高等学校化学学报 ›› 2022, Vol. 43 ›› Issue (8): 20220120.doi: 10.7503/cjcu20220120

• 物理化学 • 上一篇    下一篇

CO2在非质子溶剂与铁基离子液体复合体系中的吸收

崔伟1, 赵德银1, 白文轩2, 张晓东2, 余江2()   

  1. 1.中国石油化工股份有限公司西北油田分公司, 乌鲁木齐 830011
    2.北京化工大学化学工程学院, 环境催化与分离过程研究中心, 北京 100029
  • 收稿日期:2022-02-28 出版日期:2022-08-10 发布日期:2022-05-06
  • 通讯作者: 余江 E-mail:yujiang@mail.buct.edu.cn
  • 基金资助:
    国家自然科学基金(21076019);国家科技重大专项项目(2016ZX05017-004);国家“八六三”计划项目(2007AA06Z115)

CO2 Absorption in Composite of Aprotic Solvent and Iron-based Ionic Liquid

CUI Wei1, ZHAO Deyin1, BAI Wenxuan2, ZHANG Xiaodong2, YU Jiang2()   

  1. 1.Sinopec Northwest Oil Field Company,Urumqi 830011,China
    2.Research Center of Environmental Catalysis & Separation Process,School of Chemical Engineering,Beijing University of Chemical and Technology,Beijing 100029,China
  • Received:2022-02-28 Online:2022-08-10 Published:2022-05-06
  • Contact: YU Jiang E-mail:yujiang@mail.buct.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(21076019);the National Science and Technology Major Project, China(2016ZX05017-004);the National High-tech Research and Development Program of China(2007AA06Z115)

摘要:

选用非质子型有机溶剂聚乙二醇二甲醚(NHD)与N, N-二甲基乙酰胺(DMAC), 分别与BmimFeCl4复配, 构建了BmimFeCl4/NHD和BmimFeCl4/DMAC复合铁基离子液体体系. 考察了温度、 BmimFeCl4/溶剂的质量 比以及压力对CO2在复合铁基离子液体体系中溶解行为的影响. 结果表明, 高压低温的吸收条件更利于CO2 的溶解, 当BmimFeCl4/DMAC质量比为7∶3时, CO2在BmimFeCl4/DMAC复合体系中的亨利系数为0.9181 MPa·L·mol-1, 低于同等条件下BmimFeCl4/NHD体系的亨利系数. 在常压、 363.2 K条件下进行再生, 经5次循环后, CO2在BmimFeCl4/NHD和BmimFeCl4/DMAC中的溶解度分别为初次吸收量的92.53%和99.04%. 傅里叶变换红外光谱(FTIR)结果表明, 铁基离子液体复配体系吸收CO2为物理吸收过程. 密度泛函理论(DFT)计算与IRI分析的结果表明, 在复配DMAC的体系中, CO2更倾向与阳离子和溶剂分子作用, 而在复配NHD的体系中, CO2则更容易与阴离子和溶剂分子作用.

关键词: 铁基离子液体, 二氧化碳, 亨利系数, 吸收, 非质子溶剂

Abstract:

Two kinds of aprotic solvents, polyethylene glycol dimethyl ether(NHD) and NN-dimethylacetamide (DMAC), which have excellent desulphurization and decarbonization ability, were selected to construct composite of BmimFeCl4 and solvent as novel decarbonization agents. The effects of temperature, mass ratio of BmimFeCl4/solvent and pressure on CO2 solubility were investigated. The results show that high pressure and low temperature are more conducive to the dissolution of CO2. The Henry coefficient of BmimFeCl4/DMAC(7∶3) with 0.9181 MPa·L·mol-1 at 298.2 K, is lower than BmimFeCl4/NHD under the same conditions, indicating that the former has a larger absorption capacity for carbon dioxide. Fourier transform infrared spectroscopy(FTIR) spectra show that the absorptions of carbon dioxide by the two composites depends on physical absorption between CO2 molecule and the functional groups of BmimFeCl4 before and after CO2 absorption. After five absorption-regeneration cycles of CO2 with the two kinds of the iron-based ionic liquid composites, the amounts of CO2 absorption reached 92.53% and 99.04% of the first absorption for BmimFeCl4/NHD and BmimFeCl4/DMAC, respectively. density functional theory(DFT) calculations and IRI analyses show that CO2 is more likely to interact with [Bmim]+ cations and DMAC molecules in BmimFeCl4/DMAC, nevertheless, in BmimFeCl4/NHD, CO2 is more likely to interact with [FeCl4- anions and NHD molecules.

Key words: Iron-based ionic liquid, Carbon dioxide, Henry coefficient, Absorption, Aprotic solvent

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