Two-Dimensional MOF Constructed by a Binuclear-Copper Motif for High-Performance Electrocatalytic NO Reduction to NH<sub>3</sub>
Rong Luo, Bao-Jing Li, Zhanpeng Wang, Mingguang Chen, Gui‐Lin Zhuang, Quan Li, Jia‐Ping Tong, Wentai Wang, Yuhua Fan, Feng Shao
Abstract
High Resolution Image Download MS PowerPoint Slide Ambient electrochemical NO reduction presents a dual solution for sustainable NO reduction and NH 3 synthesis. However, their complex kinetics and energy demands necessitate high-performance electrocatalysts to ensure effective and selective process outcomes. Herein, we report that a two-dimensional Cu-based metal–organic framework (MOF), {[Cu(HL)]·H 2 O} n, ( Cu-OUC, H 3 L = 5-(2′-carboxylphenoxy)isophthalic acid) acts as a stable electrocatalyst with high efficiency for NO-to-NH 3 conversion. Electrochemical experimental studies showed that in 0.1 M K 2 SO 4 solution, the as-prepared Cu-OUC achieved a peak Faradaic efficiency of 96.91% and a notable NH 3 yield as high as 3415.82 μg h –1 mg –1 . The Zn–NO battery in aqueous solution can produce electricity possessing a power density of 2.04 mW cm –2 while simultaneously achieving an NH 3 yield of 616.92 μg h –1 mg –1 . Theoretical calculations revealed that the surface of Cu-OUC effectively facilitates NO activation through a two-way charge transfer mechanism of “electron acceptance and donation”, with the *NO formation step being the potential-determining stage. The study pioneers the use of a MOF as an electrocatalyst for ambient NO-to-NH 3 conversion.