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Ionic microenvironment constructed in quaternary ammonium modified polyacrylonitrile fiber for efficient CO2 fixation
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2021-05-03 , DOI: 10.1016/j.jcou.2021.101559
Hao Geng , Chenlu Zhang , Minli Tao , Ning Ma , Wenqin Zhang

Fiber-supported quaternary ammonium catalysts for the fixation of CO2 with epoxides were designed and prepared via amination and quaternization of polyacrylonitrile fiber, followed by ion exchange with different anions. The impact of different quaternary ammonium structures and counter anions on the reaction yields was investigated. A fiber catalyst (PANT-UdAF-I) with a C11 carboxylic acid chain and iodide counter anion exhibited excellent catalytic activity in the fixation of CO2 with epoxides under mild and solvent-free conditions (80 °C, 0.1 MPa) with a very low catalyst amount (0.5 mol%), and diverse cyclic carbonates were obtained in yields between 24–99 %. PANT-UdAF-I could be conveniently separated by filtration and showed good recyclability and durability till the 4th cycle. Novel cooperative catalytic mechanism is proposed where the ionic microenvironment plays a crucial role to stabilize the ionic intermediates and lowers the activation energy of the reaction.



中文翻译:

在季铵改性聚丙烯腈纤维中构建的离子微环境可有效固定CO 2

通过聚丙烯腈纤维的胺化和季铵化,然后与不同的阴离子进行离子交换,设计并制备了用于环氧化物固定CO 2的纤维负载季铵催化剂。研究了不同季铵结构和抗衡阴离子对反应产率的影响。具有C 11羧酸链和碘化物抗衡阴离子的纤维催化剂(PAN T-UdA F-I)在温和且无溶剂的条件下(80°C,0.1 MPa)的条件下,在用环氧化物固定CO 2时表现出出色的催化活性。催化剂用量极低(0.5 mol%),并且获得了多种环状碳酸酯,收率在24–99%之间。潘T达FI可以方便地通过过滤分离,并显示出良好的可回收性和耐久性,直到第4个循环。提出了新型的协同催化机理,其中离子微环境在稳定离子中间体和降低反应活化能方面起着至关重要的作用。

更新日期:2021-05-03
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