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打破用于可持续酸性水氧化的RuO催化剂的Ru-O-Ru对称性。

Breaking the Ru-O-Ru Symmetry of a RuO Catalyst for Sustainable Acidic Water Oxidation.

作者信息

Wang Yi, Lei Xue, Zhang Bo, Bai Bing, Das Pratteek, Azam Tasmia, Xiao Jianping, Wu Zhong-Shuai

机构信息

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, P. R. China.

University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2024 Jan 15;63(3):e202316903. doi: 10.1002/anie.202316903. Epub 2023 Dec 6.

DOI:10.1002/anie.202316903
PMID:37997556
Abstract

Proton exchange membrane water electrolysis is a highly promising hydrogen production technique for sustainable energy supply, however, achieving a highly active and durable catalyst for acidic water oxidation still remains a formidable challenge. Herein, we propose a local microenvironment regulation strategy for precisely tuning In-RuO /graphene (In-RuO /G) catalyst with intrinsic electrochemical activity and stability to boost acidic water oxidation. The In-RuO /G displays robust acid oxygen evolution reaction performance with a mass activity of 671 A g at 1.5 V, an overpotential of 187 mV at 10 mA cm , and long-lasting stability of 350 h at 100 mA cm , which arises from the asymmetric Ru-O-In local structure interactions. Further, it is unraveled theoretically that the asymmetric Ru-O-In structure breaks the thermodynamic activity limit of the traditional adsorption evolution mechanism which significantly weakens the formation energy barrier of OOH*, thus inducing a new rate-determining step of OH* absorption. Therefore, this strategy showcases the immense potential for constructing high-performance acidic catalysts for water electrolyzers.

摘要

质子交换膜水电解是一种极具前景的可持续能源供应制氢技术,然而,开发一种用于酸性水氧化的高活性且耐用的催化剂仍然是一项艰巨的挑战。在此,我们提出一种局部微环境调控策略,用于精确调节具有本征电化学活性和稳定性的In-RuO₂/石墨烯(In-RuO₂/G)催化剂,以促进酸性水氧化。In-RuO₂/G表现出稳健的析氧反应性能,在1.5 V时质量活性为671 A g⁻¹,在10 mA cm⁻²时过电位为187 mV,在100 mA cm⁻²下具有350 h的持久稳定性,这源于不对称的Ru-O-In局部结构相互作用。此外,理论上揭示了不对称的Ru-O-In结构打破了传统吸附演化机制的热力学活性极限,显著削弱了OOH的形成能垒,从而诱导了OH吸附的新速率决定步骤。因此,该策略展示了构建用于水电解槽的高性能酸性催化剂的巨大潜力。

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