Electrochemical Oxidation of Nitrogen towards Direct Nitrate Production on Spinel Oxides

被引：127
作者：
Dai, Chencheng [1 ,2 ]
Sun, Yuanmiao [1 ]
Chen, Gao [1 ]
Fisher, Adrian C. [2 ,3 ]
Xu, Zhichuan J. [1 ,2 ,4 ,5 ]
机构：
[1] Nanyang Technol Univ, Sch Mat Sci & Engn, 50 Nanyang Ave, Singapore 639798, Singapore
[2] Cambridge Ctr Adv Res & Educ Singapore, 1 CREATE Way, Singapore 138602, Singapore
[3] Dept Chem Engn & Biotechnol, West Cambridge Site Philippa Fawcett Dr, Cambridge CB3 0AS, England
[4] Nanyang Technol Univ, Solar Fuels Lab, Singapore 639798, Singapore
[5] Nanyang Technol Univ, Energy Res Inst, 50 Nanyang Ave, Singapore 639798, Singapore
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2020年 / 59卷 / 24期
关键词：
electrochemical oxidation; electrocatalysis; nitrate; nitrogen oxidation; spinel oxides; AMMONIA;
D O I：
10.1002/anie.202002923
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Nitrates are widely used as fertilizer and oxidizing agents. Commercial nitrate production from nitrogen involves high-temperature-high-pressure multi-step processes. Therefore, an alternative nitrate production method under ambient environment is of importance. Herein, an electrochemical nitrogen oxidation reaction (NOR) approach is developed to produce nitrate catalyzed by ZnFexCo2-xO4 spinel oxides. Theoretical and experimental results show Fe aids the formation of the first N-O bond on the *N site, while high oxidation state Co assists in stabilizing the absorbed OH- for the generation of the second and third N-O bonds. Owing to the concerted catalysis, the ZnFe0.4Co1.6O4 oxide demonstrates the highest nitrate production rate of 130 +/- 12 mu mol h(-1) g(MO)(-1) at an applied potential of 1.6 V versus the reversible hydrogen electrode (RHE).
引用
收藏
页码：9418 / 9422
页数：5
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