Self-separation ionic liquid catalyst for the highly effective conversion of H_(2)S by α,β-unsaturated carboxylate esters under mild conditions  

作　　者：Wenjie Xiong Xiaomin Zhang Xingbang Hu Youting Wu 

机构地区：[1]Key Laboratory of Mesoscopic Chemistry of MOE,School of Chemistry and Chemical Engineering,Nanjing University,Nanjing,210023,China [2]The Institute of Green Chemistry and Engineering,School of Chemistry and Chemical Engineering,Nanjing University,Suzhou,Jiangsu,215163,China

出　　处：《Green Energy & Environment》2024年第9期1440-1448,共9页绿色能源与环境（英文版）

基　　金：sponsored by the National Natural Science Foundation of China (Nos. 22208140 and 22078145)。

摘　　要：The deep-processing utility of pure hydrogen sulfide (H_(2)S) is a significant direction in natural gas chemical industry.Herein,a brand-new strategy of H_(2)S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids (ILs) as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third component.It can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H_(2)S to a,β-unsaturated carboxylate esters.Also,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were investigated.Furthermore,the proposed interaction mechanism of H_(2)S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical calculation.The approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically benign.High-efficiency reaction activity can still be maintained after ten cycles of the catalyst.Therefore,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and cost-effective.It is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H_(2)S utilization,which will guide its application on an industrial scale.

关 键 词：Ionic liquid Cascade reaction Self-separation H_(2)S conversion Catalysis 

分 类 号：TQ426[化学工程] X701[环境科学与工程—环境工程]