Supported Ionic Liquid Membranes with Dual-Site Interaction Mechanism for Efficient Separation of CO2

Supported Ionic Liquid Membranes with Dual-Site Interaction Mechanism for Efficient Separation of CO2
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具有双位点相互作用机制的负载离子液体膜可有效分离CO2

DOI:
10.1021/acssuschemeng.9b01604
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发表时间:
2019-06-17
影响因子:
8.4
通讯作者:
Hu, Xingbang
Hu, Xingbang
中科院分区:
化学1区
文献类型:
--
作者:
Zhang, Xiaomin;Xiong, Wenjie;Hu, Xingbang

文献摘要

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选择性地分离烟气中的二氧化碳符合可持续社会的标准。本论文设计并制备了一系列具有双中心相互作用中心的咪唑基酚类离子液体(ILS),通过支撑离子液膜(SILM)实现CO2与氮气的分离。测量了这些ILS的密度、粘度和CO2的溶解度。系统地考察了取代基吸电子或给电子能力对阴离子的影响、操作温度和分压对CO2透过率的影响以及CO2/N_2的理想选择性。含15wt%H2O的1-丁基-3-甲基咪唑酚([bmim][pho])在加湿条件下具有较高的渗透率(高达2540桶)和二氧化碳/氮气选择性(高达127)。根据核磁共振、红外光谱和理论计算结果,提出了二氧化碳从卡宾向酚化阴离子转移的新的促进迁移机理。这条新的途径被认为提供了一种替代方案。
Selective separation of CO2 from flue gas conforms to the criterion of sustainable society. Herein, a series of imidazolium-based phenolate ionic liquids (ILs) that have dual-site interaction centers to isolate CO2 from N2 by supported ionic liquid membranes (SILMs) is designed and prepared. Density, viscosity, and CO2 solubility in these ILs were measured. The effects of the electron-withdrawing or electron-donating ability of the substituents on the anion, the operation temperature and partial pressure on the permeability of CO2, and the ideal selectivity of CO2/N2 were investigated systematically. High permeability (up to 2540 barrers) and selectivity of CO2/N2 (up to 127) are achieved in 1-butyl-3-methylimidazolium phenolate ([bmim][PhO]) containing 15 wt % H2O under humidified condition. A novel facilitated transport mechanism, transfer of CO2 from carbene to phenolated anion, is proposed based on NMR, FT-IR, and theoretical calculation results. The new pathway is believed to offer an alternative opp...