Journal
GREEN ENERGY & ENVIRONMENT
Volume 8, Issue 1, Pages 296-307Publisher
KEAI PUBLISHING LTD
DOI: 10.1016/j.gee.2021.04.008
Keywords
CO2 transformation; Carbonylation; Ionic liquids; Synergistic effect; Theoretical analysis
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The Ru-catalyzed carbonylation of alkenes using CO2 and imidazole chlorides as the promotor was studied through computational and experimental analysis. The efficiency of hydroesterification and hydroformylation was found to be correlated with the conversion rate of CO2 to CO, which was facilitated by chloride additives, particularly BmimCl and B3MimCl > BmmimCl > LiCl. In the hydroesterification reaction with MeOH, BmimCl with C-H functionality at the C2 site of the cation acted as a hydrogen donor medium, with the anion and cation working synergistically. The insertion of CO2 into the formed Ru-H bond with the assistance of chloride anion produced the Ru-COOH species, accelerating the activation of CO2.
The Ru-catalyzed carbonylation of alkenes with CO2 as a C1 surrogate and imidazole chlorides as the promotor is investigated by a combination of computational and experimental study. The conversion rate of CO2 to CO is positively correlated with the efficiency of both hydroesterification and hydroformylation, which is found facilitated in the presence of chloride additives with a decreasing order of BmimCl similar to B3MimCl > BmmimCl similar to LiCl. Taking the hydroesterification with MeOH as a representative example, BmimCl bearing C-H functionality at the C2 site of the cation assists the reduction of CO2 to CO as a hydrogen donor medium, with the anion and cation acting in a synergistic fashion. Subsequent insertion of CO2 into the formed Ru-H bond with the assistance of chloride anion produces the Ru-COOH species, which ultimately accelerates the activation of CO2. (c) 2021 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communi-cations Co., Ltd.
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