Enhancing electroreduction activity and selectivity of N2-to-NH3 through proton-feeding adjustments in Ag@AgP2@Ni-CoP@C core-shell nanowires

The synthesis of NH3 via electrochemical N2 fixation at ambient conditions has been proposed as a promising alternative to the traditional Haber-Bosch process. However, the development of highly efficient and selective electrocatalysts remains a challenge. In this study, uniform [email protected]2 @[email protected] core-shell nanowires were synthesized using a template-engaged strategy. The merging of conductive Ag core with active AgP2 and porous carbon-coated Ni-doped CoP shells favors the mass and electron transfers, effectively lowering the activation energy toward the reduction of N2 to NH3. Density functional theory (DFT) calculations further indicates that the sandwiched AgP2 layer plays crucial roles in promoting electrocatalytic kinetics and suppressing the competitive hydrogen evolution reactions. Benefiting from these advantages, the titled catalyst achieved a high NH3 yield of 16.84 μg h−1 mg–1cat. at −0.4 V (vs. reversible hydrogen electrode, RHE) and a high Faradaic efficiency of 21.7 % at −0.3 V vs. RHE, as well as high electrochemical and structure stability.