Single‐Atom Bi Alloyed Pd Metallene for Nitrate Electroreduction to Ammonia
Kai Chen, Ziyu Ma, Xingchuan Li, Jilong Kang, Dongwei Ma, Ke Chu
Abstract
Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) holds a great promise for attaining both NH 3 electrosynthesis and wastewater purification. Herein, single‐atom Bi alloyed Pd metallene (Bi 1 Pd) is reported as a highly effective NO 3 RR catalyst, showing a near 100% NH 3 ‐Faradaic efficiency with the corresponding NH 3 yield of 33.8 mg h −1 cm −2 at −0.6 V versus RHE, surpassing those of almost all ever reported NO 3 RR catalysts. In‐depth theoretical and operando spectroscopic investigations unveil that single‐atom Bi electronically couples with its neighboring Pd atoms to synergistically activate NO 3 − and destabilize *NO on Bi 1 Pd, leading to the reduced energy barrier of the potential‐determining step (*NO→*NOH) and enhanced protonation energetics of NO 3 − ‐to‐NH 3 pathway.