Electrocatalytic CO2 Reduction with Half-Sandwich Cobalt Catalyst: Selectivity towards CO.
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2020
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Abstract
We present herein a Cp*Co(III)-half-sandwich catalyst system for electrocatalytic CO 2 reduction in aqueous acetonitrile solution. In addition to an electron-donating Cp* ligand (Cp* = pentamethylcyclopentadienyl), the catalyst featured a proton-responsive pyridyl-benzimidazole-based N,N-bidentate ligand. Owing to the presence of a relatively electron-rich Co center, the reduced Co(I)-state was made prone to activate the electrophilic carbon center of CO 2 . At the same time, the proton-responsive benzimidazole scaffold was susceptible to facilitate proton-transfer during the subsequent reduction of CO 2 . The above factors rendered the present catalyst active toward producing CO as the major product over the other potential 2e/2H + reduced product HCOOH, in contrast to the only known similar half-sandwich CpCo(III)-based CO 2 -reduction catalysts which produced HCOOH selectively. The system exhibited Faradaic efficiency (FE) of ~70% while the overpotential for CO production was found to be 0.78 V as determined by controlled-potential electrolysis experiment.
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pandey2020electrocatalyticchemistry
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| Authors | Pandey, Indresh Kumar;Kumar, Abhishek;Choudhury, Joyanta; |
| Journal | Chemistry, an Asian journal |
| Year | 2020 |
| DOI |
10.1002/asia.201901805
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