APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Xiang Li,Wangchuan Zhu,Feng Yue,Huijuan Pang,Chuantao Wang,Danjun Wang,Yuxuan Lu,Chunming Yang
Copper-based compounds exhibit broad prospects in the electrocatalytic oxidation of biomass for sustainable production of high-value-added chemicals due to their passivated oxygen evolution reaction (OER) competitiveness. However, the sluggish reaction kinetics remain the main challenge in constraining their scalable application. Herein, a highly selective electrooxidation of 5-hydroxymethylfurfural (HMF) to 2, 5-furandicarboxylic acid (FDCA) on CuO is achieved via photoinduced surface reconstruction. The experimental results confirmed that the photogenerated hole accumulation on the surface of CuO with matched valence band position can promote the CuOOH active phase generation. Density functional theory (DFT) calculations and the overall relationship between structure and selectivity indicate the CuOOH species can accelerate the spontaneous dehydrogenation process of hydroxyl group . Therefore, the activated CuO electrode under illumination can effectively regulate the conversion of 5-Hydroxymethyl-2-furancarboxylic acid (HMFCA) key intermediates and exhibits accelerated reaction kinetics, FDCA yield increased by 17.79 % compared to dark condition. Additionally, a general enhancement effect on the oxidation of benzyl alcohol and furfuryl alcohol was also revealed. This work introduces photoassistance effect for the first time in HMF oxidation, opening up prospects for the application of photoelectric synergy in biomass value-added conversion and providing insights into the activity mechanism of Cu-based catalysts in organic oxidation.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
MOLECULES
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2025
·Vol. 30
·期 8
·1780
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IF 4.6
Shiying Yang,Xin Jin,Bin Zhu,Dan Yang,Xiaoyue Wan,Yihu Dai,Chunmei Zhou,Yuguang Jin,Yanhui Yang
5-Hydroxymethylfurfural (HMF) serves as an important bridge connecting biomass resources with fossil fuels. Its downstream product, 2,5-furandicarboxylic acid (FDCA), is a renewable alternative to terephthalic acid (TPA) in the synthesis of various polymer materials. In this study, we successfully synthesized four ruthenium-based catalysts with varying valence states supported on carbon nanotubes (CNTs) and compared the performance of HMF electrooxidation. Among these, the Ru+2.9catalyst demonstrated the highest activity for the electrochemical oxidation of HMF to FDCA in the neutral medium (0.1 M K2SO4). Notably, the FDCA yield reached 90.2% under an applied potential of 0.95 V (vs. Ag/AgCl) after 24 h. Mechanistic analysis revealed that the superior specific capacitance of the Ru+2.9catalyst significantly facilitated the reaction process. This work represents a more cost-effective approach to avoid the need for excessive alkaline additives during catalyst preparation and the HMF oxidation process, and FDCA separated easily after cooling the reaction solution down.
研究领域:
能源化学
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催化化学
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生物质转化
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2018
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IF 6.759
Tianyu Gao,Jing Chen,Wenhao Fang,Qiue Cao,Weiping Su,Franck Dumeignil
Mn-Ce mixed oxides-supported Ru nanoparticles (Ru/Mn X Ce 1 O Y ) with enhanced oxygen mobility and strong metal-support interaction were prepared and applied to the aerobic oxidation of 5 -hydroxymethylfurfural (HMF) to 2,5 -furandicarboxylic acid (FDCA) without addition of any base additives. Oxygen and water were used as green oxidant and solvent, respectively. The catalysts were characterized in depth by XRD, H 2 -TPR, O 2 -TPD, UV–Vis DRS, XPS and TEM, to reveal materials properties from bulk to surface. The influence of Mn/Ce molar ratios in support materials and reaction parameters ( i.e. , HMF/Ru ratio, O 2 pressure, reaction temperature and time) was systematically studied and optimized. The reaction route and rate-determining step for oxidation of HMF to FDCA over the Ru/Mn X Ce 1 O Y catalysts were investigated by kinetic analysis. Well-dispersed metallic Ru nanoparticles with a mean size of 4.4 nm deposited on the support were found essential to activate and oxidize the HMF molecule. The Mn/Ce molar ratio was found to affect not only conversion of HMF but also distribution of products. The Ru/Mn 6 Ce 1 O Y catalyst demonstrated an exceptional yield (≥99%) of FDCA, which corresponds in our conditions to one of the best productivity (5.3 mol FDCA ·mol Ru −1 ·h −1 ) ever reported in literature. The superior activity of the Ru/Mn 6 Ce 1 O Y catalyst was mainly associated with (i) the strong metal-support interaction and (ii) the synergistic effect between manganese and cerium oxides. This catalyst showed the highest surface concentrations in Mn 4+ and Ce 3+ among the series, which, as a consequence, enhanced the availability and mobility of active oxygen species. This catalyst was shown resistant to deactivation during eight recycling uses thanks to a strong metal-support interaction between Ru nanoparticles and the Mn-Ce mixed oxide used as a support.
研究领域:
催化化学
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绿色化学
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材料科学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2023
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IF 2.2
Ke Wang,Jia Wu,Shuyi Zheng,Shibin Yin
Construction of highly active and stable bifunctional catalysts for 5-hydroxymethylfurfural oxidation reaction (HMFOR) and hydrogen evolution reaction (HER) is meaningful but remains a challenge. Herein, the NiCo–Mo 2 N heterostructure nanosheets catalyst with excellent HMFOR/HER performance is obtained by a simple hydrothermal and calcination method. The heterogeneous interface between NiCo and Mo 2 N induces electron redistribution, regulating the electronic structure of the catalyst and thus optimizing the adsorption/desorption behavior of HMFOR/HER intermediates. Consequently, NiCo–Mo 2 N/NF exhibits superior catalytic activity with a potential of 1.14 V RHE /−17 mV RHE (HMFOR/HER) at ±10 mA cm −2 , and the HMF conversion rate, FDCA yield, and Faradaic efficiency (FE) are ∼100%, 99.98%, and 98.65%, respectively. Besides, it only requires a low voltage of 1.36 V to achieve 100 mA cm −2 for HMFOR-assisted H 2 production. This study provides a strategy for the development of efficient bifunctional catalysts for sustainable production of high value-added products and hydrogen.
研究领域:
催化
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电化学
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材料科学
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可持续化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）