CO2 activation and carbonate intermediates: an operando AP-XPS study of CO2 electrolysis reactions on solid oxide electrochemical cells
Literature Information
Yi Yu, Baohua Mao, Aaron Geller, Rui Chang, Karen Gaskell, Zhi Liu, Bryan W. Eichhorn
Through the use of ambient pressure X-ray photoelectron spectroscopy and specially designed ceria-based solid oxide electrochemical cells, carbon dioxide (CO2) electrolysis reactions (CO2 + 2e− → CO + O2−) and carbon monoxide (CO) electro-oxidation reactions (CO + O2− → CO2 + 2e−) over cerium oxide electrodes have been investigated in the presence of 0.5 Torr CO–CO2 gas mixtures at ∼600 °C. Carbonate species (CO32−) are identified on the ceria surface as reaction intermediates. When CO2 electrolysis is promoted on ceria electrodes at +2.0 V applied bias, we observe a higher concentration of CO32− over a 400 μm-wide active region on the ceria surface, accompanied by Ce3+/Ce4+ redox changes. This increase in the CO32− steady-state concentration suggests that the process of pre-coordination of CO2 to the ceria surface to form a CO32− intermediate (CO2(g) + O2−(surface) → CO32−(surface)) precedes a rate-limiting electron transfer process involving CO32− reduction to give CO and oxide ions (CO32−(surface) + 2Ce3+ → CO(g) + 2O2−(surface) + 2Ce4+). When the applied bias is switched to −1.5 V to promote CO electro-oxidation on ceria, the surface CO32− concentration slightly decreases from the equilibrium value, suggesting that the electron transfer process is also a rate-limiting process in the reverse direction.
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