Abstract
Electrochemical reduction of nitrate to ammonia (eNO3RR) is proposed as a sustainable solution for high-rate ammonia synthesis under ambient conditions. The complex, multistep eNO3RR mechanism necessitates the use of a catalyst for the complete conversion of nitrate to ammonia. Our research focuses on developing a novel Pd-PdO doped in a reduced graphene oxide (rGO) composite catalyst synthesized via a laser-assisted one-step technique. This catalyst demonstrates dual functionality: palladium (Pd) boosts hydrogen adsorption, while its oxide (PdO) demonstrates considerable nitrogen adsorption affinity and exhibits a maximum ammonia yield of 5456.4 ± 453.4 μg/h/cm2 at -0.6 V vs reversible hydrogen electrode (RHE), with significant yields for nitrite and hydroxylamine under ambient conditions in a nitrate-containing alkaline electrolyte. At a lower potential of -0.1 V, the catalyst exhibited a minimal hydrogen evolution reaction of 3.1 ± 2.2% while achieving high ammonia selectivity (74.9 ± 4.4%), with the balance for nitrite and hydroxylamine. Additionally, the catalyst's stability and activity can be regenerated through the electrooxidation of Pd.