Investigation and mitigation of degradation mechanisms in Cu2O photoelectrodes for CO2 reduction to ethylene

Guiji Liu, Fan Zheng, Junrui Li, Guosong Zeng, Yifan Ye, David M. Larson, Junko Yano, Ethan J. Crumlin, Joel W. Ager, Lin-wang Wang and Francesca M. Toma ()
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Guiji Liu: Lawrence Berkeley National Laboratory
Fan Zheng: Lawrence Berkeley National Laboratory
Junrui Li: Lawrence Berkeley National Laboratory
Guosong Zeng: Lawrence Berkeley National Laboratory
Yifan Ye: Lawrence Berkeley National Laboratory
David M. Larson: Lawrence Berkeley National Laboratory
Junko Yano: Lawrence Berkeley National Laboratory
Ethan J. Crumlin: Lawrence Berkeley National Laboratory
Joel W. Ager: Lawrence Berkeley National Laboratory
Lin-wang Wang: Lawrence Berkeley National Laboratory
Francesca M. Toma: Lawrence Berkeley National Laboratory

Nature Energy, 2021, vol. 6, issue 12, 1124-1132

Abstract: Abstract The chemical transformations that occur in metal oxides under operating conditions limit their applications for artificial photosynthesis. Understanding these chemical changes is a prerequisite to achieve sustainable production of solar fuels and chemicals. Herein, we use a correlative approach to unravel how cuprous oxide (Cu2O) photoelectrodes change under reaction conditions and, consequently, provide a protection scheme to mitigate degradation. In agreement with theoretical predictions, we find that under illumination the Cu2O concurrently undergoes reduction by photoelectrons and oxidation by holes in the material at electrolyte-dependent degradation rates. These mechanistic insights led us to design a protection scheme that uses a silver catalyst to accelerate transfer of photogenerated electrons and a Z-scheme heterojunction to extract holes. The resulting photocathode exhibits a stable photocurrent for CO2 reduction with ~60% Faradaic efficiency for ethylene with a balance of hydrogen for hours, whereas bare Cu2O degrades within minutes.

Date: 2021
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DOI: 10.1038/s41560-021-00927-1

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