A mechanistic study and computational prediction of iron, cobalt and manganese cyclopentadienone complexes for hydrogenation of carbon dioxide.
A series of cobalt and manganese cyclopentadienone complexes are proposed and examined computationally as promising catalysts for hydrogenation of CO2to formic acid with total free energies as low as 20.0 kcal mol-1in aqueous solution. Density functional theory study of the newly designed cobalt and manganese complexes and experimentally reported iron cyclopentadienone complexes reveals a stepwise hydride transfer mechanism with a water or a methanol molecule assisted proton transfer for the cleavage of H2as the rate-determining step.
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, People's Republic of China. xyang@iccas.ac.cn and University of Chinese Academy of Sciences, Beijing 100049, People's Republic of China.
Hongyu
H
Ge
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, People's Republic of China. xyang@iccas.ac.cn and University of Chinese Academy of Sciences, Beijing 100049, People's Republic of China.
Xiangyang
http://orcid.org/0000-0002-6981-7022
X
Chen
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, People's Republic of China. xyang@iccas.ac.cn.
Xinzheng
X
Yang