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Electrocatalytic synthesis of value-added chemicals is attracting significant research attention owing to its mild reaction conditions, environmental benignity, and potentially scalable application to organic synthetic chemistry. Herein, we report the preparation of a single-crystalline NiS2 nanostructure film of ~ 50 nm thickness grown directly on a carbon fiber cloth (NiS2/CFC) by a facile vapor-phase hydrothermal (VPH) method. NiS2/CFC as an electrocatalyst exhibits activity for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) in alkaline media. Furthermore, a series of alcohols (2-propanol, 2-butanol, 2-pentanol, and cyclohexanol) were electrocatalytically converted to the corresponding ketones with high selectivity, efficiency, and durability using the NiS2/CFC electrode in alkaline media. In the presence of 0.45 M alcohol, a remarkably decreased overpotential (~ 150 mV, vs. RHE) at the NiS2/CFC anode compared with that for water oxidation to generate O2, i.e., the OER, in alkaline media leads to significantly improved H2 generation. For instance, the H2 generation rate in the presence of 0.45 M 2-propanol is almost 1.2-times of that obtained for pure water splitting, but in a system that employs an applied voltage at least 280 mV lower than that required for water splitting to achieve the same current density (20 mA·cm–2). Thus, our results demonstrate the applicability of our bifunctional non-precious-metal electrocatalyst for organic synthesis and simultaneous H2 production.


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Vapor-phase hydrothermal growth of single crystalline NiS2 nanostructure film on carbon fiber cloth for electrocatalytic oxidation of alcohols to ketones and simultaneous H2 evolution

Show Author's information Tianxing Wu1Xiaoguang Zhu1Guozhong Wang1( )Yunxia Zhang1Haimin Zhang1( )Huijun Zhao1,2
Key Laboratory of Materials PhysicsCentre for Environmental and Energy NanomaterialsAnhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsChinese Academy of SciencesHefei230031China
Centre for Clean Environment and EnergyGriffith UniversityGold Coast CampusNathanQueensland4222Australia

Abstract

Electrocatalytic synthesis of value-added chemicals is attracting significant research attention owing to its mild reaction conditions, environmental benignity, and potentially scalable application to organic synthetic chemistry. Herein, we report the preparation of a single-crystalline NiS2 nanostructure film of ~ 50 nm thickness grown directly on a carbon fiber cloth (NiS2/CFC) by a facile vapor-phase hydrothermal (VPH) method. NiS2/CFC as an electrocatalyst exhibits activity for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) in alkaline media. Furthermore, a series of alcohols (2-propanol, 2-butanol, 2-pentanol, and cyclohexanol) were electrocatalytically converted to the corresponding ketones with high selectivity, efficiency, and durability using the NiS2/CFC electrode in alkaline media. In the presence of 0.45 M alcohol, a remarkably decreased overpotential (~ 150 mV, vs. RHE) at the NiS2/CFC anode compared with that for water oxidation to generate O2, i.e., the OER, in alkaline media leads to significantly improved H2 generation. For instance, the H2 generation rate in the presence of 0.45 M 2-propanol is almost 1.2-times of that obtained for pure water splitting, but in a system that employs an applied voltage at least 280 mV lower than that required for water splitting to achieve the same current density (20 mA·cm–2). Thus, our results demonstrate the applicability of our bifunctional non-precious-metal electrocatalyst for organic synthesis and simultaneous H2 production.

Keywords: vapor-phase hydrothermal, single-crystalline NiS2 film, carbon fiber cloth, electrocatalytic oxidation of alcohols to ketones, H2 generation

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Publication history
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Acknowledgements

Publication history

Received: 07 April 2017
Revised: 09 June 2017
Accepted: 11 June 2017
Published: 04 August 2017
Issue date: February 2018

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© Tsinghua University Press and Springer-Verlag GmbH Germany 2017

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 51672277, 51432009, and 51602315), the Postdoctoral Science Foundation of China (No. 2017M612101), and the CAS Pioneer Hundred Talents Program and the CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China.

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