Affiliation:
1. State Key Laboratory of Coordination Chemistry Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical Engineering Nanjing University Nanjing 210023 P. R. China
2. Institute of Green Chemistry and Engineering Nanjing University Suzhou 215163 P. R. China
3. Jiangsu Key Laboratory of Advanced Organic Materials Nanjing University Nanjing 210023 P. R. China
Abstract
AbstractRemoval of trace impurities for natural gas purification coupled with waste gas conversion is highly desired in industry. We here report a type of porous ionic liquids (PILs) that can realize the continuous flow separation of CH4/CO2/H2S and the conversion of the captured H2S to useful products. The PILs are synthesized through a step‐by‐step surface modification of ionic liquids (ILs) onto UiO‐66‐OH nanocrystals. The introduction of free tertiary amine groups on the nanocrystal surface endows these PILs with an exceptional ability to enrich H2S from CO2 and CH4 with impressive selectivity, while the permanent pores of UiO‐66‐OH act as containers to store an exceptionally higher amount of the selectively captured H2S than the corresponding nonporous ILs. Simultaneously, the tertiary amines as dual functional moieties offer effective catalytic sites for the conversion of the H2S stored in PILs into 3‐mercaptoisobutyric acid, a key intermediate required for the synthesis of Captopril (an antihypertensive drug). Molecular dynamics, density functional theory calculations and Grand Canonical Monte Carlo simulations help understand both the mechanisms of separation and catalysis performance, confirming that the tertiary amines as well as the permanent pores in UiO‐66‐OH play vital roles in the whole procedure.
Funder
National Natural Science Foundation of China
Basic Research Program of Jiangsu Province
Fundamental Research Funds for the Central Universities