Zhang Bocheng, Dai Zechuan, Chen Yanxu, Cheng Mingyu, Zhang Huaikun, Feng Pingyi, Ke Buqi, Zhang Yangyang, Zhang Genqiang
Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui, 230026, China.
Nat Commun. 2024 Apr 1;15(1):2816. doi: 10.1038/s41467-024-47025-w.
Nitrate can be electrochemically degraded to produce ammonia while treating sewage while it remains grand challenge to simultaneously realize high Faradaic efficiency and production rate over wide-range concentrations in real wastewater. Herein, we report the defect-rich Cu nanowire array electrode generated by in-situ electrochemical reduction, exhibiting superior performance in the electrochemical nitrate reduction reaction benefitting from the triple synergistic modulation. Notably, the defect-rich Cu nanowire array electrode delivers current density ranging from 50 to 1100 mA cm across wide nitrate concentrations (1-100 mM) with Faradaic efficiency over 90%. Operando Synchrotron radiation Fourier Transform Infrared Spectroscopy and theoretical calculations revealed that the defective Cu sites can simultaneously enhance nitrate adsorption, promote water dissociation and suppress hydrogen evolution. A two-electrode system integrating nitrate reduction reaction in industrial wastewater with glycerol oxidation reaction achieves current density of 550 mA cm at -1.4 V with 99.9% ammonia selectivity and 99.9% nitrate conversion with 100 h stability, demonstrating outstanding practicability.
在处理污水时，硝酸盐可通过电化学降解产生氨，但要在实际废水中的宽浓度范围内同时实现高法拉第效率和产率仍然是一个巨大的挑战。在此，我们报道了通过原位电化学还原生成的富含缺陷的铜纳米线阵列电极，由于三重协同调制，在电化学硝酸盐还原反应中表现出优异的性能。值得注意的是，富含缺陷的铜纳米线阵列电极在宽硝酸盐浓度（1-100 mM）范围内提供50至1100 mA cm的电流密度，法拉第效率超过90%。原位同步辐射傅里叶变换红外光谱和理论计算表明，有缺陷的铜位点可以同时增强硝酸盐吸附、促进水离解并抑制析氢。将工业废水中的硝酸盐还原反应与甘油氧化反应相结合的双电极系统在-1.4 V时实现了550 mA cm的电流密度，氨选择性为99.9%，硝酸盐转化率为99.9%，具有100小时的稳定性，展现出卓越的实用性。
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