纳米团簇
催化作用
材料科学
动力学
电化学
化学工程
无机化学
钌
电催化剂
氧化还原
纳米技术
物理化学
化学
电极
工程类
物理
量子力学
冶金
生物化学
作者
Zhongfen Nie,Linlin Zhang,Xin Ding,Meiyu Cong,Fanfan Xu,Lehui Ma,Mingxia Guo,Mingzhu Li,Lixue Zhang
标识
DOI:10.1002/adma.202108180
摘要
Electrochemical N2 oxidation reaction (NOR), using water and N2 in the atmosphere, represents a sustainable approach for nitric production to replace the conventional industrial synthesis with high energy consumption and greenhouse gas emission. Meanwhile, owing to chemical inertness of N2 and sluggish kinetics for 10-electron transfer, emerging electrocatalysts remain largely underexplored. Herein, Ru-nanoclusters-coupled Mn3 O4 catalysts decorated with atomically dispersed Ru atoms (Ru-Mn3 O4 ) are designed and explored as an advanced electrocatalyst for ambient N2 oxidation, with an excellent Faraday efficiency (28.87%) and a remarkable NO3- yield (35.34 µg h-1 mg-1cat. ), respectively. Experiments and density functional theory calculations reveal that the outstanding activity is ascribed to the coexistence of Ru clusters and single-atom Ru. The synergistic effect between the Ru clusters and Mn3 O4 can effectively activate the chemically inert N2 , lowering the kinetic barrier for the vital breakage of N≡N. The intensive *OH supply and enhanced conductivity are used to regulate the catalytic kinetics for optimized performance. This work provides brand-new ideas for the rational design of electrocatalysts in complicated electrocatalytic reactions with multiple dynamics-different steps.
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