Luo Rong, Li Bao-Jing, Wang Zhan-Peng, Chen Ming-Guang, Zhuang Gui-Lin, Li Quan, Tong Jia-Ping, Wang Wen-Tai, Fan Yu-Hua, Shao Feng
Key Laboratory of Marine Chemistry Theory and Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Ocean University of China, Qingdao 266100, China.
Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, China.
JACS Au. 2024 Oct 1;4(10):3823-3832. doi: 10.1021/jacsau.4c00475. eCollection 2024 Oct 28.
Ambient electrochemical NO reduction presents a dual solution for sustainable NO reduction and NH 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)]·HO} , (, HL = 5-(2'-carboxylphenoxy)isophthalic acid) acts as a stable electrocatalyst with high efficiency for NO-to-NH conversion. Electrochemical experimental studies showed that in 0.1 M KSO solution, the as-prepared achieved a peak Faradaic efficiency of 96.91% and a notable NH yield as high as 3415.82 μg h mg. The Zn-NO battery in aqueous solution can produce electricity possessing a power density of 2.04 mW cm while simultaneously achieving an NH yield of 616.92 μg h mg. Theoretical calculations revealed that the surface of 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 conversion.
环境电化学法还原NO为可持续的NO还原和NH合成提供了双重解决方案。然而，其复杂的动力学和能量需求需要高性能的电催化剂来确保有效和选择性的过程结果。在此，我们报道了一种二维铜基金属有机框架（MOF），{[Cu(HL)]·H₂O}ₙ ，（HL = 5-(2'-羧基苯氧基)间苯二甲酸）作为一种稳定的电催化剂，对NO到NH的转化具有高效率。电化学实验研究表明，在0.1 M K₂SO₄溶液中，所制备的催化剂实现了96.91%的峰值法拉第效率和高达3415.82 μg h⁻¹ mg⁻¹的显著NH产率。水溶液中的Zn-NO电池可以产生功率密度为2.04 mW cm⁻²的电力，同时实现616.92 μg h⁻¹ mg⁻¹的NH产率。理论计算表明，其表面通过“电子接受和给予”的双向电荷转移机制有效地促进了NO的活化，其中*NO形成步骤是电位决定阶段。该研究开创了使用MOF作为环境中NO到NH转化的电催化剂的先河。
