{"title":"la掺杂诱导的RuO2晶格应变和电子态调制在酸性溶液中电催化析氧","authors":"Min Zhu, Juan Gao* and Chao Zhang*, ","doi":"10.1021/acs.inorgchem.4c0558510.1021/acs.inorgchem.4c05585","DOIUrl":null,"url":null,"abstract":"<p >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<sub>2</sub> in acidic media. The introduction of La into RuO<sub>2</sub> 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<sub>2</sub>. Meanwhile, La doping modulates the electronic structure of RuO<sub>2</sub> and optimizes the adsorption energy of the reaction intermediates, thereby enhancing the electrocatalytic OER activity. Notably, the optimized La<sub>0.05</sub>-RuO<sub>2</sub> electrocatalyst presents an excellent OER performance in 0.5 M H<sub>2</sub>SO<sub>4</sub> electrolyte, which delivers a low overpotential of 190 mV at 10 mA cm<sup>–2</sup> and sustains 150 h without obvious decay at 50 mA cm<sup>–2</sup>. More importantly, a PEM electrolyzer is constructed by using our La<sub>0.05</sub>-RuO<sub>2</sub> as the anode catalyst, which acquires 200 h stability at 1 A cm<sup>–2</sup>, highlighting its strong potential for practical industrial applications. This work sheds new light on designing high-performance OER catalysts toward PEM electrolyzer applications.</p>","PeriodicalId":40,"journal":{"name":"Inorganic Chemistry","volume":"64 9","pages":"4571–4579 4571–4579"},"PeriodicalIF":4.7000,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"La-Doping-Induced Lattice Strain and Electronic State Modulation in RuO2 for Electrocatalytic Oxygen Evolution in Acidic Solutions\",\"authors\":\"Min Zhu, Juan Gao* and Chao Zhang*, \",\"doi\":\"10.1021/acs.inorgchem.4c0558510.1021/acs.inorgchem.4c05585\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >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<sub>2</sub> in acidic media. The introduction of La into RuO<sub>2</sub> 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<sub>2</sub>. Meanwhile, La doping modulates the electronic structure of RuO<sub>2</sub> and optimizes the adsorption energy of the reaction intermediates, thereby enhancing the electrocatalytic OER activity. Notably, the optimized La<sub>0.05</sub>-RuO<sub>2</sub> electrocatalyst presents an excellent OER performance in 0.5 M H<sub>2</sub>SO<sub>4</sub> electrolyte, which delivers a low overpotential of 190 mV at 10 mA cm<sup>–2</sup> and sustains 150 h without obvious decay at 50 mA cm<sup>–2</sup>. More importantly, a PEM electrolyzer is constructed by using our La<sub>0.05</sub>-RuO<sub>2</sub> as the anode catalyst, which acquires 200 h stability at 1 A cm<sup>–2</sup>, highlighting its strong potential for practical industrial applications. 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引用次数: 0
摘要
在酸性条件下寻求高活性和稳定的ru基析氧反应催化剂是推进质子交换膜(PEM)水电解槽的重要内容。不幸的是,钌基催化剂的稳定性不足,特别是在大电流密度下,仍然阻碍了它的实际应用。在此,我们报道了一种La掺杂策略,可以同时增强RuO2在酸性介质中的OER活性和稳定性。在RuO2中引入La引起拉伸应变,有效地削弱了Ru-O键的共价。这种结构修饰明显抑制了Ru的溶解,从而大大提高了RuO2的稳定性。同时,La掺杂调节了RuO2的电子结构,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La0.05-RuO2电催化剂在0.5 M H2SO4电解质中表现出优异的OER性能,在10 mA cm-2下可提供190 mV的低过电位,在50 mA cm-2下可维持150 h而无明显衰减。更重要的是,利用La0.05-RuO2作为阳极催化剂构建了PEM电解槽,该电解槽在1 a cm-2下获得了200 h的稳定性,突出了其在实际工业应用中的强大潜力。本研究为PEM电解槽高性能OER催化剂的设计提供了新的思路。
La-Doping-Induced Lattice Strain and Electronic State Modulation in RuO2 for Electrocatalytic Oxygen Evolution in Acidic Solutions
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 RuO2 in acidic media. The introduction of La into RuO2 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 RuO2. Meanwhile, La doping modulates the electronic structure of RuO2 and optimizes the adsorption energy of the reaction intermediates, thereby enhancing the electrocatalytic OER activity. Notably, the optimized La0.05-RuO2 electrocatalyst presents an excellent OER performance in 0.5 M H2SO4 electrolyte, which delivers a low overpotential of 190 mV at 10 mA cm–2 and sustains 150 h without obvious decay at 50 mA cm–2. More importantly, a PEM electrolyzer is constructed by using our La0.05-RuO2 as the anode catalyst, which acquires 200 h stability at 1 A cm–2, highlighting its strong potential for practical industrial applications. This work sheds new light on designing high-performance OER catalysts toward PEM electrolyzer applications.
期刊介绍:
Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.