Anodic Oxidation Enabled Cation Leaching for Promoting Surface Reconstruction in Water Oxidation

Yan Duan; Jun Yan Lee; Shibo Xi; Yuanmiao Sun; Jingjie Ge; Samuel Jun Hoong Ong; Yubo Chen; Shuo Dou; Fanxu Meng; Caozheng Diao; Adrian C. Fisher; Xin Wang; Günther G. Scherer; Alexis Grimaud; Zhichuan J. Xu

doi:10.1002/anie.202015060

Anodic Oxidation Enabled Cation Leaching for Promoting Surface Reconstruction in Water Oxidation

Yan Duan, Jun Yan Lee, Shibo Xi, Yuanmiao Sun, Jingjie Ge, Samuel Jun Hoong Ong, Yubo Chen, Shuo Dou, Fanxu Meng, Caozheng Diao, Adrian C. Fisher, Xin Wang, Günther G. Scherer, Alexis Grimaud^*, Zhichuan J. Xu^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

195 Citations (Scopus)

Abstract

A rational design for oxygen evolution reaction (OER) catalysts is pivotal to the overall efficiency of water electrolysis. Much work has been devoted to understanding cation leaching and surface reconstruction of very active electrocatalysts, but little on intentionally promoting the surface in a controlled fashion. We now report controllable anodic leaching of Cr in CoCr₂O₄ by activating the pristine material at high potential, which enables the transformation of inactive spinel CoCr₂O₄ into a highly active catalyst. The depletion of Cr and consumption of lattice oxygen facilitate surface defects and oxygen vacancies, exposing Co species to reconstruct into active Co oxyhydroxides differ from CoOOH. A novel mechanism with the evolution of tetrahedrally coordinated surface cation into octahedral configuration via non-concerted proton-electron transfer is proposed. This work shows the importance of controlled anodic potential in modifying the surface chemistry of electrocatalysts.

Original language	English
Pages (from-to)	7418-7425
Number of pages	8
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	13
DOIs	https://doi.org/10.1002/anie.202015060
Publication status	Published - Mar 22 2021
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2021 Wiley-VCH GmbH

ASJC Scopus Subject Areas

Catalysis
General Chemistry

Keywords

Co-based materials
controllable leaching
OER
site occupancy
surface reconstruction

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10.1002/anie.202015060

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Duan, Y., Lee, J. Y., Xi, S., Sun, Y., Ge, J., Ong, S. J. H., Chen, Y., Dou, S., Meng, F., Diao, C., Fisher, A. C., Wang, X., Scherer, G. G., Grimaud, A., & Xu, Z. J. (2021). Anodic Oxidation Enabled Cation Leaching for Promoting Surface Reconstruction in Water Oxidation. Angewandte Chemie - International Edition, 60(13), 7418-7425. https://doi.org/10.1002/anie.202015060

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abstract = "A rational design for oxygen evolution reaction (OER) catalysts is pivotal to the overall efficiency of water electrolysis. Much work has been devoted to understanding cation leaching and surface reconstruction of very active electrocatalysts, but little on intentionally promoting the surface in a controlled fashion. We now report controllable anodic leaching of Cr in CoCr2O4 by activating the pristine material at high potential, which enables the transformation of inactive spinel CoCr2O4 into a highly active catalyst. The depletion of Cr and consumption of lattice oxygen facilitate surface defects and oxygen vacancies, exposing Co species to reconstruct into active Co oxyhydroxides differ from CoOOH. A novel mechanism with the evolution of tetrahedrally coordinated surface cation into octahedral configuration via non-concerted proton-electron transfer is proposed. This work shows the importance of controlled anodic potential in modifying the surface chemistry of electrocatalysts.",

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AU - Dou, Shuo

AU - Meng, Fanxu

AU - Diao, Caozheng

AU - Fisher, Adrian C.

AU - Wang, Xin

AU - Scherer, Günther G.

AU - Grimaud, Alexis

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AB - A rational design for oxygen evolution reaction (OER) catalysts is pivotal to the overall efficiency of water electrolysis. Much work has been devoted to understanding cation leaching and surface reconstruction of very active electrocatalysts, but little on intentionally promoting the surface in a controlled fashion. We now report controllable anodic leaching of Cr in CoCr2O4 by activating the pristine material at high potential, which enables the transformation of inactive spinel CoCr2O4 into a highly active catalyst. The depletion of Cr and consumption of lattice oxygen facilitate surface defects and oxygen vacancies, exposing Co species to reconstruct into active Co oxyhydroxides differ from CoOOH. A novel mechanism with the evolution of tetrahedrally coordinated surface cation into octahedral configuration via non-concerted proton-electron transfer is proposed. This work shows the importance of controlled anodic potential in modifying the surface chemistry of electrocatalysts.

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Anodic Oxidation Enabled Cation Leaching for Promoting Surface Reconstruction in Water Oxidation

Abstract

Bibliographical note

ASJC Scopus Subject Areas

Keywords

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