Highly Active Manganese-Based CO2 Reduction Catalysts with Bulky NHC Ligands:
A Mechanistic Study
Posted on 2020-06-25 - 21:04
Because of the strong
σ-donor and weak π-acceptor of the N-heterocyclic carbene
(NHC), Mn-NHC complexes were found to be active for the reduction
of CO2 to CO with high activity. However, some NHC-based
manganese complexes showed low catalytic activity and required very
negative potentials. We report herein that complex fac-[MnI(bis-MesNHC)(CO)3Br] [1; bis-MesNHC = 3,3-bis(2,4,6-trimethylphenyl)-(1,1′-diimidazolin-2,2′-diylidene)methane]
could catalyze the electrochemical reduction of CO2 to
CO with high activity (TOFmax = 3180 ± 6 s–1) at a less negative potential. Due to the introduction of the bulky
Mes groups, a one-electron-reduced intermediate {[Mn0(bis-MesNHC)(CO)3]0 (2•)} was isolated as a packed “dimer” and crystallographically
characterized. Stopped-flow Fourier-transform infrared spectroscopy
was used to prove the direct reaction between doubly reduced intermediate fac-[Mn(bis-MesNHC)(CO)3]− and CO2; the tetracarbonyl Mn complex [Mn+(bis-MesNHC)(CO)4]+ ([2-CO]+) was captured, and its further reduction proposed
as the rate-limiting step.
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Yang, Yong; Zhang, Zhenyu; Chang, Xiaoyong; Zhang, Ya-Qiong; Liao, Rong-Zhen; Duan, Lele (1753). Highly Active Manganese-Based CO2 Reduction Catalysts with Bulky NHC Ligands:
A Mechanistic Study. ACS Publications. Collection. https://doi.org/10.1021/acs.inorgchem.0c01364
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AUTHORS (6)
YY
Yong Yang
ZZ
Zhenyu Zhang
XC
Xiaoyong Chang
YZ
Ya-Qiong Zhang
RL
Rong-Zhen Liao
LD
Lele Duan