Artificial Frustrated Lewis Pairs for Ampere-Level Ammonia Synthesis and High-Power-Density Zinc-Nitrate Battery

Cu-based electrocatalysts exhibit superior reduction kinetics in the electrochemical nitrate reduction reaction (NO3RR) and suppress competing hydrogen evolution reaction, making NO3RR an alternative to the traditional Haber–Bosch process in NH3 production. However, the NO3RR in NH3 production involves a nine-proton and eight-electron process, and its performance is constrained by the poor capacity to generate protons. In this study, frustrated Lewis pairs (FLPs) were introduced into Cu-based catalysts to create La-doped Cu2O, in which the FLPs [Cu–O–La–Ov] (where v denotes vacancy) formed by the Lewis acidic sites Ov and Lewis basic sites O in the Cu–O–La motif served as active sites. These active sites facilitated H2O dissociation, providing ample protons for the NO3RR hydrogenation. The La9–CuOx catalyst exhibited an ultralow NH3 production overpotential of only 290 mV, achieving an NH3 current density of 1.76 A cm–2 at −0.4 V vs the reversible hydrogen electrode, with an NH3 yield rate of 139.5 mg h–1 cm–2 and Faradaic efficiency of 98.9%. Due to the superior NO3RR performance of La9–CuOx, a La9–CuOx-based Zn-NO3– battery achieved a remarkable power density of 80.6 mW cm–2, with an NH3 yield rate of 21.4 mg h–1 cm–2. This study clarifies the role of FLPs in facilitating the NO3RR and achieves an efficient Zn-NO3– battery to accomplish electricity generation and NH3 production simultaneously.