Probing the NO electroreduction mechanism in single phosphorus atom decorated defective MXene: A first-principles calculations

Abstract

The efficient electrocatalytic NO reduction (ENOR) to NH₃ is a critical reaction, offering significant economic and environmental benefits. The defective MXene embedded with the single phosphorus atom at the O vacancy were investigated for ENOR using first principles calculations. The results indicate that P@MXene can efficiently activate NO via N-end mode, with P@Cr₂CO₂ and P@MoCO₂ exhibiting particularly low limiting potentials of −0.27 V for NO conversion to NH₃. The origin of the catalytic activity of metal-free SACs is elucidated through the “reversal-activation” mechanism. After a rigorous four−stage screening process, stable P@Cr₂CO₂ exhibits high performance toward NH₃ synthesis.