Synthesis and Functionalization of Sustainable Poly(ester-co-carbonate) from Carbon Dioxide, 1,3-Butadiene, and Biosourced Diols

IF 5.1 1区化学 Q1 POLYMER SCIENCE Macromolecules Pub Date : 2025-01-02 DOI:10.1021/acs.macromol.4c02023

Kaihao Chen, Tianwen Bai, YuLing Lin, Jun Ling, Xufeng Ni

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Abstract

Chemical synthesis of polymers from carbon dioxide (CO₂) has been attracting a continuous amount of attention. This contribution explores the copolymerization of ethylidene-6-vinyltetrahydro-2H-pyran-2-one (EVL) synthesized from CO₂ and 1,3-butadiene with various cyclic carbonates (CC) derived from CO₂ and biomass diols. Following the “scrambling polymerizations” mechanism, EVL units are incorporated into polycarbonate backbones, resulting in random poly(ester-co-carbonate) P(EVL-co-CC) with functionalizable C═C double bonds. Kinetic studies and characterizations are conducted by NMR, MALDI-ToF MS, and SEC techniques. The obtained degradable P(EVL-co-CC)s having varying topologies, CO₂ and C═C double bond contents, and glass transition temperatures are suitable for diverse applications. Modification in situ or via a postpolymerization “thiol–ene” reaction produces a copolymer with tunable tensile strength and amphiphilic and hydrophilic properties. This work presents an advancement in the utilization of CO₂ to synthesize functional poly(ester-co-carbonate)s, contributing to the development of sustainable and green polymer chemistry.

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二氧化碳、1,3-丁二烯和生物源二醇可持续聚（酯-碳酸酯）的合成与功能化

以二氧化碳（CO2）为原料化学合成聚合物的研究一直备受关注。这篇论文探讨了由二氧化碳和1,3-丁二烯合成的乙基-6-乙烯基四氢- 2h -吡喃-2- 1 （EVL）与由二氧化碳和生物质二醇衍生的各种环碳酸盐（CC）的共聚反应。根据“乱序聚合”机制，EVL单元被纳入聚碳酸酯骨架中，产生具有可官能化C = C双键的随机聚（酯-共碳酸酯）P（EVL-co- cc）。动力学研究和表征是通过核磁共振，MALDI-ToF质谱和SEC技术进行的。所得的可降解P(EVL-co-CC)s具有不同的拓扑结构、CO2和C = C双键含量以及玻璃化转变温度，适合于不同的应用。原位改性或通过聚合后的“巯基”反应产生具有可调拉伸强度和两亲性和亲水性能的共聚物。本文介绍了利用CO2合成功能性聚（酯-共碳酸酯）的研究进展，为可持续和绿色高分子化学的发展做出了贡献。

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阿拉丁

Potassium methoxide (MeOK)

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.