4.8 Article

Steering CO2 electroreduction toward ethanol production by a surface-bound Ru polypyridyl carbene catalyst on N-doped porous carbon

出版社

NATL ACAD SCIENCES
DOI: 10.1073/pnas.1907740116

关键词

CO2 reduction; electrocatalysis; Ru(II) polypyridyl complex; porous carbon

资金

  1. US Department of Energy, Office of Basic Energy Sciences [DE-SC0015739]
  2. National Natural Science Foundation of China [21707016, 51708085]
  3. State Scholarship Fund from the China Scholarship Council
  4. U.S. Department of Energy (DOE) [DE-SC0015739] Funding Source: U.S. Department of Energy (DOE)

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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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