期刊
NANO RESEARCH
卷 11, 期 2, 页码 1004-1017出版社
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-017-1714-0
关键词
vapor-phase hydrothermal; single-crystalline NiS2 film; carbon fiber cloth; electrocatalytic oxidation of alcohols to ketones; H-2 generation
类别
资金
- National Natural Science Foundation of China [51672277, 51432009, 51602315]
- Postdoctoral Science Foundation of China [2017M612101]
- CAS Pioneer Hundred Talents Program
- CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China
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 similar to 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 (similar to 150 mV, vs. RHE) at the NiS2/CFC anode compared with that for water oxidation to generate O-2, i.e., the OER, in alkaline media leads to significantly improved H-2 generation. For instance, the H-2 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 H-2 production.
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