调节Co-O共价性以操控机理转变，从而提高酸性水氧化反应中的活性/耐久性。
Regulating Co-O covalency to manipulate mechanistic transformation for enhancing activity/durability in acidic water oxidation.
作者信息
Zhang Jiachen, Chen Guangbo, Sun Dongmei, Tang Yawen, Xing Wei, Sun Hanjun, Feng Xinliang
机构信息
Jiangsu Key Laboratory of New Power Batteries, Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, School of Chemistry and Materials Science, Nanjing Normal University 210023 Nanjing China
Center for Advancing Electronics Dresden (CFAED) and Faculty of Chemistry and Food Chemistry, Technische Universität Dresden 01062 Dresden Germany
出版信息
Chem Sci. 2024 Oct 1;15(43):17900-11. doi: 10.1039/d4sc05547k.
Developing earth-abundant electrocatalysts with high activity and durability for acidic oxygen evolution reaction is essential for H production, yet it remains greatly challenging. Here, guided by theoretical calculations, the challenge of overcoming the balance between catalytic activity and dynamic durability for acidic OER in CoO was effectively addressed the preferential substitution of Ru for the Co (T) site of CoO. characterization and DFT calculations show that the enhanced Co-O covalency after the introduction of Ru SAs facilitates the generation of OH* species and mitigates the unstable structure transformation direct O-O coupling. The designed Ru SAs-CoO catalyst (5.16 wt% Ru) exhibits enhanced OER activity (188 mV overpotential at 10 mA cm) and durability, outperforming most reported CoO-based and Ru-based electrocatalysts in acidic media.
开发具有高活性和耐久性的用于酸性析氧反应的地球丰富型电催化剂对于制氢至关重要，但仍然极具挑战性。在此，在理论计算的指导下，通过Ru优先取代CoO的Co（T）位点，有效解决了克服CoO中酸性OER催化活性与动态耐久性之间平衡的挑战。表征和DFT计算表明，引入Ru单原子后增强的Co-O共价性促进了OH*物种的生成，并减轻了直接O-O耦合导致的不稳定结构转变。所设计的Ru单原子-CoO催化剂（5.16 wt% Ru）表现出增强的OER活性（在10 mA cm下过电位为188 mV）和耐久性，在酸性介质中优于大多数已报道的基于CoO和基于Ru的电催化剂。
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