Towards Efficient Nitrite-to-Ammonia Conversion: DFT-Guided Design of Single-Atom Catalysts on Defective Boron Phosphide

Abstract

Ammonia is a promising zero-carbon energy carrier, yet conventional production via the Haber–Bosch process is energy-intensive and high in emissions. Electrochemical nitrite reduction to ammonia (NO2RR) offers a sustainable alternative but is limited by mechanistic complexity and catalyst performance. Using density functional theory, this study investigates transition-metal single atoms supported on defective boron phosphide (BP) substrates for NO2RR. Results show that V-anchored BP exhibits superior activity with a low limiting potential of –0.11 V, significantly outperforming pristine BP (–0.90 V). This enhancement is attributed to a reduced work function and favorable charge transfer. The work provides theoretical insights for designing efficient NO2RR electrocatalysts.