Dynamic Cation Intercalation Facilitating Chemical Oxidation of Water and Surface Stabilization During the Oxygen Evolution Reaction

IF 13 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Energy & Environmental Materials Pub Date : 2024-08-01 DOI:10.1002/eem2.12813

Huiyan Zeng, Zhongfei Liu, Jun Qi, Jiajun Chen, Yanquan Zeng, Chengyan Yang, Zhenzhong Li, Chao Wang, Long Gu, Yan Zhang, Miao Shu, Chunzhen Yang

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Abstract

A comprehensive understanding of the dynamic processes at the catalyst/electrolyte interfaces is crucial for the development of advanced electrocatalysts for the oxygen evolution reaction (OER). However, the chemical processes related to surface corrosion and catalyst degradation have not been well understood so far. In this study, we employ LiCoO₂ as a model catalyst and observe distinct OER activities and surface stabilities in different alkaline solutions. Operando X-ray diffraction (XRD) and online mass spectroscopy (OMS) measurements prove the selective intercalation of alkali cations into the layered structure of LiCoO₂ during OER. It is proposed that the dynamic cation intercalations facilitate the chemical oxidation process between highly oxidative Co species and adsorbed water molecules, triggering the so-called electrochemical-chemical reaction mechanism (EC-mechanism). The results of this study emphasize the influence of cations on OER and provide insights into new strategies for achieving both high activity and stability in high-performance OER catalysts.

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阳离子动态互螯促进水的化学氧化和氧进化反应过程中的表面稳定

全面了解催化剂/电解质界面的动态过程对于开发先进的氧进化反应（OER）电催化剂至关重要。然而，迄今为止，与表面腐蚀和催化剂降解相关的化学过程还没有得到很好的理解。在本研究中，我们以 LiCoO2 为模型催化剂，观察其在不同碱性溶液中不同的 OER 活性和表面稳定性。操作性 X 射线衍射 (XRD) 和在线质谱 (OMS) 测量证明，在 OER 过程中，碱阳离子选择性地插层到 LiCoO2 的层状结构中。研究认为，动态阳离子插层促进了高氧化性 Co 物种与吸附水分子之间的化学氧化过程，引发了所谓的电化学-化学反应机制（EC-机制）。该研究结果强调了阳离子对 OER 的影响，并为实现高性能 OER 催化剂的高活性和稳定性的新策略提供了启示。

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来源期刊

Energy & Environmental Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

17.60

自引率

6.00%

发文量

期刊介绍： Energy & Environmental Materials (EEM) is an international journal published by Zhengzhou University in collaboration with John Wiley & Sons, Inc. The journal aims to publish high quality research related to materials for energy harvesting, conversion, storage, and transport, as well as for creating a cleaner environment. EEM welcomes research work of significant general interest that has a high impact on society-relevant technological advances. The scope of the journal is intentionally broad, recognizing the complexity of issues and challenges related to energy and environmental materials. Therefore, interdisciplinary work across basic science and engineering disciplines is particularly encouraged. The areas covered by the journal include, but are not limited to, materials and composites for photovoltaics and photoelectrochemistry, bioprocessing, batteries, fuel cells, supercapacitors, clean air, and devices with multifunctionality. The readership of the journal includes chemical, physical, biological, materials, and environmental scientists and engineers from academia, industry, and policy-making.