Synthesis of bio-based polycarbonate via one-step melt polycondensation of isosorbide and dimethyl carbonate by dual site-functionalized ionic liquid catalysts,Green Chemistry

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Synthesis of bio-based polycarbonate via one-step melt polycondensation of isosorbide and dimethyl carbonate by dual site-functionalized ionic liquid catalysts
Green Chemistry ( IF 9.3 ) Pub Date : 2020-11-19 , DOI: 10.1039/d0gc03247f
Zifeng Yang _{1,

2,

3,

4,

5} , Xue Li _{1,

2,

3,

4,

5} , Fei Xu _{1,

2,

3,

4,

5} , Weiwei Wang _{1,

2,

3,

4,

5} , Yongqing Shi _{1,

2,

3,

4,

5} , Zhencai Zhang _{1,

2,

3,

4,

5} , Wenjuan Fang _{1,

2,

3,

4,

5} , Lei Liu _{1,

2,

3,

4,

5} , Suojiang Zhang _{1,

2,

3,

4,

5}

Affiliation

The synthesis of green products using renewable bio-monomers has become a research trend with the requirement of sustainable development. In this work, we reported a green pathway to synthesize poly(isosorbide carbonate) (PIC) via one-step melt polycondensation of biomass-derived isosorbide (ISB) and CO₂-derived dimethyl carbonate (DMC) catalyzed by eco-friendly dual site-functionalized ionic liquids; a series of these catalysts were synthesized for the first time to the best of our knowledge and their effects on the molecular weight and terminal groups of PIC were systematically investigated. The results showed that the steric structure of cations and anions of catalysts could significantly influence their catalytic performance in polymer synthesis reactions. Meanwhile, it was found that the ability of catalysts to activate the reaction substrate gradually increased with decreasing steric hindrance of cations and anions. Among our exploited ionic liquid catalysts, the selectivity of carboxymethylated products was increased significantly by using bis-tetraethylammonium hydroquinone ([N₂₂₂₂]₂ [HQ]), and a PIC with a weight average molecular weight (M_w) of 53 600 along with an ISB conversion up to 99.0% was obtained. As far as we know, the catalyst of [N₂₂₂₂]₂ [HQ] was the most efficient catalyst for PIC one-step synthesis compared with the existing traditional ionic liquid catalysts. Besides, according to the detected intermediates of the reaction process and the results of various analytical means, a possible mechanism for the synergetic catalysis of cations–anions promoting the chain growth was proposed.

中文翻译：

双位官能化离子液体催化剂通过异山梨醇和碳酸二甲酯的一步熔融缩聚合成生物基聚碳酸酯

利用可再生生物单体合成绿色产品已成为可持续发展的研究趋势。在这项工作中，我们报告了通过生物质衍生的异山梨醇（ISB）和CO ₂的一步熔融缩聚反应合成聚异山梨碳酸酯（PIC）的绿色途径环保双位官能化离子液体催化衍生的碳酸二甲酯（DMC）；据我们所知，首次合成了一系列这类催化剂，并系统地研究了它们对PIC分子量和端基的影响。结果表明，阳离子和催化剂的阴离子的空间结构可以显着影响它们在聚合物合成反应中的催化性能。同时，发现随着阳离子和阴离子的空间位阻的降低，催化剂活化反应底物的能力逐渐提高。在我们开发的离子液体催化剂中，使用双四乙基对苯二酚氢醌（[N ₂₂₂₂ ] ₂[HQ]），获得具有53600的重均分子量（M _w）和高达99.0％的ISB转化率的PIC 。据我们所知，与现有的传统离子液体催化剂相比，[N ₂₂₂₂ ] ₂ [HQ]催化剂是最有效的PIC一步合成催化剂。此外，根据反应过程中所检测到的中间体和各种分析手段的结果，提出了一种可能的阳离子-阴离子协同催化促进链增长的机理。

更新日期：2020-12-09

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