由双核-铜基团构建的二维 MOF,用于高性能电催化 NO 还原成 NH3。

IF 8.5 Q1 CHEMISTRY, MULTIDISCIPLINARY JACS Au Pub Date : 2024-10-01 eCollection Date: 2024-10-28 DOI:10.1021/jacsau.4c00475
Rong Luo, Bao-Jing Li, Zhan-Peng Wang, Ming-Guang Chen, Gui-Lin Zhuang, Quan Li, Jia-Ping Tong, Wen-Tai Wang, Yu-Hua Fan, Feng Shao
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引用次数: 0

摘要

环境电化学还原氮氧化物是一种可持续还原氮氧化物和合成 NH3 的双重解决方案。然而,它们复杂的动力学和能量需求要求高性能的电催化剂,以确保有效和选择性的工艺结果。在此,我们报告了一种二维铜基金属有机框架(MOF){[Cu(HL)]-H2O} n(Cu-OUC,H3L = 5-(2'-羧基苯氧基)间苯二甲酸)可作为一种稳定的电催化剂,高效地实现 NO 到 NH3 的转化。电化学实验研究表明,在 0.1 M K2SO4 溶液中,制备的 Cu-OUC 的峰值法拉第效率达到 96.91%,显著的 NH3 产率高达 3415.82 μg h-1 mg-1。水溶液中的 Zn-NO 电池可产生功率密度为 2.04 mW cm-2 的电能,同时实现 616.92 μg h-1 mg-1 的 NH3 产量。理论计算显示,Cu-OUC 表面通过 "电子接受和捐赠 "的双向电荷转移机制有效促进了 NO 的活化,而 *NO 的形成步骤是电位决定阶段。该研究开创性地将 MOF 用作常温 NO-NH3 转化的电催化剂。
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Two-Dimensional MOF Constructed by a Binuclear-Copper Motif for High-Performance Electrocatalytic NO Reduction to NH3.

Ambient electrochemical NO reduction presents a dual solution for sustainable NO reduction and NH3 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)]·H2O} n , (Cu-OUC, H3L = 5-(2'-carboxylphenoxy)isophthalic acid) acts as a stable electrocatalyst with high efficiency for NO-to-NH3 conversion. Electrochemical experimental studies showed that in 0.1 M K2SO4 solution, the as-prepared Cu-OUC achieved a peak Faradaic efficiency of 96.91% and a notable NH3 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 NH3 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-NH3 conversion.

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