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首页> 外文期刊>ACS Sustainable Chemistry & Engineering >Tailoring Molecular Weight of Bioderived Polycarbonates via Bifunctional Ionic Liquids Catalysts under Metal-Free Conditions
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Tailoring Molecular Weight of Bioderived Polycarbonates via Bifunctional Ionic Liquids Catalysts under Metal-Free Conditions

机译：通过双官能离子液体催化剂在无金属条件下纵向聚碳酸酯的分子量

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摘要

Synthesis of bioderived high-molecular-weight polycarbonates over metal-free catalysts is of great importance but also challenging. In this work, a series of 1-butyl-3-methylimidazolium (Bmim) ionic liquids (ILs) were prepared as catalysts for a melt polycondensation reaction of isosorbide and diphenyl carbonate. By modifying the structures of ILs' anions, the number-average molecular weight (M-n) of poly(isosorbide carbonate) (PIC) was effectively tailored. In the presence of a trace amount (0.05 mol % based on isosorbide) of bifunctional [Bmim][CH3CHOHCOO], the synthesized PIC possessed high M-n of 61,700 g/mol and a glass transition temperature of 174 degrees C, both the highest so far to the best of our knowledge. Besides, it was found that the anions with stronger electronegativity and hydrogen bond formation ability were more efficient for the formation of PIC with higher M-n. To modify the flexibility of PIC, poly(aliphatic diol-co-isosorbide carbonate)s with M-n ranging from 34,000 to 75,700 g/mol were also formulated by incorporating with various aliphatic diols. Additionally, based on the experimental results and nuclear magnetic resonance spectroscopy, a possible mechanism of cooperative nucleophilic-electrophilic activation through hydrogen bond formation and electrostatic interactions by the ILs catalyst was proposed.
机译：在无金属催化剂上合成生物化的高分子量聚碳酸酯是非常重要的，但也具有挑战性。在这项工作中，制备了一系列1-丁基-3-甲基咪唑鎓（BMIM）离子液体（ILS）作为异山梨醇和二苯基酯的熔融缩聚反应的催化剂。通过改变ILS阴离子的结构，有效地定制了聚（异山梨醇碳酸酯）（PIC）的数均分子量（M-N）。在存在双官能[Bmim] [Bmim] [Bmim] [Bmim] [Bmim] [Bmim] [Bmim] [CH3CHOHCOO]的痕量（0.05mol％）中，合成的PIC具有61,700g / mol的高Mn，玻璃化转变温度为174℃，迄今为止最高据我们所知。此外，发现具有较强的电阻性和氢键形成能力的阴离子对于具有较高M-N的PIC的形成更有效。为了改变PIC的柔韧性，通过掺入各种脂族二醇，还配制了具有M-N的PIC（脂族二醇 - 碳化物碳酸碳酸酯）S，其具有34,000至75,700g / mol。另外，基于实验结果和核磁共振光谱，提出了通过ILS催化剂的氢键形成和静电相互作用的协同亲核 - 亲电子激活的可能机制。

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    Ma Congkai; Xu Fei; Cheng Weiguo; Tan Xin; Su Qian; Zhang Suojiang;

  • 作者单位

    Chinese Acad Sci State Key Lab Multiphase Complex Syst Beijing Key Lab Ion Liquids Clean Proc Inst Proc Engn Key Lab Green Proc &

    Engn 1 North Second St Beijing 100190 Peoples R China;

    Chinese Acad Sci State Key Lab Multiphase Complex Syst Beijing Key Lab Ion Liquids Clean Proc Inst Proc Engn Key Lab Green Proc &

    Engn 1 North Second St Beijing 100190 Peoples R China;

    Chinese Acad Sci State Key Lab Multiphase Complex Syst Beijing Key Lab Ion Liquids Clean Proc Inst Proc Engn Key Lab Green Proc &

    Engn 1 North Second St Beijing 100190 Peoples R China;

    Chinese Acad Sci State Key Lab Multiphase Complex Syst Beijing Key Lab Ion Liquids Clean Proc Inst Proc Engn Key Lab Green Proc &

    Engn 1 North Second St Beijing 100190 Peoples R China;

    Chinese Acad Sci State Key Lab Multiphase Complex Syst Beijing Key Lab Ion Liquids Clean Proc Inst Proc Engn Key Lab Green Proc &

    Engn 1 North Second St Beijing 100190 Peoples R China;

    Chinese Acad Sci State Key Lab Multiphase Complex Syst Beijing Key Lab Ion Liquids Clean Proc Inst Proc Engn Key Lab Green Proc &

    Engn 1 North Second St Beijing 100190 Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学工业;
  • 关键词

    Bioderived polycarbonate; Bifunctional ionic liquids; Catalysis; Hydrogen bond;

    机译：生物化的聚碳酸酯;双官能离子液体;催化;氢键;

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