Rationally manipulating the in situ formed catalytically active surface of catalysts remains a tremendous challenge for a highly efficient water electrolysis. Here we present a cationic redox-tuning method to modulate in situ catalyst leaching and to redirect the dynamic surface restructuring of layered LiCoO2–xClx (x = 0, 0.1 or 0.2), for the electrochemical oxygen evolution reaction (OER). Chlorine doping lowered the potential to trigger in situ cobalt oxidation and lithium leaching, which induced the surface of LiCoO1.8Cl0.2 to transform into a self-terminated amorphous (oxy)hydroxide phase during the OER. In contrast, Cl-free LiCoO2 required higher electrochemical potentials to initiate the in situ surface reconstruction to spinel-type Li1±xCo2O4 and longer cycles to stabilize it. Surface-restructured LiCoO1.8Cl0.2 outperformed many state-of-the-art OER catalysts and demonstrated remarkable stability. This work makes a stride in modulating surface restructuring and in designing superior OER electrocatalysts via manipulating the in situ catalyst leaching.
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We acknowledge the National Research Foundation of Korea (NRF) grants funded by the Korean government (MSIT) (no. NRF-2018M1A2A2063868, no. NRF-2019R1A4A1025848, no. NRF-2019M3E6A1065102, no. 2015M3D1A1070639, and no. NRF-2018R1C1B6006854). J. Lim also acknowledges support from the Samsung Science and Technology Foundation under project no. SRFC-MA2002-04. We express thanks to the staff and crew of the Seoul National University Electron Microscopy Facility (NCIRF), Research Institute of Advanced Materials (RIAM), the Institute of Applied Physics of Seoul National University and the Seoul National University Co-operative Flexible Transformative (SOFT) Foundry. J.W. gratefully acknowledges the SNU Science Fellowship (NRF-2019R1A6A1A10073437) funded by the Korean government (MSIT).
The authors declare no competing interests.
Peer review information Nature Catalysis thanks Marcel Risch, Kirsten Winther and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Wang, J., Kim, SJ., Liu, J. et al. Redirecting dynamic surface restructuring of a layered transition metal oxide catalyst for superior water oxidation. Nat Catal 4, 212–222 (2021). https://doi.org/10.1038/s41929-021-00578-1
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