Electrical‐Driven Directed‐Evolution of Copper Nanowires Catalysts for Efficient Nitrate Reduction to Ammonia

Abstract

AbstractThe electrocatalytic conversion of nitrate (NO3−) to NH3 (NO3RR) at ambient conditions offers a promising alternative to the Haber–Bosch process. The pivotal factors in optimizing the proficient conversion of NO3− into NH3 include enhancing the adsorption capabilities of the intermediates on the catalyst surface and expediting the hydrogenation steps. Herein, the Cu/Cu2O/Pi NWs catalyst is designed based on the directed‐evolution strategy to achieve an efficient reduction of NO3‾. Benefiting from the synergistic effect of the OV‐enriched Cu2O phase developed during the directed‐evolution process and the pristine Cu phase, the catalyst exhibits improved adsorption performance for diverse NO3RR intermediates. Additionally, the phosphate group anchored on the catalyst's surface during the directed‐evolution process facilitates water electrolysis, thereby generating Hads on the catalyst surface and promoting the hydrogenation step of NO3RR. As a result, the Cu/Cu2O/Pi NWs catalyst shows an excellent FE for NH3 (96.6%) and super‐high NH3 yield rate of 1.2 mol h−1 gcat.−1 in 1 m KOH and 0.1 m KNO3 solution at −0.5 V versus RHE. Moreover, the catalyst's stability is enhanced by the stabilizing influence of the phosphate group on the Cu2O phase. This work highlights the promise of a directed‐evolution approach in designing catalysts for NO3RR.