One-Pot Upcycling of Heterogeneous Polyester Waste to Biodegradable Thermoplastics: A Cost-Effective Solution for a Circular Economy

Mira Shin , Minjin Kim , Giyoung Shin , Sung Bae Park , Hyeonyeol Jeon , Dongyeop X. Oh , Jun Mo Koo , Wangyun Won , Jeyoung Park

SusMat ›› 2025, Vol. 5 ›› Issue (6) : e70046

PDF
SusMat ›› 2025, Vol. 5 ›› Issue (6) :e70046 DOI: 10.1002/sus2.70046
RESEARCH ARTICLE
One-Pot Upcycling of Heterogeneous Polyester Waste to Biodegradable Thermoplastics: A Cost-Effective Solution for a Circular Economy
Author information +
History +
PDF

Abstract

The efficient recycling of poly(ethylene terephthalate) and poly(butylene terephthalate), the most extensively produced plastics, is essential for reducing global carbon emissions and the current dependence on fossil resources. However, the chemical recycling of polyesters primarily involves polymer-to-monomer and monomer-to-polymer processes, resulting in significant greenhouse gas emissions owing to significant electricity and fuel consumption. Herein, this research reports a simple and efficient one-pot polymer-to-polymer upcycling process that directly converts these two polyester wastes into biodegradable thermoplastic poly(ether ester)s using poly(tetramethylene ether) glycol (PTMG). The synthesized series of poly((ET-co-BT)-mb-PTMG) (PEBTG) exhibit a maximum tensile strength of 68 MPa, with 85% weight loss after 20 weeks in composted soil. Techno-economic analysis and life cycle assessment indicate that PEBTG is more cost-competitive and environmentally beneficial than currently existing plastics derived from fossil fuels, such as polypropylene and polybutylene adipate terephthalate. Once de-risked, the proposed upcycling strategy for polymer waste can be extended to expedite the development of a sustainable plastic economy.

Keywords

chemical upcycling / life cycle assessment / one-pot upcycling / polyester recycling / thermoplastic polyether ester elastomers

Cite this article

Download citation ▾
Mira Shin, Minjin Kim, Giyoung Shin, Sung Bae Park, Hyeonyeol Jeon, Dongyeop X. Oh, Jun Mo Koo, Wangyun Won, Jeyoung Park. One-Pot Upcycling of Heterogeneous Polyester Waste to Biodegradable Thermoplastics: A Cost-Effective Solution for a Circular Economy. SusMat, 2025, 5(6): e70046 DOI:10.1002/sus2.70046

登录浏览全文

4963

注册一个新账户 忘记密码

References

[1]

A. Kulkarni, G. Quintens, and L. M. Pitet, “Trends in Polyester Upcycling for Diversifying a Problematic Waste Stream,” Macromolecules 56 (2023): 1747–1758.

[2]

T. N. Tsironi, S. M. Chatzidakis, and N. G. Stoforos, “The Future of Polyethylene Terephthalate Bottles: Challenges and Sustainability,” Packaging Technology and Science 35 (2022): 317–325.

[3]

N. Thachnatharen, S. Shahabuddin, and N. Sridewi, “The Waste Management of Polyethylene Terephthalate (PET) Plastic Waste: A Review,” IOP Conference Series: Materials Science and Engineering 1127 (2021): 012002.

[4]

A. Ganguly, P. Channe, R. Jha, S. Mitra, and S. Saha, “Review on Transesterification in Polycarbonate–Poly (Butylene Terephthalate) Blend,” Polymer Engineering & Science 61 (2021): 650–661.

[5]

S. A. Vyavahare, B. M. Kharat, and A. P. More, “Polybutylene Terephthalate (PBT) Blends and Composites: A Review,” Vietnam Journal of Chemistry 62 (2024): 579–589.

[6]

J.-P. Lange, “Managing Plastic Waste─Sorting, Recycling, Disposal, and Product Redesign,” ACS Sustainable Chemistry & Engineering 9 (2021): 15722–15738.

[7]

M. Chu, W. Tu, S. Yang, et al., “Sustainable Chemical Upcycling of Waste Polyolefins by Heterogeneous Catalysis,” SusMat 2 (2022): 161–185.

[8]

A. Ghosh, “Performance Modifying Techniques for Recycled Thermoplastics,” Resources, Conservation and Recycling 175 (2021): 105887.

[9]

L. D. Ellis, N. A. Rorrer, K. P. Sullivan, et al., “Chemical and Biological Catalysis for Plastics Recycling and Upcycling,” Nature Catalysis 4 (2021): 539–556.

[10]

A. Vlasopoulos, J. Malinauskaite, A. Żabnieńska-Góra, and H. Jouhara, “Life Cycle Assessment of Plastic Waste and Energy Recovery,” Energy 277 (2023): 127576.

[11]

M. Tejaswini, P. Pathak, S. Ramkrishna, and P. S. Ganesh, “A Comprehensive Review on Integrative Approach for Sustainable Management of Plastic Waste and Its Associated Externalities,” Science of the Total Environment 825 (2022): 153973.

[12]

C. Li, L. Tong, S. Wang, et al., “Nitrogen Doping Induced by Intrinsic Defects of Recycled Polyethylene Terephthalate-Derived Carbon Nanotubes,” SusMat 3 (2023): 431–440.

[13]

V. Sinha, M. R. Patel, and J. V. Patel, “PET Waste Management by Chemical Recycling: A Review,” Journal of Polymers and the Environment 18 (2010): 8–25.

[14]

J. Payne and M. D. Jones, “The Chemical Recycling of Polyesters for a Circular Plastics Economy: Challenges and Emerging Opportunities,” ChemSusChem 14 (2021): 4041–4070.

[15]

W.-H. Xu, L. Chen, S. Zhang, et al., “New Insights Into Urethane Alcoholysis Enable Chemical Full Recycling of Blended Fabric Waste,” Green Chemistry 25 (2023): 245–255.

[16]

Y. Liu, X. Wang, Q. Li, et al., “Photothermal Catalytic Polyester Upcycling Over Cobalt Single-Site Catalyst,” Advanced Functional Materials 33 (2023): 2210283.

[17]

H. Abedsoltan, “A Focused Review on Recycling and Hydrolysis Techniques of Polyethylene Terephthalate,” Polymer Engineering & Science 63 (2023): 2651–2674.

[18]

S. Zhang, Q. Hu, Y.-X. Zhang, et al., “Depolymerization of Polyesters by a Binuclear Catalyst for Plastic Recycling,” Nature Sustainability 6 (2023): 965–973.

[19]

X. Bai, D. R. Aireddy, A. Roy, and K. Ding, “Solvent-Free Depolymerization of Plastic Waste Enabled by Plastic-Catalyst Interfacial Engineering,” Angewandte Chemie International Edition 62 (2023): e202309949.

[20]

J. Cao, H. Liang, J. Yang, et al., “Depolymerization Mechanisms and Closed-Loop Assessment in Polyester Waste Recycling,” Nature Communications 15 (2024): 6266.

[21]

E. Lorusso, Y. Feng, J. Schneider, et al., “Investigation of Aminolysis Routes on PET Fabrics Using Different Amine-Based Materials,” Nano Select 3 (2022): 594–607.

[22]

K. Chan and A. Zinchenko, “Conversion of Waste Bottles' PET to a Hydrogel Adsorbent via PET Aminolysis,” Journal of Environmental Chemical Engineering 9 (2021): 106129.

[23]

A. Jain and R. Soni, “Spectroscopic Investigation of End Products Obtained by Ammonolysis of Poly(ethylene Terephthalate) Waste in the Presence of Zinc Acetate as a Catalyst,” Journal of Polymer Research 14 (2007): 475–481.

[24]

J. Liang, J. Fu, H. Lin, et al., “Valorization of Polyethylene Terephthalate Wastes to Terephthalamide via Catalyst-Free Ammonolysis,” Journal of Industrial and Engineering Chemistry 132 (2024): 578–587.

[25]

L. Shen, E. Worrell, and M. K. Patel, “Open-Loop Recycling: A LCA Case Study of PET Bottle-to-Fibre Recycling,” Resources, Conservation and Recycling 55 (2010): 34–52.

[26]

M. Iturrondobeitia, L. Alonso, and E. Lizundia, “Prospective Life Cycle Assessment of Poly (Ethylene Terephthalate) Upcycling via Chemoselective Depolymerization,” Resources, Conservation and Recycling 198 (2023): 107182.

[27]

S. Tang, J. Li, R. Wang, et al., “Current Trends in Bio-Based Elastomer Materials,” SusMat 2 (2022): 2–33.

[28]

G. Holden, “Thermoplastic Elastomers,” in Applied Plastics Engineering Handbook (Elsevier, 2024).

[29]

S. Deng, R. Chen, S. Duan, Q. Jia, X. Hao, and L. Zhang, “Research Progress on Sustainability of Key Tire Materials,” SusMat 3 (2023): 581–608.

[30]

T. Yang, F. Liu, R. Gao, J. Li, J. Wang, and J. Zhu, “Rational Design for the Development of Thermoplastic Poly(ether-Ester) Elastomers From Bio-Based 2, 5-Furandicarboxylic Acid With High Elasticity,” European Polymer Journal 198 (2023): 112385.

[31]

A. S. Mohite, Y. D. Rajpurkar, and A. P. More, “Bridging the Gap Between Rubbers and Plastics: A Review on Thermoplastic Polyolefin Elastomers,” Polymer Bulletin 79 (2022): 1309–1343.

[32]

H. J. Kim, C. Jeong, A. Oh, Y.-S. Seo, H. Jeon, and Y. Eom, “Elevated Volatile Organic Compound Emissions From Coated Thermoplastic Polyester Elastomer in Automotive Interior Parts: Importance of Plastic Swelling,” Journal of Hazardous Materials 461 (2024): 132614.

[33]

L. Yu, Z. Yu, L. Yang, S. Wen, and Z. X. Zhang, “Development of Thermoplastic Polyether Ester Elastomer Microcellular Foam With High Resilience: Effect of Chain Extension on Foaming Behavior and Mechanical Properties,” Journal of Applied Polymer Science 140 (2023): e53912.

[34]

T. N. Jen, K. Behera, Y. H. Chang, and F. C. Chiu, “Improving the Ductility, Toughness, and Electrical Conductivity of Poly(lactic Acid) by Forming Poly(lactic Acid)/Thermoplastic Polyester Elastomer Blend and Blend-Based Nanocomposites,” Polymer Composites 44 (2023): 767–777.

[35]

J.-H. Ho, K.-C. Kuo, T.-Y. Lo, et al., “Upcycling Fabrics: Valorization of Recycled Polyethylene Terephthalate (r-PET) Plastic Waste Into Thermoplastic Polyester Elastomers (TPEE) for Fiber Spinning,” ACS Applied Polymer Materials 6 (2024): 552–560.

[36]

J.-J. Fang and L.-M. Shen, “Compression Property of TPEE-3D Fibrous Material and Its Application in Mattress Structural Layer,” Polymers 15 (2023): 3681.

[37]

J. Wang, X. Zhang, X. Fei, et al., “Synthesis of High Thermal-Resistant Poly(ester-Ether) Elastomers From Bio-Based 2, 5-Furandicarboxylic Acid,” ACS Sustainable Chemistry & Engineering 10 (2022): 13595–13606.

[38]

W. Wu, M. Li, Y. Zhong, et al., “Themoxidative Stability and Char Formation Mechanism for the Introduction of CNTs and MoS 2 Into Halogen-Free Flame Retarding TPEE,” RSC Advances 6 (2016): 3267–3275.

[39]

E. Marten, R.-J. Müller, and W.-D. Deckwer, “Studies on the Enzymatic Hydrolysis of Polyesters. II. Aliphatic–Aromatic Copolyesters,” Polymer Degradation and Stability 88 (2005): 371–381.

[40]

Y. Chen, L. Tan, L. Chen, Y. Yang, and X. Wang, “Study on Biodegradable Aromatic/Aliphatic Copolyesters,” Brazilian Journal of Chemical Engineering 25 (2008): 321–335.

[41]

B. Ahn, H. Sohn, J. J. Liu, and W. Won, “A System-Level Analysis for Long-Distance Hydrogen Transport Using Liquid Organic Hydrogen Carriers (LOHCs): A Case Study in Australia–Korea,” ACS Sustainable Chemistry & Engineering 12 (2024): 8630–8641.

[42]

C. Gong, S. Lee, and W. Won, “Process Development and Analyses for the Co-Production of 2-Methyltetrahydrofuran and 1, 4-Pentanediol From Lignocellulosic Biomass,” GCB Bioenergy 15 (2023): 900–915.

[43]

S. Backson, A. Kenwright, and R. Richards, “A 13C Nmr Study of Transesterification in Mixtures of Poly(ethylene Terephthalate) and Poly(butylene Terephthalate),” Polymer 36 (1995): 1991–1998.

[44]

W. J. Yoon, S. Y. Hwang, J. M. Koo, Y. J. Lee, S. U. Lee, and S. S. Im, “Synthesis and Characteristics of a Biobased High-T G Terpolyester of Isosorbide, Ethylene Glycol, and 1, 4-Cyclohexane Dimethanol: Effect of Ethylene Glycol as a Chain Linker on Polymerization,” Macromolecules 46 (2013): 7219–7231.

[45]

R. Yamadera and M. Murano, “The Determination of Randomness in Copolyesters by High Resolution Nuclear Magnetic Resonance,” Journal of Polymer Science Part A-1: Polymer Chemistry 5 (1967): 2259–2268.

[46]

A. Escala and R. S. Stein, “Crystallization Studies of Blends of Polyethylene Terephthalate and Polybutylene Terephthalate,” in Multiphase Polymers, 1st ed., ed. S. L. Cooper (American Chemical Society, Inc., 1979), 455–487.

[47]

D. Qiu, P. Zhang, S. Zhang, J. Sun, J. J. Wang, and L. Dai, “Synthesis and Non-Isothermal Crystallization Kinetics of Poly(ethylene Terephthalate)-co-Poly(propylene Glycol) Copolymers,” Polymers for Advanced Technologies 26 (2015): 1130–1140.

[48]

T. Yang, F. Liu, R. Gao, et al., “Fabrication of Thermoplastic Poly(ether-Ester) Elastomers With High Melting Temperature and Elasticity From Bio-Based 2, 5-Furandicarboxylic Acid,” ACS Sustainable Resource Management 1 (2024): 1520–1533.

[49]

M. Nofar and H. Oğuz, “Development of PBT/Recycled-PET Blends and the Influence of Using Chain Extender,” Journal of Polymers and the Environment 27 (2019): 1404–1417.

[50]

M. Sono, K. Kinashi, W. Sakai, and N. Tsutsumi, “Spin-Trapping Analysis and Characterization of Thermal Degradation of Thermoplastic Poly(ether–Ester) Elastomer,” Macromolecules 51 (2018): 1088–1099.

[51]

B. Ucpinar Durmaz, C. Ozturk, and A. Aytac, “Reduced Graphene Oxide Reinforced PET/PBT Nanocomposites: Compatibilization and Characterization,” Polymer Engineering & Science 60 (2020): 2606–2618.

[52]

W. Li, A. J. Ryan, and I. K. Meier, “Morphology Development via Reaction-Induced Phase Separation in Flexible Polyurethane Foam,” Macromolecules 35 (2002): 5034–5042.

[53]

W. Zhou, Y. Zhang, Y. Xu, et al., “Synthesis and Characterization of Bio-Based Poly(butylene Furandicarboxylate)-b-Poly(tetramethylene Glycol) Copolymers,” Polymer Degradation and Stability 109 (2014): 21–26.

[54]

D. Abdo, A. Gleadall, and V. V. Silberschmidt, “Damage and Damping of Short-Glass-Fibre-Reinforced PBT Composites Under Dynamic Conditions: Effect of Matrix Behaviour,” Composite Structures 226 (2019): 111286.

[55]

J. Fitoussi, M. Bocquet, and F. Meraghni, “Effect of the Matrix Behavior on the Damage of Ethylene–Propylene Glass Fiber Reinforced Composite Subjected to High Strain Rate Tension,” Composites Part B: Engineering 45 (2013): 1181–1191.

[56]

S. Sbrescia, J. Ju, T. Engels, E. Van Ruymbeke, and M. Seitz, “Morphological Origins of Temperature and Rate Dependent Mechanical Properties of Model Soft Thermoplastic Elastomers,” Journal of Polymer Science 59 (2021): 477–493.

[57]

S. Thomas and P. Visakh, Handbook of Engineering and Speciaalty Thermoplastics, Volume 3: Polyethers and Polyesters, ed. N. Jersey (John Wiley & Sons, 2011).

[58]

J. V. John, K. R. Kim, S. T. Baek, J. H. Yoon, H. Suh, and I. Kim, “Effect of Chain-Extender Modification on the Structure and Properties of Thermoplastic Poly(ether Ester) Elastomers,” Journal of Applied Polymer Science 133 (2016): app.42888.

[59]

R. Mouhoubi, M. Lasschuijt, S. Ramon Carrasco, H. Gojzewski, and F. R. Wurm, “End-of-Life Biodegradation? How to Assess the Composting of Polyesters in the Lab and the Field,” Waste Management 154 (2022): 36–48.

[60]

Y. Wei, J. Li, D. Shi, G. Liu, Y. Zhao, and T. Shimaoka, “Environmental Challenges Impeding the Composting of Biodegradable Municipal Solid Waste: A Critical Review,” Resources, Conservation and Recycling 122 (2017): 51–65.

[61]

E. Hartley, H. Moon, and A. Neves, “Biodegradable Synthetic Polymers for Tissue Engineering: A Mini-Review,” Reinvention: An International Journal of Undergraduate Research 15 (2022): 1.

[62]

S. Ju, G. Shin, M. Lee, et al., “Biodegradable Chito-Beads Replacing Non-Biodegradable Microplastics for Cosmetics,” Green Chemistry 23 (2021): 6953–6965.

[63]

V. Titone, M. C. Mistretta, L. Botta, and F. P. L. Mantia, “Investigation on the Properties and on the Photo-Oxidation Behaviour of Polypropylene/Fumed Silica Nanocomposites,” Polymers 13 (2021): 2673.

[64]

H. Zhao, H. Liu, Y. Liu, and Y. Yang, “Blends of Poly(butylene Adipate-co-Terephthalate)(PBAT) and Stereocomplex Polylactide With Improved Rheological and Mechanical Properties,” RSC Advances 10 (2020): 10482–10490.

[65]

L. Sobczak, R. W. Lang, and A. Haider, “Polypropylene Composites With Natural Fibers and Wood–General Mechanical Property Profiles,” Composites Science and Technology 72 (2012): 550–557.

[66]

B. K. Ratshoshi, S. Farzad, and J. F. Görgens, “A Techno-Economic Study of Polybutylene Adipate Terephthalate (PBAT) Production From Molasses in an Integrated Sugarcane Biorefinery,” Food and Bioproducts Processing 145 (2024): 11–20.

[67]

M. L. Broeren, L. Kuling, E. Worrell, and L. Shen, “Environmental Impact Assessment of Six Starch Plastics Focusing on Wastewater-Derived Starch and Additives,” Resources, Conservation and Recycling 127 (2017): 246–255.

[68]

G. Yadav, A. Singh, A. Dutta, et al., “Techno-Economic Analysis and Life Cycle Assessment for Catalytic Fast Pyrolysis of Mixed Plastic Waste,” Energy & Environmental Science 16 (2023): 3638–3653.

[69]

B. Ahn, S. Jo, J. Na, J. Jay Liu, Y.-J. Kim, and W. Won, “Maximizing Biomass Utilization: An Integrated Strategy for Coproducing Multiple Chemicals,” Journal of Energy Chemistry 100 (2025): 180–191.

[70]

T. Kwon, B. Ahn, K. H. Kang, W. Won, and I. Ro, “Unraveling the Role of Water in Mechanism Changes for Economically Viable Catalytic Plastic Upcycling,” Nature Communications 15 (2024): 1–15.

[71]

R. Davis, L. Tao, E. Tan, et al., “Process Design and Economics for the Conversion of Lignocellulosic Biomass to Hydrocarbons: Dilute-Acid and Enzymatic Deconstruction of Biomass to Sugars and Biological Conversion of Sugars to Hydrocarbons,” NREL/TP-5100-60223 (National Renewable Energy Lab.(NREL), 2013).

[72]

C. Gong, H. Na, H. Kim, S. Yun, H. Cho, and W. Won, “Energy-Efficient and Sustainable Design of a Hydrogen Refueling Station Utilizing the Cold Energy of Liquid Hydrogen,” ACS Sustainable Chemistry & Engineering 12 (2024): 13763–13773.

[73]

Technical Committee ISO/TC 207 EM, Environmental Management-Life Cycle Assessment-Principles and Framework (International Organization for Standardization, 2006).

[74]

ISO, Environmental Management—Life Cycle Assessment—Requirements and Guidelines, ISO 14044:2006/AMD 2:2020 (ISO, 2006).

[75]

H. Kim, B. Saremi, S. Park, et al., “Comparative Life Cycle Assessment for the Sustainable Production of Fermentation-Based L-Methionine,” Journal of Cleaner Production 462 (2024): 142700.

RIGHTS & PERMISSIONS

2025 The Author(s). SusMat published by Sichuan University and John Wiley & Sons Australia, Ltd.

PDF

4

Accesses

0

Citation

Detail

Sections
Recommended

/