Статья

Understanding the sulphur-oxygen exchange process of metal sulphides prior to oxygen evolution reaction

Yang HuFrontiers Science Center for Rare Isotopes, Lanzhou University, Lanzhou, 730000, ChinaYao ZhengSchool of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005, AustraliaJing JinState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, ChinaYantao WangState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, ChinaYong PengElectron Microscopy Centre, Lanzhou University, Lanzhou, 730000, China. [email protected]Jie YinFrontiers Science Center for Rare Isotopes, Lanzhou University, Lanzhou, 730000, ChinaWei ShenState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, ChinaYichao HouState Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000, ChinaLiu ZhuElectron Microscopy Centre, Lanzhou University, Lanzhou, 730000, ChinaLi AnFrontiers Science Center for Rare Isotopes, Lanzhou University, Lanzhou, 730000, ChinaMin LuFrontiers Science Center for Rare Isotopes, Lanzhou University, Lanzhou, 730000, ChinaPinxian XiFrontiers Science Center for Rare Isotopes, Lanzhou University, Lanzhou, 730000, China. [email protected]Chun‐Hua YanBeijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China

2023en

ABI

Аннотация

Abstract Dynamic reconstruction of metal sulphides during electrocatalytic oxygen evolution reaction (OER) has hampered the acquisition of legible evidence for comprehensively understanding the phase-transition mechanism and electrocatalytic activity origin. Herein, modelling on a series of cobalt-nickel bimetallic sulphides, we for the first time establish an explicit and comprehensive picture of their dynamic phase evaluation pathway at the pre-catalytic stage before OER process. By utilizing the in-situ electrochemical transmission electron microscopy and electron energy loss spectroscopy, the lattice sulphur atoms of (NiCo)S 1.33 particles are revealed to be partially substituted by oxygen from electrolyte to form a lattice oxygen-sulphur coexisting shell surface before the generation of reconstituted active species. Such S-O exchange process is benefitted from the subtle modulation of metal-sulphur coordination form caused by the specific Ni and Co occupation. This unique oxygen-substitution behaviour produces an (NiCo)O x S 1.33-x surface to reduce the energy barrier of surface reconstruction for converting sulphides into active oxy/hydroxide derivative, therefore significantly increasing the proportion of lattice oxygen-mediated mechanism compared to the pure sulphide surface. We anticipate this direct observation can provide an explicit picture of catalysts’ structural and compositional evolution during the electrocatalytic process.

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Идентификаторы

DOI: 10.1038/s41467-023-37751-y

Цитирования и источники

Цитирований: 2Использованных источников: 0

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