Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 122, Issue 37, Pages 21151-21161Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.8b05312
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Understanding of the CO2 electroreduction mechanism at the three-phase boundary (TPB) is of great importance for the development of a solid oxide electrolysis cell (SOEC). In this study, the effect of oxygen vacancy locations on the CO2 reduction reaction (CO2RR) at the TPB of Ni(111)/ samarium-doped ceria (SDC) surface was investigated using periodic density functional theory (DFT) + U calculations. It was found that interface oxygen vacancy can notably boost CO, adsorption and reduction. Based on DFT results, a microkinetic analysis was conducted to determine the rate-controlling step under various solid oxide electrolysis cell operating voltages at 1000 K. Possible charge transfer steps, including one- or two-electron charge transfer, were considered and discussed. The analysis reveals that, on Ni/SDC with noninterface oxygen vacancy, the rate-controlling step will change from the oxygen spillover step to the CO desorption step with an increase in cathode overpotential. On Ni/SDC with interface oxygen vacancy, CO desorption is the rate-controlling step regardless of the electrode overpotentials.
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