Steering Co2 Electroreduction Toward Ethanol Production By A Surface-Bound Ru Polypyridyl Carbene Catalyst On N-Doped Porous Carbon

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA(2019)

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摘要
Electrochemical reduction of CO2 to multicarbon products is a significant challenge, especially for molecular complexes. We report here CO2 reduction to multicarbon products based on a Ru(II) polypyridyl carbene complex that is immobilized on an N-doped porous carbon (RuPC/NPC) electrode. The catalyst utilizes the synergistic effects of the Ru(II) polypyridyl carbene complex and the NPC interface to steer CO2 reduction toward C-2 production at low overpotentials. In 0.5 M KHCO3 /CO2 aqueous solutions, Faradaic efficiencies of 31.0 to 38.4% have been obtained for C-2 production at -0.87 to -1.07 V (vs. normal hydrogen electrode) with 21.0 to 27.5% for ethanol and 7.1 to 12.5% for acetate. Syngas is also produced with adjustable H-2/CO mole ratios of 2.0 to 2.9. The RuPC/NPC electrocatalyst maintains its activity during 3-h CO2-reduction periods.
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关键词
CO2 reduction, electrocatalysis, Ru(II) polypyridyl complex, porous carbon
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