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Tuning electronic structure of RuO2 by single atom Zn and oxygen vacancies to boost oxygen evolution reaction in acidic medium
Journal of Energy Chemistry ( IF 14.0 ) Pub Date : 2023-09-22 , DOI: 10.1016/j.jechem.2023.09.010
Qing Qin , Tiantian Wang , Zijian Li , Guolin Zhang , Haeseong Jang , Liqiang Hou , Yu Wang , Min Gyu Kim , Shangguo Liu , Xien Liu

The poor stability of RuO2 electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers. To dramatically enhance the durability of RuO2 to construct activity-stability trade-off model is full of significance but challenging. Herein, a single atom Zn stabilized RuO2 with enriched oxygen vacancies (SA Zn-RuO2) is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction (OER). Compared with commercial RuO2, the enhanced Ru–O bond strength of SA Zn-RuO2 by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru, while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation. Simultaneously, the optimized surrounding electronic structure of Ru sites in SA Zn-RuO2 decreases the adsorption energies of OER intermediates to reduce the reaction barrier. As a result, the representative SA Zn-RuO2 exhibits a low overpotential of 210 mV to achieve 10 mA cm−2 and a greatly enhanced durability than commercial RuO2. This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.



中文翻译:

通过单原子Zn和氧空位调节RuO2的电子结构以促进酸性介质中的析氧反应

RuO 2电催化剂稳定性差一直是其在聚合物电解质膜电解槽中实际应用的主要障碍。大幅提高RuO 2的耐久性,构建活性与稳定性的权衡模型,具有重要意义,但也具有挑战性。在此,开发了具有富氧空位的单原子Zn稳定的RuO 2 (SA Zn-RuO 2 )作为用于酸性析氧反应(OER)的氧化铱的有前途的替代品。与商业RuO 2相比,SA Zn-RuO 2通过形成Zn-O-Ru局域结构基序而增强了Ru-O键强度,有利于稳定表面Ru,而电子从Zn单原子转移到相邻Ru原子则保护了RuO 2 。 Ru 活性位点来自过度氧化。同时,SA Zn-RuO 2中Ru位点周围电子结构的优化降低了OER中间体的吸附能,从而降低了反应势垒。结果,代表性的SA Zn-RuO 2表现出210 mV的低过电势以实现10 mA cm -2 ,并且比商业RuO 2大大提高了耐久性。这项工作通过耦合单原子掺杂和空位来权衡酸性 OER 的高活性和催化稳定性,提供了一种有前景的双工程策略。

更新日期:2023-09-22
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