Electrochemical Oxidation of Nitrogen towards Direct Nitrate Production on Spinel Oxides

被引：140

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

页码：9418 / 9422

页数：5

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