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Effect of Cation and Anion Vacancies in Ruthenium Oxide on the Activity and Stability of Acidic Oxygen Evolution
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-11-15 , DOI: 10.1021/acscatal.4c02779
Jiao Yang, Keyu An, Zhichao Yu, Lulu Qiao, Youpeng Cao, Yujuan Zhuang, Chunfa Liu, Lun Li, Lishan Peng, Hui Pan

Electrocatalysts capable of working efficiently in acidic media for the oxygen evolution reaction (OER) are highly demanded for the large-scale utilization of proton exchange membrane (PEM) water electrolysis. This study focuses on the design and fabrication of cation/oxygen vacancy-enriched RuO2 catalysts to investigate the impact of defect types on the OER activity and stability of RuO2. The comprehensive blend of experimental and theoretical approaches elucidates that the presence of Ru vacancies in Ru1–xO2 modulates the d-band center and optimizes the adsorption energy of the OER intermediates, thereby augmenting the intrinsic OER activity. Conversely, the presence of oxygen vacancies in RuO2-x diminishes the strength of Ru–O bonds, suppressing the involvement of the lattice oxygen oxidation mechanism (LOM) and Ru dissolution, consequently enhancing long-term stability. Notably, Ru1–xO2 exhibits the lowest overpotential of 212 mV at 10 mA cmgeo–2, while RuO2–x demonstrates superior stability, enduring 400 h under 10 mA cmgeo–2, surpassing many catalysts for acidic OER in the literature. Our findings demonstrate that defect engineering is a promising strategy to achieve electrocatalysts with super catalytic performance in acid media for water electrolysis.

中文翻译:


氧化钌中阳离子和阴离子空位对酸性析氧活性和稳定性的影响



能够在析氧反应 (OER) 的酸性介质中高效工作的电催化剂对于质子交换膜 (PEM) 水电解的大规模利用非常必要。本研究侧重于阳离子/氧空位富 RuO2 催化剂的设计和制造,以研究缺陷类型对 RuO2 的 OER 活性和稳定性的影响。实验和理论方法的全面结合阐明了 Ru 1-xO2 中存在的 Ru 空位调节了 d 带中心并优化了 OER 中间体的吸附能,从而增强了内在的 OER 活性。相反,RuO2-x 中存在氧空位会降低 Ru-O 键的强度,抑制晶格氧氧化机制 (LOM) 和 Ru 溶解的参与,从而增强长期稳定性。值得注意的是,Ru 1-xO2 在 10 mA cm geo-2 处表现出 212 mV 的最低过电位,而 RuO 2-x 表现出卓越的稳定性,在 10 mA cm geo-2 下可承受 400 小时,超过了文献中的许多酸性 OER 催化剂。我们的研究结果表明,缺陷工程是一种很有前途的策略,可以在水电解的酸性介质中获得具有超级催化性能的电催化剂。
更新日期:2024-11-16
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