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

作者：Shaoce Zhang, Dong Chen, Rong Zhang, Xinru Yang, Xintao Ma, Chuan Li, Huilin Cui, Zhiquan Wei, Yiqiao Wang, Peng Chen, Xun Guo, Shixun Wang, Johnny C. Ho, Ying Guo, Chunyi Zhi · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c11084 · 被引用次数：27 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、CO2 Reduction Techniques and Catalysts、Advanced Photocatalysis Techniques

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.