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通过Ta掺杂调控RuO的Ru-O键和氧空位用于酸性介质中的电催化析氧反应

Regulating Ru-O Bond and Oxygen Vacancies of RuO by Ta Doping for Electrocatalytic Oxygen Evolution in Acid Media.

作者信息

Bai Jirong, Zhang Hanyu, Zhang Chunyong, Qin Hengfei, Zhou Pin, Xiang Mei, Lian Yuebin, Deng Yaoyao

机构信息

Research Center of Secondary Resources and Environment, School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou, 213022, China.

School of Chemistry and Environmental Engineering, Jiangsu University of Technology, Changzhou 213001, China.

出版信息

Inorg Chem. 2024 Oct 28;63(43):20584-20591. doi: 10.1021/acs.inorgchem.4c03227. Epub 2024 Oct 14.

Abstract

Proton exchange membrane water electrolysis (PEMWE) is considered an ideal green hydrogen production technology with promising application prospects. However, the development of efficient and stable acid electroanalytic oxygen electrocatalysts is still a challenging bottleneck. This progress is achieved by adopting a strategic approach with the introduction of the high valence metal Ta to regulate the electronic configuration of RuO by manipulating its local microenvironment to optimize the stability and activity of the electrocatalysts. The Ta-RuO catalysts are notable for their excellent electrocatalytic activity, as evidenced by an overpotential of only 202 mV at 10 mA cm, which significantly exceeds that of homemade RuO and commercial RuO. Furthermore, the Ta-RuO catalyst exhibits exceptional stability with negligible potential reduction observed after 50 h of electrolysis. Theoretical calculations show that the asymmetric configuration of Ru-O-Ta breaks the thermodynamic activity limitations usually associated with adsorption evolution, weakening the energy barrier for the formation of the OOH* formation. The strategic approach presented in this study provides an important reference for the development of a stable active center for acid water splitting.

摘要

质子交换膜水电解(PEMWE)被认为是一种具有广阔应用前景的理想绿色制氢技术。然而,开发高效稳定的酸性析氧电催化剂仍然是一个具有挑战性的瓶颈。通过采用一种策略性方法,引入高价金属Ta来调节RuO的电子构型,通过操纵其局部微环境来优化电催化剂的稳定性和活性,从而取得了这一进展。Ta-RuO催化剂以其优异的电催化活性而著称,在10 mA cm时过电位仅为202 mV,这明显超过了自制RuO和商业RuO。此外,Ta-RuO催化剂表现出卓越的稳定性,在电解50小时后观察到的电位降低可忽略不计。理论计算表明,Ru-O-Ta的不对称构型打破了通常与吸附演化相关的热力学活性限制,削弱了形成OOH*的能量屏障。本研究中提出的策略性方法为开发用于酸性水分解的稳定活性中心提供了重要参考。

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