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

Autor: 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
Přispěvatelé: School of Materials Science and Engineering
Rok vydání: 2022
Předmět:
Zdroj: Advanced materials (Deerfield Beach, Fla.).
ISSN: 1521-4095
Popis: 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 CoFe2 S4 , and its reconstruction chemistry for a high OER activity. The reconstruction of CoFe2 S4 gives a mixture with both Fe-S component and active oxyhydroxide (Co(Fe)Ox Hy ) because Co is more inclined to reconstruct as oxyhydroxide, while the Fe is more stable in Fe-S component in a major form of Fe3 S4 . The interface spin channel is demonstrated in the reconstructed CoFe2 S4 , which optimizes the energetics of OER steps on Co(Fe)Ox Hy 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. Ministry of Education (MOE) National Research Foundation (NRF) Submitted/Accepted version The authors thank the support from the Singapore Ministry of Education Tier 2 Grant (MOE-T2EP10220-0001) and the Singapore National Research Foundation under its Campus for Research Excellence and Technological Enterprise (CREATE) programme, through the Cambridge Center for Carbon Reduction in Chemical Technology (C4T) and eCO2EP programmes.
Databáze: OpenAIRE