RSC PET Review

Industrial Chemistry & Materials
Chemical Recycling of PET Plastics – An alternative to obtain

value added products: A REVIEW
Journal: Industrial Chemistry & Materials
Manuscript ID Draft
Article Type: Review Article
Date Submitted by the

n/a
Author:
Complete List of Authors: Bhanderi, Khodidas; ISTAR, Industrial chemistry

Joshi, Jeimin; ISTAR, Industrial Chemistry
Patel, Jigar; ISTAR, Industrial Chemistry
Page 1 of 25 Industrial Chemistry & Materials
1 Chemical Recycling of PET Plastics – An alternative to obtain value added products: A

2 REVIEW
3 Khodidas K. Bhanderi, Jeimin R. Joshi & Dr. Jigar V. Patel*
4 Industrial Chemistry, Institute of Science & Technology for Advanced Studies and Research, Vallabh
5 Vidyanagar, Anand, 388120, Gujarat, India.
6 [Emails: bhanderikhodidask@gmail.com, Jeimin17@gmail.com, *pramukhprit@gmail.com]
7
8 Abstract
9 Waste management is become one of the world's most pressing issues. Plastic is one of the most widely
10 utilised materials in the modern world. Plastic manufacturing and usage have risen globally in recent decades due
11 to its low weight and outstanding mechanical properties. Plastic has a wide range of applications due to such good
12 properties include lightweight, high strength, and extended durability. Because of plastics are non- or low-
13 biodegradable, a vast quantity of plastic waste is generated every day, making waste disposal the most pressing
14 matter globally. Furthermore, improper waste disposal pollutes the environment. An ecologically friendly
15 approach is necessary to locket these issues. One of the solutions is to recycle this sort of garbage. There are many
16 plastic recycling technologies available, however practically all of them have certain restrictions. Chemical
17 recycling of plastic, on the other hand, has been shown to be more efficient than other recycling methods. This
18 article provides a quick overview of chemical recycling of PET post-consumer waste and the synthesis of
19 potentially value-added products such as dye or dyestuffs, bolaform surfactant, bio-degradable polyesters, drug
20 carrier, Metal-organic framework (MOF), bio-degradable polymeric scaffolds, polyurethane foam and coating
21 materials etc.
22
23 Keywords: Environmental pollution, PET waste, Recycling, Value-added product, Waste management.
24
Page 1 of 25
Industrial Chemistry & Materials Page 2 of 25
25 1.0 Introduction
26 There was a lot of research done on numerous sectors by researchers throughout the eighteenth and nineteenth
27 centuries, and one of the most notable discoveries is "polymer or plastics materials" to this day. Since the
28 introduction of polymer into our lives, there have been numerous applications of polymer in various fields. As the
29 need for polymer grows, more research is being conducted in these fields for the synthesis of various more useful
30 polymers and their applications in other fields. Because polymer is widely used in our daily lives and in our
31 products, it will exacerbate a key problem: the accumulation of solid waste. It will now open a new field for
32 various researchers to solve this problem using various ways and doing various experiments in these sectors, and
33 there are now solutions for reducing solid waste by recycling of polymer waste materials using various recycling
34 processes.
35 “A polymer is a complex molecule made up of monomers, which are interconnected repeating subunits in
36 chains or rings.” Polymers have large molecular weights because they are made up of numerous monomers. The
37 prefix “poly” which means "many," and the suffix “mer”, which means "parts," form the term polymer. Swedish
38 scientist Jons Jacob Berzelius (1779–1848) created the term in 18331, and "Plastics are semi-organic compounds
39 derived from petroleum or oil. They are often referred to as polymers since they are made up of polymers.
40 Condensation and addition polymerization processes generate plastics."2–4. "The primary distinction between
41 polymer and plastic is that plastic is a form of polymer." Plastic is made up of a lengthy chain of polymers, each
42 of which is made up of smaller, homogeneous molecules."4“Plastic is a lightweight, hygienic and resistant material
43 which can be moulded in a variety of ways and utilized in a wide range of applications.To better understand the
44 challenges of recycling these polymeric materials, we should first understand their types and characteristics.
45 Thermoplastics and thermosets are the two most common types of polymeric materials5,6.
46 They are divided into one of two categories:
47 1) Thermosetting polymers/plastics
48 2) Thermoplastic polymers/plastics
49 “Thermosetting polymers solidify into a permanent design and shape. Thermoplastic polymers can be heated
50 and remolded for an unlimited amount of time”2–4,7,8. “Thermoset is a polymer that is cured by heat or chemical
51 reaction and becomes infusible and in- soluble material. Thermoset polymers have a permanent irreversible
52 polymerization”. “Thermoplastic is a plastic that softens upon heating and hardens when cooled”7. Figure 1
53 presents an illustrated overview of the two main categories of plastics”9. In today's world, it's impossible to
54 imagine a world without plastic or polymer. Despite this, their manufacture dates only from 1950. Bakelite was
55 the first synthetic plastic, debuting in the early twentieth century10.
56 Figure 1:The two main categories of plastics and their single-use applications9
Thermoplastics: A plastics that can be melted when heated & hardened when applied
cooling. That is why it is recyclyble.
Types of For Example:Polyethyleneterephtalate,Polyethylene,Polypropylene,Polystyrene,
Polyvinyl chloride,polylactic acid etc..
Plastics
Thermosets: A plastics that undergo a chemical change whaen heated, creating a three
dimension network. After they are heated and formed these plastics cannot be re-melte
and reshaped, and that is why it is recyclyble plastics.
For Example: Polyurethane,Phenolic resins,Epoxy resins,Vinyl ester,Urea
formaldehyde resins etc..
57
58 1.1 Plastics production
Page 2 of 25
59 The plastics business originated in the United States in the early 1900s, when Leo Hendrik Baekeland
60 developed the first synthetic plastic. Since 1950, yearly worldwide plastics manufacturing has risen from 1.5
61 million metric tonnes to 359 million metric tonnes. Plastic manufacturing has already surpassed eight billion
62 metric tonnes globally, and output will continue to rise significantly in the next few decades. Because plastic
63 manufacturing is expanding every day, it has become a severe global concern. Plastic products generated in the
64 previous 70-80 years have ended up in landfills, polluting the environment severely. The Great Pacific Ocean is
65 one of the most well-known instances of plastic pollution, with a concentration of plastic debris spanning over a
66 million square kilometres. Plastic may take hundreds or thousands of years to degrade in water, and the resulting
67 pieces, macro- and micro-plastics, are often released into the environment and consumed by living organisms.
68 Prior to 2018, China was the primary export destination for plastic garbage. Following that, China chose to stop
69 accepting plastic trash and other recyclables from other countries, putting pressure on major exporting countries
70 like the United States, Germany, and the United Kingdom to find other garbage destinations. Malaysia was the
71 leading destination for garbage exports by the end of 201811. In 2019, total worldwide plastics output was
72 estimated to be approximately 368 million metric tonnes. COVID-19's effects on the industry are expected to
73 reduce it by around 0.3 percent over the next several years 11,12. Plastics manufacturing has continued to expand
74 year after year. Plastics' market worth continues to rise in lockstep with that increase. Plastics are employed in a
75 variety of products and have replaced traditional materials such as wood, metal, and glass in areas where plastics
76 currently dominate. The yearly output of plastics across the globe is shown in the graph illustrated in Figure 11,12.
77 In the year 2019, Europe alone generated almost 57.9 million metric tonnes of plastic. China is one of the world's
78 largest manufacturers of plastics, accounting for more than a quarter of worldwide output. Plastic imports into the
79 United States are steadily growing, with China becoming as the world's leading provider. where China's plastic
80 exports have increased dramatically over the previous three decades, from 14.4 billion dollars in 2009 to 48.3
81 billion dollars in 2019 11,12.
82 Figure 2 : Annual production of plastics world-wide 8,9
Annual production of plastics world-wide

348 359 368 367
400 322 335
production volume in
299 311
million metric tons
270 279 288

300 245 250
200
200
100
100 50
1.5
0
1950 1976 1989 2002 2008 2009 2010 2011 2012 2013 2014 2015 2016 2017 2018 2019 2020
production volume in million metric tons
83 In world-wide waste was generated by various sector out of the packing sector is one of the major waste
84 plastics generations in our world. which came in first with 141 million tons of waste production 13,14.
85
Plastics waste generation in million metric tons
160 141
140
120
100
80
60 42 38 37
40 13 17 13
20 1
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Page 3 of 25
du
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industrial sector
86 Figure 3:Plastics waste generation by different industrial sectors 13,14
87 Global plastic waste volume was 6.3 billion metric tonnes in 2015, with an anticipated value of roughly
88 12 billion metric tonnes in 2050, as illustrated in the figure 15.
Plastic waste volume worldwide

14
WASTE VOLUME IN BILLION METRIC TONS
12
12
10
8 6.3
6
4
2
0
2015 2050
YEARS
89 Figure 4:Plastic waste volume worldwide in 2015 and 2050 15
90 The average per capita use of plastic in India is around 11 kilogrammes, according to the Ministry of
91 Petroleum and Natural Gas estimate.
92 By 2022, the annual per capita consumption in India will reach 20 kilogrammes. According to CPCB
93 estimates, plastic makes about 8% of total solid trash, with Delhi generating the most, followed by Kolkata and
94 Ahmedabad. Only 60% of the total plastic garbage gets recycled further. Water and soft drink bottles create the
95 most plastic garbage in households. Around 43% of produced plastics in India are used for packaging, with the
96 majority being single-use.16 Thermoplastics contribute for 80-85 percent of all plastics used worldwide, and are
97 mostly employed in packaging and textile fibres. Approximately half of them is employed in single-use
98 applications17, while the rest are used in long-term infrastructures such as pipelines, cable coatings, and structural
99 components. The rest is utilised for long-lasting consumer items like electronics, furniture, and automobiles 18.
100 Thermoset plastics, on the other hand, were employed as a long-term useful material6.
120 109
Waste generation plastics in (Kgs)
100
80 65
60
38
40 32 28
20 11
0
US Europe China Brazil Global India
average
country’s name
101 Figure 5:Per capita consumption of plastic 16
102 There are many thermoplastic polymers that we use in our daily life, each with its own plastics code to
103 identify which kind of plastic it is and to classify it into distinct categories.19–22 which are shown in figure.
Page 4 of 25
104
105
106
107
108
109 SIP codes for
Different
110 Plastics
111
112
113
114
115
116
117 Figure 6: SPI codes for different types of plastic take from19
118
119 Out of all polymeric materials demand most demanding polymer or plastics was PET (poly ethylene
120 terephthalate), and the production of polyethylene terephthalate (PET) bottles worldwide an in 2016, some around
121 485 billion of PET bottles were produced, and it is increase in end of 2021 was some around 583.3 billion of PET
122 plastic bottles will be produced and it will increase day by day by increasing use of PET plastics which are show
123 in given figure in below23. Global PET production capacity was 30.3 million tons out of maximum production
124 capacity was 30.80% of China, and into second number was Africa was 21%.
Global PET bottle production 2004-2021

PET PRODUCTION (IN BILLIONS)
583.3
600 475 485
500
400 300
300
200
100
0
2004 2014 2016 2021*
YEARS OF PRODUCTION
Global PET bottle production
Page 5 of 25
125 Figure 7 : Global PET bottle production 2004-2021
126 Figure 8 : Global PET production capacity21
127 1.2 Polyethylene terephthalate (PET)
128 PET or PETE stands for Polyethylene Terephthalate Plastics, which is the world's most widely used
129 polymer. PET is known as poly (oxyethylene oxyterephthaloyl) based on its systematic structure, according to
130 IUPAC polymer nomenclature. It is also reinforced with glass fibres and carbon to improve material strength.
131 PET is still very strong for its lightweight nature even without the addition of those additives24,25. In the textile
132 sector, it is known as "Polyester," and it is commonly used as a fabric for garments because it is a good moisture
133 barrier. It is also used for bottling and packaging. The majority of PET plastic manufactured contains synthetic
134 fibre up to 60% of the total world demand, with the remaining 30% used for bottle manufacturing. By the mid-
135 1940s, the first PET had been developed in the United States. PET is an integral element of your daily routine.
136 Many businesses manufacture virgin PET under many trade names across the world 26,27. The table below lists
137 some of the most frequent trade names for PET that are commercially available 28.
138 Trade name Manufacture

Arnite DSM Engineering Plastics
Diolen ENKA-Glazstoff
Global PET production capacity (%)
Eastapac Eastman chemical company
Hostadur totleFarbwerke
capacity 30.3 million
Hoechst AG tons (2017)
Mylar E.I. Du Point de Nemours & Co. Inc
Asia(Excluding
Melinex Imperial Chemical Indusatries Ltd
China) 2.30%
Rynite Du Point de Nemours & Co. Inc
21%
Africa
30.80% China
South america
Middle East
Europe
16.90%
North America
4.10% Asia(Excluding China)
10.20%
14.20%
139
140
141
142
143 Figure 9:commercially available PET 28
144 1.2.1 Production of PET
145 PET is made primarily by the reaction of bi-functional acids and alcohols in the presence of a metal catalyst
146 28. It's an aliphatic polyester that can be made in two ways:
147 1. Esterification process between terephthalic acid and ethylene glycol.

148 2. Trans-esterification process between ethylene glycol and dimethyl terephthalate 29–32.
149
Page 6 of 25
OH
O O
OH
H 3C O O CH3
Ethylene
Dimethyl terephthalate (DMT) glycol (EG)
O
O
2nCH3OH
Methenol
O n
150 Poly(ethylene terephthalate) or PET
151 Figure 10: Ethylene glycol and dimethyl terephthalate by Trans-esterification reaction
152 Another laboratory approach for producing PET is to combine Terephthalic acid with ethylene glycol in
153 the presence of a catalyst. PET may be made by combining terephthoyl chloride with ethylene glycol. PET
154 production is a simple process, however terephthoyl chloride is more costly than terephthalic acid 28.
COOH
O
O
OH O
H 2O -2nH2O
Ethylene glycol (EG)

n
O
COOH Poly(ethylene terephthalate), or
Terephthalic acid (TPA) PET
155
156 Figure 11:Tterephthalic acid and ethylene glycol by esterification reaction.
157
158 1.2.2 Physical properties
159 PET is a glass-like amorphous substance. PET transforms from a stiff glass-like condition to a rubbery elastic
160 state when heated over 72°C. Because the polymer was semi-crystalline 28. PET plastics are the most widely used
161 thermoplastics in the packaging and textile sectors. They have excellent properties such as:
162  It is a semi-crystalline plastic that is translucent.

163  It is very strong and stiff.
164  It has excellent heat resistance.
165  It is lightweight and so transportable.
166  Its electrical insulating characteristics are outstanding.
167  It is stable owing to its minimal water absorption.
168  It is useful for consumable packaging because it has excellent resistance to various chemicals (or does
169 not react with) and water 33.
170  PET possesses a glass-like clarity, as well as appropriate gas barrier characteristics for carbonation
171 retention. It also has a high toughness-to-weight ratio, allowing for lightweight, large-capacity, safe,
Page 7 of 25
172 unbreakable containers. It is one of the primary reasons for its widespread popularity 28,34. Because of
173 these beneficial properties, PET is the most widely used thermoplastic in various sectors.
174 1.2.3 Application of PET
175 Plastic manufacturing and usage have risen globally in recent decades due to its low weight and
176 outstanding mechanical qualities. Plastic has a broad range of applications due to qualities such as lightweight,
177 high strength, and extended durability. PET plastic is used in a variety of industries, including transportation,
178 automotive, electronics, home appliances, packaging, and textiles. Because of the poor or non-degradability of
179 this type of polymer or plastics materials, a huge amount of waste plastic was generated in our daily lives. To deal
180 with this type of problems, follow the three "R" rules: "REDUCE," "REUSE," and "RECYCLE." To minimize
181 plastic waste by reducing the usage of plastics, reusing them for a longer period of time, or recycling them. Other
182 methods for reducing waste include landfills and incineration plants where polymer waste burning to generate the
183 energy.
184 1.3 What is recycling
185 "The process of recovering scrap or waste plastics and reprocessing the material into value-added
186 products, often radically different in form from their initial condition," according to Wikipedia.35 The term
187 recycling refers to the process of recovering monomer from a previously processed polymer so that it may be
188 reused by the industry36–39. The primary motivation for recycling and reprocessing waste PET stems from public
189 knowledge and concern about pollution. Out of the six most prevalent polymers used in packaging, PET has the
190 highest recycling rate. In the next several years, we expect 68% of PET bottles to be collected internationally. In
191 2018, 19.7 million tonnes of food-grade PET bottles were manufactured, with 845,000 tonnes being mechanically
192 recycled back into food-grade PET bottles. We estimate that it will reach 30.4 million tonnes in the next few years,
193 with over 3 million tonnes mechanically recycled. Danone and Pepsi Coca-Cola have both requested that RPET
194 be used in 50% of their bottles.40
195 The recycling rate of PET plastic bottles in selected countries in 2018* was Norway was the world
196 leader in recycling with a % recycling rate for PET (polyethylene terephthalate) plastic bottles in 2018. In the
197 United States, just 29 percent of these plastic bottles were recycled shown in figure below. (* Data is from 2017,
198 ** 65% is recycled at registered facilities, 15% in the unorganized sector) The effective deposit return process in
199 Norway explains the country's high recycling rate. When customers buy plastic bottles, they pay a modest charge
200 on top of the product price and are compensated when they return them to reverse vending machines. Because the
201 system has been so successful, other countries have followed suit. In the United Kingdom, 86 percent of
202 consumers favour supermarket deposit return systems for plastic, glass, and beverage cans41.
Page 8 of 25
PET plastics Recycling Rate
97%
100% 84.80% 84%

80%
90%
80% 58.20%
70%
60%
50% 28.90%
40%
30%
20%
10%
0%
ay
n*
en
n*
es
a*
at
rw
pa
ed
io
di
St
Un
No
Ja
Sw
In
d
n
ite
ea
Un
p
ro
Eu
203 Figure 12 : Recycling rate of PET plastic bottles in selected countries in 201841
204 Various polymer recycling technologies have been developed to handle these issues which are describe
205 in flow charts figure 28. There are four primary methods for recycling PET waste plastics that have been presented
206 in this article 34.
Plastics
recycling
method
Chemical Mechanical Plastic waste

Recycling recycling menagement
Energy Recovery secondary Primary

Tertairy recycling Landfilling
or Quaternary recycling Recycling
Recycling
2)
1) 4)
Amminolysis/a 3) Hydrolysis 5) Pyrolysis 6) Glycolysis
Methanolysis Hydrogenation
monolysis
207 Figure 13:Different method for PET plastics recycling28,39,42,43
208 1.3.1 Mechanical recycling
Page 9 of 25
209 Mechanical recycling is the most common and commonly used method for plastic recycling, and it
210 consists of multiple phases such as collecting, screening, automatic or manual sorting, washing, shredding,
211 extrusion, and granulation39,44–47.figure 14. Mechanical recycling is categorised as primary or secondary based on
212 the kind of initial material treated. Primary recycling, also known as re-extrusion and closed-loop recycling, is the
213 most common method of reusing discarded plastics. For instance, an aluminium can is recycled into another
214 aluminium can, while a plastic pot is recycled into another identical plastic pot 43,48–51. one of the drawbacks of
215 This method is used to keep the number of cycles for each material to a minimum 43,48–51.
216 Figure 14: Step of mechanical recycling of plastics39
217 Physical recycling is another name for secondary or mechanical recycling method. Melt extrusion is used
218 to extract the polymer from the waste and reprocess it into granules. It entails trash sorting and separation, size
219 reduction, melt filtering, and plastic material reforming.18,43 The used polymer products are transformed to various
220 end products. for example, rubber Tyres may be recycled into various rubber products. There are some positive
221 and negative points which are described in shown in figure 15. in 2018, 19.7 million tonnes of food-grade PET
222 bottles were manufactured, with 845,000 tonnes being mechanically recycled back into food-grade PET bottles.
223 We estimate that it will reach 30.4 million tonnes in the next few years, with over 3 million tonnes mechanically
224 recycled. Danone and Pepsi Coca-Cola have both requested that RPET be used in 50% of their bottles.28
225
Advantage Disadvantage
-This procedure is reasonably priced. -Thermoplastic polymers are the only ones that can be
recycled.
-The recycling procedure is -The amount of waste plastic will be drastically
straightforward.51 decreased.
-It requires a significant initial expenditure.
-It has little or no environmental -Each cycle results in a loss of product qualities owing to
consequences.52,53 the recycled resin's reduced molecular weight.18,42,54
-When compared to virgin polymers, the applications of
recycled plastics were less demanding.47
-Melt viscosity is reduced as a result of hydrolytic and
thermal deterioration.55
-Printability and dyeability of the final PET product are
affected by the formation of cyclic and linear oligomers55.
-PET yellowing caused by oxidation and intramolecular
cross-linking.55
226 Figure 15 : Advantages and Dis-advantages of mechanical recycling of PET plastics 18,43,48,52–56
227 1.3.2 Energy Recovery or Quaternary Recycling
Page 10 of 25
228 The plastic is burned to recover the energy content of the plastic and to utilise the heat it creates as an
229 energy source. Incineration is an energy-recovery technique that is used to recycle plastic waste in a Quaternary
230 manner. When dealing with polymeric waste is difficult or not economically feasible, this procedure is utilised.
This method creates a large volume of
This process results in the melt residue.28
creation of monomers, which are Toxic airborne compounds such as
used to make polymers. dioxins (in the case of heavy metals,
It produces a significant amount chlorine-containing polymers, toxic
carbon, and oxygen-based free radicals)
of energy from waste pose a significant health risk.17,50,58–60
plastics.17,42,50 all the recycling techniques listed here,
chemical recycling is the only one that is
suitable according to the principles of
sustainable development since it recovers
a raw material (monomers) from which
the polymer is made.28,61
231 Figure 16 : Advantages & dis-advantages of quaternary recycling method 17,28,43,51,57–60
232
233 This procedure was carried out in incinerators reactors, where wastes were burned in the presence of air,
234 and plastic hydrocarbons were converted to carbon dioxide and water. The heat generated is superheated steam,
235 which may be used to generate power using turbine generators.28
236 1.3.3 Advanced recycling: feedstock or chemical recycling
237 The structural breakdown of a substance into its raw product component and subsequent transformation
238 into an entirely new product. Chemical recycling is described as "a chemical reaction in which polymers are
239 chemically transformed to monomers or partly depolymerized to oligomers (a change in the polymer's chemical
240 structure)." The end product may be used to create additional polymerizations in order to replicate the original or
241 another value-added product. The leftover plastic material may be converted into tiny monomer molecules using
242 this method.43,50,51 The following chemical processes are employed to decompose polymers into monomers such
243 as Hydrogenation, Glycolysis, Gasification, Hydrolysis, Pyrolysis, Methanolysis, Chemical depolymerization,
244 Thermal cracking, Catalytic cracking and reforming, Photodegradation, Ultrasound degradation, Degradation in
245 microwave reactor etc.
By breaking down PET scrap Chemical recycling is still in
into monomers, oligomers, its infancy, which is why only
and other compounds utilising a few businesses are pursuing
this method.56 it.51
A pure monomer and other This process is more costly
valuable compounds have than other methods of
been produced, requiring no recycling.42,50,51,57–59
additional purification.
246 Figure 17 : advantages & dis-advantages of chemical recycling method 43,51,52,57,58,61,62
247 1.3.4 Chemical recycling of PET
Page 11 of 25
248 Chemical recycling of PET is a process that incorporates many kinds of depolymerization procedures to
249 break down the polymers of waste PET into valuable chemicals in the form of oligomers and monomers. The
250 advantage of chemical recycling is that it can achieve the quality of virgin PET. PET waste chemical recycling
251 include depolymerization by several procedures such as methanolysis, hydrolysis, glycolysis, aminolysis, and
252 ammonolysis.
253 Figure 18 : different chemical recycling routes of waste PET
254 Various depolymerization procedures are employed in many journals research papers for the most commonly used
255 PET polymers. However, depolymerization plastics create monomer or recycling chemicals using a variety of
256 chemical reaction mechanisms, but the most useful and commercially accessible are alcoholysis (methanolysis)
257 and glycolysis.28
258
259 1.3.4.1 Hydrolysis
260 To break the polymer chain and create monomers such terephthalic acid (TPA) and ethylene glycol
261 (EG).28Hydrolysis depolymerizes the most valuable plastic PET. There are three types of hydrolysis:
262 1. Acid hydrolysis

263 2. Alkaline hydrolysis
264 3. Neutral (water) hydrolysis
265 PET waste is treated with NaOH or KOH in alkaline hydrolysis to produce terephthalate salt, which is further
266 acidified to produce monomer TPA The effect usually carried out for 3-5 hours at temperatures ranging from 210-
267 250 °C at a high pressure24,63–65. An alkaline hydrolysis procedure is normally carried out with the use of
268 an aqueous alkaline solution of NaOH, KOH, at a concentration of 4-20 wt% EG & salt of disodium or
269 dipotassium terephthalate.66,67 Alkaline hydrolysis has the benefit of being able to employ highly
270 contaminated PET waste and the process is much simpler and less expensive than methanolysis.28,67
271 Hot water or hot steam is used in neutral hydrolysis. This procedure requires the use of high-pressure autoclaves,
272 Temperatures of 200-300 °C and pressures ranging from 1-4 MPa the primary by products are EG and TPA 24,63–
273 65. In acid hydrolysis, PET waste is depolymerized with water in an acidic atmosphere to create TPA
274 and EG. To depolymerize waste PET into TPA and EG, strong acid (87 % weight H2SO4, H3PO4, and
275 HNO3) was utilised. There are no further requirements, such as high temperature or pressure. However,
276 if the acid concentration is too low and the temperature is too low, the acid hydrolysis process will be
277 sluggish. But the problem with this hydrolysis method for depolymerizing PET. The reagent H2SO4 is
278 often used in acid hydrolysis. As a result, it has generated a large amount of liquid waste containing
279 inorganic salt and H2SO4.42,58 However, the acid hydrolysis process has become expensive at the
280 industrial level due to the need for recycling of large amounts of waste liquid generated in the acid
Page 12 of 25
281 hydrolysis process, as well as the purification of EG from H2SO4. Acid hydrolysis has been used to
282 recover chemicals like TPA and EG from waste PET.28
283 1.3.4.2 Aminolysis
284 Different aqueous amine solutions are used in the aminolysis of PET waste to produce the
285 corresponding diamides of TPA and EG. In this process, primary amine aqueous solutions such as
286 methylamine, ethylamine, and ethanolamine are often used at temperatures ranging from 20-100 °C.
287 Acid, sodium acetate, and potassium sulphate are utilized as catalysts in this process. With the presence
288 of catalysts, pure bis (2- hydroxy ethylene) terephthalamide (BHETA) is synthesized with sufficiently
289 high yields 68. PET chemical recycling has seldom employed aminolysis methods. Numerous research studies
290 have been conducted on the partial aminolytic depolymerization of PET for industrial use.69–75 Methylamine,
291 ethylamine71–73, and butylamine73,74, ethanolamine 73, and triethylenetetramine 75 are the most often utilised
292 aminolysis agents. The use of basic chemicals such as glacial acetic acid or simple salts to depolymerize PET
293 fibre waste was examined by S.R Shukla, Ajay M. Harad. 76 Through numerous chemical reactions, the BHETA
294 product of this method was utilised to produce a valuable product. 28
295 1.3.4.3 Ammonolysis
296 Ammonia is reacted with PET waste to produce terephthaldiamide in ammonolysis. This primary product can
297 be transformed to terephthalonitrile or another chemical. For 1-7 hours, the reaction is carried out under pressure
298 of about 2 MPa at temperatures ranging from 120 -180 °C. The amide generated is filtered, washed with distilled
299 water, and dried at 80 °C. The product has a very high purity level of at least 99% 77. Anhydrous ammonia reacts
300 with waste PET in an ethylene glycol environment and it will produce terephthalic acid amide. This can be
301 converted into terephthalic acid nitrile and further to p-xylylene diamine or 1,4-bis(aminoethyl)cyclohexane.28,78
302 Waste PET depolymerization by this process was carried out at about 2 MPa pressure in a temperature range of
303 120–180◦C for 1–7 h. after the reaction completion filter the reaction mass, rinsed with water, and dried at an
304 80◦C temperature. To get 90% yield of the product.28,78
305 1.3.4.4 Methanolysis
306 Because methanol is utilised as a reagent in this reaction, it is also known as alcoholysis. Chandra R
307 investigated the depolymerization of PET by methanol at high temperatures and pressure. The primary products
308 of PET depolymerization by methanolysis reaction were dimethyl terephthalate (DMT) and ethylene glycol
309 (EG).28 The key benefits of this technology are the easy recovery and recycling of ethylene glycol and methanol.
310 It has difficult and expensive separation and refining of the mixture of reaction products (glycol, alcohols, and
311 phthalate derivatives).28 In recent years, PET depolymerization by supercritical fluid has been focused by using
312 supercritical water, and supercritical methanol has been introduced to the depolymerization of PET.28,58,79–88
313 1.3.4.5 Glycolysis
314 Glycolysis is the solvolytic breakdown of PET in which the ester linkages are broken and hydroxyl
315 functionalities are replaced. To get BHET and other oligomers, PET must react with appropriate glycols such as
316 EG, DEG or PG, DPG, and so on. Whereas BHET may be utilised as the starting material for PET synthesis,
317 finished oligomers can be used to make polymers such as unsaturated polyesters, polyurethanes, vinyl esters,
318 epoxy resins, and polymeric concretes. To achieve full depolymerization in an adequate time period at a consistent
319 rate, a transesterification different oxide salt as a catalyst was used 28,81,89,90.
320 Glycolysis is the cleavage of ester linkages by a different glycol, resulting in various oligomers or
321 oligoesters with hydroxyl terminal group.28,91 In general, the glycolysis process involves cutting up pre-consumed
322 PET bottles into small pieces, washing them with detergent solution, and drying them in a dryer. The
323 depolymerization process will then be carried out using various glycols in the presence of various catalysts in an
324 inert atmosphere at temperatures ranging from 190 -220◦C.26,74–77,78–80 Omrani et al. studied the depolymerization
325 of PET waste using propylene glycol (PG) in the presence of a catalyst in an inert atmosphere at various reaction
326 time and weight ratios of PET. It was discovered that the presence of a catalyst accelerates the depolymerization
Page 13 of 25
327 reaction process. To compare the depolymerization of PET using PG, two different grades of PET were employed,
328 and the results were identical. Free glycol was eliminated. The glycolization products were characterised using
329 FTIR, GPC, DSC, and hydroxyl value determination, among other methods. Unsaturated resins and certain kinds
330 of polyurethanes may be easily made using the oligomeric glycolizates product.28 Size exclusion chromatography
331 was used by Chen et al. to investigate the oligomer distribution in glycolized products. It was also discovered that
332 in the presence of zinc acetate catalyst, the glycolysis process of PET fibre progresses more quickly. Excess
333 ethylene glycol (EG) and polyethylene terephthalate (PET) oligomers were used in the studies, which were
334 conducted in the presence of zinc acetate. During the ongoing glycolysis reaction of PET, the monomer and dimer
335 were discovered to be contained in the liquid phase. The catalyst was discovered to have boosted the glycolysis
336 rate.28,94 Mansour and Ikladious was investigated that the depolymerizing of PET waste using 1,4 Butane diol and
337 tri-ethylene glycol in the presence of zinc acetate as a catalyst. The finished products were analysed by hydroxyl
338 and acid value, as well as other analytical elemental analysis such as GPC, 1H NMR, 13C NMR, differential
339 scanning calorimeter (DSC), and mass spectra.28,99 Xi, Lu, and Sun was studied that how to depolymerize PET
340 waste by using glycolysis with high purity and a considerable yield of BHET product. Depolymerization of PET
341 waste utilising ethylene glycol (EG) as a reagent and zinc acetate as a catalyst. The yield of the end product,
342 BHET, was 85.6 %. IR, DTA (differential thermal analysis), 1H NMR, and 13C NMR were used to analysed it.28,95
343 But in convectional catalyst are not much better because catalyst was used to decrease the reaction time to increase
344 the rate of reaction but convectional metal salt of oxide catalyst not much decrease the reaction time, so than new
345 bio-derived or nano catalyst was introduced into these sectors to using them the reaction time of chemical
346 recycling of waste plastics was up to 3-4 hr which are batter than 8 hr reaction time, and which will be cost down
347 the product by recycling of this type of catalyst. PET waste glycolyzed by various glycols such as polypropylene
348 glycol ,100 Di propylene glycol , propylene glycol (PG). 28 In recent years, researchers have focused on developing
349 new types of catalysts, such as bio-waste-derived catalysts, nano-particles or nano tubes as nano-catalysts, and
350 catalysts that bond to supporting materials for use as catalysts, among others. By utilizing nano-catalyst as a
351 glycolysis catalyst, Zengwei Guo discovered a novel catalyst for depolymerization of waste PET. PET was
352 cryogenically pulverized into fine particles in this study, and then used for depolymerization using ethylene glycol
353 and a nano-catalyst101. Fernanda Reis Veregue invented a new cobalt nanoparticle that can be used as a catalyst
354 in the glycolysis of waste PET. The very first ultrasmall cobalt nanoparticle was dispersed into ethylene glycol
355 using an ultrasonic bath or sonicator, according to the researchers. Following the addition of waste PET flaks, the
356 solution was heated to 180°C for different time intervals, and the end product BHET was identified using 13C
357 NMR and DSC techniques102. Yujun Zhao proposed a study in which waste PET flaks were glycolized with
358 ethylene glycol as a reagent and heterogeneous CaO (SrO, BaO)/MCF as highly active and recyclable catalysts,
359 which were prepared and used in the glycolysis reaction for 0.5-4 hours at 175-195°C, yielding 100% PET
360 conversion and 80% yield of the desired product. It was analysed by several types of analysis techniques103. Boron
361 nitride nanosheets coated with Fe3O4 nanoparticles were investigated by Mohammad Reza Nabid as a magnetic
362 bifunctional catalyst for PET waste recycling through glycolysis. The author can first produce hexagonal boron
363 nitride nanosheets in this study, which will be used as a catalyst in the PET depolymerization process. In the
364 reaction, waste PET and ethylene glycol were combined with a small amount of catalyst, and the reaction was
365 carried out at 200°C for 5 hours. After the reaction was completed, the final product was recovered using a hot
366 water and then filtered using a vacuum filter. Various analytical methods were used to conform the final product
367 BHET, including 1H NMR, FT-IR, HPLC, Mass spectrometry etc104. Emine Sert has reported on a new tradition
368 of depolymerization of waste PET utilizing a novel solvent medium/catalyst. The author can use deep eutectic
369 solvents as a catalyst for glycolysis of waste PET, which are made up of two components: hydrogen bond acceptor
370 (HBA) and hydrogen bond donor (HBD) (HBD). First, waste PET and ethylene glycol were charged into the RBF,
371 and the reaction was run until the desired reaction temperature was reached. After that, a solvent was added to the
372 system as a catalyst, and the reaction was run until the waste PET conversion was completed. The final product
373 was derived using the workup technique once the reaction was completed, and it was verified by FT-IR105. The
374 use of waste ostrich eggshell as a bio-catalyst in the depolymerization of waste PET was examined as a new bio-
375 waste use which was reported by Isti Yunita. The author prepares a bio-catalyst from waste ostrich eggshell using
376 a calcined technique, then adds waste PET, reagent, and prepared bio-catalyst to RBF and runs the reaction at
377 192°C for 4 hours. After the reaction was completed, we achieved our desired product through multiple stages of
378 workup, which was confirmed by 1H NMR, 13CNMR, FT-IR, and mass spectral data106. Jean Halison de Oliveira
Page 14 of 25
379 presented a novel study of nickel nano-catalyst efficiency in the degree of PET conversion under different
380 conditions. The Pechini method was used to produce the nano-catalysts, and nickel oxide nanoparticles were used
381 as a catalyst in the depolymerization reaction of PET via glycolysis once they were made. He developed a factorial
382 design with a central point using software, with the following variables: the synthesis temperature of nano-
383 catalysts, the period of the depolymerization reaction, and the number of nano-particles employed in mass. The
384 depolymerization was carried out in the presence of ethylene glycol at a temperature of 185°C at atmospheric
385 pressure using a nano-catalyst reaction temperature of 185°C. Multiple filtering was used to obtain the desired
386 product. Different analytical instruments were used to examine and analyse it107. Gabrielle R. Lima discovered
387 that waste PET depolymerization utilising two distinct catalysts, sodium titanate nanotubes (NaTNT) and zinc
388 titanate nanotubes (ZnTNT), at 196°C for 2, 3, and 4 hours yielded 67-85 % yield of end product (BHET) during
389 various reaction time periods108. Another technique proposed by Gabrielle R. Lima was to use a sodium/protonated
390 nanotube catalyst in the depolymerization of waste PET at 196°C for 3 hours, yielding more than 80% of the final
391 BHET product, which was confirmed by 1H NMR and 13C NMR spectroscopy109. Israel Cano proposed a study
392 utilizing paramagnetic ionic liquid-coated SiO2@Fe3O4 nanoparticles as a next-generation recoverable nano-
393 catalyst for glycolysis of waste PET. PET depolymerization was accomplished using glycol at 190°C for 24 hours,
394 following which the end product was extracted using hot water and the catalyst was recovered using an external
395 magnet110. Zathang Laldinpuii was reported to have developed a bio-waste derived catalyst for PET waste
396 glycolyzed with Ethelene glycol in the presence of a bio-catalyst at 190°C for 3.5 hours, yielding 83% of the
397 required product. The FT-IR will confirm it. Another method utilised by this author to depolymerize waste PET
398 was to use another bio-waste based bio-catalyst, which resulted in a 79 % yield of the desired product. Different
399 analytical methods will be used to characterize it 96,97. Ren-Xuan Yang and Yen-Tsz Bieh developed a novel
400 heterogeneous Metal Azolate Framework 6 Catalyst with a High Zinc Density, which will be utilized as a catalyst
401 for Enhanced Polyethylene Terephthalate (PET) Conversion in glycolysis111. Erik Adolfsson proposed work was
402 a Nanostructured micro particle of Magnetic Mg-Al-O@Fe3O4 as a low-cost and sustainable catalyst in the
403 recycling of PET fibre waste, in the reaction process first micro particle of Mg-Al-O@Fe3O4 was prepared and
404 used in depolymerization of waste PET waste fibre ethylene glycol was used as a glycolyzing agent charged into
405 RBF and run the reaction at required temperature and pressure until the rection is complete, then recover the final
406 product and analyse it using various analytical techniques112. Using ultrasmall CeO2 nanoparticles with rich
407 oxygen defects as novel catalysts for efficient glycolysis of PET, ling-xia yun recently investigated a very rapid
408 way of glycolysis process. PET was depolymerized utilising CeO2 nanoparticales with a size of 2.7 nm that were
409 dispersed in ethylene glycol and the reaction was carried out at 196°C for 15 minutes with a conversion rate of
410 98.6% and a yield of 90.3 % BHET monomer113. Yonghwan Kim investigated a new source of heterogeneous
411 catalyst derived from bio-waste, which was utilised to depolymerize waste PET using the glycolysis technique in
412 the presence of bio-catalyst at 195°C for 1 hour, yielding 64.98 %BHET product. FT-IR, 1H NMR, 13C NMR, and
413 other techniques will be used to characterise it a thorough examination114. Zishuai Wang presented work based on
414 the discovery of novel catalysts that are more efficient than those previously identified. The experiment used
415 waste PET depolymerization utilising a cyanamide catalyst in a glycolysis process that yielded 100% PET
416 conversion at 150°C115. Other some glycolysis reaction data given below table no.1
Reagent ratio Reaction Used catalyst Solvent / ionic % Of yield Reference

condition liquid of BHET
PET:EG (1:2) 190◦C for 1.5 cobalt acetate - - 89,116
hr
PET:EG 220◦C for 3 hr zinc acetate & lead acetate - - 89,117
PET:EG (1:10) 190◦C for 2 hr 1-butyl-3- 1-butyl-3- 71.2 % 89,118
methylimidazolium methylimidazolium
hydroxyl ([Bmim]OH), hydroxyl ([Bmim]OH),
1-butyl-3-
methylimidazolium
bicarbonate
([Bmim]HCO3), 1-
butyl3-
methylimidazolium
chloride ([Bmim]Cl),
and 1-butyl-3-
Page 15 of 25
methylimidazolium
bromide ([Bmim]Br)
PET:EG 196◦C for 1.25 Zn/Al mixed oxide - 79 % 89,119
hr
PET:EG Tetragonal a novel set of catalysts, - 92.2 % 89,120
ZnMn2O4 pure oxides (ZnO, Co3O4,

spinel catalyst and Mn3O4) and mixed-
at 260◦C, 5 oxide spinel (ZnMn2O4,
atm, for 60 CoMn2O4, and ZnCo2O4)
minutes
PET:EG 190◦C for 3 hr Lewis base acetate-based - 52.8 % 89,121
(3gm:20gm) ionic liquid as the catalyst

PET:EG 170-175◦C into 1-butyl-3-methyl - 64 % 89,122
microwave imidazolium bromide

([bmim]Br) as a catalyst
PET:EG Reaction run 1 % zinc acetate - 78 % 89,123
into microwave
power of 500
W and at 196◦C
only for 35
minutes
PET:EG (1:05) at 240°C for 2 Mg-Al double oxides - - 124
hrs pellets as catalyst

PET:EG (1:05) Reaction metal organic framework - - 125
temperature at catalysts (ZIF8, ZIF-67,

160–200 °C for MOF-5)
0.5–4 h under
the
atmospheric
pressure
PET:EG (1:02) For only 1–20- zinc acetate as catalyst solvents used such as 82 % 126
minute reaction aniline, nitrobenzene,

time in DMSO 1-methyl-2-
at 190°C pyrrolidinone (NMP)
or dimethyl sulfoxide
(DMSO)
1:5:50 wt% ratio of at 240°C for 1 zwitterionic 1,3- - 60 % 127
catalyst: PET:EG h dimethylimidazolium-2-

carboxylate as a catalyst
(or catalyst-precursor)
417 Table 1: glycolysis reaction parameters with % Yield
418 1.4 Value-added products from recycling chemicals
419 Chemical recycling of PET waste using several recycling methods When waste plastics are
420 depolymerized using various recycling methods, chemicals such as ethylene glycol (EG), di-methyl ester of
421 terephthalate (DMT), terephthalic acid (TPA), bis (2-hydroxy ethylene) terephthalamide (BHETA),
422 Terephthalamide, and bis(2-hydroxyethyl) terephthalate (BHET) are produced. BHET is the most interesting and
423 useful of these compounds due to its wide range of applications compared to the other chemicals obtained from
424 chemical depolymerization of waste PET polymers.
425
426
427 Dye/Dyestuff
pH-sensitive
428 Polyurethane
Drug carrier
-Alginate
429 nanoparticles
430
Polyurethane
foam/coating BHET (bis(2- Bolaform
surfactants Page 16 of 25
materials
hydroxyethyl)
terephthalate)
431
432
433
434
435
436
437
438
439
440 Figure 19 : Application of glycolized product (BHET) of waste PET
441 Andrew C. A. Wan proposed a number of biodegradable poly- (phosphoester) ionomers utilising recycled
442 BHET from waste PET. Another approach presented by Mao, Hai-Quan was to synthesize biodegradable
443 polymers with desirable physicochemical and biological characteristics by synthesising a series of
444 poly(terephthalate-co-phosphate)s128,129.
445 Using Bis (2-hydroxyethyl) terephthalate glycolyzed product of PET, one of the methods for synthesis of
446 Flame Retardant Polyurethane Coating. Vacuum distillation was used to obtain the pure product.130
447 S.R. Shukla reported chemical recycling of PET waste to produce hydrophobic textile dyestuffs from
448 glycolyzed product and apply them to polyester fabric.131
449 Xing Zhou investigated the synthesis and characterization of waterborne polyurethane dispersions from
450 glycolyzed waste polyethylene terephthalate used as soft and hard segments in the synthesis of novel waterborne
451 polyurethane dispersions (PUDs) using a simple and environmentally friendly process.22
452 The study of synthesis of biodegradable polymer was examined by Hai-Quan Mao and Irina Shipanova-
453 Kadiyala utilising a two-step polycondensation polymerization procedure. In the reaction process,
454 dimethylaminopyridine (DMAP) and methylene chloride were dissolved appropriately in RBF with recycled
455 BHET from waste PET. After that, the solution was cooled to -40°C, and ethyl phosphorodichloridate (EOP) in
456 methylene chloride was added dropwise to the solution. After adding EOP, the mixture was stirred at room
457 temperature for 4 hr before adding a drop-wise solution of terephthaloyl chloride (TC) in methylene chloride to
458 the RBF flask. The temperature was gradually increased to 50°C, and the reaction was allowed to take place
459 overnight. The solvent and residue were evaporated and re-dissolved into chloroform, respectively, and the final
460 reaction mass was washed with salt solution before being anhydrous with Na2SO4. After quenching the solution
461 in cold methanol and drying it in a 60°C oven, the final product was obtained. With an 82 percent yield, the
462 poly(terephthalate-co-phosphate) P (BHET-EOP, 80: 20) was synthesized. It will also be analysed using the GPC
463 technique. Various different polymers can be synthesised by changing the reagent ratio129.
464 A. S. Sabnis proposed research for the synthesis of polyester polyol from recycled chemicals derived from
465 waste PET. BHET, adipic acid, phthalic anhydride, and neopentyl glycol were charged into RBF using p-toluene
466 sulphonic acid (p-TSA) as a catalyst and xylene as a solvent. This polyesterification reaction was carried out at a
467 temperature of 180-190°C in parallel with the complection reaction. This polyester was used on mild steel panels
468 as a coating material132.
469 A novel work was proposed by I.Duque-Ingunza to synthesise unsaturated polyester resin from glycolyzed
470 postconsumer PET wastes. It was reported that BHET was react with (MA) malic anhydride, which is frequently
471 used in the manufacture of resin, and polyesterification was accomplished in a three-neck RBF in an inert
Page 17 of 25
472 environment at 135-180°C. Hydroquinone was then added to stop the reaction. After cooling the reaction mass, it
473 is dissolved in the appropriate solvent for further curing or moulding133.
474 Mengjuan Li presented a unique synthesis of azo dispersion dyestuffs utilising BHET monomer. 134,135
475 Kishor Sarkar discovered one of the ways for production of bio-degradable poly ester, which are utilised as
476 drug binder or drug carrier, in which glycolyzed waste of PET waste (BHET) was reacts with sebacic, citric acid
477 & D-Menitol as a raw material. The bio-degradable poly ester manufactured by melt condensation polymerization
478 using glycolyzed PET as the monomer and sebacic, citric, and D-Menitol as the monomer. This biodegradable
479 poly ester was made without the use of a catalyst and under severe conditions. This poly ester is biphasic in nature
480 and is used to transport drugs. Which may be characterised using a variety of analytical techniques like as NMR,
481 SEM, FTIR, and in vitro degradation.136,137
482 M. Ben Gara's proposed study was Synthesis of Aliphatic-Aromatic Co-polyesters from Glycolized Waste
483 PET. In this study, ring-opening polymerization was used to create BHET/Caprolactone co-polyesters by reacting
484 BHET with caprolactone. The reaction took place in an inert environment at 160°C, and once the mixture became
485 homogenous, catalyst tin octoate was added to the reaction mixture. After adding the catalyst, raise the temperature
486 to 220°C and conduct the reaction for 6 hours. Finally, following the complection reaction, the required product
487 was collected and analysed using several analytical methods138.
488 New aromatic-aliphatic biodegradable polyesters were studied by Fouad Malek. First, BHET, succinic
489 anhydride, and 4-dimethyl aminopyridine (DMAP) were charged into RBF, together with 1,4-dioxan as a reaction
490 medium, and the reaction was carried out at 50°C. After the reaction had been performed for 12 hours, the solvent
491 was removed, and the residual product was solubilized using chloroform. After that, we removed the excess
492 succinic acid residue by washing the reaction mixture with water and passing it through Na2SO4 to remove the
493 water residue. The last solvent evaporated, producing a solid product. After that, hydroxytelechelic poly (-
494 caprolactone) oligomer and dibutyl tin dilaurate (DBTDL) were added to the product in RBF. The reaction
495 mixture was heated to 220°C for 5 hr. After the reaction was completed, the reaction mass was cooled, and the
496 co-polyester was dried in an oven at 60°C for 72 hr. Random co-polyester was also synthesised by this researcher
497 using BHET, Succinic anhydride (AS), and poly(ε-caprolactone) diol (α,ω−ΟΗ oligo-PCL) reaction was run at
498 220°C and dibutyl tin dilaurate (DBTDL) was used as a catalyst into this reaction139.
499 Aditi Bhattacharyya proposed a task to build pH-sensitive Polyurethane-Alginate nanoparticles for safe and
500 effective oral insulin administration in an animal model using recycled value-added chemicals BHET from waste
501 PET. First, polyurethane was prepared by adding BHET to RBF and heating it to 110°C in an inert environment.
502 Hexamethylene di-isocyanate (HMDI) was added to RBF after melting and the temperature was raised to 130°C.
503 After 1 hour, (PEG) polyethylene glycol-600 was added to the reaction mass as a chain extender, and the
504 temperature was increased to 180°C. The finished product was dissolved in a suitable solvent to create a
505 polyurethane film. The film was then mixed with sodium alginate to make pH-sensitive Polyurethane-Alginate
506 nanoparticles for insulin administration through oral140.
507 Rapeseed oil and recycled poly (ethylene terephthalate) polyols were produced using a two-step continuous
508 synthesis method with varied rapeseed oil and poly (ethylene terephthalate) concentrations. The polyols that
509 resulted were utilised to make hard polyurethane foams, which were then analysed using different procedures to
510 determine their properties.141
511 Assem K. Merekenova has introduced novel value-added products derived from waste PET. The goal of the
512 research was to create a monoalkyl phosphate ester from a glycolized waste PET product. BHET was synthesised
513 from waste PET in this process, and it was then charged with N, N-dimethylforamide and mixed properly at 70°C.
514 After that, polyphosphoric acid was added while maintaining continual stirring at a temperature of 70°C to 140°C
515 for 12 hr to reaction time. water was used to neutralise the reaction mass after reaction completed for 3 hr at
516 80°C142.
517 Amit Kumar A. Barot described the preparation of polyurethane coatings using synthesised polyols as a base
518 component and Toluene di-isocynate (TDI) or Hexamethylene di-isocynate (HMDI) adducts as a hardener
Page 18 of 25
519 component. FT-IR, 1H NMR & 31P NMR, MASS spectrometry, and gel permeation chromatographic (GPC) are
520 among of the analytical techniques used to characterise it130.
521 Supaluck Kawkumpa researched the synthesis of polyurethane BHET utilising ZnO as a catalyst. Author
522 BHET and PEG (400) were dissolved in their respective solvents into RBF established the remaining assembly
523 and heated the reaction at 60°C for several minutes in this study. The reaction was then treated with 98% iso
524 phorone diisocyanate (IPDI), followed by the addition of catalyst. The reaction was performed at 70oC for 3 hr,
525 following which the reaction mixture was cooled to room temperature and cast by pouring into the fixed shape
526 material for curing143.
527 Amandeep Singh proposed a study for the synthesis of biodegradable porous polymeric scaffolds for
528 osteoblast cell regeneration in the human/animal body to be used in the restoration of damaged bone tissues. First
529 prepolymer synthesis from BHET in this study. In this reaction, BHET is charged into the RBF, which sets the
530 reaction conditions by purging nitrogen gas for an inert environment and gradually increasing the temperature to
531 110°C. Hexamethylene di-isocyanate (HMDI) was slowly added when BHET was completely melted, and the
532 temperature was steadily increased up to 130°C. A dense wine-colored product was formed after 1 hr of reaction.
533 As a chain extender, different glycols were utilised. Finally, polyurethane was synthesised. The manufacture of
534 different PU-GO/(Hap) composites and scaffolds utilizing graphene oxide GO/hydroxyapatite (Hap)144.
535 There has recently been an increasing interest in biodegradable polyester. Krishana Ghosal proposed another
536 method for tissue regeneration using bio-resorbable polyester made from recovered PET waste react with
537 soyabean oil. The product was characterised by FTIR, NMR, DSC, TGA, XRD, and in vitro degradation, and it
538 was manufactured utilising BHET as the raw material monomer, which was generated by depolymerisation of
539 waste PET by glycolysis 136, However, there are several biopolymers for interfacial tissue regeneration that have
540 yet to be found. Almost every biopolymer has some use in bone regeneration or cartilage creation. It is challenging
541 to rebuild tissue interfaces such as bone-cartilage with this bio-polymer due to its complicated chemical
542 composition and mechanical characteristics. Because of the high cost of manufacture, employing this biopolymer
543 for tissue regeneration is restricted. However, this bio-polymer, created by Krishana Ghosal using waste or
544 renewable resources, may be able to fix the issue. They are inspired from the previous studies 145,146 and
545 investigated that a new approach for tissue engineering application was evolved by incorporating soyabean oil by
546 epoxidation into BHET, SA(sebacic acid), CA(citric acid), and MA(malic anhydride) based bio-polymers.
547 Because of the presence of an aromatic ring and a long aliphatic hydrocarbon chain in BHET and soyabean oil,
548 this polyester offers hard and soft segments, which is why it is used in tissue interfaces such as bone-cartilage for
549 interfacial tissue engineering (ITE).147
550 Pavel A. Mikhaylov investigated the synthesis of thermotropic co-polyesters based on recycled chemical
551 BHET from waste PET. A series of novel co-polyesters are synthesised in this study using melt polycondensation
552 of bis(2-hydroxyethyl) terephthalate (BHET) and 4'-acetoxybiphenyl-4-carboxylic acid (ABCA) as co-monomers
553 and Sb2O3 as a catalyst in reaction. Different analytical methods validated it148.
554 Potential biomedical application of a new Metal–organic frameworks (MOF) based on a derived from bis(2-
555 hydroxyethyl) terephthalate (BHET) work proposed by DENIS A CABRERA-MUNGUIA. MOF was synthesised
556 in this study by mixing aluminium nitrate nonahydrate (Al (NO3)3.9H2O) and BHET in distilled water. The
557 resulting mixture was charged into RBF and heated for 72 hours at 200°C. After the reaction was completed, the
558 reaction mass was cooled to room temperature and the required product was collected using filtering. The product
559 was neutralised by washing it with water to eliminate the excess nitric acid. The product was dried for 24 hr at
560 80°C149.
561 Tânia Marina Palhano Zanela invented a different type of application. He presented a study to synthesise
562 bolaform surfactants from BHET derived from waste PET. First, BHET and triethyl phosphate (OP(OEt)3) were
563 charged into a three-neck RBF equipped with a reflux condenser, temperature monitoring, and magnetic stirring.
564 The system was operated at 100°C for 72 hours to collect the desired product, which would be analysed using
565 different analytical methods150.
566
Page 19 of 25
567 1.5 Conclusion
568 Over the next several decades, the need for plastics will rise, and as a result of this increased demand and
569 usage, plastic trash will rise as well. By using various chemical recycling processes, various building block
570 chemicals and various value-added products can be obtained. This review paper discusses the method of waste
571 plastics recycling step by step, as well as various building block chemicals and value-added products and their
572 major applications in today's market.
573 1.6 Future aspects of Plastics Recycling
574 In the near future, the globe will become more ecologically aware, with a greater focus on recycling.
575 Because recovery, reuse, and recycling of any waste material, such as plastics, paper, and glass, is an effective
576 and long-term approach for enhancing the industry's and society's sustainability. The primary motivations for
577 recycling plastic garbage are to conserve natural resources and waste, as well as to reduce solid waste on our
578 world. Plastic waste recycling was used to create a variety of derivatives or value-added products using recycled
579 chemicals or building blocks. About half of the world's population will utilise biodegradable or recycled plastics
580 and value-added products in the future. We can lessen the amount of plastic garbage in our environment this way.
581 1.7 Acknowledgement
582 The authors acknowledge financial assistance from SHODH - ScHeme of Developing High Quality Research,
583 Knowledge Consortium of Gujarat, Education Department, Government of Gujarat.
584 1.8 Funding
585 SHODH - ScHeme of Developing High Quality Research, Knowledge Consortium of Gujarat,
586 (Education Department, Government of Gujarat. Letter Reference no: KCG/SHODH/2020-21/ & Grant number:
587 202010820003.
588
589 1.9 Declaration of conflicting interests
590  Consent to participate Not applicable.

591  Consent to publish Not applicable
592  The author(s) declared no potential conflicts of interest with respect to the research, authorship, and/or
593 publication of this article, and the authors also declare that they have no known competing financial
594 interests or personal relationships that could have appeared to influence the work reported in this paper.
595 1.10 Author Contributions
596  Dr. Jigar V. Patel have given guidance’s & idea about this work, and he have supervised, monitored, and
597 revised the manuscript. Khodidas K. Bhanderi & Jeimin R. Joshi have collected data, designed the
598 manuscript and written the main text and revised the manuscript. All authors have read and agreed to the
599 published version of the manuscript.
600 1.11 Ethical Approval
601  We hereby declare that this work is original and not copied from anywhere else. We approve that this
602 work is not submitted in this language or any other language to any other journal nor it is submitted for
603 simultaneous consideration.
604
605 1.12 REFERANCE
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607 8, 2022).
608 2 Plastics vs. Polymers, https://omicoplastics.com/blog/plastics-polymers-difference/, (accessed
609 March 15, 2022).
Page 20 of 25
610 3 Polymer Vs Plastic, https://www.rspinc.com/blog/plastic-injection-molding/polymer-vs-plastic/,

611 (accessed March 15, 2022).
612 4 Polymer vs Plastic, https://www.osborneindustries.com/news/polymers-vs-plastics/, (accessed
613 March 15, 2022).
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Industrial Chemistry & Materials

Chemical Recycling of PET Plastics – An alternative to obtain

Journal: Industrial Chemistry & Materials

Article Type: Review Article

Date Submitted by the

Complete List of Authors: Bhanderi, Khodidas; ISTAR, Industrial chemistry

1 Chemical Recycling of PET Plastics – An alternative to obtain value added products: A

46 They are divided into one of two categories:

58 1.1 Plastics production

82 Figure 2 : Annual production of plastics world-wide 8,9

Annual production of plastics world-wide

270 279 288

86 Figure 3:Plastics waste generation by different industrial sectors 13,14

Plastic waste volume worldwide

89 Figure 4:Plastic waste volume worldwide in 2015 and 2050 15

101 Figure 5:Per capita consumption of plastic 16

Global PET bottle production 2004-2021

Global PET bottle production

125 Figure 7 : Global PET bottle production 2004-2021

126 Figure 8 : Global PET production capacity21

127 1.2 Polyethylene terephthalate (PET)

138 Trade name Manufacture

144 1.2.1 Production of PET

147 1. Esterification process between terephthalic acid and ethylene glycol.

150 Poly(ethylene terephthalate) or PET

Ethylene glycol (EG)

162  It is a semi-crystalline plastic that is translucent.

174 1.2.3 Application of PET

184 1.3 What is recycling

PET plastics Recycling Rate

100% 84.80% 84%

Chemical Mechanical Plastic waste

Energy Recovery secondary Primary

207 Figure 13:Different method for PET plastics recycling28,39,42,43

208 1.3.1 Mechanical recycling

216 Figure 14: Step of mechanical recycling of plastics39

227 1.3.2 Energy Recovery or Quaternary Recycling

231 Figure 16 : Advantages & dis-advantages of quaternary recycling method 17,28,43,51,57–60

236 1.3.3 Advanced recycling: feedstock or chemical recycling

246 Figure 17 : advantages & dis-advantages of chemical recycling method 43,51,52,57,58,61,62

247 1.3.4 Chemical recycling of PET

253 Figure 18 : different chemical recycling routes of waste PET

262 1. Acid hydrolysis

283 1.3.4.2 Aminolysis

295 1.3.4.3 Ammonolysis

305 1.3.4.4 Methanolysis

313 1.3.4.5 Glycolysis

Reagent ratio Reaction Used catalyst Solvent / ionic % Of yield Reference

PET:EG (1:10) 190◦C for 2 hr 1-butyl-3- 1-butyl-3- 71.2 % 89,118

ZnMn2O4 pure oxides (ZnO, Co3O4,

(3gm:20gm) ionic liquid as the catalyst

microwave imidazolium bromide

hrs pellets as catalyst

temperature at catalysts (ZIF8, ZIF-67,

minute reaction aniline, nitrobenzene,

catalyst: PET:EG h dimethylimidazolium-2-

418 1.4 Value-added products from recycling chemicals

567 1.5 Conclusion

573 1.6 Future aspects of Plastics Recycling

581 1.7 Acknowledgement

584 1.8 Funding

590  Consent to participate Not applicable.

595 1.10 Author Contributions