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	Antagonism effect of residual S triggers the dual-path mechanism for water oxidation
	Liu, Li1; Cao, Jinming1; Hu, Siqi1; Liu, Tinghui1; Xu, Can1; Fu, Wensheng1; Ma, Xinguo2; Yang, Xiaohui3
	2024-06-01
摘要	Transition metal chalcogenides (TMCs) are recognized as pre-catalysts, and their (oxy)hydroxides derived from electrochemical reconstruction are the active species in the water oxidation. However, understanding the role of the residual chalcogen in the reconstructed layer is lacking in detail, and the corresponding catalytic mechanism remains controversial. Here, taking Cu1_XCoXS as a platform, we explore the regulating effect and existence form of the residual S doped into the reconstructive layer for oxygen evolution reaction (OER), where a dual-path OER mechanism is proposed. First-principles calculations and operando 18O isotopic labeling experiments jointly reveal that the residual S in the reconstructive layer of Cu1_XCoXS can wisely balance the adsorbate evolution mechanism (AEM) and lattice oxygen oxidation mechanism (LOM) by activating lattice oxygen and optimizing the adsorption/desorption behaviors at metal active sites, rather than change the reaction mechanism from AEM to LOM. Following such a dual-path OER mechanism, Cu0.4Co0.6S-derived Cu0.4Co0.6OSH not only overcomes the restriction of linear scaling relationship in AEM, but also avoids the structural collapse caused by lattice oxygen migration in LOM, so as to greatly reduce the OER potential and improved stability. (c) 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
关键词	Electrochemical reconstruction Adsorbate evolution mechanism Lattice oxygen oxidation mechanism Oxygen evolution reaction Residual sulfur
DOI	10.1016/j.jechem.2024.02.028
发表期刊	JOURNAL OF ENERGY CHEMISTRY
ISSN	2095-4956
卷号	93页码:568-579
通讯作者	Fu, Wensheng(fuwensheng@cqnu.edu.cn) ; Ma, Xinguo(maxg@hut.edu.cn) ; Yang, Xiaohui(yangxiaohui@cigit.ac.cn)
收录类别	SCI
WOS记录号	WOS:001225748300001
语种	英语