Jie Liu, Gao Y, Fanghua Ning, Linlin Wang, Yuyu Liu
The nitrate electroreduction reaction (NO 3 RR) to ammonia (NH 3 ) is an effective method for producing ammonia and treating wastewater. However, its effectiveness is hindered by the multi‐step proton‐electron transfer mechanism and the difficulty of synergistically modulating intermediate adsorption energies. Herein, we report a wet‐chemical reduction approach to create P‐doped CoBO x electrocatalysts, which demonstrated exceptional NO 3 RR activity in neutral media. According to experimental studies, 5P‐CoBO x exhibits outstanding activity for NO 3 RR, featuring an impressive NH 3 yield rate (4.18 mg h −1 cm −2 ) and a high Faraday efficiency (96.87%) at −0.65 V versus RHE, far superior to that of CoBO x and P‐Co 3 O 4 . The exceptional performance of 5P‐CoBO x can be attributed to synergetic catalysis among Co, B, and P sites. The improved electrical structure of several active sites at Co and B sites improves nitrate adsorption, allowing for nitrate reduction to intermediate products. The P site efficiently generates *H through hydrolyzation, thereby promoting the selective conversion of the intermediate to NH 3 . In addition to demonstrating the effectiveness of synergistic electrocatalysis, this work creates new opportunities for the creation of extremely effective multisite catalysts.