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

Wu, Tianze1; Sun, Yuanmiao1; Ren, Xiao1; Wang, Jiarui1; Song, Jiajia1; Pan, Yangdan2; Mu, Yongbiao2; Zhang, Jianshuo2; Cheng, Qiuzhen3,4; Xian, Guoyu3,4; Xi, Shibo5; Shen, Chengmin3,4; Gao, Hong-Jun3,4; Fisher, Adrian C.6,7; Sherburne, Matthew P.8,9; Du, Yonghua10; Ager, Joel W.8,9; Gracia, Jose11; Yang, Haitao3,4; Zeng, Lin2; Xu, Zhichuan J.1

2022-12-01

10.1002/adma.202207041

ADVANCED MATERIALS   Impact Factor & Quartile

0935-9648

1521-4095

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.

electrochemical reconstruction membrane electrode assembly spin sulfides water oxidation

SCI

English

NI Journal Papers

Corresponding

Singapore Ministry of Education Tier 2 Grant[MOE-T2EP10220-0001] ; DOE Office of Science by Brookhaven National Laboratory[DE-SC0012704]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000896590200001

WILEY-V C H VERLAG GMBH

MATERIALS SCIENCE

Web of Science

1.Nanyang Technol Univ, Sch Mat Sci & Engn, 50 Nanyang Ave, Singapore 639798, Singapore
2.Southern Univ Sci & Technol, Dept Mech & Energy Engn, Shenzhen 518055, Guangdong, Peoples R China
3.Chinese Acad Sci, Beijing Natl Lab Condensed Matter Phys, Beijing 100190, Peoples R China
4.Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China
5.ASTAR, Inst Sustainabil Chem Energy & Environm, 1 Pesek Rd, Singapore 627833, Singapore
6.Univ Cambridge, Dept Chem Engn, Cambridge CB2 3RA, England
7.Cambridge Ctr Adv Res & Educ Singapore, 1 CREATE Way, Singapore 138602, Singapore
8.Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA
9.Berkeley Educ Alliance Res Singapore Ltd, 1 CREATE Way, Singapore 138602, Singapore
10.Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY 11973 USA
11.MagnetoCat SL, Gen Polavieja 9 3I, Alicante 03012, Spain

Wu, Tianze,Sun, Yuanmiao,Ren, Xiao,et al. Reconstruction of Thiospinel to Active Sites and Spin Channels for Water Oxidation[J]. ADVANCED MATERIALS,2022.

Wu, Tianze.,Sun, Yuanmiao.,Ren, Xiao.,Wang, Jiarui.,Song, Jiajia.,...&Xu, Zhichuan J..(2022).Reconstruction of Thiospinel to Active Sites and Spin Channels for Water Oxidation.ADVANCED MATERIALS.

Wu, Tianze,et al."Reconstruction of Thiospinel to Active Sites and Spin Channels for Water Oxidation".ADVANCED MATERIALS (2022).