PdNi nanosheets boost nitrate electroreduction to ammonia

Electrochemical NO3−-to-NH3 reduction reaction (NO3RR) represents an environmentally-friendly way to not only degrade NO3− in contaminated water, but also produce value-added NH3 with a high efficiency. Herein, we first demonstrate Ni-alloyed PdNi nanosheets as a high-performing NO3RR catalyst, which presents the maximum NH3 yield rate of 16.7 mg h−1 mg−1 at − 1.2 V (RHE) and the highest FE of 87.9% at − 0.6 V (RHE), together with the good catalytic durability. Combined density functional theory and molecular dynamics simulations reveal that Ni alloying can effectively modulate the electronic configuration of Pd to enable the favorable desorption of produced NH3, resulting in decreased hydrogenation energy barrier and boosted NO3RR energetics.