氨
法拉第效率
傅里叶变换红外光谱
产量(工程)
无机化学
化学
电化学
氧化物
材料科学
化学工程
电极
有机化学
物理化学
工程类
冶金
作者
Yanbo Li,Chuanqi Cheng,Shuhe Han,Yanmei Huang,Xi‐Wen Du,Bin Zhang,Yifu Yu
出处
期刊:ACS energy letters
[American Chemical Society]
日期:2022-03-01
卷期号:7 (3): 1187-1194
被引量:83
标识
DOI:10.1021/acsenergylett.2c00207
摘要
Electrocatalytic nitric oxide (NO) reduction represents a sustainable route from the point of view of environmental protection and ammonia generation. However, conversion from NO to ammonia under low NO concentrations is still a big challenge. Herein, Ru nanosheets with low coordination numbers (Ru-LCN) are prepared and exhibit high performance for electrocatalytic NO (1% v/v) reduction to ammonia under −0.2 V vs RHE (Faradaic efficiency, 65.96%; yield rate, 45.02 μmol·h–1·mgcat–1), obviously outperforming its counterpart of high coordination number Ru nanosheets (Faradaic efficiency, 37.25%; yield rate, 25.57 μmol·h–1·mg–1). Colorimetric methods and 1H nuclear magnetic resonance spectroscopy are performed to quantify ammonia. Through the combination of online differential electrochemical mass spectrometry (DEMS) and electrochemical in situ Fourier transform infrared (FTIR) spectroscopy with density functional theory calculations, the possible reaction pathway and enhanced mechanism are revealed. Constructing low coordination number Ru active sites is conducive to facilitating the adsorption of NO and reducing the reaction energy barrier of the potential-determining hydrogenation step.
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