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Electrochemical Oxidation of Nitrogen towards Direct Nitrate Production on Spinel Oxides
Author(s) -
Dai Chencheng,
Sun Yuanmiao,
Chen Gao,
Fisher Adrian C.,
Xu Zhichuan J.
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202002923
Subject(s) - oxidizing agent , spinel , catalysis , electrochemistry , inorganic chemistry , nitrate , chemistry , nitrogen , redox , oxidation state , oxide , electrode , materials science , metallurgy , organic chemistry
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 ZnFe x Co 2− x O 4 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 ZnFe 0.4 Co 1.6 O 4 oxide demonstrates the highest nitrate production rate of 130±12 μmol h −1 g MO −1 at an applied potential of 1.6 V versus the reversible hydrogen electrode (RHE).