P‐Modified Single‐Atom Cu Catalyst Boosting Electrocatalytic Performance of NO<sub>3</sub><sup>−</sup> Reduction to NH<sub>3</sub>
Honghai Wang, Yan‐an Yao, Jiayu Zhan, Yangting Jia, Yao Tong, Lu‐Hua Zhang, Fengshou Yu
Abstract
Abstract Electrochemical conversion of NO 3 − to NH 3 production is of great environmental significance for water pollution treatment and can artificially close the nitrogen cycle. However, direct nine protons and eight electrons transfer lead to low Faraday efficiency (FE) and yield. Herein, the single copper site immobilized on N,P co‐doped carbon substrates (Cu−N 4 /P) was prepared for efficient NO 3 − ‐to‐NH 3 conversion. Benefiting from the electronic redistribution of the Cu site induced by the introduction of the less electronegative element P, the Cu−N 4 /P catalyst exhibited a high Faraday efficiency of FE (95.89 %) for NH 3 product formation at a potential of −0.6 V vs . RHE and 100 % conversion of NO 3 − −N was achieved after 5 hours of electrolysis. Density functional theory (DFT) explains the effective operation mechanism that P doping can promote the spontaneous hydrogenation of *NO to form *NOH, thus promoting the formation of NH 3 from NO 3 − reduction reaction. The heteroatom doping strategy mentioned proposes a new approach for promoting NO 3 − ‐to‐NH 3 conversion at atomic level catalytic sites.