Edge-Driven Nitrate Reduction Catalysis for Efficient Ammonia Production on InSe Nanoribbons

Abstract

The electrocatalytic nitrate reduction reaction (NO3RR) enables the simultaneous removal of nitrate (NO3–) pollutants and production of valuable ammonia (NH3), offering an environmentally friendly route for nitrogen fixation. Recently, p-block metals have emerged as promising electrocatalysts for this process. Edge sites in catalysts contain undercoordinated atoms that often exhibit enhanced catalytic activity. Accordingly, we systematically investigated nitrate-to-ammonia conversion at the edge sites of InSe nanoribbons using first-principles density functional theory (DFT) calculations. Nitrate adsorption and N–O bond activation arise from electron donation and back-donation between In sites and NO3–. Strong p–p orbital hybridization facilitates efficient NH3 production, with a low limiting potential of −0.10 V. In addition, competing byproduct formation and hydrogen evolution are effectively suppressed, resulting in excellent selectivity. This work demonstrates the potential of In-based selenides for tuning catalyst–intermediate interactions at edge-exposed active sites for NH3 synthesis and provides a theoretical framework to guide future experimental studies.