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Peer-reviewedCC BY-NC-ND 4.0Proceedings of the National Academy of Sciences of the United States of America

Mechanistic insight into conflicting valence fluctuation of Cu(I) photocorrosion pathways: The role of charge behaviors

  • Yi-Cheng Wang1
  • Chenyu Xu2
  • Peng-Fei Sui1
  • Renfei Feng3
  • Yi Liu2
  • Hanxiao Zhang1
  • Hongbo Zeng1
  • Xiaolei Wang1
  • Jing-Li Luo1,4
4 affiliations
  1. 1Department of Chemical and Materials Engineering, University of Alberta, Edmonton, AB T6G 1H9, Canada
  2. 2State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, People’s Republic of China
  3. 3Canadian Light Source Inc., Saskatoon, SK S7N 0X4, Canada
  4. 4College of Materials Science and Engineering, Shenzhen University, Shenzhen 518060, Guangdong, People’s Republic of China
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Abstract

Photocorrosion remains a major challenge that hinders the development of photoelectrochemical (PEC) solar fuel production. Although Cu2O is a promising photocathode material due to its suitable band structure and visible light absorption, both oxidative and reductive photocorrosion pathways have been reported, with no consensus established in the research community in the PEC system. In this work, we fabricate three Cu2O photocathodes with distinct charge transport properties to investigate the correlation between charge accumulation and photocorrosion behavior. Both oxidative and reductive photocorrosion were observed depending on the type and location of charge accumulation. Notably, we propose a refined oxidative photocorrosion mechanism in which photogenerated holes induce surface Cu2O dissolution to Cu2+, followed by coordination with adsorbed *OH to form Cu(OH)2/CuO under illumination, which is contrary to the widely assumed direct oxidation from Cu2O to CuO. This work not only provides a unified understanding of the dual photocorrosion pathways in Cu2O, but also offers a generalizable framework for understanding photo-induced degradation in metal oxide photocathodes and for guiding the design of more robust PEC systems through charge transport engineering.

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Cite

BibTeXRIS
BibTeX
@article{wang2026mechanistic,
  title = {{Mechanistic insight into conflicting valence fluctuation of Cu(I) photocorrosion pathways: The role of charge behaviors}},
  author = {Yi-Cheng Wang and Chenyu Xu and Peng-Fei Sui and Renfei Feng and Yi Liu and Hanxiao Zhang and Hongbo Zeng and Xiaolei Wang and Jing-Li Luo},
  journal = {Proceedings of the National Academy of Sciences of the United States of America},
  year = {2026},
  month = oct,
  doi = {10.1073/pnas.2611567123},
  url = {https://doi.org/10.1073/pnas.2611567123},
  note = {CC BY-NC-ND 4.0},
}
RIS
TY  - JOUR
TI  - Mechanistic insight into conflicting valence fluctuation of Cu(I) photocorrosion pathways: The role of charge behaviors
AU  - Yi-Cheng Wang
AU  - Chenyu Xu
AU  - Peng-Fei Sui
AU  - Renfei Feng
AU  - Yi Liu
AU  - Hanxiao Zhang
AU  - Hongbo Zeng
AU  - Xiaolei Wang
AU  - Jing-Li Luo
PY  - 2026
DA  - 2026/10/22
JO  - Proceedings of the National Academy of Sciences of the United States of America
DO  - 10.1073/pnas.2611567123
UR  - https://doi.org/10.1073/pnas.2611567123
AB  - Photocorrosion remains a major challenge that hinders the development of photoelectrochemical (PEC) solar fuel production. Although Cu2O is a promising photocathode material due to its suitable band structure and visible light absorption, both oxidative and reductive photocorrosion pathways have been reported, with no consensus established in the research community in the PEC system. In this work, we fabricate three Cu2O photocathodes with distinct charge transport properties to investigate the correlation between charge accumulation and photocorrosion behavior. Both oxidative and reductive photocorrosion were observed depending on the type and location of charge accumulation. Notably, we propose a refined oxidative photocorrosion mechanism in which photogenerated holes induce surface Cu2O dissolution to Cu2+, followed by coordination with adsorbed *OH to form Cu(OH)2/CuO under illumination, which is contrary to the widely assumed direct oxidation from Cu2O to CuO. This work not only provides a unified understanding of the dual photocorrosion pathways in Cu2O, but also offers a generalizable framework for understanding photo-induced degradation in metal oxide photocathodes and for guiding the design of more robust PEC systems through charge transport engineering.
SN  - 0027-8424
SN  - 1091-6490
ER  -