Theoretical Investigation of Reverse Water Gas Shift Reaction Catalyzed by Ruthenium Halogen Carbonyl Complexes

摘要

In this paper we present theoretical study of the reverse water gas shift (RWGS) reaction catalyzed by ruthenium halogen carbonyl complexes. Three mechanisms, including hydrogen chloride, formic acid and oxidation-reduction mechanism, have been explored by density functional theory. The calculations indicate that the oxidation-reduction mechanism contributes to the TDI and TDTS in the ESM TOF calculations. Bimetallic catalysts would be likely to be more highly active than monometallic catalyst for the RWGS reaction. Among bimetallic catalysts studied, both bimetallic catalysts [Ru(mu-Cl)Cl(CO)(3)](2) and [Ru(mu-CO)Cl(CO)(3)](2) shows higher activity than [Ru(mu-Cl)(CO)(4)](2) catalyst with [Ru(mu-CO)Cl(CO)(3)](2) considering as the most efficient catalyst for RWGS reaction.