Antiperovskite nitride Cu3N nanosheets for efficient electrochemical oxidation of methanol to formate

Perovskite oxides with flexible compositions and electronic structures have great potential for application in electrocatalytic water oxidation reactions. However, few studies have focused on the application of perovskite oxides in electrocatalytic oxidation reactions of organic molecules, probably...

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Bibliographic Details
Published in:Science China materials 2023-05, Vol.66 (5), p.1820-1828
Main Authors: Zhao, Lei, Sun, Qijiao, Li, Mao, Zhong, Yafei, Shen, Peiqi, Lin, Yunxiang, Xu, Kun
Format: Article
Language:English
Subjects:
Absorption spectroscopy
Chemistry and Materials Science
Chemistry/Food Science
Conversion
Core-shell structure
Electrocatalysts
Electrochemical oxidation
Electron transport
High resolution electron microscopy
Infrared reflection
Infrared spectroscopy
Mass spectrometry
Materials Science
Methanol
Nanosheets
Nitrides
Organic chemistry
Oxidation
Perovskites
Raman spectroscopy
Surface chemistry
X ray absorption
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Summary:Perovskite oxides with flexible compositions and electronic structures have great potential for application in electrocatalytic water oxidation reactions. However, few studies have focused on the application of perovskite oxides in electrocatalytic oxidation reactions of organic molecules, probably due to the absence of active species because of the poor conductivity and high energy barrier of the surface reconstruction. Herein, we report Cu 3 N nanosheets with a typical antiperovskite structure as electrocatalysts for selectively converting methanol to formate. The as-prepared antiperovskite nitride Cu 3 N samples exhibit a Faradic efficiency exceeding 90% for methanol to formate over a wide potential range, which was further confirmed by online electrochemical mass spectrometry and in situ infrared reflectance absorption spectroscopy. Moreover, the high-resolution transmission electron microscopy, X-ray absorption spectroscopy, and in situ Raman spectroscopy results indicate that the core-shell structure formed by generating surface Cu(II) species triggers the electrocatalytic methanol oxidation reaction activity, whereas the pristine Cu 3 N core facilitates the electron transport inside the catalyst during the electrocatalytic process. This study provides a modelable scheme for the highly selective conversion of methanol and introduces a novel nonoxide perovskite material for the electrochemical conversion of small-organic molecules.
ISSN:2095-8226
2199-4501
DOI:10.1007/s40843-022-2311-y