Sustainable Terephthalic Polyesters with Medium/Long Methylene Sequence: Structure–Property Relationships and Closed-Loop Chemical Recycling

IF 5.1 1区化学 Q1 POLYMER SCIENCE Macromolecules Pub Date : 2024-12-23 DOI:10.1021/acs.macromol.4c01793

Junfeng Liu, Jianfei Xia, Chang Zeng, Chengtao Yu, Ying Zheng, Bao Wang, Shanshan Xu, Pengju Pan

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Abstract

Traditional short-chain terephthalic polyesters such as poly(ethylene terephthalate) (PET) are among the most produced plastics in today’s polymer industry, while their large-scale chemical recycling has been a long-standing challenge. The long-chain polyesters have shown good recyclability under mild conditions, whereas the structure–property relationships and chemical recycling performance of long-chain terephthalic polyesters are still unclear. Herein, we synthesized a series of medium/long-chain terephthalic polyesters with different methylene sequence lengths (CH₂ number in diol monomer n_CH₂ = 6, 8, 10, 12) and investigated their thermal properties, crystallization behavior, mechanical properties, and chemical recycling performance. All terephthalic polyesters show good crystallizability; their melting temperature decreases, and melting enthalpy increases gradually as n_CH₂ increases from 2 to 12. All polyesters adopt a triclinic crystal lattice while slightly different crystalline lamellar structures. The medium/long-chain terephthalic polyesters exhibit improved ductility and good melt processability, enabling them to be used as three-dimensional (3D) printing materials. In addition, the medium- and long-chain terephthalic polyesters are chemically recyclable and can depolymerize under mild conditions (e.g., 140 °C in methanol). The monomers obtained by depolymerization can be reused to synthesize again the according polyesters. This study provides new inspiration for developing sustainable high-performance polyesters with great industrial potential.

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.