
carbon and oxygen has high energy efficiency, and the acti- the synthesis process, halogenated compounds promoted
vation takes place at relatively low temperatures, commonly the decomposition of polypropylene into light hydrocarbons
less than 500 ℃. The reactions in physical activation can be and aromatics, and the decomposition products promoted the
shown as Eqs. (5–9) (Zhou et al. 2021). aggregation and reconstruction of catalyst. Then, under the
catalysis of diamond shaped nickel oxide, light hydrocarbons
2 KOH + CO2 → K2 CO3 + H2 O (1) and aromatics were converted into cup-shaped carbon nano-
tubes. How to improve the carbon yield has been paid much
2 KOH + 2C → 2CO + 2 K + H2 (2) attention for catalytic carbonization of waste plastics. Car-
bon nanosheets with a yield of up to 62.8% were obtained
2 K2 CO3 + C → 2 CO + K2 O (3) from waste polypropylene by the combined catalytic action
of ferrocene and sulfur (Liu et al. 2021b). The iron parti-
K2 O + C → CO + 2 K (4) cles derived from ferrocene not only accelerated the large
dehydrogenation and aromatization of waste polypropylene,
but also reacted with high-pressure sulfur vapor to generate
2 C + O2 → 2 CO (5) ­Fe7S8 nanoparticles, forming carbon nanosheets loaded with
­Fe7S8 (Fig. 4a).
2 CO + O2 → 2 CO2 (6)
Template‑based method
C + H2 O → CO + H2 (7)
Templates can be used in carbonization of waste plastics
C + CO2 → 2 CO (8) to regulate the morphology of carbon products. Template-
based carbonization is usually divided into soft template-
based carbonization and hard template-based carbonization
CO + H2 O → CO2 + H2 (9)
based on the properties of the templates. Hard templates
In the process of preparing carbon materials, chemi- such as ­SiO2 and Zn have higher carbonization tempera-
cal modification (acid oxidation or heteroatom-doping) of ture than sacrificial templates, and porous carbon materials
carbon materials can increase their surface-active sites and are obtained after removing the templates through chemical
improve their ability to adsorb pollutants. For example, etching (Ma et al. 2020; Min et al. 2019; Wang et al. 2022a).
using waste polyethylene terephthalate urea, and sodium The plastics are converted into carbon material in an inert
hydroxide as the carbon source, nitrogen source, and acti- atmosphere, and the void or pore between particles in the
vator, N-doped microporous carbon was synthesized and templates is infiltrated by plastic precursor that transforms
exhibited high ­CO2 absorption capacity (Yuan et al. 2020a). from solid to liquid during carbonization. In addition, the
metal additives in polyvinyl chloride were used as a hard

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Environmental Chemistry Letters (2023) 21:3127–3158 3135

Fig. 4  Preparation of carbon materials using different carboniza- from polyurethane waste plastics using in situ atmosphere pyrolysis
tion methods. a Formation of carbon nanosheets loaded with F ­ e7S8: and KOH activation. Reprinted with permission of Elsevier from
pyrolysis of polypropylene into carbon atoms, iron particles from fer- Zhou et al. (2022). c Preparation of porous carbon scaffolds with sul-
rocene pyrolysis reacted with high-pressure sulfur vapor to generate fonic groups by sulfonation reaction and microwave carbonization.
­Fe7S8 nanoparticles. Reprinted with permission of Elsevier from Liu Reprinted with permission of American Chemical Society from Kim
et al. (2021b). b N-doped gradient porous carbon materials extracted et al. (2018)

template to recover up to 92% of calcium and titanium com- formation of carbon materials during the carbonization pro-
pounds in polyvinyl chloride through KOH activation and cess. For example, the organically modified montmorillonite
acid washing, which was conducive to the development of active template not only controlled the morphology of car-
micropores and ­CO2 adsorption (Liu et al. 2022b). bon materials, but also catalyzed polymer degradation and
Soft templates can not only serve as a sacrificial precur- improved the carbonization yield (Ma et al. 2020; Min et al.
sor for porous carbon, but also catalyze and promote the 2019; Gong et al. 2014c). In addition, to improve the thermal

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3136 Environmental Chemistry Letters (2023) 21:3127–3158

stability and flame retardancy of plastics during carboniza- Other methods for carbonization of waste plastics
tion, basic magnesium carbonate pentahydrate was added
to waste polyethylene plastics to provide MgO templates. For oxygen-containing plastics, they can be carbonized
The prepared porous carbon had excellent capacitance per- directly under oxygen-limited conditions, while for oxy-
formance and excellent cycling stability in supercapacitors gen-free plastics, templates or catalysts need to be used
(Lian et al. 2019a, 2019b). to promote the formation of carbon materials from small
molecules generated by plastic pyrolysis, thereby improving
Pressure carbonization carbon yield. In addition, the self-generated pressure formed
by plastic pyrolysis can also improve carbon yield. In order
Pressure carbonization refers to the high-pressure carboniza- to quickly and efficiently obtain high-quality graphene and
tion of waste plastics in a sealed reactor. Based on different carbon nanotubes, flash Joule heating and microwave car-
pressure sources, pressure carbonization can be divided into bonization are also good choices.
direct pressure carbonization and hydrothermal carboniza- Flash Joule heating is a promising method for rapid syn-
tion with self-generated pressure. Direct pressure carboniza- thesis of high-quality graphene. In the carbonization process,
tion either uses additive substituents or catalysts, or requires there is no need for a furnace, solvent, or reaction gas, nor
higher pressure conditions exceeding 30 MPa. The used for purification steps. The plastic is heated to high tempera-
catalysts or additives may pollute the environment, while ture in a short period of time, and most non-carbon atoms are
the latter requires stringent equipment requirement (Chen removed through sublimation to obtain high-quality turbine
et al. 2022). The autogenous pressure generated by plastic layer flash graphene, with a yield of over 90% (Luong et al.
carbonization promotes the carbonization process, which is 2020). The conversion of waste rubber to turbine layer flash
simple to operate and does not need to add external pres- vaporized graphene was optimized using flash Joule heating.
sure. Moreover, autogenous pressure carbonization greatly Carbon black derived from waste rubber tires was converted
improves the carbonization yield. Low density polyethylene, into graphene, which was used as a reinforcing additive in
as a precursor, will not produce carbon products during car- cement materials (Advincula et al. 2021). Through flash
bonization at atmospheric pressure, while 45% of carbon joule heating technology, the byproduct of waste plastics
yield can be obtained by autogenous pressure carbonization beneficiation process was rapidly converted into high-purity
in a closed system (Zhang et al. 2019b). The polyurethane turbine layer flash graphene (Wyss et al. 2021).
foam was pyrolyzed into N-doped porous carbon under Similar to rapid Joule heating, the carbonization of waste
in situ atmosphere, and the yield of hierarchical porous car- plastics assisted by microwave greatly shortens heating time
bon obtained by KOH activation reached 55.0% (Fig. 4b) and prepares high-value carbon materials and hydrogen fuels
(Zhou et al. 2022). (Suresh et al. 2021). Using inexpensive iron-based catalysts
The hydrothermal carbonization takes place under as microwave sensors, a rapid catalytic decomposition pro-
pressurized conditions containing water or solvent vapor. cess of plastic was initiated for 30–90 s, converting mechani-
According to the hydrothermal reaction temperature, hydro- cally crushed commercial plastics into 55.6 mmol/g high
thermal carbonization can be divided into low-temperature yield hydrogen and multi walled carbon nanotubes (Jie et al.
carbonization below 250 °C and high-temperature carboni- 2020). In addition, it was found that microwave promoted
zation above 250 °C. Low-temperature hydrothermal car- the sulfonation reaction of low-density polyethylene, and
bonization produces hydrogen carbon through dehydration induced a large number of pores in the sulfonated low-den-
and decarboxylation, while high-temperature hydrothermal sity polyethylene plastic (Fig. 4c). The sulfonation reaction
carbonization produces highly graphitized carbon products cooperated with microwave successfully prepared the porous
such as graphite carbon, activated carbon, and carbon nano- carbon scaffold with sulfonic group from low-density poly-
tubes as the reaction temperature increases (Chen et al. 2020, ethylene plastic (Kim et al. 2018).
2022). Low-temperature hydrothermal carbonization can be
employed for dehydrochlorination of waste polyvinyl chlo-
ride, which is crucial for the subsequent formation of poly- Carbon materials derived from waste
vinyl chloride dichloride and aromatic structure (Xu et al. plastics
2022). In addition to the temperature, solvent also affects
the physical properties of carbon materials obtained from Waste plastics can be converted into different forms of car-
hydrothermal carbonization. For example, the higher the bon materials, depending on plastic types and carboniza-
concentration of hydrogen peroxide solution, the smaller tion method. Compared to other plastics, polyethylene is
the particle size of photoluminescence carbon nanoparticles an excellent precursor for producing carbon nanotubes, as
synthesized by hydrothermal carbonization of waste plastic it can produce light hydrocarbons that contribute to the
bags in hydrogen peroxide solution (Hu et al. 2014b). formation of carbon nanotubes during the carbonization

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Environmental Chemistry Letters (2023) 21:3127–3158 3137

process (Cai et al. 2021). Similar to polyethylene, polypro- graphene layer grew at the same angle, forming an angle
pylene is an excellent precursor for producing carbon nano- of 17–25° with its growth axis, resulting in the formation
tubes, graphene, and carbon spheres. During the carboni- of cup-shaped carbon stacked nanotubes.
zation process, polypropylene undergoes random cleavage
of C–C bonds to form oligomers, which then undergoes Graphene
β-Cracking to further decomposes into small molecules
such as hydrogen, methane, and propylene, which are then Chemical vapor deposition and flash joule heating are
catalyzed and carbonized to form carbon nanotubes, gra- effective methods for converting waste plastics into gra-
phene, and carbon spheres (Vollmer et al. 2020). phene (Algozeeb et al. 2022; Cui et al. 2017). In the pro-
Due to the presence of benzene ring in polystyrene and cess of chemical vapor deposition, graphene layers are
polyethylene terephthalate, aromatics and oil compounds controlled by adjusting the flow rate of ­H2 or Ar (Sharma
are easily formed during carbonization, which are the main et al. 2014). Although flash Joule heating cannot control
raw materials for the formation of amorphous carbon (Cai the graphene layer, it can quickly and effectively convert
et al. 2021; Zhang et al. 2021b). Polystyrene and polyethyl- mixed waste plastics into graphene within a few seconds,
ene terephthalate can also be converted into porous carbon and the carbon yield of graphene is higher than that of
after activation. Compared with other plastics, polyvinyl chemical vapor deposition, reaching 20–30 wt% (Algozeeb
chloride has the lowest carbon content and is prone to gen- et al. 2022). During the heating process, the thermal sta-
erating harmful gases such as HCl during carbonization. bility of plastics will affect the rate of carbon generation
Apart from being used for synthesizing porous carbon, during the flash Joule heating process. Choosing plastics
polyvinyl chloride is not an ideal raw material for synthe- with high stability during the carbonization process will
sizing other carbon materials. The type of waste plastics, result in slower thermal decomposition, slower carbon
carbonization processes, and catalyst types are important supply, and more time for the generated carbon to react
factors that affect the morphology and properties of carbon with metal catalysts, thereby increasing carbon production
materials. Choosing appropriate plastics as carbon sources, (Cui et al. 2017). Cu and Ni are the most commonly used
carbonization conditions, and carbonization methods can metal catalysts in method of chemical vapor deposition.
generate ideal carbon materials. The preparation of carbon Single-layer graphene can be synthesized in different gas
materials from waste plastics reported in recent studies is environments using the low carbon source solubility of Cu.
summarized in Table 3. Carbon materials derived from Compared to Cu, Ni's low carbon source solubility has a
waste plastics exhibit different carbon yield due to the dif- stronger chemical adsorption on graphene and is easier to
ference of plastics, reaction equipment and conditions. form graphene (Ren et al. 2022).

Carbon nanotubes Carbon nanosheets

For the production of carbon nanotubes, catalyst, tempera- The main reactors for preparing nanosheets include quartz
ture, and carbonization method are decisive factors in the tube reactors and sealed reactors. The quartz tube reactor is
carbonization process. In terms of carbonization methods, simple to operate and has a high security, while the sealed
the traditional method is to use transition metal catalysts to autoclave reactor can prevent carbon volatiles from escap-
produce carbon nanotubes from waste plastics. Recently, ing with the gas and improve the carbon yield. It is reported
microwave carbonization has attracted much attention as that the carbonization of plastic polymers containing polycy-
a new method for efficiently and rapidly converting waste clic aromatic hydrocarbons can produce more carbon prod-
plastics into carbon nanotubes and hydrogen (Jie et al. ucts, such as polystyrene, which is easy to produce carbon
2020). Meanwhile, increasing the carbonization tempera- nanosheets under the same conditions (Ma et al. 2018). MgO
ture is beneficial for the decomposition of plastic polymers and the organically modified montmorillonite are reported
and obtaining high-quality and highly graphitized carbon as the template catalysts for the production of carbon
nanotubes. In addition, the morphology and particle size nanosheets. Porous MgO template can not only promote the
of metal catalysts have a profound impact on the mor- decomposition of polymers, but also promote the formation
phology of carbon nanotubes. For example, the diamond of porous carbon nanosheets as a sacrificial template, while
shape of nickel catalysts can promote the formation of organically modified montmorillonite, as an active template,
cup-shaped stacked carbon nanotubes (Shah et al. 2022). can introduce more Brønsted acid sites to catalyze the decom-
Graphene layer was first formed on the surface of the cat- position of plastics and improve carbon emissions, but it can-
alyst was parallel to its surface. Later, due to the angle not generate pores on carbon nanosheets (Wen et al. 2019).
between the two sides of the diamond shaped catalyst, the Compared with other plastics, aromatic-rich polystyrene is

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Table 3  Carbon materials prepared from waste plastics


Carbonization Plastics Reaction equip- Reaction condi- Carbon material Carbon yield References
method ment tions (wt%)

Flash Joule heat- Polyethylene tere- Quartz or ceramic Greater than 3000 Graphene 80–90 Luong et al. (2020)
ing phthalate, high- tube K, ~ 400 V, Less
or low-density than 100 m s
polyethylene,
polyvinyl chlo-
ride, polypropyl-
ene polyacryloni-
trile, rubber tires
Microwave con- Low-density Microwave reactor ~ 573 K, 220V, Carbon nanotubes 57.6–73.1 Jie et al. (2020)
version polyethylene, 30–90 s
high-density
polyethylene,
polypropylene
and polystyrene
Oxygen-limited Polyethylene tere- Quartz tube 973 K, 2 h Activated carbon – Kaur et al. (2019b)
carbonization phthalate furnace
Oxygen-limited Polyethylene tere- Quartz tube 998 K, 2 h Activated carbon 22.0 Moura et al. (2018)
carbonization phthalate furnace
Oxygen-limited Polyethylene tere- Quartz tube 773 K or 1073 Activated carbon – de Castro et al.
carbonization phthalate furnace K, 2 h (2018)
Oxygen-limited Polyethylene tere- Quartz tube 873 K, 1 h Porous carbon – Yuan et al. (2020a)
carbonization phthalate furnace
Oxygen-limited Polyethylene tere- Horizontal cylin- 873 K, 1 h Porous carbon – Yuan et al. (2020c)
carbonization phthalate drical furnace
Oxygen-limited Polyethylene tere- Tube furnace 873 K, 2 h Porous carbon – Zhu et al. (2021)
carbonization phthalate
Oxygen-limited Polyethylene tere- Quartz tube 773 K, 1 h Porous carbon – Liu et al. (2020)
carbonization phthalate furnace
Oxygen-limited Polyethylene tere- Horizontal cylin- 873 K, 1 h Porous carbon – Yuan et al. (2020b)
carbonization phthalate drical furnace
Oxygen-limited Polyethylene tere- Autoclave reactor 873 K or 1073 Graphene – Elessawy et al.
carbonization phthalate K, 5 h (2019)
Catalytic carboni- Polypropylene Quartz tube 773 K, 20 min Carbon nanotubes – Yao and Wang
zation furnace 2020),
Catalytic carboni- Polyethylene Tube furnace 773–1073 K, 2 h Carbon nanotubes 59.0 Huang et al. (2021)
zation
Catalytic carboni- High-density Quartz tube 773 K, 3 h Carbon nanotubes – Nath et al. (2021)
zation polyethylene furnace
Catalytic carboni- Low-density poly- Tubular furnace 723 K and 1123 Carbon nanotubes – Ribeiro et al. (2022)
zation ethylene K, 1 h
Catalytic carboni- Polypropylene Crucible 973 K, 5 min Carbon nanotubes – Gong et al. (2014d)
zation
Catalytic carboni- Polyethylene tere- Quartz tube 973 K, 2 h Carbon nanosheets 45.2 Wen et al. (2020)
zation phthalate furnace
Catalytic carboni- Polypropylene Autoclave 973 K, 1.5 h Carbon nanosheets 62.8 Liu et al. (2021b)
zation
Catalytic carboni- Polypropylene Tube furnace 873 K, 2 h Nanowires – Li et al. (2022a)
zation
Catalytic carboni- Polystyrene Reaction kettle, 973 K, 1 h Porous carbon – Ma et al. (2020)
zation tube furnace
Template-based Polystyrene Autoclave 973 K, 2 h Porous carbon – Min et al. (2019)
method flakes
Template-based Polystyrene Reaction kettle 973 K, 1 h – Ma et al. (2019a)
method

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Table 3  (continued)
Carbonization Plastics Reaction equip- Reaction condi- Carbon material Carbon yield References
method ment tions (wt%)

Template-based Polystyrene Tube furnace 1173 K, 3 h – Wang et al., 2018)


method
Template-based Polytetrafluoro- Tube furnace 973 K, 2 h Porous carbon – Chen et al. (2014),
method ethene
Template-based Polyethylene Tube furnace 1173 K, 1 h – Lian et al. (2019a)
method
Template-based Polyvinyl chloride Tube furnace 873–1073 K, 1 h Activated carbon – Liu et al. (2022b)
method
Template-based Polypropylene, Autoclave reactor 1073 K, 3 h Porous carbon – Min et al. (2022)
method polyethylene, flakes loaded
polystyrene with hollow
and polyvinyl carbon spheres
chloride
Template-based Poly(vinylidene Tube furnace 1073 K, 3 h Carbon spheres – Li et al. (2021c)
method chloride)
Pressure carboni- Polypropylene Autoclave reactor 673 K, 4 h Hetero carbon – Mir et al. (2020b)
zation Polyethylene tere- Autoclave reactor 973 K, 0.5 h Activated carbon – Zhang et al. (2021b)
phthalate,
Pressure carboni- Low-Density Autoclave reactor 873 K, 0.5 h Carbon Spheres – Zhang et al. (2019b)
zation Polyethylene
Polyurethane Autoclave reactor 973 K, 0.5 h Porous carbon 55.0 Zhou et al. (2022)

an ideal candidate for preparing carbon nanosheets. Using plastics, plastics such as polyethylene terephthalate and
MgO and organically modified montmorillonite as template polyvinyl chloride are more likely to produce porous car-
and catalyst, carbonization in a sealed autoclave effectively bon than polyethylene and polypropylene (Algozeeb et al.
increases the porosity and yield of carbon nanosheets. 2022). Currently, the most common template is MgO, and
Mg(OH)2 that can be converted into MgO at high tempera-
Carbon spheres tures. Other materials such as silica are also hard templates
for synthesizing porous carbon. Among various activators,
Generally, carbon spheres are synthesized from waste the most commonly used KOH is mainly used to promote
plastics through self-generated pressure carbonization and the formation of a large number of micropores and a small
atmospheric pressure carbonization. Self-generated pres- amount of mesopores in carbon materials. Z ­ nCl2 as an acti-
sure carbonization can obtain carbon sphere with smooth vator only produces mesopores, but promotes the graphitiza-
surfaces, while atmospheric pressure carbonization obtains tion degree of carbon materials. The activation process of
carbon sphere with rough surfaces and aggregated carbon ­K2CO3 introduces a large number of defect structures and
(Gong et al. 2014a; Zhang et al. 2019b). The carbonization oxygen-containing groups on the carbon surface. Compared
of oxygen-free plastics such as polypropylene and poly- to KOH, ­K2CO3 has less corrosiveness (Liew et al. 2019;
ethylene will form oil containing aromatic hydrocarbons, Min et al. 2020; Zhang et al. 2021b, 2018).
which is an ideal raw material for carbon sphere synthesis. In
addition, increasing the carbonization time and temperature Other carbon materials derived from waste plastics
can improve the graphitization degree of carbon spheres.
Therefore, in order to obtain high-quality carbon spheres Carbon nanodots are spherical carbon nanoparticles with
with smooth surface, it is recommended to use appropriate a size of 1–10 nm, mainly containing s­ p3 hybrid carbon,
plastics and increase the carbonization temperature and reac- and the most distinctive property is strong photolumines-
tion time (Ren et al. 2022). cence (Georgakilas et al. 2015). Hydrothermal carboniza-
tion, carbonization or oxidation are usually used to pro-
Porous carbon duce carbon nanodots from polymers (Arpita et al. 2023).
Hydrothermal carbonization can control the size and surface
The fabrication of porous carbon involves the carboniza- chemical properties of carbon nanoparticles, and has been
tion of plastics and the generation of pores. Among different used for carbonization of discarded plastics in recent years

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Environmental Chemistry Letters (2023) 21:3127–3158 3141

◂Fig. 5  Carbon materials derived from polyethene terephthalate for long life, fast charging or discharging and wide operating
energy applications. a Mechanism for the generation of porous car- temperature range are preferred for energy storage devices
bon during the autogenic pressure carbonization. Reprinted with
permission of Elsevier from Zhang et al. (2021b). b Synthesis of car-
(Pandey et al. 2021). Carbon materials obtained from waste
bon composite materials doped with NiO nanoparticles using waste plastics, such as carbon nanotubes, carbon spheres, car-
plastics. Reprinted with permission of Elsevier from Al-Enizi et al. bon nanosheets, layered porous carbon, and carbon-based
(2020b). c Effects of two carbonization temperatures on the proper- composites, have been applied in supercapacitors due to
ties of carbon materials prepared from waste plastics. Reprinted with
permission of Elsevier from Liu et al. (2020)
the unique properties such as porosity, large surface area,
controllable morphology, and heteroatom-doping (Uteti-
wabo et al. 2020). Activated carbon with abundant surface
(Adolfsson et al. 2018). Combustion oxidation is suitable for groups and high surface area can also be prepared by using
aromatic polymers as they are prone to pyrolysis into carbon the autogenous carbonization (Zhang et al. 2021b; Zhu et al.
nanoparticles. Waste polystyrene was carbonized in an oxy- 2021). Activated carbon as supercapacitor electrodes showed
gen-free environment and then oxidized to produce green excellent specific capacitance of 325 F/g when the current
fluorescent onion like carbon nanoparticles (MalikaáTripathi density was 0.5 A/g. Waste polyethylene terephthalate was
and KumaráSonkar 2014). The use of strong acid oxidation first decomposed and deoxygenated, and under autogenic
can easily lead to low product yield. Therefore, it is crucial pressure pyrolysis, the oxygen-containing components were
to seek green and efficient methods to manufacture carbon completely deoxygenated to form aromatics, which further
nanodots from waste polymers. condensed to form polycyclic aromatic hydrocarbons of dif-
Electrospinning is the main equipment for mass produc- ferent sizes. Smaller aromatics formed carbon spheres, while
tion of carbon fibers or porous carbon nanofibers. The pro- larger aromatics formed blocky carbon materials (Fig. 5a).
duced fiber materials have the advantages of large specific Metal oxide nanoparticles NiO, ZnO and C ­ o3O4 were
surface area, chemical composition, morphology, adjustable loaded into the metal–organic framework with high surface
fiber diameter, and high porosity (Zhu and Nie 2021). Dur- area and excellent porosity transformed by polyethylene
ing the spinning process, the concentration of waste polymer terephthalate, which improved the capacitance and stabil-
solution is the most important factor affecting the fiber diam- ity of carbon materials, thus improving the performance of
eter. With the increase of the proportion of waste polymer, supercapacitors (Al-Enizi et al. 2020a, 2020b; Ubaidullah
the fiber diameter of electrospinning will also increase (Bon- et al. 2021). To further improve the conductivity and sta-
fim et al. 2021). In addition, adding other metal coordina- bility of metal–organic frameworks, the benzene-1,4-dicar-
tion compounds and N-containing precursors to the polymer boxylic acid after polyethylene terephthalate depolymeriza-
solution could regulate the chemical composition and poros- tion was mixed with two other reagents, and the obtained
ity of carbon fibers (Li et al. 2018b). Using electrospinning Ni-metal–organic framework crystal was carbonized at high
to produce carbon fiber is a potential attractive choice. temperature to form a porous carbon composite material
loaded with NiO (Fig. 5b). The prepared carbon material
as a composite electrode showed improved conductivity
Application of carbon materials derived and stability, exhibiting an excellent specific capacitance
from waste plastics of 581.30 F/g in supercapacitors (Al-Enizi et al. 2020b).
In addition, the ultra-long carbon fiber with uniform diam-
Carbon materials synthesized from waste plastics through eter produced by electrospinning technology was a mixture
carbonization have different characteristics and can be of amorphous carbon and reduced graphite oxide, which
applied to different fields. Carbon materials with electrocata- increased pseudocapacitance in capacitors, providing an
lytic activity, good conductivity, and pore structure can be opportunity for further mass production of carbon materi-
applied in batteries, capacitors, and water electrolysis, play- als with high capacitance in the future (Mirjalili et al. 2020).
ing an important role in sustainable green energy systems. Porous carbon with high surface area and reasonable
Additionally, carbon materials with high surface area, large micropores, mesopores, and macroporous layered structures
porosity, and abundant surface groups have shown great is an ideal electrode material for capacitors. By utilizing
potential in pollutant removal, solar evaporation, and ­CO2 catalytic carbonization and KOH activation, polyethylene
capture. This section summarizes the applications of carbon terephthalate from waste beverage bottles was effectively
materials derived from waste plastics based on plastic types. converted into layered porous carbon nanosheets with ultra-
high specific surface area, and exhibited excellent electro-
Polyethene terephthalate chemical performance in capacitors (Wen et al. 2019). After
high-temperature carbonization, waste polyethylene tereph-
In order to effectively store and use energy, supercapacitors thalate mainly generates ­sp2 hybrid carbon, and the acti-
with high specific power density, good cycle stability and vated microporous carbon exhibits lower capacitance. Under

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3142 Environmental Chemistry Letters (2023) 21:3127–3158

low-temperature carbonization conditions, waste polyethyl- including ­H3PO4, NaOH, Z ­ nCl2 and H
­ 2SO4 (Adibfar et al.
ene terephthalate generates ­sp2/sp3 hybrid carbon, which, 2014; Yuan et al. 2020b). On this basis, the optimal ratio of
after activation, generates layered pores in the carbon mate- KOH and appropriate carbonization temperature were fur-
rial, exhibiting good capacitance (Fig. 5c). The co-etching ther studied to prepare carbon materials with a large surface
effect of ­sp2/sp3 hybrid carbon prepared at low temperature area of 1690 m ­ 2/g, obtaining a maximum ­CO2 absorption
was utilized to generate layered porous carbon with a high capacity of 2.31 mmol/g at 30 °C (Kaur et al. 2019a, 2019b).
specific surface area of 2238 m ­ 2/g. Using porous carbon as The high alkalinity provided by nitrogen functional groups
electrode material, the specific capacitance of the capacitor increased the affinity for attaching acidic ­CO2 molecules,
was increased to 413 F/g at 0.5 A/g, with a good energy stor- and N-doping improved the absorption and selectivity of
age capacity of 25 W h/kg (Liu et al. 2020). By changing the carbon materials towards C ­ O2 (El-Mahdy et al. 2020). The
surface composition of carbon materials and doping N, O, carbon material obtained from the carbonization of waste
S, and other heteroatoms, the conductivity, surface wettabil- plastic bottles at 600 ℃ was first activated with KOH, and
ity, and pseudocapacitance of carbon materials in capacitors then injected with urea, which was called two-pot pyrolysis.
could be further improved (Hossain and Sahajwalla 2021). The simultaneous activation of carbon materials with urea
The 3D sponge shaped N-doped graphene electrode material and KOH in a tubular furnace was called one-pot synthesis.
prepared by mixing waste polyethylene terephthalate with N-doped carbon materials synthesized by one-pot method
urea had a specific capacitance of 405 F/g at 1 A/g, and exhibited a maximum adsorption capacity of 6.23 mmol/g
its energy density and the maximum power density reached for ­CO2 at 0 °C and 1 atmospheric pressure (Yuan et al.
68.1 W/h kg and 558.5 W/kg (Elessawy et al. 2019). 2020a).
Hydrogen energy is considered as the most promising The method of utilizing solar-driven interface evapora-
clean energy because of its high energy density and zero tion and limited heating of the water–air interface has been
carbon emission. And, hydrogen energy plays an important widely used for water purification, seawater desalination,
role in achieving carbon neutrality. Water electrolysis for and steam generation due to its low heat loss and high photo-
hydrogen production is considered a green and environmen- thermal conversion efficiency. Using porous carbon materi-
tally friendly method, and it is divided into oxygen evolution als with high porosity, low thermal conductivity, and wide
reaction and hydrogen evolution reaction (Ubaidullah et al. absorption rate as photothermal materials, the evaporation
2020). The efficiency of water electrolysis largely depends rate of the photothermal conversion interface can be greatly
on the electrocatalytic performance of the used catalysts. improved in solar steam power generation systems (Chen
Economical, stable, efficient, and highly active electrocata- et al. 2019; Li et al. 2019a, 2019b, 2017b). Irregular and
lysts are crucial for efficient hydrogen and oxygen evolution interconnected layered nano-porous carbon was obtained by
reactions. Carbon materials prepared from waste plastics carbonization of waste polyethylene terephthalate assisted by
with excellent properties make them suitable as catalysts molten salt of Z­ nCl2 and NaCl, showing high surface area,
for water electrolysis reactions (Chen et al. 2020). N-doped high evaporation rate, high conversion efficiency, and low
mesoporous carbon functionalized zinc oxide synthesized thermal conductivity. The porous carbon exhibited an evapo-
from waste polyethylene terephthalate as catalyst provided ration rate of up to 1.68 kg/m2 per hour and had an energy
a large number of active sites and easy charge transfer for conversion efficiency of up to 97% in seawater (Zhang et al.
water electrolysis (Ubaidullah et al. 2020). The composite 2019a).
material effectively promoted the oxygen evolution reac- Partial destruction of the cross-linked structure during
tion, with Tafel slope and overpotential of ~ 318 mV/dec the heating process results in a reduction of the surface
and ~ 0.57 V, respectively. area of carbon materials. The addition of molten salt is
Adsorbents used for gas separation or storage through an effective strategy to solve this problem. The presence
physical adsorption should have some ideal characteristics: of melamine during the carbonization process not only
mainly micropores, high surface area, hydrophobic surface, introduced nitrogen groups but also reacted with the deg-
and good selectivity for the adsorbed gas (Wiersum et al. radation products of polyethylene terephthalate to form a
2013). Waste polyethylene terephthalate underwent physical strong cross-linked structure, resulting in a more stable
activation to obtain a series of nano-porous carbon (Moura N-doped porous carbon which had a high C ­ O 2 adsorp-
et al. 2018). By determining the adsorption and selectiv- tion capacity of 6.47 mmol/g and an evaporation rate of
ity of porous carbon on C ­ O2 under different conditions, it 1.62 kg/(m2·h) (Song et al. 2022). To introduce hydrophilic
was found that the higher the activation degree of carbon groups, reduce the water evaporation enthalpy of foam car-
favored the adsorption of C ­ O2, while narrow carbon pore bon and significantly increase the evaporation rate, waste
was beneficial for C­ O2 selectivity. Carbon materials derived polyethylene terephthalate, melamine and molten salt were
from polyethylene terephthalate activated by KOH have the carbonized by at a low temperature of 340 °C to generate
highest ­CO2 adsorption capacity compared to activators N- and O-doped foam carbon with super hydrophilicity

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Fig. 6  Carbon materials derived from polyethene terephthalate for ety from Bai et al. (2022). b Preparation of a porous carbon coated
solar evaporation. a Carbon foam prepared from waste polyethyl- wood double layer solar evaporator for solar steam power generation
ene terephthalate carbonized at low temperature for interfacial solar to produce fresh water. Reprinted with permission of Wiley from Liu
evaporation. Reprinted with permission of American Chemical Soci- et al. (2022a)

and ultra-low thermal conductivity. The modification not evaporator had an evaporation rate of up to 2.38 kg/(m2·h).
only achieved about 99% light absorption and photother- The natural wood structure is conducive to the rapid trans-
mal conversion, but also promoted the formation of water mission of water, and the graded porous carbon coated on
groups, reducing the evaporation enthalpy of about 37% wood with oxygen-containing groups is beneficial for light
water (Fig. 6a) (Chen et al. 2019). Firstly, polyethylene absorption (Liu et al. 2022c).
terephthalate was carbonized under the catalysis of ZnO Adsorption is efficient, cost-effective, easy and prac-
to prepare structurally controllable porous carbon materi- tical method for removing pollutants (Wang and Wang
als. Then, porous carbon was coated on the top surface of 2018; Kang et al. 2022). Due to the developed porosity,
the wooden block to construct a wood-based bilayer solar large surface area, high adsorption efficiency, and chemi-
evaporator (Fig. 6b). Due to the synergistic advantage of cal stability, carbon materials are often used as excellent
wood and porous carbon, the wood-based bilayer solar adsorbents to remove pollutants (Wei and Kamali 2020).

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The effects of physical and chemical activation methods, Polyethylene


as well as the types of activators, on the pore structure and
surface properties of activated carbon prepared from poly- Polyethylene can be easily decomposed into small molecules
ethylene terephthalate were studied (Mendoza-Carrasco upon heating due to its unstable molecular chains. The melt-
et al. 2016). Although the surface area of activated carbon ing point of low-density polyethylene is between 120 °C and
obtained by steam activation reached 1235 ­m2/g, which was 180 °C, resulting in poor thermal stability during carboni-
greater than that obtained by potassium hydroxide activa- zation (Khan et al. 2017; Li et al. 2018a). Layered porous
tion. The yield of activated carbon prepared by potassium carbon with large surface area and abundant surface groups
hydroxide reached 24.62–32.07%, which was significantly was obtained after carbonization and activation of low-den-
higher than that obtained by steam activation. The influence sity polyethylene under autogenous pressure (Zhang et al.
of the impregnation state and potassium hydroxide addition 2019b). Gas substances generated from thermal decompo-
on the preparation of activated carbon was explored. The sition of polyethylene formed a high-pressure environment
dry impregnation with a weight ratio of 1:5 polyethylene and the short chain aliphatic hydrocarbons underwent aro-
terephthalate to potassium hydroxide achieved a maximum matization and further condensed to form a carbon layer.
activation rate of 75.8%, and the activated carbon had a sur- The capacitance of the porous carbon electrode reached 355
face area of 1990 ­m2/g, which had a layered porous structure F/g under the condition of 0.2 A/g, and the power density
and was more favorable for the adsorption of bisphenol A was 450 W/kg.
(Gomez-Serrano et al., 2021). ­ZnCl2 and K ­ 2CO3 were used In order to avoid the use of expensive and toxic N­ H3 as
as activators for the preparation of carbon materials (de Cas- activators, graphene/mesoporous carbon composites with
tro et al. 2018). The mesoporous carbon prepared by K ­ 2CO3 large surface area and a large number of mesopores were
activation had a surface area of 1400 ­m2/g, much higher obtained by adding the optimal proportion of graphite oxide.
than that prepared by Z ­ nCl2 activation, and the adsorption The combined action of alkaline magnesium carbonate and
of methylene blue and Victoria blue B reached 625 mg/g and graphite oxide improved the thermal stability and flame
323 mg/g, respectively. retardancy of waste polyethylene, thus greatly increasing the
In addition to the porous structure and large surface final carbon yield (Lian et al. 2019b). The composite carbon
area, the π–π bond interaction and electrostatic attraction material had an energy density of 63.3 W h/kg in symmetric
between the adsorbent and the adsorbate are important supercapacitors, and the cycling stability improved to 89.3%
factors affecting the adsorption process. To improve the after 5000 cycles (Lian et al. 2019b, 2019a).
conductivity of carbon materials and provide more π–π Sulfonation is a crosslinking method that can improve
interactions to adsorb more aromatic ion dyes, a two-step the thermal stability of polyethylene. In order to achieve
method based on air carbonization and thermal oxidation deep sulfonation, porous polyethylene reprecipitation blocks
control was proposed to convert polyethylene terephthalate were prepared in toluene and water mixed system (Li et al.
into porous carbon materials with conductivity of 37 S/m, 2016). The thermal stability of polyethylene was signifi-
demonstrating excellent adsorption performance for methyl cantly improved, and the carbonization yield at 700 °C was
orange (Wei and Kamali 2020). To increase active adsorp- 51.9%. However, the carbon yield of the method is limited
tion sites on the surface of carbon materials, ferromagnetic for potential application. The innovative solvent thermal
iron oxide was embedded into the activated carbon matrix, cycling method generated high pressure at low tempera-
and obtained a composite material with an adsorption capac- tures and improved polyethylene sulfonation, increasing
ity of 71.42 mg/g for cephalexin, which was three times the total mass retention rates of low-density polyethylene
higher than that of pristine activated carbon (Rai and Singh and high-density polyethylene in sulfonated materials to
2018). The carbon matrix served as a stable carrier, while 50% and 46% (Villagomez-Salas et al. 2018). Lithium ion
magnetic metal oxides not only provided magnetic mobil- battery composite anodes using carbon materials derived
ity and facilitated controlled navigation of composites in from low-density polyethylene and high-density polyethyl-
the application process, but also provided Fe–O bonds as ene generated specific capacities of 230 and 350 m Ah/g,
nucleation sites to enhance cephalexin adsorption. The poly- respectively. In addition, the use of microwave technology
ethylene terephthalate derived carbon had a high porosity not only promoted the sulfonation of low-density polyethyl-
and available Cu (II) adsorption center, with an adsorption ene, but also induced a large number of pores in the carbon
capacity of up to 62.9 mg/g for dibenzothiophene (Fayazi derived from sulfonated polyethylene (Kim et al. 2018). The
and Ghanei-Motlagh 2021). The tomatoes and carrots were as-prepared porous carbon was a conductive support with
combined with polyethylene terephthalate after activation to negative charge. When the porous carbon was used as the
prepare a composite adsorbent and the adsorption capacity intermediate layer of lithium-sulfur battery, the capacity of
was 312.50 mg/g Co (II) (Changmai et al. 2018)). the sulfur cathode at 0.5 C was 776 mA h/g, and the cycle
retention rate reached 79% in 200 cycles.

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Environmental Chemistry Letters (2023) 21:3127–3158 3145

Carbon materials derived from waste plastics have been of amaranth (Kwon et al. 2021). The catalytic ability of the
used as catalysts for oxidation degradation of organic pollut- composite well maintained after 10 cycles for amaranth deg-
ants in wastewater (Wang et al. 2022b, 2023). Photocatalysis radation. Carbon nanotubes produced from waste plastics
is an attractive strategy to utilize renewable solar energy to were tested in advanced oxidation process for persulfate
degrade pollutants (Ivanets et al. 2021). During the pho- activation to remove micropollutants (Ribeiro et al. 2022).
tocatalytic process, when exposed to light of appropriate Using low-density polyethylene as carbon source, carbon
wavelengths, photocatalysts generate excited electrons and nanotubes were grown on A ­ l2O3, Ni, Fe and Al catalysts
strong oxidation holes, which can quickly degrade pollut- by chemical vapor deposition, and the carbon nanotubes
ants. In addition, hydroxyl radicals can be generated during showed the best performance of venlafaxine removal of
the photocatalytic process, breaking down organic pollutants 3.17 mg/g/h in ultrapure water.
into non-toxic or less toxic compounds such as C ­ O2 and ­H2O In order to increase the high yield of carbon nanotubes,
(Li et al. 2021a; Liu et al. 2022c; Wang et al. 2022c). Multi- oleamine can be used as a protective agent. Using waste pol-
walled carbon nanotubes or carbon and metal oxide com- yethylene and cobalt nitrate as carbon sources and catalyst
posites have been used as photocatalysts to degrade organic precursors, carbon nanotubes with the yield of 59.0% were
pollutants under visible light (Mohamed and Alsanea 2020; obtained under the protection of oleamine, and the adsorp-
Nath et al. 2021). The band gap of nickel oxide–multiwall tion capacity for methylene blue reached 107.1 mg/g. By
carbon nanotube composite derived from waste polyethylene combining carbon nanotubes with graphite oxide through
was 3.02 eV, which absorbed visible light and induced the hydrothermal and freeze-drying processes, graphene carbon
degradation of methylene blue, with an efficiency of 92.4% nanotube aerogel was successfully prepared and exhibited
(Nath et al. 2021). The conduction band and valence band of low density, high porosity and excellent hydrophobicity,
nickel oxide-multiwall carbon nanotube generated electrons manifesting high adsorption capacity of 410 mg/g oil or
and holes separately under visible light irradiation (Eq. 10). organic solvent (Huang et al. 2021).
Hydroxyl ions adsorbed on nickel oxide–multiwall carbon
nanotube catalysts containing holes to generate hydroxyl Waste from halogenated plastic
radicals (Eq. 11). The electrons in the conduction band
reacted with dissolved oxygen to generate oxygen radicals Waste plastic containing F and Cl can emit extremely dan-
(Eq. 12). Subsequently, free radicals reacted with methylene gerous byproducts during carbonization, such as C ­ l2, HCl,
blue dye for decolorization (Eq. 13). and organic chlorinated compounds. Therefore, halogenated
plastics need to be dehalogenated before carbonization. An
NiO − MWCNT + hv (visible) → NiO − MWCNT + e− + h+
effective dehalogenation method of converting polyvinyl
(10)
chloride into carbon materials was by ball milling with KOH

and N- or S-doping, while forming clean KCl and H ­ 2O by-
( +)
NiO − MWCNT h + OH → NiO − MWCNT + OH⋅
(11) products. In water-based symmetrical supercapacitors, car-
NiO − MWCNT (e−) + O2 (dissolved) → NiO − MWCNT + O⋅− bon materials derived from polyvinyl chloride were used as
2
(12) electrodes and exhibited excellent performance. At 1.0 A/g,
the specific capacitance reached 399 F/g (Chang et al. 2018).
MB∗ + OH ⋅ ∕O⋅−
2
∕h+ → MB Intermediates A simple in situ synthesis method of S-doped graphitized
(13)
+ Mineralized products carbon composite using polyvinyl chloride as a carbon
source was reported (Gao et al. 2015). Pyrolysis of polyvi-
In addition, advanced oxidation process is another effec- nyl chloride underwent dehalogenation, producing carbon
tive way to degrade organic pollutants, based on the activa- monomers and hydrocarbons (Eq. 14). ­KMnO4 was also
tion of persulfates or hydrogen peroxide to produce active thermally decomposed and reduced, producing ­MnOx and
radicals for oxidation of pollutants (Liu et al. 2023a, b). emitting ­CO2 and O ­ 2 (Eq. 15). ­(NH4)2Fe(SO4)2 serves as a
With its high chemical stability, low cost and high oxidation graphitization catalyst and doped S source. Polyvinyl chlo-
potential, persulfates have been widely used as oxidants in ride carbon reduced ­Fe2+ ions to Fe metals at high tempera-
the in situ chemical oxidation of groundwater or soil reme- ­ O42− anion was also reduced by carbon to S,
tures, and the S
diation (Wu et al. 2021). Non-noble metals such as Co and allowing S to be doped into the graphitized carbon during
Fe can activate persulfates without any light source or heat, the graphitization process (Eq. 16). Under the catalysis of
and porous materials as anchoring support of metal particles Fe, polyvinyl chloride underwent thermal decomposition and
greatly enhance the activation ability (Pi et al. 2019; Pu et al. carbonization, ultimately forming an S-doped graphitized
2020; Zhang et al. 2019c). The iron carbon composite pre- carbon supported M ­ nOx hybrid. The oxides of Mn and S in
pared by co-carbonization of polyethylene and goethite acti- the composite improved the catalytic activity of oxygen evo-
vated persulfate to produce OH· and ­SO4·− for the oxidation lution and oxygen reduction reactions. Molybdenum carbide

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3146 Environmental Chemistry Letters (2023) 21:3127–3158

is one of the transition metal carbides. Due to the change of The removal rates of Cu (II) and Cr (VI) by polyvinyl chlo-
its electronic characteristics, it has reached a special level ride derived carbon were 81.2% and 60.3%, respectively (Xu
similar to Pt as a catalyst and has received special attention. et al. 2022).
The synthesis of molybdenum carbide carbon nanocompos-
ites using waste plastics promoted electrocatalytic activity Polypropylene and polystyrene
and exhibited stable electrocyclic performance (Mir and
Pandey 2019). Due to the high carbon content of waste polystyrene, it has
been studied for the preparation of carbon materials suitable
(14)
( )
CH2 Cl n → C + HCl + Cx Hy for different fields. Using MgO as a template and KOH as an
activator, the carbon nanosheets produced by the carboni-
C + KMnO4 → MnOx (embedded) + K2 O + O2 + CO2 zation of polystyrene exhibited good specific capacitance
(15) and rate capacity, as well as excellent cycling stability (Ma
( ) ( )
C + NH4 2 Fe SO4 2 → Fe + S(doped) + NH3 + CO2 + H2 O
et al. 2020). Iron coagulation can effectively separate poly-
styrene microplastics from aqueous solution (Wang et al.
(16)
2021, 2022d). Then the high-temperature carbonization of
The recovery of calcium-based compounds in polyvinyl coagulated waste plastics promoted the reduction of iron,
chloride through activation and acid washing was beneficial improved the catalytic activity of iron and carbon nano-
for the formation of micropores and the adsorption of car- materials, and the removal rate of Rhodamine B reached
bon dioxide (Liu et al. 2022b). Structural characterization 97.57%. A series of porous carbon nanosheets were pre-
showed that the prepared carbon had a high specific sur- pared using templates such as MgO, Mg(OH)2, ­MnO2, and
face area and pore volume, up to 2507 ­m2/g and 1.11 ­cm3/g, ­Fe2O3. The carbon nanosheets used as electrodes showed
respectively. Porous carbon materials prepared from polyvi- improved electrochemical performance of supercapacitors
nyl chloride exhibited excellent ­CO2 adsorption capacity of (Ma et al. 2020; Min et al. 2019). Using MgO as a tem-
6.90 mmol/g. Spherical carbon materials reduced the flow plate and KOH as an activator, the carbon nanosheets with
resistance and wear inside the adsorption bed at the macro mesopores, micropores, and high surface area were produced
level, and had a large surface area, high chemical stability, by carbonization of polystyrene. Porous carbon nanosheets
and good recyclability at the micro level, thus possessing exhibited good specific capacitance and rate capacity, as
large ­CO2 capture ability (Pardakhti et al. 2019). well as excellent cycling stability (Ma et al. 2020). As a
Polyvinylidene chloride and melamine were used as transition metal oxide, ­MnO2 is one of the most promising
carbon source and nitrogen source for co- carbonization in pseudo-capacitor materials. To improve the inherent conduc-
alginate gel beads to develop a high compressive strength tivity, ­MnO2 was deposited on the porous carbon nanosheets
N-doped porous carbon, showing excellent C ­ O2 capture from polystyrene. The high surface area and conductivity
capacity (Li et al. 2021c). During the carbonization process, of the porous carbon had a positive synergistic effect with
melamine was not only used as a nitrogen source, but also the inherent specific capacity of ­MnO2. The obtained com-
as a template for macroporous structures. Due to the ther- posite exhibited excellent capacitance retention of 93.4%
moplastic nature of polyvinyl chloride, direct carbonization at 10,000 cycles of 10 A/g (Min et al. 2019). The addition
of polyvinyl chloride cannot produce target shapes. How- of ­Fe2O3 and urea carbonization to polystyrene resulted in
ever, the use of tetrabutylammonium bromide and NaOH the formation of 3D porous carbon. The porous carbon was
promoted dechlorination and oxidative crosslinking within activated by KOH to form a 3D hierarchically porous carbon
the polyvinyl chloride sphere, transforming thermoplastic with micropores and coexisting hollows (Fig. 7a) (Ma et al.
polyvinyl chloride into thermosetting and maintaining its 2020). When the 3D hierarchically porous carbon was used
sphericity. The porous carbon spheres obtained after car- as magnetic nanocarbon adsorbent, the adsorption capacity
bonization had a large surface area and good microporous of Tetrabromobisphenol A reached 117.0 mg/g. After five
structure, with ­CO2 adsorption capacity of 8.93 mmol/g at cycles, the adsorption capacity of Tetrabromobisphenol A
0 °C (Wang et al. 2020). remained about 85.5%.
Hydrothermal treatment at a relatively low temperature Polypropylene is investigated for preparing carbon mate-
of 160–300 °C can be used for dehydrochlorination of waste rials such as carbon nanosheets, carbon nanotubes, porous
polyvinyl chloride (Ma et al. 2019). Sulfonation introduces carbon, and carbon composites. To increase the yield of car-
a large number of surface groups of carbon materials, such bon nanosheets, the combination catalyst of ferrocene and
as –OH, –COOH and lactone, as well as –SO3H groups, thus sulfur was used for efficient carbonization of waste polypro-
improving the hydrophobic properties (Konwar et al. 2019). pylene into carbon nanosheets. After catalytic activation, the
Carbon derived from polyvinyl chloride was synthesized thickness of the nanosheets was only 4–4.5 nm, exhibiting a
through hydrothermal treatment and sulfonation reaction. porous structure and a high specific capacitance of 349 F/g

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Environmental Chemistry Letters (2023) 21:3127–3158 3147

Fig. 7  Carbon materials with different morphology obtained from tor. Reprinted with permission of Beilstein-Institut from Schneider-
polystyrene, polyurethane, and polyethylenimine. a Synthesis of 3D mann et al. (2019). c Preparation of N-doped activated carbon by
porous carbon prepared by carbonization of polystyrene. Reprinted the carbonization of polyethylenimine. Reprinted with permission of
with permission of Elsevier from Ma et al. (2020). b N-doped porous Elsevier from Zhang et al. (2019d)
carbon prepared from carbonized polyurethane foam for supercapaci-

(Liu et al. 2021b). Although high surface area and porous materials can reduce the internal resistance of electrodes.
structure help improve the accessibility of electrolyte ions, A method of combining catalyst and template was reported
improving the graphitization and crystallinity of carbon to obtain graphitic carbon with high surface area and

13
3148 Environmental Chemistry Letters (2023) 21:3127–3158

conductivity (Urgunde et al. 2020). Using nickel composite (Liu et al. 2019; Mir and Pandey 2018; Wei et al. 2018). On
ink as a catalyst and macroporous sugar as a soft template, this basis, a method of loading M ­ o2C onto N-doped carbon
the conductive carbon graphite obtained as an electrode had was developed in autoclave using waste plastic as carbon
a specific capacitance of about 158 F/g at 1 A/g, exhibiting source. The synergistic effect of N-doped carbon coating
excellent cycling stability. and ­Mo2C improved the electronic conductivity and charge
After the COVID-19 epidemic, a large number of dis- storage capacity of the composite, and the material surface
posal masks were discarded, which caused some pollution provided a large number of active sites, which enhanced the
to the environment (Jiang et al. 2022b, 2022c; Dharmaraj activity and stability of hydrogen evolution reaction, show-
et al. 2022). The preparation of valuable carbon materials ing a higher current density of 60 mA/cm2, and the stability
from waste disposal masks mainly composed of polypropyl- reached 2000-V ampere cycles (Mir et al. 2020a).
ene through different carbonization methods is a promising In order to explore the relationship between the morphol-
solution (Mghilia et al. 2022). Using melt blown cloth from ogy of carbon materials and the performance of solar steam
discarded masks as precursor and nickel metal catalysis, generators, a method for preparing Ni and carbon nanocom-
carbon-based composites were obtained and used as nega- posite was proposed through carbonization of waste polypro-
tive electrode materials for lithium-ion batteries, providing pylene, NiO, and poly (ionic liquid) (Song et al. 2020). The
a specific capacity of 479 m Ah/g (Li et al. 2022a). Another composites had a large surface area and three-dimensional
sulfonation and carbonization method produced a type of network structures with porous structure. The morphology
carbon electrode material with a hollow fiber porous struc- and structural properties of the composite material was
ture (Hu and Lin 2021). Due to the combined action of sul- adjusted by adding a small amount of poly(ionic liquid). The
fonic acid groups and KOH, the formation of dense porous synergistic effect of Ni and cup-shaped carbon nanotubes
carbon structure was promoted, which favored the rapid in solar energy absorption endowed the composites with
diffusion of ions, resulting in a high specific capacitance excellent photothermal conversion performance, resulting in
of 328.9 F/g at 1 A/g. In addition, the problem of low car- excellent performance in solar energy absorption, water per-
bon yield during the chemical vapor deposition in catalytic meability, and thermal conductivity. This composite material
carbonization has been solved through microwave assisted had a high moisture evaporation rate of 1.67 kg/m2/h and an
hydrothermal method and catalytic carbonization (Gong excellent solar steam conversion efficiency of 94.9%.
et al. 2014b; Lee et al. 2022). The polypropylene-based dis- In addition to using catalysts to induce the formation of
posable masks were sulphonated by sulfuric acid and then carbon nanotubes on its surface, the combination of halo-
heated to 2400 °C to convert into non-graphitized carbon gen compounds and NiO catalysts effectively synthesized
powder. Used as the anode material of sodium-ion battery, cup-shaped carbon nanotubes, exhibiting high performance
the graphitized carbon electrode had the highest reversible in adsorbing heavy metals and organic dyes (Gong et al.
capacity of 340 m Ah/g and superior rate performance at a 2014d). Low content halogenated compounds promoted
current of 0.01 A/g (Lee et al. 2022). the formation of light hydrocarbons and aromatic hydrocar-
In recent decades, efforts have been made to develop low- bons, improved the aggregation and reconstruction of NiO
cost, efficient, and stable hydrogen evolution reaction elec- catalysts towards diamond-shaped structures. The diamond-
trocatalysts to replace low abundance and high cost platinum shaped NiO catalyzed the conversion of light hydrocarbons
based electrocatalysts. A key challenge in designing elec- and aromatic hydrocarbons into cup-shaped carbon nano-
trocatalysts is to obtain a large surface area, and the hetero tubes. Moreover, polypropylene is considered as an excel-
carbon structure prepared by high-pressure carbonization of lent additive for biomass carbonization, which can be used
waste plastics has a higher surface area compared to other as a hydrogen supplement to promote pore formation and
reports, making it an efficient and low-cost candidate for generate porous carbon materials (Li et al. 2021b). The
hydrogen evolution reaction electrocatalysts (Louisia et al. porous carbon obtained from the carbonization of blue-green
2018; Mir et al. 2020b; Padilla et al. 2018). algae and polypropylene plastic had a high surface area and
Molybdenum carbide is considered to be the most prom- pore volume, exhibiting excellent adsorption capacity of
ising electro-catalyst to replace platinum-based catalysts due 667 mg/g for methylene blue (Li et al. 2022b).
to its high conductivity and similar D band structure (Miao
et al. 2017). The composite formed by loading M ­ o2C onto a Polyurethane
carbon material derived from waste polypropylene exhibited
higher stability and improved electrocatalytic hydrogen evo- Polyurethane is an ideal raw material for preparing N-doped
lution reaction in acidic media (Mir and Pandey 2018). By porous carbon due to its high C and N content. However,
comparing the impacts of amorphous and graphite coatings during the carbonization process, the cracking of polyu-
on the properties of the composite, amorphous carbon coat- rethane bonds and the evaporation of volatile products
ings exhibited better electrocatalytic stability in acidic media result in a particularly low yield of carbon materials. The

13
Environmental Chemistry Letters (2023) 21:3127–3158 3149

polyurethane foam was successfully converted into N-doped polyacrylonitrile had excellent specific capacitance, large
porous carbon by in situ atmosphere carbonization and KOH surface area, high mesoporous content, and fast ion trans-
activation, and the N-doped porous carbon as capacitor elec- port ability. N-doped porous carbon as an electrode material
trode had a high specific capacitance of 342 F/g at 0.5A/g, for capacitive deionization provided high electro adsorption
energy density of 11.3 W h/kg, and power density of 250 capacity of 19.61 mg/g and had the ability to remove heavy
W/kg (Zhou et al. 2022). In addition, N-containing carbon metal ions such as ­Pb2+, ­Cd2+, and ­Cu2+, with capacities of
materials synthesized by mechanical milling and carboniza- 21.5, 30.02, and 36.3 mg/g, respectively (Wang et al. 2022a).
tion of polyurethane foam had high surface area and poros- Doping sulfur-containing groups into the carbon matrix
ity, which enhanced the amplification ability of supercapaci- can obtain carbon materials which had unique physical and
tors (Fig. 7b) (Schneidermann et al. 2019). chemical properties such as good conductivity, excellent
Waste polyurethane contains abundant O and N het- catalytic activity and excellent chemical stability (Kiciński
eroatoms, which can improve the adsorption capacity of et al. 2014). The S-doping process makes the sulfur group
carbon materials. The ­CO2 adsorption capacity of porous uniformly distributed in the whole matrix and permanently
carbon prepared from waste polyurethane foam under the fused into the carbon skeleton. The obtained carbon showed
optimal conditions was 6.67 mg/g at 0 °C. Physical adsorp- excellent performance in the activation of persulfate and was
tion dominated by micropores played an important role in used for the catalytic oxidation of aqueous organic pollutants
­CO2 adsorption, with approximately 80% of C ­ O2 adsorption (Guo et al. 2017, 2018a, c). Using polyphenylene sulfide
capacity coming from physical adsorption, and the remain- as precursor and KOH as activator, the S-doped activated
ing 20% from chemical adsorption caused by the interac- carbon was prepared and exhibited high performance in the
tion between alkaline N groups and acidic C ­ O2 molecules adsorption and oxidation removal of phenol organic com-
(Duan et al. 2018; Ge et al. 2016). After carbonization of pounds (Guo et al. 2018b). In this process, the organics were
waste polyurethane, it was beneficial for the preservation and preferentially degraded in situ to accelerate adsorption, and
utilization of nitrogen and oxygen elements in carbon mate- then adsorption and oxidation synergize to promote the
rials, and did not cause secondary pollution. Activated car- effective removal of organics.
bon prepared by carbonization and physical activation had
a maximum adsorption capacity of 1428 mg/g for malachite Mixed plastics
green dye. The malachite green in wastewater was removed
through physical adsorption, and electrostatic attraction, Previously reported methods were mostly limited to single
oxygen-containing groups, and π–π interactions were the plastic, while "real world" waste plastics typically contain
driving forces for the excellent adsorption performance (Li many components, such as polypropylene, polyethylene,
et al. 2021d). polystyrene, polyethylene terephthalate, and polyvinyl chlo-
ride, severely hindering the application of previous methods
Other waste plastics (López et al. 2011). Wen et al. carbonized the waste plastics,
such as waste woven bags, waste containers, waste foam
In order to prepare highly active carbon materials, N, B, P sheets, waste beverage bottles and waste sewage pipes to
and S atoms were doped into carbon matrix, and this can produce porous carbon nanosheets with multi-stage porous
adjust the electronic state and create active sites. However, structure and high surface area (Wen et al. 2019). Zhao et al.
nitrogen sources into carbon materials have the drawbacks used industrial waste plastics such as melamine and polyure-
of low doping and uneven mixing. Due to that low boil- thane to prepare conductive N-doped carbon carrier through
ing point or decomposition temperature, nitrogen sources combining with highly catalytic ­MoS2 nanosheets, and it
such as ­NH3, aminomethane, urea are prone to decomposi- improved the conductivity and electrocatalytic activity of the
tion under high-temperature carbonization, resulting in low composite material and promoted the progress of hydrogen
nitrogen doping in carbon materials. Some nitrogen sources evolution reaction (Zhao et al. 2020). In order to improve
have low solubility in a range of solvents, making it difficult the photocatalytic activity of carbon materials for pollutant
to form a uniform mixture with plastics. Polyethyleneim- degradation, carbon-based T ­ iO2 nanocomposite from waste
ide has excellent water solubility and high viscosity, which car bumper was used as catalyst for photocatalytic degrada-
delayed the diffusion of nitrogen atoms in the process of tion of methylene blue (Mohamed and Alsanea 2020).
nitrogen doping, extended the contact time with carbon at Waste printer plastics, waste bicycle rubber tubes, and
high temperature, and improved the nitrogen doping level waste blister packs were used to prepare high-performance
of carbon materials. N-doping was successfully obtained carbon materials. Using waste printer plastic as the precursor
through mixing activated carbon and polyethyleneimide obtained the activated porous carbon which exhibited excel-
and high temperature carbonization (Fig. 7c) (Zhang et al. lent rate capacity with a transmission capacity of reached
2019d). The N-doped layered porous carbon derived from 3 mA h/g at 190 mA/g (Kumar et al. 2019). The defective

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3150 Environmental Chemistry Letters (2023) 21:3127–3158

engineering graphene turbine layer carbon prepared by the abundant surface groups, improving the removal perfor-
waste blister packs at a higher activation temperature had mance of dye. The removal efficiency of thymol blue dye
a pleated shape similar to graphene. When it was used as was up to 98.05% observed on the activated carbon (Kumari
anode of lithium-ion battery, it provided excellent electro- et al. 2022).
chemical characteristics and promoted faster L ­ i+ diffusion. The adsorption capacity of char derived from was plas-
At a current rate of 0.1 C, the storage capacity of Li-ion was tics for absorb arsenic not only depended on the char dos-
594 mA h/g after 200 cycles (Kumar et al. 2022). age or the solution pH, but also on the sources of plastics
Recently, a large number of studies showed that electro- (Singh et al. 2020). The adsorption effect of low-cost carbon
chemical activity of lithium ion battery anode was developed synthesized by carbonization of waste polyvinyl chloride,
by carrying metal oxide core and porous carbon shell struc- polyethylene terephthalate, and polyethylene on arsenic was
ture (Hong et al. 2021; Liu et al. 2021a). Min et al. obtained compared, and polyethylene and polyvinyl chloride mixed
the core–shell structure of S ­ nO2 loaded on porous carbon char had the highest removal rate of arsenic, ranging from
sheets by uniformly inserting nano-SnO2 spheres and cubes, 71.6% to 99.4%. Through a more environmentally friendly
block shaped ­SnO2 sheets and blocks into hollow carbon and economical carbon dioxide capture route, porous carbon
spheres derived from waste plastics. The high storage capac- with high ­CO2 capture capacity was obtained by using waste
ity ­SnO2 egg yolk and hollow carbon shells were closely plastic for carbonization in the presence of potassium salt
connected, providing sufficient internal space, limiting the (Algozeeb et al. 2022).
fragmentation of nanospheres and cubic S ­ nO2, enhancing
the storage capacity and capacity of ­Li+ (Min et al. 2022).
In addition, in order to limit the gradual diffusion of Perspective
lithium polysulfide from the cathode interface caused by
the shuttle effect, which disrupted the cycling stability of One of the main challenges in producing carbon materials
lithium-sulfur batteries, the pyrolysis residue of waste plas- from waste plastics is the economic feasibility of the produc-
tic was used as the cathode sulfur main body of lithium- tion process. Currently, although waste plastics have a wide
sulfur batteries to limit the shuttle effect. The significant N range of sources and low price, their composition are com-
defects in the prepared carbon material facilitated chemical plex and lacking efficient and cost-effective carbonization
interaction with the Li portion in polysulfides, while the methods. The production cost of carbon derived from waste
­TiO2-x formed after heat treatment effectively inhibited the plastics is higher than that of traditional carbon materials. It
diffusion of intermediates. N defects and T ­ iO2-x inhibited is particularly important to explore the preparation methods
the escape of lithium polysulfide from the bulk electro- of mixed plastics, providing more methods and avenues for
lyte through chemical adsorption, resulting in a decrease treating mixed plastic products in the environment.
in the decay rate of the prepared carbon at 1 C to 0.089% Another challenge is the environmental impact associated
per cycle until 500 cycles, with a capacity of 512 mA h/g with the carbonization of waste plastics. For the pretreatment
(Kim et al. 2022). In addition, a barrier layer outside the of oxygen free polymers such as polypropylene, polystyrene,
cathode to suppress the shuttle effect was studied (Lee et al. polyvinyl chloride, it is necessary to stabilize the carbon
2019; Park et al. 2020). Through heat treatment of waste chain using sulfuric acid or use catalyst templates to cata-
plastics with ­CaCO3 nanoparticles and boric acid, the porous lyze the production of carbon materials, and then remove the
bridge carbon was obtained and used as lithium sulfur bat- templates through acid washing. If the former is not properly
teries modified separator (Gim et al. 2021). The co-doping controlled, it generates harmful emissions, such as volatile
of boron and nitrogen provided strong attraction for lithium organic compounds and greenhouse gases. If the latter is
polysulfide, accelerating the electrochemical redox reaction not properly handled, strong corrosive acids may pollute the
and exhibited excellent electrochemical performance and environment and even the public health.
cycle stability. From the perspective of carbon source selection, the com-
Based on the porous carbon nanosheets which obtained position of waste plastics is complex and it is difficult to
from carbonization of mixed waste plastics, the adsorption extract individual plastic components. Moreover, previous
capacity of porous carbon nanosheets for pollutants was methods are mostly used to prepare carbon-based materials
further studied. The adsorption capacity of porous carbon from single plastic, while it remains challenging for pre-
nanosheets for methylene blue was 769.2 mg/g, significantly paring carbon materials from mixed plastics. Therefore, we
higher than most reported adsorbents, and carbon nanosheets should explore more effective carbonization methods to treat
had excellent recyclability. After 10 cycles, approximately mixed waste plastics, and reduce the harm of waste plastics
90% of porous carbon nanosheets were recovered (Gong to the environment.
et al. 2015, 2014c). In addition, waste plastics were con- It is worth noting that the use of flash Joule heating and
verted into activated carbon with large surface area and microwave conversion technology can quickly and efficiently

13
Environmental Chemistry Letters (2023) 21:3127–3158 3151

produce high-quality graphene and carbon nanotubes. In the the electrochemical, adsorption, and catalytic performance
carbonization process, we should pay more attention to the of carbon materials in batteries, supercapacitors, pollutant
process optimization of the methods and explore feasible removal by adsorption or degradation, solar evaporation, and
methods on a large scale. It is particularly important for carbon dioxide capture systems are improved. Transforming
quickly treating accumulated waste plastics and reducing waste plastics into functional carbon materials enables the
environmental pressure. recycling of waste plastics and the mitigation of environ-
Designing low-cost catalysts is crucial for converting mental pollution, favoring circular economy.
plastics into carbon materials. Although carbon materi-
als and their composites derived from waste plastics using
Author contributions All authors contributed to the study conception
catalysts have shown good performance in applications, the and design. Material preparation, data collection and analysis were
mechanism by which they catalyze the formation of carbon performed by YL and CW. EL, XL, and HJ contributed to the revision
materials during the experimental process is still unclear. of the manuscript.
The use of instruments to monitor the in situ conversion of
plastics is crucial for understanding their catalytic mecha- Declarations
nisms and designing low-cost catalysts. Conflict of interest The authors have no relevant financial or non-fi-
Several factors need to be considered in the design of nancial interests to disclose.
the next generation of functional carbon materials derived
from waste plastics. First of all, it is important to design Consent for publication All authors read the manuscript and approved
for publication.
the porosity of carbon materials. Existing chemical activa-
tion methods which improve the porosity and surface area
of carbon may be harmful to the environment, and more
green methods should be explored to mitigate environmental References
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1016/j.​scito​tenv.​2021.​145309 Publisher's Note Springer Nature remains neutral with regard to
Zhang Y, Wang Q, Yalikun N, Wang H, Wang C, Jiang H (2023) A jurisdictional claims in published maps and institutional affiliations.
comprehensive review of separation technologies for waste plas-
tics in urban mine. Resour Conserv Recycl 197:107087. https://​ Springer Nature or its licensor (e.g. a society or other partner) holds
doi.​org/​10.​1016/j.​resco​nrec.​2023.​107087 exclusive rights to this article under a publishing agreement with the
Zhao Y, Zhao J, Li Q, Gu C, Zhang B, Liu C, Qiao S (2020) Degra- author(s) or other rightsholder(s); author self-archiving of the accepted
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electrocatalyst: high-nitrogen dependent activity for hydrogen such publishing agreement and applicable law.
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