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首页> 外文期刊>Catalysis science & technology >Acylamido-based anion-functionalized ionic liquids for efficient synthesis of poly(isosorbide carbonate)
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Acylamido-based anion-functionalized ionic liquids for efficient synthesis of poly(isosorbide carbonate)

机译：基于酰基胺的阴离子官能化离子液体，用于有效合成聚（异氧化碳酸盐）

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摘要

Using biomass and renewable feedstocks to prepare high value-added products instead of conventional petrochemicals has received extensive attention recently. In this work, a facile and phosgene-free approach for synthesizing bio-based polycarbonate is developed via melt polycondensation of isosorbide (ISB) and dimethyl carbonate (DMC), which are both derived from renewable biomass resources and CO2. Several kinds of acylamido-based anion-functionalized ionic liquids (ILs) are prepared and used as catalysts to promote the reaction of ISB and DMC. Their catalytic performances in the transesterification stage and the polycondensation stage are evaluated. Results show that acylamido-based ILs with a low anion–cation interaction energy and a high natural population analysis atomic charges of the nitrogen atom exhibited good catalytic performance. Furthermore, by using tetrabutylphosphonium phthalimide as the catalyst, the selectivity of carboxymethylation of DMC and conversion of ISB significantly increased to 99.6% and 99.0%, respectively. Quantum chemical calculations reveal that the dramatic enhancement of endo-OH reactivity originated from the interactions between the acylamido and –OH groups. Based on the NMR data and DFT calculations, a plausible synergistic catalytic mechanism involving cation–anion is proposed. This work not only provides guidance for the design and synthesis of efficient IL catalysts, but also is applicable to exploring the industrial possibilities of developing value-added bioproducts from renewable feedstocks.
机译：最近，使用生物质和可再生原料来制备高增值产品，而不是传统的石化产品，最近受到了广泛的关注。在这项工作中，通过异糖层（ISB）和二甲基碳酸盐（DMC）开发了一种可合成生物基聚碳酸盐的便利和无磷酸化方法，这些方法均来自可再生生物量资源和CO2。制备了几种基于酰基胺的阴离子官能化离子液体（ILS），并用作促进ISB和DMC反应的催化剂。评估了他们在跨二元阶段和多偏阶段的催化性能。结果表明，基于低阴离子 - 阳离子相互作用能和高自然人口分析的基于酰基胺的IL氮原子的原子电荷表现出良好的催化性能。此外，通过使用邻苯二甲酰亚胺作为催化剂，DMC的羧甲基化的选择性和ISB转化分别显着增加到99.6％和99.0％。量子化学计算表明，内OH反应性的显着增强起源于酰基胺和–OH基团之间的相互作用。基于NMR数据和DFT计算，提出了涉及阳离子 - 氨基的合理协同催化机制。这项工作不仅为有效IL催化剂的设计和合成提供了指导，而且还适用于探索从可再生原料开发增值生物产品的工业可能性。

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