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Heterogeneous conversion of CO2 into cyclic carbonates at ambient pressure catalyzed by ionothermal-derived meso-macroporous hierarchical poly(ionic liquid)s

机译:离子热衍生的介孔-大分子多级聚离子液体在环境压力下将CO2非均相转化为环状碳酸酯

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摘要

Meso-macroporous hierarchical poly(ionic liquid)s (MPILs) with extremely high ionic site densities and tunable pore structures were ionothermally synthesized through the free radical self-polymerization of our newly designed rigid bis-vinylimidazolium salt monomer. The synthesis avoided the use of any templates, gave a high yield (>99%) and allowed recycling of the IL solvent; thus it is facile, atom-efficient, environmentally friendly and sustainable. The synthesized MPILs possessed distinctive features of polycation matrices, abundant halogen anions, and large surface areas. They not only presented enhanced CO2 capture, but led to breakthroughs in the heterogeneous catalytic conversion of CO2 into cyclic carbonates: (1) unprecedented high activity at atmospheric pressure and low temperature; (2) good substrate compatibility, even being active towards the extremely inert aliphatic long carbon-chain alkyl epoxides. This result renders the first occasion of a metal–solvent–additive free recyclable heterogeneous cycloaddition of CO2 at such mild conditions.
机译:通过我们新设计的刚性双乙烯基咪唑鎓盐单体的自由基自聚合,通过离子热合成了具有极高离子位点密度和可调节孔结构的介孔-宏观聚(离子液体)(MPIL)。合成过程避免使用任何模板,产率高(> 99%),并可以回收IL溶剂;因此,它是轻便,高效,环保和可持续的。合成的MPIL具有聚阳离子基质,丰富的卤素阴离子和大表面积的独特特征。它们不仅提高了CO2的捕集率,而且还导致了CO2多相催化转化为环状碳酸酯的突破:(1)在大气压和低温下前所未有的高活性; (2)良好的底物相容性,甚至对极惰性的脂肪族长碳链烷基环氧化物都有活性。这一结果使得在这种温和条件下首次出现了金属-溶剂-添加剂的可自由循环利用的二氧化碳异质环加成反应。

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