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

Abstract

Cu-based electrocatalysts exhibit superior reduction kinetics in the electrochemical nitrate reduction reaction (NO 3 RR) and suppress competing hydrogen evolution reaction, making NO 3 RR an alternative to the traditional Haber–Bosch process in NH 3 production. However, the NO 3 RR in NH 3 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 Cu 2 O, in which the FLPs [Cu–O–La–O v ] (where v denotes vacancy) formed by the Lewis acidic sites O v and Lewis basic sites O in the Cu–O–La motif served as active sites. These active sites facilitated H 2 O dissociation, providing ample protons for the NO 3 RR hydrogenation. The La 9 –CuO x catalyst exhibited an ultralow NH 3 production overpotential of only 290 mV, achieving an NH 3 current density of 1.76 A cm –2 at −0.4 V vs the reversible hydrogen electrode, with an NH 3 yield rate of 139.5 mg h –1 cm –2 and Faradaic efficiency of 98.9%. Due to the superior NO 3 RR performance of La 9 –CuO x, a La 9 –CuO x -based Zn-NO 3 – battery achieved a remarkable power density of 80.6 mW cm –2, with an NH 3 yield rate of 21.4 mg h –1 cm –2 . This study clarifies the role of FLPs in facilitating the NO 3 RR and achieves an efficient Zn-NO 3 – battery to accomplish electricity generation and NH 3 production simultaneously.

The authors' abstract, as published at the source. Journal of the American Chemical Society, 2025 · DOI ↗