Molecular Catalysis
·
2024
·
IF 3.9
Yuwei Liang,Chunling Hu,Peng Chen,Qi Li,Jianning Wu,Zhiyong Liu,Jichang Liu,Yanlong Tai
5-hydroxymethylfurfural (HMF) can catalyte into 2,5-diformylfuran (DFF) which had received much attention as a potential biomass resource. Here, we used a simple and effective method to construct hollow CdS quantum dot (CdS QDs)/MIL-101 heterostructures with high contact area and multiple active sites. The structure of heterostructures could improve photocatalytic activity by charge transfer, photogenerated carrier separation and the multiple refractions of light supported within the hollow-structured CdS QDs. The detailed catalytic mechanism was illustrated by trap agent experiments and electron paramagnetic resonance (EPR) spectroscopy, in which superoxide radicals (·O 2 - ) play a decisive role in the catalytic oxidation of HMF to DFF. Furthermore, the large specific surface area of MIL-101 adsorbs O 2 from the reaction system thereby accelerating the ·O 2 - formation process. Under environmental conditions, 70 % CdS QDs/MIL-101 exhibited optimal catalytic performance. Comparing with pure CdS QDs, the photocurrent enhances 1.8 times, HMF conversion is 1.5 times and DFF selectivity is 1.2 times. This work provide a useful way to improve the conversion of biomass by Z-heterostructures under ambient conditions.
研究领域:
化学工程
·
材料科学
·
环境科学
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Wenhui Li,Yuqiu Wu,Si Long,Zhi Chen,Liangzhi Li,Xin Ju
The cascade of sugar isomerases is one of the most practical methods for producing rare sugars, and enzyme immobilization endows it with high economic efficiency, operational convenience and reusability. However, the most employed cross-linker glutaraldehyde (GA) has the disadvantages of enzyme deactivation and limitation of substrate binding. Herein, three compounds, glyoxal, GA, and 2,5-furandicarboxaldehyde (DFF) were evaluated within a previously developed cascade comprising ribose-5-phosphate isomerase and D-tagatose-3-epimerase to prepare D-ribulose form D-xylose. Analyses of surface morphology, element and chemical bond revealed that all compounds effectively cross-linked the isomerases. High concentration of the cross-linkers was generally beneficial for binding protein and preventing enzyme leak during reusing cycles. Glyoxal performed the highest immobilization rate, though it hadn't been employed as a cross-linker for enzyme immobilization. DFF mediated cross-linking revealed the highest activity recovery, substrate conversion and residual activity after reusing cycles, suggesting better biocompatibility than glyoxal and GA. After 8 rounds of recycling, the residual activity of enzyme immobilized by DFF was 61.4 %, ∼30 % higher than that of GA. This study proved a potential alternative cross-linker DFF for the immobilization of enzyme cascade with high activity recovery and reusability, which could promote the efficient production of high value-added products from biomass monosaccharides.
研究领域:
生物化学
·
酶工程
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DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2026
·
IF 3.4
Chu Sun,Rui Bi,Chunhui Song,Deyang Zhao,Zhiguo Zhu,Kaixuan Yang,Christophe Len,Hongying Lü,Ting Su
2,5-Diformylfuran (DFF) is an important biomass-derived platform chemical, widely recognized as a key intermediate building block in the synthesis of biodegradable polymers and pharmaceutical compounds. The mild and sustainable nature of photocatalysis has attracted considerable attention for such valorization processes, highlighting the need for in-depth exploration of heterostructure-based photocatalysts to enhance catalytic performance. In this study, we report the fabrication and photocatalytic application of a Nb2CTx MXene/ZnIn2S4 (ZIS) Schottky heterojunction with intimate interfacial contact. This heterostructure significantly enhances the separation efficiency of photogenerated charge carriers while prolonging their lifetime. The observed enhancement is attributed to the synergistic interaction between the n-type ZIS semiconductor and the two-dimensional metallic conductor MXene, which induces favorable band bending in ZIS and facilitates the formation of a Schottky barrier at the MXene–ZIS interface. This barrier effectively inhibits electron backflow, thereby promoting charge carrier separation and enhancing interfacial charge dynamics. Compared to pristine ZIS, the Nb2CTx/ZIS heterojunction catalyst achieves a significantly higher DFF yield under ambient temperature and pressure, without the need for additional oxidants. This finding not only demonstrates a highly efficient route for DFF production under mild conditions but also offers a new design strategy for MXene-based Schottky heterojunctions in biomass valorization via photocatalysis.
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ChemCatChem
·
2026
·Vol. 18
·期 5
·e70637
·
IF 4.1
Yintao Song,Hang Zheng,Mengyuan Huang,Quanwei Deng,Luhui Lin,Yaqi Shi,Jiacheng Li,Chenting Yang,Lu Lin,Changlong Wang,Xing Tang
We have developed a highly efficient and stable non-noble metal-based heterogeneous catalyst for the selective oxidation of HMF to DFF. Mixed oxide catalysts with different Mn/Ni molar ratios were synthesized using the urea precipitation method. The Mn 6.6 NiO X catalyst exhibited a 95.33% HMF conversion rate and a 99.39% DFF selectivity under the conditions of 110°C, 2 h, 1 MPa O 2 , and N,N -dimethylformamide. Experimental results indicate that the introduction of NiO can effectively regulate the crystal structure of MnO 2 , forming an amorphous Mn─O─Ni interface, which significantly increases the specific surface area (SSA) of the catalyst while reducing the binding energy of surface lattice oxygen (O L ), promoting the generation of oxygen vacancies (O V ), and thereby enhancing the adsorption and activation capabilities of O 2 . Combined adsorption experiments and kinetic analysis revealed that Ni species preferentially anchor the hydroxymethyl group in HMF molecules, enhancing reaction selectivity. Further experiments demonstrated that the Mn 6.6 NiO x catalyst, under certain conditions, could achieve an HMF conversion rate of 87.52% and a DFF selectivity of 85.81% even at a high substrate concentration of 10 wt% HMF.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Bo Zhang,Xinlei Ma,Jing Zhang,Neyha Rubab Syed,Leilei Dai,Roger Ruan
This study presents a novel strategy of piezocatalysis driven by ball milling (BM) for the anaerobic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to high-value 2,5-diformylfuran (DFF) with simultaneous hydrogen (H₂) production. A rationally designed Schottky heterojunction (CS/MB) composed of 1D CdS nanorods (CS) and 2D MoB MBene nanosheets (MB) is synthesized, demonstrating strong interfacial coupling and efficient electron transfer (from CS to MB). The unique piezocatalytic system operates under mild mechanical energy input (600 rpm), achieving an exceptional 80.36% HMF conversion with 78.00% DFF yield (97.07% selectivity) and an H 2 evolution rate of 0.147 μmol/(mg catalyst ·h). This substantial enhancement, which achieved a 2.7-fold increase in DFF formation kinetics and a 1.8-fold boost in H₂ generation over pristine CS, signifies a clear breakthrough in piezocatalytic systems for coupled biomass oxidation and proton reduction. Mechanistic investigations via ESR spectroscopy and DFT calculations reveal that carbon-centered radicals mediate the selective oxidation pathway, while the Schottky junction at the CS/MB interface enhances charge separation, thereby suppressing recombination. By replacing conventional thermal/chemical inputs with mechanical activation, this work pioneers a self-sustaining bio-refinery paradigm where piezoelectric polarization and catalytic active sites cooperate as a unified energy-harvesting reactor. This strategy demonstrates a promising potential pathway for simultaneously advancing green chemical synthesis and renewable energy production.
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高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 48
·18473-18479
·
IF 4.569
Yan Zhou,Shanshan Lv,Han Li,Qikang Wu,Taiyu Chen,Shaohuan Liu,Wanying Li,Wenjuan Yang,Zheng Chen
The development and transformation of biomass-derived platform compounds is a sustainable way to deal with the fossil fuel crisis. 5-Hydroxymethylfurfural (HMF) can be reduced or oxidized to produce many high-value compounds; however, it is challenging to effectively produce 2,5-diformylfuran (DFF) due to overoxidation. In this work, a carbon-doped V2O5 (C–V2O5) material was obtained through pyrolysis of MIL-47(V) nanorods, a typical metal–organic framework material. The X-ray diffraction patterns and X-ray photoelectron spectra showed that the graphitized carbon species were incorporated in C–V2O5. High-efficiency HMF oxidation, high specific selectivity for DFF and excellent recycling could be achieved with the C–V2O5 catalyst. Fourier-transform infrared spectroscopy combined with density functional theory (DFT) calculation revealed that graphitized carbon weakens the VO bond and promotes the formation of oxygen vacancies in C–V2O5, thus improving the catalytic activity in the oxidation of furfuryl alcohols. The V4+ induced by oxygen vacancies will be oxidized by O2 to form V5+, so that the cycle can be realized. It exhibits remarkable selectivity in the oxidation of different alcohols produced from biomass based on the relatively constant active sites in C–V2O5.
研究领域:
材料科学
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催化
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化学工程
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可持续化学
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DOI
PubMed
高影响因子
Science China-Materials
·
2023
·Vol. 67
·期 1
·162-169
·
IF 8.1
Yang Bixia,Zhu Mengyao,Jiang Xingpeng,Shao Wenlei,Wang Zhiqi,Yan Jiawei,Zheng Yanting,Zhuang Zanyong,Yu Yan
The photooxidation of renewable bioderivatives into value-added chemicals is highly significant; however, it typically exhibits low selectivity owing to the challenges in controlling the oxidative species and managing the desirable reaction pathways. In this work, we used the Bi 2 O 2 CO 3 /ZnIn 2 S 4 heterostructure, prepared by a CO 2 -mediated solid–solid phase transition, to catalyze the photooxidation of bioderived 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) with a high selectivity of 98.1% and a yield rate of 882.6 µmol g −1 h −1 . The metal carbonate/oxide heterointerface enables the effective transfer of photoactive electrons and holes, optimizes surface oxygen activation, and facilitates the synergy of ·OOH and holes to selectively convert HMF into DFF. The findings unravel how the tailoring and coupling of the electron–hole pairs and reactive oxygen species on heterostructured materials can promote the usage of renewable feedstocks for sustainable development.
研究领域:
光催化
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环境化学
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材料科学
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绿色化学
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可再生能源
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DOI
高影响因子
ChemSusChem
·
2014
·Vol. 7
·期 12
·3496-3504
·
IF 7.117
Zehui Zhang,Ziliang Yuan,Dingguo Tang,Yongshen Ren,Kangle Lv,Bing Liu
Graphical Magnetic attraction: We have demonstrated an efficient and environmentally benign magnetic catalyst for the aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF). A high DFF yield of 89.1 % and an HMF conversion of 100 % were obtained after 4 h at 90 °C. Magnetic γ-Fe 2 O 3 nanocrystallites encapsulated by hydroxyapatite (HAP), HAP @ γ-Fe 2 O 3 , were prepared followed by cation exchange of Ca 2+ on the external HAP surface with Ru 3+ to give the γ-Fe 2 O 3 @ HAP-Ru catalyst. The structure of the as-prepared catalyst was characterized, and its catalytic activity was studied in the aerobic oxidation of 5-hydroxymethylfurfural (HMF). γ-Fe 2 O 3 @ HAP-Ru showed a high catalytic activity for the aerobic oxidation of HMF into 2,5-diformylfuran (DFF). A high DFF yield of 89.1 % with an HMF conversion of 100 % was obtained after 4 h at 90 °C. Importantly, the synthesis of DFF from fructose was realized by two consecutive steps. The dehydration of fructose in the presence of a magnetic acid catalyst (Fe 3 O 4 @SiO 2 SO 3 H) produced HMF in a yield of 90.1 %. Then the Fe 3 O 4 @SiO 2 SO 3 H catalyst was removed from the reaction solution with a permanent magnet, and HMF in the resulting solution was further oxidized to DFF with a yield of 79.1 % based on fructose. The synthesis of DFF from fructose by two steps avoids the tedious separation of the intermediate HMF, which saves time and energy.
研究领域:
催化
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材料科学
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绿色化学
·
有机合成
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DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Chenhui Xu,Yang Yang,Chengyang Hui,Pengfei Tang,Genlei Zhang,Jialun Liu,Zhenzhen Yang
Highly efficient synthesis of 2,5-diformylfuran (DFF) from 5-hydroxymethylfurfural (HMF) or fructose has attracted much attention in recent years. Herein, one-dimensional MoO2@a-NCx core–shell nanorods that oxygen vacancy-rich molybdenum dioxide (MoO2) coated with porous amorphous nitrogen-doped carbon layer (a-NC) are synthesized via pyrrole polymerization followed by pyrolysis, using orthorhombic molybdenum trioxide (α-MoO3) nanorods as a precursor. Benefiting from the well-engineered architecture and the strong interfacial interaction between MoO2 and surface carbon, the optimized MoO2@a-NC9 with an a-NC layer thickness of ∼9 nm exhibits considerable catalytic activity and stability in oxidation of HMF/fructose to DFF. Under optimal reaction conditions, MoO2@a-NC9 achieves nearly quantitative DFF yield of 99.1% with complete HMF conversion (100%) in the aerobic oxidation of HMF. A possible reaction mechanism involving a Mo4+/Mo3+ redox cycle is proposed for MoO2@a-NC9-catalyzed oxidation of HMF to DFF, based on experimental and characterization results. Furthermore, MoO2@a-NC9 served as a bifunctional catalyst for direct conversion of fructose to DFF via a “one-pot, two-step” approach, achieving a high DFF yield of 82.5%. Notably, this catalyst exhibits excellent recyclability, maintaining its catalytic performance over at least six reaction cycles without significant activity decay.
研究领域:
催化
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纳米材料
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绿色化学
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有机合成
·
能量转换
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Thi Le Cham-Bich,Nguyen Trinh Hao,Thi Le Mai Ngoc,Liem The Ho,Phuong Hoang Tran
The selective oxidation of biomass-derived carbohydrates into high-value platform chemicals represents a promising avenue for sustainable chemical production. In our work, we explored the catalytic performance of a bimetallic Fe/Cu loaded in carbon decorated with nitrogen-sulfur (Fe/Cu@NSC) in the conversion of fructose/glucose into 2,5-diformylfuran (DFF). The catalyst exhibited remarkable efficiency, particularly with fructose, achieving a peak DFF yield of 61.1% under optimized conditions. In contrast, glucose conversion proved less effective, with a maximum DFF yield of 29.1% at 160 °C for 15 h. Methodical examinations of reaction parameters, such as solvent composition, and reaction time, yielded crucial insights into the determinants of product dispersion and catalytic efficacy. Moreover, reusability evaluations demonstrated a slow reduction in catalytic activity throughout repeated cycles; yet, this negligible fall still affirms the promise of catalysts in green chemistry. In addition, the catalyst structure was evidenced by FTIR, XPS, HRTEM, SEM, BET, ICP-MS, NH 3 -TPD, EDX, elemental mapping analyses, and the thermal stability of the catalyst was evaluated by TGA. These findings underscore the potential of Fe/Cu@NSC as an effective and recyclable catalyst for DFF synthesis while highlighting the necessity for further optimization to enhance its long-term stability and performance.
研究领域:
催化化学
·
绿色化学
·
生物质利用
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可持续化学品生产
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材料科学
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DOI
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 5
·1335-1344
·
IF 5
Mei Hong,Yuxiang Liu,Haidi Sun,Liping He,Junkai Zhu,Huixian Wang,Shifa Wang,Licheng Li
Lignocellulosic biomass is a potential sustainable feedstock to replace fossil fuels. Utilization of lignocellulosic biomass in a green and effective way is of great significance for sustainable development. The direct, one-pot, one-step catalytic conversion of glucose to 2,5-diformylfuran is a challenging task. In this work, Al(NO3)3 has been heterogeneously supported on porous carbon derived from Na-lignosulfonate or a mixture of Na-lignosulfonate and Na-polystyrene sulfonate via ice-templating, mild pyrolysis (350 and 450 °C) and H+ exchange techniques to obtain bifunctional carbocatalysts (Al(NO3)3@LH or Al(NO3)3@LH–PH). The catalysts were characterized by Fourier transform infrared (FT-IR), pyridine adsorption infrared (Py-IR), X-ray diffraction (XRD), X-ray photoelectron spectra (XPS), field emission scanning electron microscopy (FE-SEM), energy dispersive X-ray spectroscopy (EDS) and Brunauer–Emmett–Teller (BET) analyses. A novel one-step cascade method of producing DFF directly from glucose through the binary catalyst Al(NO3)3@LH or Al(NO3)3@LH–PH with AlBr3 in 99% DFF yield without the need for a strong oxidant is described. Mechanistic studies show that the cascade conversion of glucose involves isomerization, dehydration and successive Kornblum-type oxidation. Moreover, the catalysts could be reused in consecutive runs, exhibiting a slightly lower activity in the synthesis of DFF from glucose.
研究领域:
化学工程
·
催化
·
可再生能源
·
绿色化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）