Self-separation ionic liquid catalyst for the highly effective conversion of H2S by α, (3-unsaturated carboxylate esters under mild conditions

被引:19
|
作者
Xiong, Wenjie [1 ]
Zhang, Xiaomin [1 ,2 ]
Hu, Xingbang [1 ,2 ]
Wu, Youting [1 ,2 ]
机构
[1] Nanjing Univ, Sch Chem & Chem Engn, Key Lab Mesoscop Chem MOE, Nanjing 210023, Peoples R China
[2] Nanjing Univ, Inst Green Chem & Engn, Sch Chem & Chem Engn, Suzhou 215163, Jiangsu, Peoples R China
基金
中国国家自然科学基金;
关键词
Ionic liquid; Cascade reaction; Self-separation; H 2 S conversion; Catalysis; HYDROGEN-SULFIDE; EFFICIENT; CAPTURE; SOLUBILITY; ABSORPTION;
D O I
10.1016/j.gee.2023.03.001
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The deep-processing utility of pure hydrogen sulfide (H2S) is a significant direction in natural gas chemical industry. Herein, a brand-new strategy of H2S conversion by c,,(3-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 H2S to c,,(3-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 H2S 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 H2S utilization, which will guide its application on an industrial scale. (c) 2023 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co., Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
引用
收藏
页码:1440 / 1448
页数:9
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