电合成
化学
电催化剂
催化作用
氨生产
法拉第效率
产量(工程)
选择性
共价键
基质(水族馆)
氨
硝酸盐
化学工程
共价有机骨架
组合化学
金属有机骨架
聚苯胺
氢
纳米技术
制氢
无机化学
反应中间体
光化学
混合材料
多相催化
氢键
可逆氢电极
电化学
反应中间体
动力学
反应机理
作者
Warisha Tahir,Yuqin Wei,Mao Wang,Islam E. Khalil,Prasenjit Das,Ting Wang,C.H. Cheng,Shuang Li,Arne Thomas
摘要
Nitrate electroreduction to ammonia offers a dual opportunity: decarbonizing NH3 production by replacing the energy-intensive Haber-Bosch process and remediating nitrate-contaminated wastewater. While copper-based catalysts show promise for this transformation, their practical implementation is hindered by sluggish kinetics and competing hydrogen evolution pathways. Here, we report the integration of covalent organic framework (COF) layers onto a Cu2O surface, which enables rapid proton/electron transfer and substrate activation for efficient NH3 electrosynthesis from NO3– in neutral media. By growing pyridine- or imidazole-decorated COF shells with varying thickness on Cu2O nanocubes, we achieve precise control over the microenvironment of the electrocatalyst surface. The pyridine-COF on Cu2O demonstrates 84% Faradaic efficiency for NH3 production with 92.11% selectivity and a record yield of 2.3 mg h–1 cm–2. In situ spectroscopic investigations reveal that the COF shells have multifunctional roles: they selectively transport reactants, stabilize key intermediates through hydrogen bonding interactions, and steer the reaction along an associative pathway that bypasses common side reactions. Our findings establish COF-gated core–shell architectures as a generalizable platform for designing efficient, selective, and durable electrocatalysts for broad applications.
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