JOURNAL OF CATALYSIS
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2025
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IF 6.5
Xinyu Liu,Jiansong Wang,He Li,Xiaoliang Qu,Yipu Xu,Liu-Liu Shen,Gui-Rong Zhang,Donghai Mei
Electrochemical oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) offers a sustainable route for biomass valorization. The technoeconomic viability of this promising route, however, hinges on developing efficient electrocatalysts. Moving beyond conventional structural engineering of catalysts, we introduce a surface modification strategy using a small amount of hydrophobic ionic liquids (ILs) to adjust the local electrochemical microenvironment. Specifically, by modifying a porous conductive metal organic framework (Ni-HHTP) with [MTBD][NTf 2 ], the FDCA yield and Faradaic efficiency (FE) are significantly enhanced to 99.9% and 97.0%, respectively, along with a threefold increase in FDCA production rate compared to the unmodified catalyst. Mechanistic studies reveal that the ILs facilitate HMF enrichment at the catalyst surface while preventing water-induced blockage of active sites. This work highlights the transformative potential of interfacial engineering with ILs as a versatile strategy for advancing electrocatalytic systems in biomass conversion applications.
研究领域:
电化学
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催化
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生物质转化
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材料科学
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绿色化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zhe-Hui Zhang,Meng-Ying Liu,Zhuohua Sun,Katalin Barta,Tong-Qi Yuan
Funneling complex lignocellulose into simple and valuable building blocks has garnered significant interest in the field of biorefinery as a competitor to the petrochemical industry. Reductive Catalytic Fractionation (RCF) of lignocellulose, an innovative biorefinery technology, provides a promising strategy for complete valorization of lignocellulose into various valuable chemicals. In this study, integrated processes utilizing RCF strategies were developed to achieve complete conversion of lignocellulose into various simple and valuable platform chemicals. The core of this system is the flexible use of commercial Ni catalysts including Raney Ni and Ni/SiO 2 -Al 2 O 3 which brings great benefits for future upscale and industrial applications. Surprisingly, both monomers derived from lignin and high molecular weight fractions could be converted to 4-ethylcyclohexanol while carbohydrate pulp was converted to furfural and 5-methoxymethylfurfural (MMF) in one-pot. MMF could be further upgraded to 2,5-Furandicarboxylicacid (FDCA) via catalytic oxidation by Ru/C catalysts. This work could inspire the development of more sustainable and economically viable biorefinery processes.
研究领域:
生物精炼
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化学工程
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催化
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可持续化学
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产品关联
DOI
高影响因子
ChemCatChem
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2016
·Vol. 8
·期 23
·3636-3643
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IF 4.724
Zhenyou Gui,Wenrong Cao,Shunmugavel Saravanamurugan,Anders Riisager,Lifang Chen,Zhiwen Qi
Graphical Efficient noble alloy : Au–Pd supported on zinc hydroxycarbonate (ZOC) catalysts shows high activity for 5-hydroxymethylfurfural oxidation. The basicity of ZOC can play a crucial role in enhancing the yield of FDCA. Moreover, Au–Pd/ZOC can be recycled at least six times without significant loss of its activity. Bimetallic catalysts with Au–Pd supported on zinc hydroxycarbonate (ZOC) were synthesized by a simple deposition–precipitation method and analyzed by transmission electron microscopy to have a narrow-size distribution of predominantly 1–2 nm. The prepared Au–Pd/ZOC catalysts exhibited excellent activity towards 5-hydoxymethylfurfural (HMF) oxidation in water in the presence of the base NaHCO 3 at benign conditions of 80 °C and 3 bar O 2 , resulting in quantitative yield of 2,5-furandicarboxylic acid (FDCA). The addition of base not only enhanced the yield of FDCA but also stabilized the support ZOC by preventing ZOC from the reaction with formed carboxylic acid intermediates/products, thus allowing Au–Pd/ZOC to be recycled for at least six times without significant loss of activity. The basicity of ZOC could play an important role in obtaining the improved yield of FDCA as compared to other supports.
研究领域:
催化化学
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绿色化学
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化学工程
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材料科学
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有机合成
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环境科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Yingying Li,Xueli Ma,Wei Lv,Hong Chen,Linhao Yu,Zewei Ma,Sen Wang,Yongdan Li
Cr-doped ZnAl mixed oxide catalysts (Zn0.75CrAl-x-c) were obtained via calcining the Zn0.75CrAl-x hydrotalcite precursors and were applied in the selective oxidation of 5-hydroxymethylfurfural (5-HMF) to 2,5-furandicarboxylic acid (FDCA). Cr doping significantly enhanced the catalytic activity. A 95.1% 5-HMF conversion with an 88.1% FDCA selectivity was achieved over the Zn0.75CrAl-6-c catalyst at 130 °C under 0.6 MPa oxygen for 4 h. The good performance was associated with the high specific surface area and high oxygen vacancy concentration. Moreover, the Zn0.75CrAl-6-c catalyst was used for five cycles without a significant activity loss indicating excellent stability.
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
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2022
·
IF 13.599
Hao Zhang,Yinghao Wang,Qizhao Zhang,Bang Gu,Qinghu Tang,Qiue Cao,Kun Wei,Wenhao Fang
The base-free aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) in water is recognized as an important and sustainable upgrading process for cellulosic carbohydrates. However, selectivity control still remains a challenge. Here, we disclose that the unique synergy in magnetic Ni x Co 1 O y ( x = 1, 3 and 5) bimetallic oxides can induce reactive oxygen defects and simultaneously stabilize small-sized metallic Au nanoparticles in the Au/Ni x Co 1 O y catalysts. Such catalytic features render effective adsorption and activation of O 2 , OH and C O groups, realizing selective oxidation of HMF to FDCA . On a series of magnetic Au/Ni x Co 1 O y catalysts with almost identical Au loadings (ca. 0.5 wt%) and particle sizes (ca. 2.7 nm), the variable Ni/Co molar ratios give rise to the tunable electron density of Au sites and synergistic effect between NiO and CoO y . The initial conversion rates of HMF and its derived intermediates (i.e., DFF, HMFCA and FFCA) show a volcano-like dependence on the number of oxygen defects (i.e., O 2 − and O − ) and electron-rich Au 0 sites. The optimum Au/Ni 3 Co 1 O y catalyst exhibits a highest productivity of FDCA (12.5 mmol FDCA mol Au - 1 h −1 ) among all the Au catalysts in the literature and achieves > 99% yield of FDCA at 120 °C and 10 bar of O 2 . In addition, this catalyst can be easily recovered by a magnet and show superior stability and reusability during six consecutive cycling tests. This work may shed a light on Au catalysis for the base-free oxidation of biomass compounds by smartly using the synergy in bimetallic oxide carriers.
研究领域:
催化
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材料科学
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化学工程
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可持续化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2020
·
IF 7.632
Heng Ban,Youdi Zhang,Shuaibo Chen,Youwei Cheng,Teng Pan,Lijun Wang,Xi Li
In this contribution, readily available 5-methyl furfural (MF) derived from biomass was used as an excellent substitute of the chemically unstable 5-hydroxymethylfurfural (HMF) for preparing the commercial precursor 2,5-furandicarboxylic acid (FDCA). MF was catalytically oxidized by air into FDCA in acetic acid over homogeneous Co/Mn/Br catalysts at 130–170 °C. It was found that both the substitute reactivity and the ring chemical stability have a remarkable impact on the yield of aromatic dicarboxylic acids. The effects of reaction temperature, pressure, catalyst composition and concentration, water concentration in the solvent, and substrate/solvent mass ratio on both the main reaction and the side reaction were investigated systematically and thoroughly using HPLC and an online tail gas monitoring system. Under optimized conditions, the oxidation of MF gave 100% conversion of MF and 75.8% yield of FDCA with 99.6% purity. It was also proven that the addition of 200 ppm cerium could work well at low temperatures (130–140 °C) for enhancing FDCA selectivity via suppressing the side reactions.
研究领域:
化学工程
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催化
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有机化学
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绿色化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2023
·
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
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Xiangdong Ma,Shan Yue,Rui Liu,Hui Kan,Jiayi Gao,Mingjing Zhao,Haijiao Xie,Xiaohong Xia
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMFOR) is an effective way to realize the upgrading of high value-added chemicals coupled with electrolytic water to produce hydrogen under green conditions. However, the oxygen evolution reaction competition of the anodic water decomposition of HMFOR electrocatalysts at high current densities hinders the production efficiency of 2, 5-furan dicarboxylic acid (FDCA). Although Cu has excellent electrical conductivity and small molecule affinity, it does not perform well in OER. The catalytic activities of Co and Ni in the electrochemical oxidation of small organic molecules and OER were significant. By optimizing the electronic structure and morphology of Cu, Co, and Ni, the competitive reaction of OER can be effectively inhibited, and the catalytic efficiency of HER can be strengthened. Then, we have successfully constructed a micro-Ni-doped Co phosphide grown on Cu foam (Ni m CoP/CF) with an optimized interfacial structure for adsorption and conversion of reactants. At 1.43 V vs. RHE, Ni m CoP/CF achieves high current density (100 mA cm -2 ) and selectivity for FDCA. The Co site at Ni optimized interface was identified as the catalytic center for OH⁎ adsorption by electrochemical tests and Density Functional Theory calculations, and the synergistic adsorption between Ni-doped Co 2 P and Cu 3 P interfaces greatly enhanced the adsorption of HMF, further promoting the catalytic conversion of HMF to FDCA. This work has guiding significance for the selective upgrading of high value-added chemicals hydrogen evolution through interfacial regulatory strategies for micro-metal doping.
研究领域:
电催化
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材料科学
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能量转换
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绿色化学
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表面工程
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生物质利用
✓ 已验证
产品关联
DOI
高影响因子