化学
过电位
析氧
催化作用
价(化学)
共价键
过渡金属
电子结构
钴
密度泛函理论
八面体
吸收光谱法
无机化学
结晶学
化学物理
计算化学
物理化学
电极
晶体结构
电化学
有机化学
物理
量子力学
生物化学
作者
Xiao Lin,Yucheng Huang,Zhiwei Hu,Lili Li,Jing Zhou,Qingyun Zhao,Haoliang Huang,Jian Sun,Chih‐Wen Pao,Yu‐Chung Chang,Hong‐Ji Lin,Chien‐Te Chen,Chung‐Li Dong,Jian‐Qiang Wang,Linjuan Zhang
摘要
Electronic structure modulation among multiple metal sites is key to the design of efficient catalysts. Most studies have focused on regulating 3d transition-metal active ions through other d-block metals, while few have utilized f-block metals. Herein, we report a new class of catalyst, namely, UCoO4 with alternative CoO6 and 5f-related UO6 octahedra, as a unique example of a 5f-covalent compound that exhibits enhanced electrocatalytic oxygen evolution reaction (OER) activity because of the presence of the U 5f-O 2p-Co 3d network. UCoO4 exhibits a low overpotential of 250 mV at 10 mA cm-2, surpassing other unitary cobalt-based catalysts ever reported. X-ray absorption spectroscopy revealed that the Co2+ ion in pristine UCoO4 was converted to high-valence Co3+/4+, while U6+ remained unchanged during the OER, indicating that only Co was the active site. Density functional theory calculations demonstrated that the OER activity of Co3+/4+ was synergistically enhanced by the covalent bonding of U6+-5f in the U 5f-O 2p-Co 3d network. This study opens new avenues for the realization of electronic structure manipulation via unique 5f involvement.
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