PIIS2405844022003164

Heliyon 8 (2022) e09028
Contents lists available at ScienceDirect
Heliyon
journal homepage: www.cell.com/heliyon
Review article
Plastic recycling and their use as raw material for the synthesis of
carbonaceous materials
Rodrigo A. Mun~oz Meneses a, b, Gerardo Cabrera-Papamija a, Fiderman Machuca-Martínez a, c,
Luis A. Rodríguez a, d, Jesús E. Diosa a, d, Edgar Mosquera-Vargas a, d, *
a
Centro de Excelencia en Nuevos Materiales (CENM), Universidad del Valle, Cali, Colombia
b
Faculty Gama, University of Brasilia, Gama DF, 72.444-240, Brazil
c
Grupo de Investigaci
on en Procesos Avanzados para Tratamientos Biologicos y Químicos (GAOX), Escuela de Ingeniería Química, Universidad del Valle, Cali, Colombia
d
Grupo de Transiciones de Fase y Materiales Funcionales (GTFMF), Departamento de Física, Universidad del Valle, Cali, Colombia
A R T I C L E I N F O A B S T R A C T
Keywords: Pollution by polymeric materials - in particular plastics - has a negative effect on the health of our planet.
Circular economy (CE) Approximately 4.9 billion tons of plastic are estimated to have been improperly disposed of, with the environment
Waste plastics as their final destination. This scenario comes from a linear economic system, extraction-production-consumption
Waste recovery
and finally disposal. The alarming panorama has created the need to find technological solutions that generate
Nanocarbons
new uses for discarded polymeric materials or turn them into part of the production process to produce new and
novel materials, such as carbon nanotubes, graphene, or other carbonaceous materials of high added value,
modifying the economy for a circular and sustainable production model. This review highlights the negative
impact that the disposal of plastic materials has on the environment and the research needs that allow solving the
pollution problems generated in the environment by these wastes. Also, the review highlights the current and
future directions of recovery plastic waste research-based to promote innovations in the plastic production sector
that could allow obtaining breakpoints in other industrial sectors with the technology-based companies.
1. Introduction mismanagement of plastic waste (intensive use of non-renewable re-

sources, degradation of natural systems, emission greenhouse gas emis-
For 2017 and 2018, the world production of plastic was 350 and 360 sions, among others) may be in the order of 40 billion USD per year.
million metric tons, being the most abundant anthropogenic materials Unless current consumption patterns and plastic waste management
besides steel and concrete [1, 2]. Since the beginning of its mass produc- practices change, by 2050 there will be about 12 billion tons of plastic
tion in 1950 and until 2015, around 8.300 million tons of plastic material waste (accumulated since its production in 1950) in landfills and the
have been produced. The popularity of plastic for everyday use is due to its environment.
high chemical stability, low density, and hydrophobicity. Apart from these In 2015, with the signing of the Paris Agreement on Climate Change
properties, plastics also have an excellent strength-to-weight ratio and by 195 countries [5] and the establishment of the Sustainable Develop-
longevity [3]. Despite the immense social benefits that come with the use ment Goals (SDGs) [6], the international community recognized that, to
of these types of materials, for example, medical devices, life-saving pro- achieve prosperous, safe and sustainable societies in the medium and
tective equipment, packaging that avoids food waste, etc., it is estimated long term, a transformation was necessary in the way we use natural
that around 5.8 billion tons, which represent 70 % of the total amount, resources and how we view “waste”, including plastic waste. This is why
have become waste. Of the total waste, 84 %, which is equivalent to one of the fundamental actions to achieve compliance with these
approximately 4.9 billion tons, has been disposed of in landfills or indis- agreements comes from the change of the linear economic paradigm of
criminately in the environment (the annual flow of plastic waste in the extraction-production-consumption and finally disposal, which is main-
oceans is estimated between 4.8-12.7 million tons [2]). tained at present, towards more circular and sustainable development
According to the United Nations Environment Program (UNEP) [4], models, actions that are currently included in the circular economy (CE)
the assessment of the negative externalities produced by the [7]. In itself, CE is known as a systemic approach to efficiency in the use
* Corresponding author.
E-mail address: edgar.mosquera@correounivalle.edu.co (E. Mosquera-Vargas).
https://doi.org/10.1016/j.heliyon.2022.e09028
Received 11 August 2021; Received in revised form 4 November 2021; Accepted 24 February 2022
2405-8440/© 2022 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
R.A. Mu~
noz Meneses et al. Heliyon 8 (2022) e09028
and exploitation of resources in which products and materials “at the end recycling symbol, only 14 % of plastic packaging (bottles, thin films, ad-
of their useful life” are not discarded, but rather are recycled, repaired or hesive sheets, among other formats) are collected for recycling.
reused through circular value chains through three types of activities (see The preparation of nanomaterials from plastic waste is very inter-
Figure 1), releasing added value from the resources [8]. esting because the environmental, economic, social, and technological
The added value released on implementing a circular economy (CE) aspects will have a high impact in a near future, also, the forecasting
strategy includes social aspects (e.g., job creation, health improvement), study for the nanomaterial and plastic sectors (Reports: Nanomaterials
environmental (reduction of the exploitation and use of resources as raw Market (2021–2026), Global Engineering Plastic Recycling Market
material, decrease in the generation of greenhouse gases, etc.), and (2021–2026), and Global Carbon Nanotubes Market (2016–2030),
economic (increased competitiveness of countries, decrease in waste Mordor Intelligence) show that:
treatment and disposal costs, etc.), as shown by various studies:
“The global engineering plastics market was estimated to be valued at
10,262.45 kilo metric ton in 2020 and is expected to reach 15,256.19
The Waste and Resources Action Program (WRAP) in a study con-
kiloton by 2026, registering a CAGR of 7.03 % during the forecast
ducted in 2015, suggested that switching to a CE could create up to 3
period, 2021–2026.
million additional jobs in Europe by 2030 [9].
A McKinsey analysis for the Ellen MacArthur Foundation (EMF) in The major factor driving the growth of the market studied is the
2015 projected that switching to a CE would bring material cost growing emphasis on sustainability among consumer and packaging
savings of up to 630 billion USD per year by 2025 in EU products.
manufacturing sectors [10]. Similar benefits could apply to devel-
oping countries. On the flipside, difficulty in collecting and sorting mixed plastic,
A 2018 Arup study, also for the EMF, estimated that a transition to CE along with the difficulty in removing residues, is expected to hinder
at scale in China could save businesses and households 10.4 billion growth of the market studied.
USD by 2040, equivalent to 16 % of the projected real Gross Domestic The global nanomaterial market (henceforth, referred to as the mar-
Product (GDP) of China [11].
ket studied) was reported at USD 19,928.96 million in 2020. It is
Consultants such as Accenture in 2015 identified business opportu- expected to reach USD 57,608.26 million by 2026, at an estimated
nities for 4.5 billion USD by 2030 [12]. In this regard, in India alone,
CAGR of 19.86 % over the forecast period, 2021–2026.
it is estimated that CE could create business opportunities worth 218
billion USD per year by 2030 [13]. By structure type, the Polymeric Nanomaterials segment accounted
The Material Economics consultancy suggests that the switch to a CE for 43 % of the total revenue of the global nanomaterials market, in
could reduce CO2 emissions from heavy industry in the EU by up to 56 2020. In terms of revenue, the segment was valued at USD 11,395.02
% by 2050 [14]. Along the same lines, the International Resource million in 2020 and is expected to reach USD 32,813.41 million by
Panel (IRP) points out that the most efficient practices in resources 2026 at a CAGR of 19.76 % over the forecast period.
could be critical to achieve the commitments of the Paris Agreement,
By product type, the nanotubes segment accounted the 19.93 % of the
for which it projects that the efficiency approaches of resources could
total revenue of the global nanomaterials market, in 2020. In terms of
reduce global greenhouse gas emissions by 60 % by 2050 [15].
revenue, the segment was valued at USD 13,798.02 million in 2020
and is expected to reach USD 40,134.99 million by 2026 at a CAGR of
According to an EMF study in 2017 [16], plastic used for the manu-
19.95 % over the forecast period.
facture of packaging represented, in 2016, the most significant application
with 26 % of the total volume of plastic produced (including PET fibers, In particular, the single-walled carbon nanotubes could have a value of
PP, and polyamide), where the main plastic materials in this category were USD 2700 per kg to 2800 per USD kg and Multi-walled carbon nanotubes
polyethylene (PE, 29.6 %), polypropylene (PP, 18.9 %) and polyethylene USD 1000 per kg to USD 1200 per kg in 2020”.
terephthalate (PET, 6.9 %). The study also reveals that most plastic
packaging that circulates today is used only once, so that 95 % of its value, The selected documents are related to the main topic of the review,
estimated at 80–120 billion USD annually, is lost to the economy after the Scopus and WoS database were used for scientific documents and the
initial use. The same foundation in a study carried out in 2016 [17] Espacenet Orbit, and Lens database for patents. Figure 2 shows the
pointed out that more than 40 years after the launch of the well-known structure used for searching the main papers and patents.
Figure 1. Activities of the circular economy (CE). Analysis adapted from a diagram by InnovateUK, Ref. [8].
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Figure 2. The level search strategy for scientific and technical documents.
The main objective of this review is to briefly address the main im- 2.1. Government efforts worldwide to face the problem of solid waste
pacts of plastic waste on the environment and to identify alternatives for
its use by applying the principles of circular economy. This allows the Given the huge benefits that implementing a large-scale circular
identification of gaps for the generation of new knowledge and to pro- economy (CE) strategy can bring, it is not surprising that the CE policy
mote innovations in the plastic production sector that could allow to landscape has expanded markedly in the last two decades. Although CE-
obtain break points in the academic and industrial sectors for the creation type thinking has existed since the 1970s, policies that explicitly refer to
of a technology-based company. the circular economy with a global focus only began to be introduced in
the 2000s [26]. For this reason, the countries have made different efforts
2. Global overview of the generation and disposal of solid waste and carried out cooperation at a global level for the dissemination of
initiatives, principles, and exchange of practices regarding the circular
In the last century, the development of anthropic activities has economy of plastic waste in productive sectors (Tables 1 and 2).
resulted in a massive demand for energy and consumption of resources At the level of local efforts, the European Union and China have been
that has had a serious impact on the ecosystems and biodiversity of our the world leaders in this process. However, as of 2018, the national
planet. The high rate of increase in the world population and the per policies at the global level related to the circular economy are summa-
capita needs have further accentuated the problem, turning post- rized in Table 2.
consumer industrial and human production waste into a global prob- Therefore, within the multilateral efforts focused on plastic waste
lem, both from an economic and ecological/social point of view due to (Table 1), it is important to highlight the effort led by the Ellen Mac-
costs of disposal, danger to human health, use of land for storage, Arthur Foundation (EMF) in collaboration with the UN Environment
contamination of land and water, climate change, etc. [18]. The World Program (UNEP) in this matter through the New Plastics Economy Global
Bank indicated that, in 2016, the world's cities generated 2 billion tons of Commitment program [27]. Since its launch in October 2018, the Global
solid waste, of which at least 33 % - being extremely conservative, was Commitment already unites more than 400 organizations in their
not managed in an environmentally safe way [19]. With rapid population
growth and urbanization, if current solid waste production and disposal
habits are maintained, annual waste generation is projected to increase Table 1. Multilateral efforts for the dissemination of the principles and ex-
change of practices of the circular economy in productive sectors.
by 70 % from 2016 levels to 3.4 billion tons in 2050 [20].
Some figures from the most important economic blocs show the Year Productive sectors
panorama described. For example, in 2016 most of the member coun- 2018 EU CE Mission to Japan and Indonesia
tries of the European Union (EU) generated between 1 and 2 tons of EU Strategy for Plastics in a CE
New Plastics Economy Global Commitment
waste (excluding the main mineral waste) per person per year [21],
EU Proposal on Water Reuse
where the recycling rate (including composting and digestion) was only EU's Memorandum on CE Cooperation
48 % [22]. For its part, the United States in 2015 had a solid waste EU CE Mission to India
generation of 262.4 million tons, of which 67.8 million tons (~ 26 %) 2017 World Circular Economy Forum 2017
were recycled (includes composting) [23]. In 2015, 190 million tons of G20 Resource Efficiency Dialogue
municipal waste were generated in China (the world's leading pro- First Latin American Circular Economy Forum.
EU CE Mission to Colombia
ducer), of which slightly more than 20 % were recycled [24]. In the African Circular Economy Alliance
above cases, more than 30 % of the solid waste ended up in landfills or WBSCD's Factor 10
garbage dumps. 2016 Toyama Framework on Material Cycles
Although solid waste in the widest sense (paper, cardboard, plastic, EU CE Mission to Chile
iron, etc.) is a serious problem, plastics are one of the main waste EU CE Mission to China
products to have received great attention in the last decade. This is 2015 EU Action Plan for CE
because their properties allow them to remain in the environment for a G7 Alliance on Resource Efficiency
2030 Agenda for SDGs
long time (some take up to 500 years to decompose) and when they break
2014 EU Revised Waste Directive
down in the environment, their products (for example, microplastics) are
2013 Ha Noi 3R Declaration
toxic to living things when ingested. Finally, their high volume/weight
ratio, as well as the great heterogeneity in composition, makes recycling 2011 EU Roadmap on Resource Efficiency
not economically viable for some types of plastic [25]. The situation of 2008 OECD Recommendation on Resource Productivity
Kobe 3R Action Plan
plastics is detailed in greater depth below.
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recorded. The next section presents in more detail the advances of the
Table 2. Initiatives or programs launched by country within the circular econ- applied research approaches.
omy (CE) framework.
Country Initiative/year
2.2. Solutions within the framework of the circular economy for the plastics
United Kingdom UKGBC Circular Economy Programme (2018).
sector
UK Plastics Pact (2018).
UK Industrial Strategy (2017).
UK CE Task Force (2012). Considering the problem in relation to the disposal of plastics, actions
Slovenia Slovenia Roadmap on CE (2018). from the point of view of materials and processes in the framework of the
Southern Common Market UNIDO CE Opportunities Programme (2018) circular economy (CE) for this plastics sector shows the current value
Mercosur chain of plastics of the linear type, together with the recycling and re-
Spain Spain Public Consultation on CE Strategy (2018). covery actions to take it to one of circular type [30].
Catalunya Circular (2018).
France France Roadmap for CE (2018). 2.2.1. Production of plastic from renewable raw materials
Denmark Denmark CE Strategy (2018). Renewable feedstock is primarily used to refer to feedstock of bio-
Scotland Scotland CE Investment Fund (2017). logical origin, that is, biomass, by-products derived from biomass, or
Lao PDR Lao PDR CE Strategies (2017). carbon dioxide (CO2), or methane (CH4) derived from biological pro-
USA US Circular Economy Summit (2017). cesses. It is also used to designate chemicals from CO2 or CH4 captured
US Sustainable Materials Management Plan (2015). through man-made carbon capture and utilization processes (for
US BCSD Materials Marketplace (2015). example, from industrial emission gases or atmospheric carbon). Some
South Africa South Africa Dialogue on CE (2017). examples of plastics in this category include but are not limited to: pol-
Wales Wales CE Investment Fund (2017). yhydroxyalkanoates (PHA), polylactic acid (PLA), poly (butylene succi-
Turkey Turkey Materials Marketplace (2016). nate) (PBS), polyethylene (PE), poly (trimethylene terephthalate) (PTT),
Finland Finland Roadmap for CE (2016). polypropylene (PP), polyethylene terephthalate (PET), and poly (pro-
China China CE Development Strategies Plan (2013). pylene carbonate) (PPC) [31]. Some plastics are in the research phase
China Law on CE Promotion (2008). and others are already included in the formulation of commercial prod-
China Law on Cleaner Production (2002).
ucts (for example, PET-30 in beverage bottles) [32].
Indonesia 10Y SCP Indonesia (2013).
In 2017, the world production capacity of plastics from renewable
Germany Germany Law on Closed Cycle Management and
raw materials was 2.1 million tons, which represented a market size of 6
Waste (2012).
billion USD [33]. However, as of 2018, the annual commercial supply of
South Korea South Korea Law on Recycling Resources (2008).
South Korea Wastes Control Act (2007).
these plastic was nearly 1 % of the current total volume [34]. The pro-
Japan Japan Law on Resource Efficiency (2000).
portion of non-biodegradable polymers, such as embedded bio-PE, of the
Japan Act for a Sound Material-Cycle Society (2000). total amount of bio-based plastics produced is 57 %, and the remaining
43 % is biodegradable, such as PLA and PHA. The world production
capacity of these plastics is estimated to be 2.4 million tonnes in 2022
common vision of a CE for plastics, keeping plastics in the economy and and is projected to reach a market size of 14 billion USD by 2023, at a
out of the ocean. The signatories include nearly 200 companies that are compound annual growth rate (CAGR) of 16.5 % from 2017 [35].
part of the plastic packaging/containers value chain, which together The growing demand for bioplastics from the packaging industry is
account for more than 20 % of all plastic packaging/containers used one of the main market drivers for these materials, representing in 2017
worldwide, including many of the major companies of the world of almost 60% of the total application market. The high growth of the
consumer products, retailers, and producers of plastic packaging, in packaging industry, together with the increasing regulations related to
addition to governments in the five continents, financial institutions, renewable packaging materials, is leading to a greater incorporation of
investors, and renowned university institutions. bioplastics in relation to conventional plastics. Major players include
To focus efforts at all levels, to achieve the transition of such a large NatureWorks (US), Braskem (Brazil), Novamont (Italy), BASF (Ger-
and interrelated sector as plastics, from a linear economy to a circular many), Total Corbion PLA (Netherlands), Biome Bioplastics (UK), Bio-On
economy scenario, the international community has outlined a vision of (Italy), Toray Industries (Japan), Plantic Technologies (Australia) and
the sector, identifying the points that must be improved or created, as the Mitsubishi Chemical Corporation (Japan) [33].
case may be (see Ref. [25]).
Broadly speaking, the circular economy (CE) solutions in the plastic 2.2.2. Recycling (post-industrial and post-consumer)
sector indicates that: a) the production of plastics from renewable sources The definitions of the ASTM D5033 standard for recycling [36]
must increase to significantly reduce dependence on fossil fuels; b) pro- include four categories: primary (mechanical reprocessing of waste ma-
duction processes and products should be redesigned to improve terials with controlled history in products with equivalent properties),
longevity, reuse, recyclability, as well as to avoid waste and chemical secondary (mechanical reprocessing of post-consumer materials in
contamination; c) sustainable business models should be fostered that products requiring properties lower), tertiary (recovery of valuable
promote products as services, facilitate the exchange and leasing of chemical components such as monomers/additives or other raw mate-
plastic products and increase reuse; d) end-of-life plastics must be rials for other industries) and quaternary (energy recovery).
increasingly recycled into new products or into new raw materials for
other industries (industrial symbiosis), in order to significantly reduce 2.2.2.1. Primary and secondary mechanical recycling. Primary recycling,
the volume of plastics that escape into the environment [25]. better known as re-extrusion, is used for post-industrial plastic waste
Other more local policies on plastic waste are those focused on single- management. It consists of the reintroduction in the extrusion cycle of
use plastics. According to a study carried out by Tobías et al. in 2019 waste, industrial plastic edges or simple polymer and pieces, to produce
[28], worldwide there were approximately 160 public policies at the products similar to the original material. With technological advances,
national and municipal level in 2018 regarding plastic bags in commerce. the waste generated in the transformation processes is minimal, allowing
These policies range from bans and levies to obligations to provide in- a reintroduction of more than 90 % of leftovers/surpluses in the pro-
formation on negative environmental impact. Likewise, the prohibition duction of plastics. This type of recycling is only feasible with semi-clean
of delivery of straws, stirrers, glasses, polystyrene plates, etc., in the food waste due to the high level of homogeneity required, so it is an option
service industry, tourist sites, among other sectors [28, 29] are also that is normally carried out within processing companies [37].
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Secondary recycling refers to the reprocessing of plastic waste recycled mechanically below virgin quality. Furthermore, this situation
(mainly post-consumer) by physical means to make pellets or granules. will also continue to make more than one recycling cycle not viable.
The steps involved in this approach before manufacturing the final
product are harvesting, sorting, wet cleaning, drying, shredding, 2.2.2.2. Chemical recycling (tertiary). Chemical recycling could address
pigmentation/coloring, bonding, and pelletizing/extrusion. These pellets some limitations of mechanical recycling due to mixing, contamination,
are subsequently used in the manufacture of new, but lower quality, and degradation of polymers. The term chemical recycling is used to
plastic products [38]. Lack of quality, regulations, and competitive price describe any advanced processing technology for converting plastic
makes the mechanically recycled plastics difficult to compete with virgin materials into smaller molecules in the liquid or gas phase using pro-
plastics. In addition, some post-consumer plastics collected and sorted cesses or chemical agents that directly affect the formation of the plastic
with a level of mixing and contamination that go to mechanical recycling, or polymer itself. Products obtained by tertiary recycling have proven
in combination with available processing technologies, are used pri- useful as fuel. However, the three main tertiary recycling types are
marily in new lower quality products (for example, garbage bags, con- solvent-based purification, depolymerization, and recycling of raw ma-
tainers, and basic furniture) [39]. Also, the compounds produced from terial, and they differ significantly in how they work and what results
recycled plastics as raw material are sold at a lower price (70–80% of the they produce (see Ref. [30]).
price) compared to virgin plastics [40]. This is why, to date, the economic 2.2.2.2.1. Solvent-based purification. Generally, this process is carried
arguments for incorporating recycled plastics in the plastic trans- out by dissolving the polymer in a specific solvent followed by removal of
formation chain are weak. However, in countries where the control of contaminants (pigments, additives, and other substances) by filtration or
compliance with the regulation in the use, application of recycled ma- phase extraction, and then precipitating the polymer using an antisolvent
terial, and waste management is not so strict, it thrives as a consolidated in which the polymer is insoluble. The purity of the recycled polymer
industry with low entry barriers, which depending on its scale can be depends on several process parameters, and there is always the risk of
housed in low-income sectors of the population or in industrial zones. residual contaminants due to the limited range of action of the solvents.
Regardless of the above, due to their impact on the quality of recycled However, the quality of the material is affected to a lesser extent than
material, technological developments to favor this type of recycling have mechanical recycling. Because this process does not modify the polymer
been taking place in the stages prior to shredding (collection, classifi- itself, it is susceptible to loss of properties with each reprocessing cycle.
cation, and cleaning) [41]. As such, this recycling method is not perpetual for plastics [53].
From the point of view of planning the on-site collection process and On a commercial scale, since 2002 the VinyLoop company processes
its coordination with the on-site sorting system for greater recycling ef- 10.000 tons per year of PVC waste in Italy, through its patented solvent-
ficiency, the collection bins now have sensor-based systems that can based purification process. However, in 2018 it announced the closure of
communicate in real time, indicating that type of waste they contain and operations due to the entry into force of the European Hazardous Ma-
how full they are [42]. Traditionally, the separation of plastics is carried terials regulation [54]. In 2017, the EU-funded PolyStyreneLoop coop-
out using different techniques such as separation between heavy media erative was created with the aim of recycling PS across Europe using the
(density) in conjunction with hydrocyclones [43]. Other techniques CreaSolv® process [55]. Unilever is currently testing this process in
include triboelectric separation [44] as well as X-ray fluorescent spec- Indonesia, primarily to recover PE from multi-material sachets [56].
troscopy (XRF), which is suitable for flame retardant plastics [45]. Polyolefins such as PE and PP can be purified with solvents at high
However, with the increasing introduction of new polymeric materials temperature and pressure using commercial PureCycle Technology®
and their combinations in different formats (e.g., multilayers), these [57]. In the USA, P&G has partnered with this company to purify PP
techniques have proven to be insufficient. residues for use in the packaging of household cleaning and hygiene
In this regard, trends in the development of selection and sorting products. In Europe, APK Aluminum und Kunststoffe is working on
technologies include the development of automated and integrated recycling various polymers (especially multilayer packaging) with its
sorting lines, comprising markers for tracking, sensor recognition, XRF Newcycling® technology [58].
compartment, online FTIR, robotics and artificial intelligence (AI). Despite the great advances in the technological development of this
Among the many R&D projects in this area with great potential, FP7 type of chemical recycling, a key issue is the time and energy input
Polymark [46] stands out, aiming to facilitate the identification of plastic required for the removal of solvents, which hinders economies of scale.
waste through tracking markers for easier sorting; and FP7 SupercleanQ Furthermore, the control over the impact of the solvent on the recycled
[47], developing quality control procedures for plastic waste. At a com- material is not clear - for example, traces of the solvent remaining in the
mercial level, in the field of robotics and AI, ZenRobotics [48] and output polymer and on the processing of the excess solvent, potentially
Max-AI [49] are to the fore. contaminated with plastic additives and other substances [59].
In the field of cleaning sorted plastic waste, the Spanish company 2.2.2.2.2. Depolymerization. Post-consumer chemical depolymeriza-
Cadel Deinking [50] developed a technology to remove printing inks tion of plastics produces the initial monomers that can be later re-
from plastic containers so that the recycled material is more homoge- polymerized into high-quality polymers or innovative small molecules
neous and closer in quality to virgin material. At the level of R&D, that can be used as high-value-added building blocks to create unique
whether on a laboratory or pilot scale, there are other approaches for polymeric materials or other chemicals with minimum waste. The tech-
removing mechanical inks, such as particle blasting, compression vibra- nology generates a profitable and sustainable industrial scheme, with
tion and cryogenic grinding; and chemical approaches such as hydrolysis high product performance. This would overcome the limitation on me-
through alkaline and high temperature treatment, liquid cyclone, and chanical recycling. However, because of the high stability of polymeric
melt filtration [51]. materials, forced conditions are generally required, such as microwave
Regarding processing, FP7 Ultravisc [52] stands out, in developing an assistance [60] supercritical conditions [61] or the use of catalysts [62]
ultrasonic detection technology for extrusion processes from plastic to improve the efficiency of the depolymerization reactions.
waste. Materials that have undergone research for depolymerization include
Although technological developments in relation to post-consumer the group of polyesters (PET, PLA, PHB), polyamides (PA-6 and PA-12),
classification may make the flow of plastic waste more granular/spe- polyolefins (PE and PI), polyurethanes (PU), polymethyl methacrylate
cific, if the current approach to “tailor-made” production continues with (PMMA), polystyrene (PS) and polycarbonate (PC) [63]. Examples of
market benefits (market-pull) and not in the ease of mechanical recycling projects that have reached the pilot level on an industrial scale based on
at the end of its use, in the foreseeable future it is not possible to reduce PET include GR3N [64], being part of the DEMETO consortium [65],
the cross contamination of materials (mixing of different grades of the Loop Industries [66], Ioniqa [67] and perPETual Global Technologies
same plastic and additives), which will continue to result in plastics [68]. In the case of PA, the Aquafil company converts used nylon, that is,
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a PA brand, into ECONYL yarn, adding value through the sale of yarns It is possible to some extent to control the exact composition of the
instead of raw material [69]. Companies such as Agilyx [70] and Poly- hydrocarbon mixture by varying the process parameters (e.g., oper-
styvert [71], commercialize processes for the depolymerization of PS, ating temperature, retention time, separation, reflux, etc.)
although mainly for bulk applications as insulation material. In 2018, It functions as a key complementary technology for conventional
ReVital Polymers, Pyrowave, and INEOS Styrolution launched a con- mechanical collection, sorting, and recycling.
sortium to recycle single-use PS packaging through microwave catalytic
depolymerization technology [72]. In the case of PC and PMMA, their This process on the other hand suffers from known deficiencies, such
chemical recycling through depolymerization is currently limited to the as high energy requirements, additional refinement (in case of wanting to
research level [73]. produce polymers) and exit pollutants (PAH, dioxins, fumes, among
Other advances in research on a laboratory scale are related to the others).
development of organic catalysts to replace the traditional organome- From the point of view of economic viability, the incentives for their
tallic catalysts, since the latter are difficult to separate from the crude implementation may be low, as in other chemical recycling processes,
product, which leads to lower quality final materials. This implies high especially in countries where there is no explicit demand for the resulting
costs due to the energy intensity and the decontamination required [74]. materials or recycled content. However, it should be mentioned that
Despite the great advances in the technological development of this type continuous improvements are reducing energy demand, and alternative
of chemical recycling, they need significant development to mature, methods, such as catalytic cracking and hydrocracking (addition of
especially if the result of depolymerization is the starting monomers and hydrogen (H2) by chemical reaction), could increase the specificity of
not a polymer or material with a higher added value. This scenario will production and reduce the production of pollutants, while potentially
remain in force at least in a near future if the prices of virgin polymers requiring less energy. However, such methods require catalysts and/or a
remain so affordable and competitive for the sector [75]. more sophisticated process setup [81].
2.2.2.2.3. Recycling of raw materials. Recycling of raw materials is Gasification is less sensitive to the quality of plastic waste than py-
distinguished by the fact that the results are simpler chemicals (for rolysis but requires more energy and large-scale operations. Gasification
example, hydrocarbons or syngas), that cannot be converted directly into is a process where the materials are heated at higher temperatures,
plastics, so they must be processed in several unit operations (refining- between 1000-1500 C, in the presence of oxygen (O2, a limited
conversion-polymerization) to produce a polymer again or they can serve amount) to produce synthesis gas (predominantly carbon monoxide
as raw material to manufacture other value-added products (e.g., fuels, (CO) and hydrogen (H2) mixture). Syngas can be used to produce a
carbon structures, among others). Within this recycling strategy, pyrol- variety of plastics and chemicals (i.e., via methanol or ammonia). Both
ysis (thermal cracking of polymers in inert atmosphere) and gasification chemicals are well known versatile platforms [82]. The high tempera-
are distinguished. These technologies transform plastics and a vast mature requirement means that gasification is energy intensive and relies
jority of their additives and contaminants into basic chemicals. Pyrolysis on building processing units large enough to be viable. Furthermore,
is carried out by heating plastics in an atmosphere in the absence of gasification generally needs pre-treatment to remove moisture and in-
oxygen, while gasification is carried out in an environment with a certain crease the calorific value to 14–18 MJ/kg to be sufficiently energy
amount of oxygen (air in this process is used). efficient [30].
Pyrolysis is a generic name for all thermochemical operations that Advances in this field are still on the laboratory scale and in some
involve heating in the absence of oxygen. Since most polyolefins spon- cases in the pilot stage (depending on the type of technology) with batch
taneously degrade at only a few hundred degrees Celsius, simply adding production. The technologies evaluated include fluidized bed reactor,
heat is enough to break them down into smaller fragments. However, fixed bed, jet beds, and plasma reactor, among others [83].
degradation is not controllable in the same way as depolymerization. However, there are industrial-scale units for both pyrolysis and
Instead, bond splitting occurs at random positions, leading to a distri- gasification, which could work more effectively by targeting certain
bution of the output molecular weights and structures. It usually includes products depending on the feedstock, market performance, and demand.
heavier waxy fragments, as well as very light fragments (C2–C4) that can
be separated in the condensation stage. Such a hydrocarbon mixture 2.2.2.3. Energy recovery (quaternary). Quaternary recycling refers to the
resembles the composition of oil and can be used directly as fuel [76]. recovery of the energy content of waste through incineration. This in-
While pyrolysis itself is not a sufficient unit operation to chemically volves burning plastic waste to produce energy in the form of heat, steam,
recycle polymers back to materials (starting monomers), the necessary and electricity. Currently, this is the most effective way to reduce and/or
additional processing infrastructure already exists in the mature and dispose of the volume of organic materials (with volume reduction up to
efficient value chain (chemical industry). 99 % in plastic solid waste). However, this method produces considerable
Almost two decades ago, pyrolysis had been tried for recycling plastic toxic substances in both smoke and ash and is considered ecologically
materials, but it had been discontinued several times due to economic unacceptable [84]. In addition, the presence of flame retardants difficult
challenges [77]. However, more recently, recognizing the limitations of the energy recovery process. Also, the burning processes of plastic waste
each type of recycling, small and large industrial players have proposed produce emissions of certain polluting gases such as CO2, SOx, and NOx.
novel and modified pyrolysis processes to increase the recycling rate of Other environmental (i.e., heavy metals emissions) and health (i.e.,
plastics [78]. carcinogenic substances) problems have been identified from the incin-
Some commercial examples of this technology are the Recycling eration or combustion processes of synthetic polymers such as PET, PS,
Technologies company [79], which has managed to recycle plastics that and PE to name a few [85]. Therefore, this technology is not considered
today are considered non-recyclable, such as crisp packages, multilayer strategic in the future to help meet either the Paris Agreement or the
films, black plastic, and mixed waste streams, turning them into fuel. Development Goals.
Another company is APChemi, which has developed a technology for
converting plastic waste into energy (fuels), including municipal plastics 2.2.3. Upcycling o valorization
segregated from solid waste and multilayer packaging [80]. Upcycling refers to the conversion of a waste material into a
The benefits derived from applying this process to plastic waste are: valuable product. It is a sustainable concept and prevents waste from
being dumped directly into the landfill or incinerator, which is why it
It facilitates the cleaning of additives and contaminants during the is considered a constructive approach due to the benefits of cost and
process. This occurs either by converting organic additives to hy- waste reduction [86]. As was outlined in the previous section, the
drocarbons as well or by separating the waste materials into the solid recycling that enables the closing of cycles (primary to tertiary) within
state at the end of the process. the plastic sector, presents a series of advantages and disadvantages
6
R.A. Mu~
associated with its nature and the current state of development. o Production of carbon nanomaterials (multiple walls, hollow spheres,
Likewise, regardless of the time that plastic materials can be threads, among others) for potential use in various applications
kept within the cycle resulting from the inclusion of new materials, (environment, energy, health, aerospace, etc.).
sooner or later their reprocessing will not be technically-economically o Hollow spherical carbon from polystyrene foam spheres and pyrolysis
viable. of sludge, which are then used as adsorbents to treat wastewater.
The foregoing leads us to think that in the future a certain constant o Conversion of expanded PS waste into polymeric azo dyes with sul-
flow of plastic waste will be maintained in the environment, albeit in a fonamide group for the pigment industry.
lower proportion than is currently the case. Therefore, to complement the o Preparation of doped carbon catalyst for oxygen reduction using PS
technological offer in the use of plastic waste, in recent years scientific foam, melamine and iron chloride as precursors.
interest has turned towards the development of recycling solutions with o Modification of ordinary paving asphalt, using, for example, a carbon
greater added value, mainly in synergy with other value chains (see fiber waste packaging based on PE and polyacrylonitrile over ordi-
Ref. [30]) and which is related to the number of patents and scientific nary polymer modifiers.
articles related to the upcycling of polymers or plastics. Figure 3 presents o Adsorbents to remove lead from wastewater using PS waste.
the evolution of patents and their interest on the part of applicants o High-surface composite material for CO2 adsorption, from amine-
worldwide. In addition, Figure 3 shows the economic and scientific in- functionalized PVC waste.
terest and the possible impact of the technologies associated with the use o Hyper-cross-linked polymers for CO2 capture, using the Friedel-Crafts
of plastic waste. Also, Figure 4 shows the main technologies and possible reaction with expanded PS foam as raw material and 1,2-dichloro-
applications related with the upcycling technologies. Some reported ex- ethane as solvent and cross-linking agent.
amples are [38]: o Substitution of constituents in concrete mixtures.
Figure 3. (a) Market and (b) patenting activity around upcycling of polymers and plastics.
7
R.A. Mu~
others. As of 2018, the market size was 4.55 billion USD, and it is pro-
jected that by 2023 it will be 9.84 billion USD, at a CAGR of 16.70 %
during the forecast period. To date, more than 100 companies are pro-
ducing and marketing of CNTs [90].
Since its discovery in 1991, a great deal of research and patenting
activity has been reported for this nanomaterial, as shown in Table 4.
There are four main methods to produce CNTs commercially: arc
discharge, laser ablation, chemical vapor deposition (CVD), and com-
bustion (flame) synthesis. Following the discovery of multi-walled and
then single-walled carbon nanotubes by electric arc carbon vaporization,
several varieties of this technique were described, such as metal doping,
different electrode configurations, or different types of carbon sources
[86]. Given that in the traditional process in the chemical industry 60 %–
90 % of production costs come from raw materials, being able to suc-
cessfully incorporate inexpensive raw materials into the production of
CNTs has become a challenge [91].
In this regard, several strategies have been proposed to prepare CNT
from plastic waste, for example, combined catalysts, high pressure
autoclave, pyrolysis-gasification-carbonization, pyrolysis-combustion-
carbonization, and CVD method. Meanwhile, the materials that have
been most extensively studied are polypropylene (PP), polyvinyl chloride
(PVC), low-density polyethylene (LDPE), and polystyrene (PS). However,
important production yields that allow it to move to a pilot stage have not
Figure 4. Main applications and technologies from upcycling developments. yet been achieved. Moreover, most studies use costly nickel-based cata-
lysts, hence the need to find other catalyst options [92].
2.2.3.1. Production of carbon nanomaterials from plastic waste. Of the 2.2.3.1.2. Graphene. Graphene is a single, two-dimensional sheet of
valorization approaches available at the international and national level, carbon atoms arranged in a hexagonal lattice. It was discovered in 2004
the production of carbon nanomaterials presents the greatest potential. through the adhesive tape peeling process [93]. The ideal graphene
This is because: 1) by themselves carbon nanomaterials represent a sheets are highly ordered and exhibit a high Young's modulus (1 TPa),
growing market segment (marketed as raw material), and 2) they can be high thermal conductivity (5000 W/mK) and high electron mobility
part of different products that address other markets (environment, en- (>200,000 cm2/Vs), a high specific surface area (up to 2630 cm2/g),
ergy, health, aerospace, others), with growth in demand. optical transmittance (up to 97.7%), chemical stability and quantum Hall
Due to the fact that carbon is the main component of plastics, such is effect at room temperature. Additionally, graphene is 200 times stronger
the case for example of polyethylene (85.6 % wt of carbon), poly- than steel, making it one of the strongest materials ever tested [94]. Due
propylene (85.6 % wt of carbon), polystyrene (92.2 % wt of carbon), to its impressive characteristics, graphene is used in a wide range of
terephthalate made of polyethylene (62.6 % wt carbon), and poly- applications, mainly in photonics, electronics, biomedical and environ-
acrylonitrile (67.9 % wt carbon), plastic waste can therefore provide a mental pollution control as a biosensor, drug carrier, energy storage,
carbon source to produce carbon nanomaterials [87]. Table 3 shows the nanocomposite polymers and adsorbent [95].
research and patenting activity related to upcycling of plastic waste to The global size of the graphene market was 42.8 million USD in 2017,
carbon nanomaterials. and from that date to 2025 a CAGR of 38.0 % [96] was projected, to reach
Although there are several structures, those with a defined market a market size of 552.3 million USD. To date, more than 20 companies
will be briefly highlighted. produce and market this material [97]. Since its discovery, this nano-
2.2.3.1.1. Carbon nanotubes (CNTs). These are rolled graphene material has reported great activity in research and patenting, as shown
sheets that form a cylindrical piece and depending on how the graphene in Table 5.
sheets are rolled, they can display different properties [88]. The attrac- At the commercial level there are four main methods to produce
tive properties of CNTs are essentially divided into five categories: (i) different types of graphene. Micromechanical exfoliation, chemical
electrical: semiconductor or metallic behavior, 100 times more conduc- vapor deposition (CVD), reduction of the liquid phase of graphene oxide
tive than copper; (ii) mechanical: very high tensile strength (100 times and epitaxial growth are the four different synthetic methods of graphene
greater than steel); (iii) thermal: high thermal stability and thermal [95]. These methods use traditional hydrocarbons as raw material that
conductivity; (iv) chemical: chemically inert while being related to make the process difficult to control and thus fail to achieve its scaling
chemical/biological functional groups; (v) structure: ideal potential. As such, the advantage of polymers as precursors over tradi-
one-dimensional (1D) system with anisotropic properties, with extremely tional hydrocarbons in preparing graphene lies in the easy control of the
high aspect ratios [89]. total number of carbon atoms. Hence the need to develop a method that
The applications of this nanomaterial include electronic, photovol- allows the successful incorporation of plastic waste as raw material [98].
taic, electrodes, transport, remediation, and medical devices, among Considering this, several strategies have been proposed using the CVD
method to prepare different types of graphene from plastic waste, these
being polyethylene terephthalate (PET), polyethylene (PE), polyvinyl
Table 3. Research and patenting activity related to upcycling of plastic waste to
carbon nanomaterials in the period 2000 to 2019.
Table 4. Research and patenting activity related to carbon nanotubes in the
Search criteria Activity in research Activity in
period 1991 to 2019.
patenting
Title, Abstract, Keywords/claims Database: SCOPUS Database: Lens Search criteria Activity in research Activity in Patenting
Org. Title, Abstract, Database: SCOPUS Database: Lens Org.
Reuse, valorization, upcycling, 31 scientific publications (As 10 patent Keywords/claims
value added, waste, residual, of 2010, publications on the documents (since Carbon nanotubes 109,631 scientific 37,752 patent documents
plastic/polymer þ carbon nano subject begin) 2007) publications grouped by family
8
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Table 5. Activity in research and patenting related to the graphene topic in the Table 6. Activity in research and patenting related to the activated carbon topic
period 2004 to 2019. in the period 2004 to 2020.
Search criteria Activity in research Activity in patenting Search criteria Activity in research Activity in patenting
Title, Abstract, Database: SCOPUS Database: Lens Org. Title, Abstract, Keywords/claims Database: SCOPUS Database: Lens Org.
Keywords/claims Activated carbon 100,027 scientific publications 3,178,257 patents
Graphene 121,979 scientific 59,359 patent documents
publications grouped by family
The size of the global activated carbon market was estimated at 4.72
chloride (PVC), polypropylene (PP), polystyrene (PS) and poly- billion USD in 2018. This market is expected to expand at a CAGR of 17.5
methylmethacrylate (PMMA) [99]. However, the yield of graphene is % during the following years, mainly due to its increasing demand in
low, and the size of the graphene is limited by the size of the metal water treatment applications and wastewater treatment [107]. Since its
substrate. Therefore, there is a need to develop new approaches for the discovery, this material has reported great research and patenting ac-
efficient conversion of plastic waste to graphene with high yields and tivity, as shown in Table 6.
controllable layers (single layer, bilayer, or a few layers) [100]. To produce activated carbon, the raw material is required to have a
2.2.3.1.3. Activated carbon. Activated carbon is a carbonaceous ma- porous structure, adequate mechanical resistance, null or low inorganic
terial that has a high surface area. Its internal structure is composed of material, high carbon content and, most importantly, the raw material
micropores, so these can adsorb a wide variety of substances, i.e., they must be abundant. Coal, wood, lignite, coconut shells, walnuts and al-
can attract molecules to their internal surface and therefore act as an monds, olive seeds and some polymers have traditionally been used as
adsorbent [101]. The properties of this material depend on the material raw materials [108]. It is for this reason that there is a need to develop
of its origin and its structure may be different depending on the raw methods that allow the successful incorporation of plastic waste as a raw
material from which it was made. Industrially they are produced through material to obtain activated carbon, considering that this waste is
reaction with gases, by physical activation, or through the addition of abundant and has a high carbon content.
chemicals in the process known as chemical activation. Activated carbon 2.2.3.1.4. Paints. Paints are liquid compositions that turn into a solid
is made up of primary microcrystals and is composed of structures of film after being applied in thin layers to a surface. The paints dry forming
hexagonal planes of two-dimensional carbon atoms that lack crystallo- an adapted film on the applied surface. They are compact and well
graphic order in the direction perpendicular to the sheets. They therefore adhered. They are applied to hide the primitive appearance of the sur-
present a high percentage of the highly disordered structure. Activated face, giving it color, a different look, as well as having the aim of lending
carbon is characterized by a branched pore system, in which pores of protection from attack by external agents [109].
different sizes, such as mesopores (d ¼ 2–50 nm), micropores (d ¼ Paints generally have several basic components: the vehicle, the
0.8–2.0 nm), and sub-micropores (d 0.8 nm) branch from macropores pigment, additives, etc. The vehicle, also known as an emulsifier, dis-
(d 50 nm). The pore volume of activated carbons is generally greater solves in a medium to form the liquid part of the paint (the part that is
than 0.2 ml/g. The internal surface area is generally greater than 400 polymerized). This provides homogeneity and the protective film. In
m2/g. Pore width varies from 0.3 to several thousand nanometers [97]. addition, it controls the sliding properties of the coating and helps
The conversion of plastic waste into carbon materials is generally improve its hardness and resistance. Pigment, meanwhile, is an organic
prepared by pyrolysis, in batch or continuous mode, because this process or inorganic compound whose mission is to provide paint with color and
is well known, the focus is can find the optimal operations conditions for coating power [110]. The additives cover many products that are
different materials with specific properties according to the applications generally added to paints for specific purposes. These are generally
required. Vieira et. al., [102] and Wijesekara et. al., [103] show complete products added in small amounts to cause or attribute certain effects or
reviews about the preparation methods for carbon-based materials from properties that would not be achieved with only the vehicle, pigments
plastic waste. These reviews verified that the different conditions (tem- and/or solvents [111].
perature, catalysts, flow, type of atmosphere, i.e.), used to obtain the Paints have many applications and their commercialization is
materials could be used to find different properties. Fuks et. al., [104] considered an important economic activity. Their global market is ex-
show a study for the synthesis of activated carbon from PET waste by pected to exceed a volume of 167 trillion dollars in 2022 mainly due to
pyrolysis under N2 environmental; also, Ilyas et. al., [105] produce increasing urbanization and industrialization, according to the TechSci
activated carbon from PETs bottles under controlled conditions (inert Research report entitled Global paints and coatings market by technol-
atmosphere at high temperature). Therefore, the operational conditions ogy, by application, by region, competition forecast & opportunities,
could be modified according to the specific structure, then the rapid, 2012–2022. Due to the growing demand for the use of these products, it
medium, and high pyrolysis could produce different activated carbons is also considered a viable alternative to include plastic waste in a new
with different properties. production cycle, generating added value.
Activated carbon has a wide range of applications both in its powder
presentation and in its granular presentation in liquid and/or gaseous 3. Conclusions
medium. In general, pulverized carbon is applied in a liquid medium
while granulated activated carbon can be applied in both environments. Plastic waste is highly resistant to degradation and causes a range of
Standing out among its applications in a liquid medium are: discoloration environmental concerns associated with the accumulation of waste in
of sugar liqueurs, purification of water (elimination of odor, color, nature, since in the long term it exerts toxic effects on living beings, soils,
chemical substances, bacteria), wastewater treatments, water dichlori- and water sources. To date, the recycling of plastics has not been an
nation for use in the manufacture of soft drinks, decolorization and economically viable solution and it is estimated that most household
enhancement of alcoholic beverages (wines, rums), purification of edible plastics end up being improperly disposed of in landfills or outdoors after
fats and oils, protein purification, as a medicine in the detoxification of their first use. As such, this review demonstrates that it is possible to
people, purification of blood plasma, and separation of metallic elements incorporate plastic waste into production processes that allow the pro-
(gold, silver). In a gaseous medium, its applications are also abundant, duction of carbonaceous materials with high added value, constituting a
among which are: storage and separation of gases, gas masks, anti- sustainable alternative for the final disposal of this waste. However, it
radioactive protection in nuclear plants, deodorizing of food products. should be stressed that the methods for obtaining these materials are still
In addition, today it has broad application prospects as a catalytic support in the research phase or the laboratory, so it remains a challenge to take it
and as a catalyst [106]. to an industrial scale and make it economically viable. Among the most
9
R.A. Mu~
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1. Introduction mismanagement of plastic waste (intensive use of non-renewable re-

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