Design Chemical Structures of CO2-Derived Poly(cyclohexene carbonate) Copolymers to Mediate Intra-/Intermolecular Interactions with Strong Hydrogen-Bonded Donor Homopolymer

IF 5.1 1区化学 Q1 POLYMER SCIENCE Macromolecules Pub Date : 2024-12-31 DOI:10.1021/acs.macromol.4c02295

Yen-Ling Kuan, Chih-Wei Chu, Wei-Ting Du, Shiao-Wei Kuo

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Abstract

The ring opening copolymerization (ROCOP) of CO₂-based poly(carbonate-co-ester) (PC-co-PE) copolymers was synthesized by cyclohexene oxide (CHO), anhydrides (AH), and carbon dioxide (CO₂) with various contents of AH. Herein, phthalic anhydride and 1,2-cyclohexanedicarboxylic anhydride were chosen for prepared poly(cyclohexene carbonate-co-cyclohexane carboxylate) (PCHC-CHA) and poly(cyclohexene carbonate-co-phthalate) (PCHC-PA). Polycarbonate-co-polyester and polyester copolymers possess strong intramolecular H-bonding interactions on the polycarbonate (PC) or polyester (PE) segments, which was confirmed by two-dimensional Fourier transform infrared (2D FTIR) spectroscopy analyses. Compared to the PC segment, the OH units of poly(vinylphenol) (PVPh) preferred to form intermolecular hydrogen bonding with the polyester segment and possess a higher intermolecular association equilibrium constant (K_A). The trend of intermolecular H-bonded strength was PVPh/PE-CHA > PVPh/PCHC-CHA > PVPh/PCHC-PA > PVPh/PCHC binary blends. Adjusting the PC % and PE % could improve the intra-/intermolecular hydrogen bonding ratio on the PVPh/PC-co-PE binary blend, which could be observed in the change of the q value (q value generally corresponds to the H-bonding strength of the miscible polymer blend based on the Kwei equation) from DSC analyses.

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环己烯氧化物（CHO）、酸酐（AH）和二氧化碳（CO2）以不同的酸酐含量合成了二氧化碳基聚（碳酸酯-酯）（PC-co-PE）共聚物的开环共聚（ROCOP）。这里选择邻苯二甲酸酐和 1,2-环己烷二羧酸酐来制备聚（碳酸环己烯酯-共环己烷羧酸酯）（PCHC-CHA）和聚（碳酸环己烯酯-共邻苯二甲酸酯）（PCHC-PA）。聚碳酸酯-聚酯和聚酯共聚物的聚碳酸酯（PC）或聚酯（PE）部分具有很强的分子内 H 键相互作用，二维傅立叶变换红外光谱（2D FTIR）分析证实了这一点。与 PC 段相比，聚（乙烯基苯酚）（PVPh）的羟基单元更倾向于与聚酯段形成分子间氢键，并具有更高的分子间关联平衡常数（KA）。分子间氢键强度的变化趋势为 PVPh/PE-CHA > PVPh/PCHC-CHA > PVPh/PCHC-PA > PVPh/PCHC 二元混合物。调整 PC % 和 PE % 可以改善 PVPh/PC-co-PE 二元共混物的分子内/分子间氢键比例，这可以从 DSC 分析的 q 值变化中观察到（根据 Kwei 方程，q 值一般对应于混溶聚合物共混物的氢键强度）。

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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.