期刊
DALTON TRANSACTIONS
卷 49, 期 3, 页码 891-900出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9dt04150h
关键词
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资金
- National Science Foundation [CHE-1800400]
[Mn(bpy)(CO)(3)Br] is recognized as a benchmark electrocatalyst for CO2 reduction to CO, with the doubly reduced [Mn(bpy)(CO)(3)](-) proposed to be the active species in the catalytic mechanism. The reaction of this intermediate with CO2 and two protons is expected to produce the tetracarbonyl cation, [Mn(bpy)(CO)(4)](+), thereby closing the catalytic cycle. However, this species has not been experimentally observed. In this study, [Mn(bpy)(CO)(4)][SbF6] (1) was directly synthesized and found to be an efficient electrocatalyst for the reduction of CO2 to CO in the presence of H2O. Complex 1 was characterized using X-ray crystallography as well as IR and UV-Vis spectroscopy. The redox activity of 1 was determined using cyclic voltammetry and compared with that of benchmark manganese complexes, e.g., [Mn(bpy)(CO)(3)Br] (2) and [Mn(bpy)(CO)(3)(MeCN)][PF6] (3). Infrared spectroscopic analyses indicated that CO dissociation occurs after a single-electron reduction of complex 1, producing a [Mn(bpy)(CO)(3)(MeCN)](+) species. Complex 1 was experimentally verified as both a precatalyst and an on-cycle intermediate in homogeneous Mn-based electrocatalytic CO2 reduction.
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