Doping transition metal oxide spinels with metal ions represents a significant strategy for optimizing the electronic structure of electrocatalysts. Herein, a bimetallic Fe and Ru doping strategy to fine‐tune the crystal structure of CoV2O4 spinel for highly enhanced oxygen evolution reaction (OER) is presented performance. The incorporation of Fe and Ru is observed at octahedral sites within the CoV2O4 structure, effectively modulating the electronic configuration of Co. Density functional theory calculations have confirmed that Fe acts as a novel reactive site, replacing V. Additionally, the synergistic effect of Fe, Co, and Ru effectively optimizes the Gibbs free energy of the intermediate species, reduces the reaction energy barrier, and accelerates the kinetics toward OER. As expected, the best‐performing CoVFe0.5Ru0.5O4 displays a low overpotential of 240 mV (@10 mA cm−2) and a remarkably low Tafel slope of 38.9 mV dec−1, surpassing that of commercial RuO2. Moreover, it demonstrates outstanding long‐term durability lasting for 72 h. This study provides valuable insights for the design of highly active polymetallic spinel electrocatalysts for energy conversion applications.

中文翻译：

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通过阳离子竞争调节 CoV2O4 的八面体位点以实现高效的析氧反应


用金属离子掺杂过渡金属氧化物尖晶石是优化电催化剂电子结构的重要策略。在此，提出了一种双金属 Fe 和 Ru 掺杂策略，可微调 CoV2O4 尖晶石的晶体结构，以实现高度增强的析氧反应 (OER)。在 CoV2O4 结构内的八面体位点上观察到 Fe 和 Ru 的结合，有效地调节了 Co 的电子构型。密度泛函理论计算证实 Fe 可以作为一种新的反应位点，取代 V。此外，Fe 的协同效应， Co和Ru有效优化了中间体的吉布斯自由能，降低了反应能垒，加速了OER动力学。正如预期的那样，性能最佳的 CoVFe0.5Ru0.5O4 显示出 240 mV (@10 mA cm−2) 的低过电势和 38.9 mV dec−1 的极低塔菲尔斜率，超过了商业 RuO2。此外，它还表现出出色的长期耐久性，可持续 72 小时。这项研究为能量转换应用的高活性多金属尖晶石电催化剂的设计提供了宝贵的见解。