电催化剂
催化作用
化学
无机化学
法拉第效率
电化学
傅里叶变换红外光谱
硝酸盐
介孔材料
电解
化学工程
电极
有机化学
物理化学
工程类
电解质
作者
Yuxiao Zhao,Shaozhen Liang,Yingji Zhao,Hongjuan Zhang,Xiang Zheng,Zhiqian Li,Lisong Chen,Jing Tang
标识
DOI:10.1016/j.jcis.2023.10.125
摘要
The electroreduction of nitrate (NO3-) pollutants to ammonia (NH3) provides a sustainable approach for both wastewater treatment and NH3 synthesis. However, electroreduction of nitrate requires multi-step electron and proton transfer, resulting in a sluggish reaction rate. Herein, we synthesized a Co-modified Cu/Cu2O catalyst supported on hollow mesoporous carbon substrates (Co/Cu/Cu2O-MesoC) by a one-step microwave-assisted reduction method. At -0.25 V vs. reversible hydrogen electrode (RHE), Co/Cu/Cu2O-MesoC shows a Faradaic efficiency (FE) of 100 ± 1% in 0.1 M NO3-. Notably, the maximum NH3 yield rate (YieldNH3) reaches 6.416 ± 0.78 mmol mgcat-1h-1 at -0.45 V vs. RHE, which is much better than most of the previous reports. Electrochemical evaluation and in-situ Fourier transform infrared (FTIR) spectroscopy reveal that the addition of Co could promote water electrolysis, and the generated H* is involved in the following hydrogenation of intermediates, ultimately leading to faster kinetics and energetics during electrocatalytic conversion of NO3- to NH3. This synergetic electrocatalysis strategy opens a new avenue for the development of high-activity, selectivity, and stability catalysts.
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