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电化学氧化 5-羟甲基糠醛在氮化镍/碳纳米片上的反应途径:通过原位和频发生振动光谱确定。

Electrochemical Oxidation of 5-Hydroxymethylfurfural on Nickel Nitride/Carbon Nanosheets: Reaction Pathway Determined by In Situ Sum Frequency Generation Vibrational Spectroscopy.

机构信息

State Key Laboratory of Chemo/Bio-Sensing and Chemometrics, Provincial Hunan Key Laboratory for Graphene Materials and Devices, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, P. R. China.

i-LAB, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences, Suzhou, 215123, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2019 Oct 28;58(44):15895-15903. doi: 10.1002/anie.201908722. Epub 2019 Sep 18.

DOI:10.1002/anie.201908722
PMID:31452306
Abstract

2,5-Furandicarboxylic acid was obtained from the electrooxidation of 5-hydroxymethylfurfural (HMF) with non-noble metal-based catalysts. Moreover, combining the biomass oxidation with the hydrogen evolution reaction (HER) increased the energy conversion efficiency of an electrolyzer and also generated value-added products at both electrodes. Here, the reaction pathway on the surface of a carbon-coupled nickel nitride nanosheet (Ni N@C) electrode was evaluated by surface-selective vibrational spectroscopy using sum frequency generation (SFG) during the electrochemical oxidation. The Ni N@C electrode shows catalytic activities for HMF oxidation and the HER. As the first in situ SFG study on transition-metal nitride for the electrooxidation upgrade of HMF, this work not only demonstrates that the reaction pathway of electrochemical oxidation but also provides an opportunity for nonprecious metal nitrides to simultaneously upgrade biomass and produce H under ambient conditions.

摘要

2,5-呋喃二甲酸是通过非贵金属基催化剂电氧化 5-羟甲基糠醛(HMF)得到的。此外,将生物质氧化与析氢反应(HER)相结合,提高了电解槽的能量转换效率,并在两个电极上生成了附加值产品。在这里,通过使用表面选择的和频产生(SFG)技术,在电化学氧化过程中评估了碳耦合氮化镍纳米片(Ni N@C)电极表面的反应途径。Ni N@C 电极对 HMF 氧化和 HER 具有催化活性。作为首例针对 HMF 电化学氧化升级的过渡金属氮化物的原位 SFG 研究,这项工作不仅证明了电化学氧化反应途径,而且为非贵金属氮化物在环境条件下同时升级生物质和生产 H 提供了机会。

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