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 NH₃production. However, the NO₃RR in NH₃production 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–O_v] (where v denotes vacancy) formed by the Lewis acidic sites O_vand 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–CuO_xcatalyst exhibited an ultralow NH₃production overpotential of only 290 mV, achieving an NH₃current density of 1.76 A cm^–2at −0.4 V vs the reversible hydrogen electrode, with an NH₃yield rate of 139.5 mg h^–1cm^–2and Faradaic efficiency of 98.9%. Due to the superior NO₃RR performance of La₉–CuO_x, a La₉–CuO_x-based Zn-NO₃^–battery achieved a remarkable power density of 80.6 mW cm^–2, with an NH₃yield rate of 21.4 mg h^–1cm^–2. This study clarifies the role of FLPs in facilitating the NO₃RR and achieves an efficient Zn-NO₃^–battery to accomplish electricity generation and NH₃production simultaneously.