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用于酸性溶液中电催化析氧的钌氧化物中镧掺杂诱导的晶格应变和电子态调制

La-Doping-Induced Lattice Strain and Electronic State Modulation in RuO for Electrocatalytic Oxygen Evolution in Acidic Solutions.

作者信息

Zhu Min, Gao Juan, Zhang Chao

机构信息

School of Mechanics and Optoelectronic Physics, Anhui University of Science and Technology, Huainan 232001, China.

School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026, China.

出版信息

Inorg Chem. 2025 Mar 10;64(9):4571-4579. doi: 10.1021/acs.inorgchem.4c05585. Epub 2025 Feb 25.

DOI:10.1021/acs.inorgchem.4c05585
PMID:39999997
Abstract

Pursuing highly active and stable Ru-based catalysts for the oxygen evolution reaction (OER) under acidic conditions is important in advancing proton exchange membrane (PEM) water electrolyzers. Unfortunately, the inadequate stability, especially under a large current density of Ru-based catalysts, still hinders its practical application. Herein, we report a La doping strategy that simultaneously enhances both OER activity and stability of RuO in acidic media. The introduction of La into RuO induces tensile strain, which effectively weakens the covalency of Ru-O bonds. This structural modification significantly inhibits Ru dissolution, thereby substantially enhancing the stability of RuO. Meanwhile, La doping modulates the electronic structure of RuO and optimizes the adsorption energy of the reaction intermediates, thereby enhancing the electrocatalytic OER activity. Notably, the optimized La-RuO electrocatalyst presents an excellent OER performance in 0.5 M HSO electrolyte, which delivers a low overpotential of 190 mV at 10 mA cm and sustains 150 h without obvious decay at 50 mA cm. More importantly, a PEM electrolyzer is constructed by using our La-RuO as the anode catalyst, which acquires 200 h stability at 1 A cm, highlighting its strong potential for practical industrial applications. This work sheds new light on designing high-performance OER catalysts toward PEM electrolyzer applications.

摘要

开发在酸性条件下用于析氧反应(OER)的高活性和稳定的钌基催化剂对于推进质子交换膜(PEM)水电解槽至关重要。不幸的是,稳定性不足,尤其是在大电流密度下钌基催化剂的稳定性不足,仍然阻碍了其实际应用。在此,我们报道了一种镧掺杂策略,该策略同时提高了RuO在酸性介质中的OER活性和稳定性。将La引入RuO会引起拉伸应变,这有效地削弱了Ru-O键的共价性。这种结构修饰显著抑制了Ru的溶解,从而大大提高了RuO的稳定性。同时,La掺杂调节了RuO的电子结构并优化了反应中间体的吸附能,从而提高了电催化OER活性。值得注意的是,优化后的La-RuO电催化剂在0.5 M HSO电解质中表现出优异的OER性能,在10 mA cm时具有190 mV的低过电位,在50 mA cm时可维持150 h无明显衰减。更重要的是,使用我们的La-RuO作为阳极催化剂构建了一个PEM电解槽,该电解槽在1 A cm时具有200 h的稳定性,突出了其在实际工业应用中的强大潜力。这项工作为设计用于PEM电解槽应用的高性能OER催化剂提供了新的思路。

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