Atomically isolated and unsaturated Sb sites created on Sb2S3 for highly selective NO electroreduction to NH3

Abstract

Sb₂S₃ comprising an atomically isolated and unsaturated Sb (Sb_AIU) site is demonstrated as a fascinating catalyst for highly selective electrochemical NO-to-NH₃ conversion (NORR). Theoretical calculations reveal the crucial function of Sb_AIU sites to favor the adsorption and activation of NO, accelerate the protonation energetics of the NO-to-NH₃ pathway and impede the coverage of H₂O/H species, thereby boosting both NORR activity and selectivity. Consequently, the developed Sb_AIU-rich Sb₂S₃ catalyst exhibits an excellent NO-to-NH₃ faradaic efficiency of 93.7% and a high NH₃ yield rate of 168.6 μmol h⁻¹ cm⁻², representing the highest NORR selectivity among all reported NORR catalysts.