Ab Initio Study of a Tandem PdCu Catalyst Supported on Carbon Nitride Nanosheets for Nitrate-to-Ammonia Electrochemical Reduction

Electrochemical conversion of nitrate offers an efficient approach to mitigate nitrate pollution and ammonia synthesis but is still challenged by the slow kinetics and selectivity issues of active sites. Herein, by performing density functional theory (DFT) calculations, we report a double-atom catalyst of PdCu–C 7 N 6 by incorporating Pd and Cu together embedded in C 7 N 6 frameworks, which not only shows outstanding catalytic performance with a low limiting potential of 0.36 V, but also can effectively inhibit the competing hydrogen evolution reactions. The high NO 3 RR activity on PdCu–C 7 N 6 is well explained by the polarizable bond length as well as the asymmetric charge distribution of Pd–Cu dual active sites. This DFT work opens an avenue for developing highly efficient multicomponent NO 3 RR electrocatalysts.