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Origin of Surface Reconstruction in Lattice Oxygen Oxidation Mechanism Based-Transition Metal Oxides: A Spontaneous Chemical Process
Authors:Chao Wu  Dr Xiaopeng Wang  Ying Tang  Haoyin Zhong  Xin Zhang  Anqi Zou  Prof Jiliang Zhu  Dr Caozheng Diao  Dr Shibo Xi  Prof Junmin Xue  Prof Jiagang Wu
Institution:1. College of Materials Science and Engineering, Sichuan University, Chengdu, 610065 China

Institute of Sustainability for Chemical, Energy and Environment (ISCE2), Agency for Science, Technology and Research, Singapore, 627833 Singapore

These authors contributed equally to this work.

Contribution: Funding acquisition (equal), Methodology (equal), Writing - original draft (equal);2. College of Materials Science and Engineering, Sichuan University, Chengdu, 610065 China;3. Department of Materials Science and Engineering, National University of Singapore, Singapore, 117575 Singapore;4. Singapore Synchrotron Light Sources (SSLS), National University of Singapore, Singapore, 117603 Singapore;5. Institute of Sustainability for Chemical, Energy and Environment (ISCE2), Agency for Science, Technology and Research, Singapore, 627833 Singapore

Abstract:A fundamental understanding of surface reconstruction process is pivotal to developing highly efficient lattice oxygen oxidation mechanism (LOM) based electrocatalysts. Traditionally, the surface reconstruction in LOM based metal oxides is believed as an irreversible oxygen redox behavior, due to the much slower rate of OH refilling than that of oxygen vacancy formation. Here, we found that the surface reconstruction in LOM based metal oxides is a spontaneous chemical reaction process, instead of an electrochemical reaction process. During the chemical process, the lattice oxygen atoms were attacked by adsorbed water molecules, leading to the formation of hydroxide ions (OH). Subsequently, the metal-site soluble atoms leached from the oxygen-deficient surface. This work also suggests that the enhancement of surface hydrophilicity could accelerate the surface reconstruction process. Hence, such a finding could add a new layer for the understanding of surface reconstruction mechanism.
Keywords:Electrocatalysis  Metal Oxides  Oxygen Evolution Reaction  Spontaneous Chemical Process  Surface Reconstruction
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