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首页> 外文期刊>ACS applied materials & interfaces >Hydroxyl-Exchanged Nanoporous Ionic Copolymer toward Low Temperature Cycloaddition of Atmospheric Carbon Dioxide into Carbonates
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Hydroxyl-Exchanged Nanoporous Ionic Copolymer toward Low Temperature Cycloaddition of Atmospheric Carbon Dioxide into Carbonates

机译:羟基交换纳米多孔离子共聚物对大气二氧化碳向碳酸盐的低温环加成反应

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摘要

An ionic copolymer catalyst with nanopores, large surface area, high ionic density, and superior basicity was prepared via the radical copolymerization of amino-functionalized ionic liquid bromide and divinylbenzene, followed with a hydroxyl exchange for removing bromonium. Evaluated in chemical fixation of CO, with epoxides into cyclic carbonates in the absence of any solvent and basic additive, the nanoporous copolymer catalyst showed high and stable activity, superior to various control catalysts including the halogen-containing analogue. Further, high yields were obtained over a wide scope of substrates including aliphatic long carbon-chain alkyl epoxides and internal epoxide, even under atmospheric pressure and less than 100 degrees C for the majority of the substrates. On the basis of in situ Fourier transform infrared (FT-IR) investigation and density functional theory (DFT) calculation for the reaction intermediates, we proposed a possible reaction mechanism accounting for the superior catalytic activity of the ionic copolymer. The specifically prepared ionic copolymer material of this work features highly stable, noncorrosive, and sustainable catalysis and, thus, may be a new possibility for efficient chemical fixation of CO, since it is an environmentally friendly, metal -free solid catalyst.
机译:通过氨基官能化的离子液体溴化物和二乙烯基苯的自由基共聚,然后进行羟基交换去除溴,制备了具有纳米孔,大表面积,高离子密度和优异碱性的离子共聚物催化剂。在没有任何溶剂和碱性添加剂的情况下,用环氧化物将环氧化合物化学固定在环状碳酸酯中,纳米多孔共聚物催化剂表现出高而稳定的活性,优于各种控制催化剂,包括含卤素的类似物。此外,即使在大气压下且对于大多数基材而言低于100℃,在包括脂族长碳链烷基环氧化物和内部环氧化物在内的多种基材上也获得了高收率。在对反应中间体进行原位傅里叶变换红外(FT-IR)研究和密度泛函理论(DFT)计算的基础上,我们提出了一种可能的反应机理,说明了离子共聚物的优异催化活性。这项工作专门制备的离子共聚物材料具有高度稳定,无腐蚀和可持续的催化作用,因此,由于它是一种环保,无金属的固体催化剂,因此可能成为有效化学固定CO的新方法。

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