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

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

doi:10.1002/adma.202207041

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

Journal Article · Tue Oct 25 00:00:00 EDT 2022 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202207041· OSTI ID:1984408

Wu, Tianze ^[1]; Sun, Yuanmiao ^[1]; Ren, Xiao ^[1]; Wang, Jiarui ^[1]; Song, Jiajia ^[1]; Pan, Yangdan ^[2]; Mu, Yongbiao ^[2]; Zhang, Jianshuo ^[2]; Cheng, Qiuzhen ^[3]; Xian, Guoyu ^[3]; Xi, Shibo ^[4]; Shen, Chengmin ^[3]; Gao, Hong‐Jun ^[3]; Fisher, Adrian C. ^[5]; Sherburne, Matthew P. ^[6]; Du, Yonghua ^[7]; Ager, Joel W. ^[6]; Gracia, Jose ^[8]; Yang, Haitao ^[3]; Zeng, Lin ^[2] more »

Nanyang Technological Univ. (Singapore)
Southern University of Science and Technology (SUSTech), Shenzhen (China)
Chinese Academy of Sciences (CAS), Beijing (China)
Agency for Science, Technology and Research (A*STAR) (Singapore)
Univ. of Cambridge (United Kingdom); Cambridge Centre for Advanced Research and Education in Singapore (Singapore)
Univ. of California, Berkeley, CA (United States); Berkeley Educational Alliance for Research in Singapore Ltd. (Singapore)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
MagnetoCat SL (Spain)

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)O_xH_y) 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)O_xH_y 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. Finally, this work introduces the feasibility of engineering the reconstruction chemistry of the precatalyst for high performance and durable MEA electrolyzers.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1984408

Alternate ID(s):: OSTI ID: 1902426

Report Number(s):: BNL-224472-2023-JAAM

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 2 Vol. 35; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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