journal article·2023-01Open access

Reconstruction of Thiospinel to Active Sites and Spin Channels for Water Oxidation

Tianze Wu, Yuanmiao Sun, Xiao Ren, Jiarui Wang, Jiajia Song, Yangdan Pan, Yongbiao Mu, Jianshuo Zhang, Qiuzhen Cheng, Guoyu Xian, Shibo Xi, Chengmin Shen, Hong‐Jun Gao, Adrian C. Fisher, Matthew P. Sherburne, Yonghua Du, Joel W. Ager, Jose Gracia, Haitao Yang, Lin Zeng, Zhichuan J. Xu

Advanced Materials· Volume 35· Issue 2

Abstract

Abstract Water electrolysis is a promising technique for carbon neutral hydrogen production. A great challenge remains at developing robust and low‐cost anode catalysts. Many pre‐catalysts are found to undergo surface reconstruction to give high intrinsic activity in the oxygen evolution reaction (OER). The reconstructed oxyhydroxides on the surface are active species and most of them outperform directly synthesized oxyhydroxides. The reason for the high intrinsic activity remains to be explored. Here, a study is reported to showcase the unique reconstruction behaviors of a pre‐catalyst, thiospinel CoFe2S4, and its reconstruction chemistry for a high OER activity. The reconstruction of CoFe2S4 gives a mixture with both Fe–S component and active oxyhydroxide (Co(Fe)OxHy) because Co is more inclined to reconstruct as oxyhydroxide, while the Fe is more stable in Fe–S component in a major form of Fe3S4. The interface spin channel is demonstrated in the reconstructed CoFe2S4, which optimizes the energetics of OER steps on Co(Fe)OxHy species and facilitates the spin sensitive electron transfer to reduce the kinetic barrier of O–O coupling. The advantage is also demonstrated in a membrane electrode assembly (MEA) electrolyzer. This work introduces the feasibility of engineering the reconstruction chemistry of the precatalyst for high performance and durable MEA electrolyzers.
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Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Advanced battery technologies research · Fuel Cells and Related Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Materials Science and Engineering Nanyang Technological University 50 Nanyang Avenue Singapore 639798 Singapore

Department of Mechanical and Energy Engineering Southern University of Science and Technology Shenzhen Guangdong 518055 China

Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Science Beijing 100190 China

Institute of Sustainability for Chemicals Energy and Environment A*STAR 1 Pesek Road Singapore 627833 Singapore

Department of Chemical Engineering University of Cambridge Cambridge CB2 3RA UK

The Cambridge Centre for Advanced Research and Education in Singapore 1 CREATE Way Singapore 138602 Singapore

Department of Materials Science and Engineering University of California at Berkeley Berkeley CA 94720 USA

Berkeley Educational Alliance for Research in Singapore Ltd. 1 CREATE Way Singapore 138602 Singapore

National Synchrotron Light Source II Brookhaven National Laboratory Upton NY 11973 USA

MagnetoCat SL General Polavieja 9 3I Alicante 03012 Spain

Funding

National Research Foundation Singapore · U.S. Department of Energy · Brookhaven National Laboratory

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