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NiFeCo wrinkled nanosheet electrode for selective oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid

文献类型： 外文期刊

作者： Chen, Bingkun 1 ; Yang, Bowen 2 ; Su, Yaqiong 3 ; Hou, Qidong 2 ; Smith Jr, Richard Lee 4 ; Qi, Xinhua 2 ; Guo, Haixin 1 ;

作者机构： 1.Chinese Acad Agr Sci, Agroenvironm Protect Inst, 31 Fukang Rd, Tianjin 300191, Peoples R China

2.Nankai Univ, Coll Environm Sci & Engn, 38 Tongyan Rd, Tianjin 300350, Peoples R China

3.Xi An Jiao Tong Univ, Engn Res Ctr Energy Storage Mat & Devices, Natl Innovat Platform Ctr Ind Educ Integrat Energy, Sch Chem, Xian 710049, Peoples R China

4.Tohoku Univ, Grad Sch Environm Studies, Aramaki Aza Aoba 468-1,Aoba Ku, Sendai 9808572, Japan

期刊名称：GREEN CHEMISTRY （ 影响因子：9.2； 五年影响因子：9.8 ）

ISSN： 1463-9262

年卷期： 2025 年 27 卷 7 期

页码：

收录情况： SCI

摘要： Quantitative and selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) via electrocatalysis is a crucial milestone for biomass conversion. In this study, FeCo-modified beta-Ni(OH)2 wrinkled nanosheet electrode were prepared by a hydrothermal method and used for the electrocatalytic oxidation of HMF to afford 100% conversion, 98.7% FDCA yield and a Faraday efficiency (FE) of 98%. The wrinkled nanosheet structure design increased the surface area (26.3 m2 g-1) and introduced oxygen-rich active sites (35.26%), enabling a current density of 10 mA cm-2 for HMF oxidation at 1.26 V vs. RHE. In situ electrochemical characterization established that beta-NiOOH was the actual oxidation active site. The decoration of FeCo promoted the formation of beta-NiOOH species, in which Ni3+ was converted into Ni2+via the hydroxy and aldehyde groups in HMF, while HMF was dehydrogenated to the oxidative derivative (FDCA) at the anode. Electrochemical cyclic voltammetry confirmed that the substrate and product species followed a Langmuir-Hinshelwood (L-H) adsorption mechanism. Density functional theory (DFT) calculations verified that the Gibbs free energy and adsorption energy of HMF can be adjusted through the co-doping of the FeCo composition, which was more effective in capturing protons and electrons and activating HMF. This work lays the foundation for a deeper understanding of polymetallic site synergies and provides a practical technique for the upgrading of electrochemical substance derivatives into structural unit chemicals.

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