Huang Jinzhen, Sheng Hongyuan, Ross R Dominic, Han Jiecai, Wang Xianjie, Song Bo, Jin Song
Department of Chemistry, University of Wisconsin-Madison, Madison, WI, USA.
Center for Composite Materials and Structures, Harbin Institute of Technology, Harbin, China.
Nat Commun. 2021 May 24;12(1):3036. doi: 10.1038/s41467-021-23390-8.
Developing efficient and stable earth-abundant electrocatalysts for acidic oxygen evolution reaction is the bottleneck for water splitting using proton exchange membrane electrolyzers. Here, we show that nanocrystalline CeO in a CoO/CeO nanocomposite can modify the redox properties of CoO and enhances its intrinsic oxygen evolution reaction activity, and combine electrochemical and structural characterizations including kinetic isotope effect, pH- and temperature-dependence, in situ Raman and ex situ X-ray absorption spectroscopy analyses to understand the origin. The local bonding environment of CoO can be modified after the introduction of nanocrystalline CeO, which allows the Co species to be easily oxidized into catalytically active Co species, bypassing the potential-determining surface reconstruction process. CoO/CeO displays a comparable stability to CoO thus breaks the activity/stability tradeoff. This work not only establishes an efficient earth-abundant catalysts for acidic oxygen evolution reaction, but also provides strategies for designing more active catalysts for other reactions.
开发用于酸性析氧反应的高效稳定的地球丰富型电催化剂是使用质子交换膜电解槽进行水分解的瓶颈。在此，我们表明，CoO/CeO纳米复合材料中的纳米晶CeO可以改变CoO的氧化还原性质并增强其本征析氧反应活性，并结合包括动力学同位素效应、pH和温度依赖性、原位拉曼光谱和非原位X射线吸收光谱分析在内的电化学和结构表征来理解其起源。引入纳米晶CeO后，CoO的局部键合环境可以被改变，这使得Co物种能够容易地氧化成催化活性的Co物种，绕过了决定电位的表面重构过程。CoO/CeO表现出与CoO相当的稳定性，从而打破了活性/稳定性的权衡。这项工作不仅建立了一种用于酸性析氧反应的高效地球丰富型催化剂，还为设计用于其他反应的更具活性的催化剂提供了策略。
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