基于半刚性配体的柔性超微孔金属有机骨架的合成及其尺度选择性二氧化碳捕获 |
A Flexible Ultramicroporous Metal-Organic Framework for Size-Selective Carbon Dioxide Capture Constructed from a Semirigid Ligand |
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摘要: 基于半刚性的配体3',5'-di (1H-1,2,4-triazol-1-yl)-(1,1'-biphenyl)-3,5-dicarboxylic acid (H2DTBDA)和硝酸钴制备了一个柔性超微孔的金属有机骨架{[Co (DTBDA)]·4H2O}n(FJI-H35),并对该材料的结构进行了系统的表征。FJI-H35活化以后可以发生自适应的结构转变,使得孔径从0.43 nm收缩到0.37 nm。气体吸附测试表明FJI-H35可以从氮气和甲烷中选择性捕获二氧化碳,具有很高的吸附选择性和相对低的吸附焓。突破实验进一步证实FJI-H35可以从二氧化碳/氮气(15∶85,V/V)和二氧化碳/甲烷(50∶50,V/V)混合气中高效选择性捕获二氧化碳。 |
关键词: 金属有机骨架 结构转变 二氧化碳捕获 分子筛效应 选择性吸附 |
基金项目: 国家自然科学基金(No.21871265)资助。 |
Abstract: Herein, a flexible ultramicroporous metal-organic framework {[Co(DTBDA)]·4H2O}n (FJI-H35) was prepared from a semirigid ligand 3',5'-di(1H-1,2,4-triazol-1-yl)-(1,1'-biphenyl)-3,5-dicarboxylic acid (H2DTBDA) and cobalt nitrate. After activation, FJI-H35 underwent an adaptive structural transformation, making the pore diameter shrink from 0.43 to 0.37 nm. Gas adsorption tests showed that FJI-H35 could selectively capture CO2 from N2 and CH4 with a high adsorption selectivity of 178 and a relatively low adsorption enthalpy (28.2 kJ·mol-1). Breakthrough experiments further confirmed that FJI-H35 could efficiently and selectively capture CO2 from CO2/N2 (15∶85, V/V) and CO2/CH4 (50∶50, V/V) mixtures. |
Keywords: metal-organic framework structural transformation carbon dioxide capture molecular sieve effect selective adsorption |
投稿时间:2022-09-07 修订日期:2022-11-04 |
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赵敏,吴栋,江飞龙,陈其辉,洪茂椿.基于半刚性配体的柔性超微孔金属有机骨架的合成及其尺度选择性二氧化碳捕获[J].无机化学学报,2022,38(12):2459-2468. |
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