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Understanding the sulphur-oxygen exchange process of metal sulphides prior to oxygen evolution reaction
Nature Communications ( IF 14.7 ) Pub Date : 2023-04-07 , DOI: 10.1038/s41467-023-37751-y
Yang Hu 1, 2 , Yao Zheng 3 , Jing Jin 1 , Yantao Wang 1 , Yong Peng 4, 5 , Jie Yin 1, 2 , Wei Shen 1 , Yichao Hou 1 , Liu Zhu 4, 5 , Li An 1, 2 , Min Lu 1, 2 , Pinxian Xi 1, 2 , Chun-Hua Yan 1, 2, 6
Affiliation  

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)S1.33 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)OxS1.33-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.



中文翻译:

了解金属硫化物在析氧反应之前的硫氧交换过程

电催化析氧反应 (OER) 过程中金属硫化物的动态重构阻碍了获得全面了解相变机制和电催化活性起源的清晰证据。在此,我们对一系列钴镍双金属硫化物进行建模,首次在 OER 过程之前的预催化阶段建立了对其动态相评估途径的明确而全面的描述。利用原位电化学透射电子显微镜和电子能量损失谱,(NiCo)S 1.33的晶格硫原子在重组活性物质的产生之前,颗粒被电解质中的氧部分取代,形成晶格氧硫共存壳表面。这种 SO 交换过程得益于特定 Ni 和 Co 占据引起的金属-硫配位形式的微妙调制。这种独特的氧取代行为产生 (NiCo)O x S 1.33-x表面以降低将硫化物转化为活性氧/氢氧化物衍生物的表面重建能垒,因此与纯硫化物表面相比,显着增加了晶格氧介导机制的比例。我们预计这种直接观察可以提供电催化过程中催化剂结构和组成演变的清晰画面。

更新日期:2023-04-08
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