NiO Matrix Decorated by Ru Single Atoms: Electron-Rich Ru-Induced High Activity and Selectivity toward Electrochemical N<sub>2</sub> Reduction
Xiang Huang, Jiong Wang, Changming Zhao, Li‐Yong Gan, Hu Xu
Abstract
Developing a single-atom catalyst with electron-rich active sites is a promising strategy for catalyzing the electrochemical N 2 reduction reaction (NRR). Herein, we choose NiO(001) as a model template and deposit a series of single transition metal (TM) atoms with higher formal charges to create the electron-rich active centers. Our first-principles calculations show that low-valent Ru (+2) on NiO(001) can significantly activate N 2, with its oxidation states varying from +2 to +4 throughout the catalytic cycle. The Ru/NiO(001) catalyst exhibits the best activity with a relatively low limiting potential of −0.49 V. Furthermore, under NRR operating conditions, the Ru site is primarily occupied by *N 2 rather than *H, indicating that NRR overwhelms the hydrogen evolution reaction and thus exhibits excellent selectivity. Our work highlights the potential of designing catalysts with electron-rich active sites for NRR.