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: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

243 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. © 2021 Wiley-VCH GmbH

Original language	English
Pages (from-to)	7418-7425
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	13
Online published	28 Dec 2020
DOIs	https://doi.org/10.1002/anie.202015060
Publication status	Published - 22 Mar 2021
Externally published	Yes

Funding

This work is supported by the Singapore MOE Tier 2 (MOE2018-T2-2-027) and the Singapore National Research Foundation under its Campus for Research Excellence and Technological Enterprise (CREATE) programme. The authors thank the Facility for Analysis, Characterization, Testing and Simulation (FACTS) in Nanyang Technological University for materials characterization.

Research Keywords

Co-based materials
controllable leaching
OER
site occupancy
surface reconstruction

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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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title = "Anodic Oxidation Enabled Cation Leaching for Promoting Surface Reconstruction in Water Oxidation",

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. {\textcopyright} 2021 Wiley-VCH GmbH",

keywords = "Co-based materials, controllable leaching, OER, site occupancy, surface reconstruction",

author = "Yan Duan and Lee, \{Jun Yan\} and Shibo Xi and Yuanmiao Sun and Jingjie Ge and Ong, \{Samuel Jun Hoong\} and Yubo Chen and Shuo Dou and Fanxu Meng and Caozheng Diao and Fisher, \{Adrian C.\} and Xin Wang and Scherer, \{G{\"u}nther G.\} and Alexis Grimaud and Xu, \{Zhichuan J.\}",

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doi = "10.1002/anie.202015060",

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T1 - Anodic Oxidation Enabled Cation Leaching for Promoting Surface Reconstruction in Water Oxidation

AU - Duan, Yan

AU - Lee, Jun Yan

AU - Xi, Shibo

AU - Sun, Yuanmiao

AU - Ge, Jingjie

AU - Ong, Samuel Jun Hoong

AU - Chen, Yubo

AU - Dou, Shuo

AU - Meng, Fanxu

AU - Diao, Caozheng

AU - Fisher, Adrian C.

AU - Wang, Xin

AU - Scherer, Günther G.

AU - Grimaud, Alexis

AU - Xu, Zhichuan J.

PY - 2021/3/22

Y1 - 2021/3/22

N2 - 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. © 2021 Wiley-VCH GmbH

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. © 2021 Wiley-VCH GmbH

KW - Co-based materials

KW - controllable leaching

KW - OER

KW - site occupancy

KW - surface reconstruction

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U2 - 10.1002/anie.202015060

DO - 10.1002/anie.202015060

M3 - RGC 21 - Publication in refereed journal

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SN - 1433-7851

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JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

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ER -

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

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