ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Wei Li,Zixia Hu,Chenyang Jia,Wei Guo,Weiwei Li,Ying Peng,Jiang Zheng
Human exposure to furan-containing pollutants (FCPs) has raised concerns due to their high risk of toxicity. A substantial number of approximately 8500 recorded compounds containing a furan ring exist which have been analytically or in biologically studied. A significant portion of these compounds is found in the everyday environments of individuals, particularly when ingested through food. Consequently, there is a need for a universal approach to rapidly predict the potential toxicity trends of FCPs. In this study, we developed a bromine labeling-based platform that combines LC-ICP-MS and LC-ESI-MS techniques to absolutely quantify FCP-induced protein adduction. The LC-ESI-MS approach facilitated the identification of FCP-derived protein adducts and optimized liquid chromatographic conditions for analyte separation. By employing a well-designed bromine-containing compound as a general internal standard, LC-ICP-MS-based technique enabled to absolutely assess bromine-labeled protein adduction. The protein adduction efficiencies of furan, 2-methylfuran, and 2,5-dimethylfuran were found to be 2.68, 2.90, and 0.37 molecules per 10,000 FCP molecules that primary hepatocytes received, respectively. Furthermore, we observed that 2-methylfuran exhibited the highest cytotoxicity, followed by furan and 2,5-dimethylfuran, which aligned with the order of their protein adduction. Thus, the protein adduction efficiency of FCPs could serve as a potential index for predicting their toxicity trends.
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ACS Catalysis
·
2024
·
IF 11.3
Wei Gao,Guodong Qi,Chao Wang,Qiang Wang,Jiawei Liang,Jun Xu,Feng Deng
The co-aromatization of methane and organic compounds using metal-modified zeolite catalysts represents a promising approach for the direct conversion of natural gas into valuable aromatics. In this work, we employ solid-state nuclear magnetic resonance (NMR) spectroscopy to systematically examine the reaction mechanism and evaluate the impact of co-feeding furan on methane aromatization over Mo/ZSM-5 zeolite. The results reveal a dual role of furan in promoting methane to aromatics and stabilizing the Mo/ZSM-5 zeolite catalyst in the co-aromatization. It is found that co-feeding a moderate amount of furan enhances methane conversion and boosts the selectivity to benzene, toluene, and xylene (BTX). The 12C/13C isotope switching experiments coupled with 1H and 13C MAS NMR spectroscopy reveal that furan actively participates in the methane aromatization reaction by forming an olefin pool, which promotes methane activation and contributes to the following aromatics formation. Two-dimensional 1H–95Mo heteronuclear correlation NMR spectroscopy indicates that furan facilitates the activation of Mo oxides into MoOxCy species, which serve as the active sites for methane aromatization. The co-feeding furan also helps to enhance catalyst stability by limiting the agglomeration of Mo and the deposition of coking species.
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ACS Catalysis
·
2017
·
IF 10.614
Chengtao Wang,Zhiqiang Liu,Liang Wang,Xue Dong,Jian Zhang,Guoxiong Wang,Shichao Han,Xiangju Meng,Anmin Zheng,Feng-Shou Xiao
The metal-catalyzed selective hydrogenation of biomass-derived molecules is in great demand but is challenging due to the complex reaction pathways. Herein, we report a persuasive example for achieving selective hydrogenation of furfural over Pd catalysts by controllable sorption of molecules in zeolite micropores. The key to this success is fixation of Pd nanoparticles inside of silicalite-1 zeolite with controllable wettability (Pd@S-1-OH) by functionalizing silanol groups into the zeolite framework. In the hydrogenation of furfural as a model reaction, the Pd@S-1-OH catalyst with appropriate hydrophilicity exhibits extraordinary selectivity for the formation of furan, giving furan selectivity as high as >99.9% with a complete conversion of furfural, outperforming the conventional Pd nanoparticles supported on zeolite crystals (Pd/S-1) and S-1 zeolite fixed Pd catalysts without an artificially functionalized silanol group (Pd@S-1). The extraordinary performance of Pd@S-1-OH is reasonably attributed to the controllable diffusion of molecules within the hydrophilic zeolite micropores, which favors the adsorption of furfural and a series of byproducts but promotes the desorption of furan. Very importantly, Pd@S-1-OH is stable and gives the furan productivity of ∼583.3 g gPd–1 day–1 in a continuous test.
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CHINESE JOURNAL OF POLYMER SCIENCE
·
2018
·Vol. 36
·期 6
·720-727
·
IF 2.016
Wang Jing-Gang,Liu Xiao-Qing,Zhu Jin
2,5-Furandicarboxylic acid (2,5-FDCA) has been regarded as the ideal bio-based alternative to terephthalic acid (TPA). In recent years, great efforts have been made to synthesize 2,5-FDCA through the following methods: (1) oxidation of 5-hydroxymethylfurfural (HMF) in the presence of complex biocatalyst or metallic catalyst; (2) conversion of 2-furoic acid via the well-known Henkel Reaction. Herein, a new strategy for the synthesis of 2,5-FDCA from furan and acetic anhydride under mild condition is reported. The purity of the resulted 2,5-FDCA was above 99.9%. Acetic acid and iodoform generated in the reaction were recyclable and no other harmful by-products were detected. The thus-obtained 2,5-FDCA was applied for the preparation of poly(ethylene furandicarboxylate) (PEF) of high quality in terms of high molecular weight and good appearance.
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Lingli Ni,Jiayu Xin,Kun Jiang,Lu Chen,Dongxia Yan,Xingmei Lu,Suojiang Zhang
Aromatics play essential and unique roles in the areas ranging from synthetic chemistry to the manufacturing industry. Production of aromatics from biomass is of great fundamental interest and practical importance to ease the burden of fossil resources. This work delineates a one-step route for the synthesis of renewable aromatics from various biobased furanics and dienophiles by acidic ionic liquids at mild conditions. [Bmim]HSO4 was used as a catalyst and solvent for the direct conversion of 2,5-dimethylfuran and acrylic acid into p-xylene and 2,5-dimethylbenzoic acid; up to 89% aromatic selectivity was achieved at 87% conversion of 2,5-dimethylfuran at room temperature and atmospheric pressure, and totally 84% selectivity of p-xylene can be obtained with a subsequent decarboxylation reaction. The reaction mechanism study supplemented with isotopic tracing and DFT calculations revealed the lowest-energy pathway for the two main products. Various starting materials were studied for further extensions of the method, and it turned out that electron-donating methyl groups on the furan ring played crucial roles on the activation of dehydration and decarboxylation processes. This work provided convenient access to industrial commodity aromatics from fully biomass-derived feedstocks and thus can be regarded more economically and environmentally feasible.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Xianlong Liu,Yiting Zhao,Gewei Zhang,Chengxiang Shi,Lun Pan,Xiangwen Zhang,Ji-Jun Zou
Attention has been drawn to the potential of renewable biomass as an alternative to petroleum-based feedstocks for the synthesis of high-density fuels given the depletion of petroleum resources and critical environmental issues. In this study, fused ring high-density liquid fuel precursors were directionally synthesized from biofuran derivatives by the Diels–Alder reaction. The impact of different dienophiles on the Diels–Alder reaction of 2-methylfuran facilitated by zeolites was evaluated. The influences of the catalyst, reaction temperature, and reactant ratio on the reaction were explored. Moreover, this study emphasized the specific synthesis of high density fuels by examining the significant influence of the substrate structure on the Diels–Alder reaction. When preparing polycyclic structures through Diels–Alder reactions of furan derivatives, it is advisible to consider monosubstituted furan derivatives first due to their high electron density and suitable steric resistance. The insights gleaned from this study provide substantial guidance for selecting suitable feedstocks for fuel synthesis, further contributing to sustainable energy solutions.
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TALANTA
·
2024
·
IF 5.6
Hao-Jie Bai,Hong-Wei Li,Yi Li,Zhijiu Huang,Sha Liu,Xin-He Duan,Yuqing Wu
Detecting the furfural concentration in Baijiu can be used to assess the quality of Baijiu , allowing for the optimization of processing techniques and the enhancement of overall quality. In this paper, a fluorescence-enhanced method based on carbon dots ( o -CDs) is developed for the furfural determination in Chinese Baijiu . In an environment full-filled with · SO 4 ‐ and · OH , furfural undergone a direct surface reaction with the ortho -diamino groups at o -CDs. The created furan-based imidazole increased the surface electron density, leading an emission enhancement and color changes from orange to green. Thereby, a linear fluorescence response of o -CDs-TA to furfural is established in water with a detection limit of 30.5 nM. Finally, after ethanol correction it is used to determine furfural in Chinese Baijiu with high precision and reproducibility, providing a new strategy with low-cost and high sensitivity. In particular, the idea of covalently connecting target molecule to the CDs surface via the assistance of free radical opens a new avenue to merge the nanoscale and molecular realms through implementing chemical role into carbon nanostructures.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Huichun Huang,Changhong Wang,Tingting Wu,Zhuohui Wu,Junxin Zheng
Thermal stress resulting from excessive temperatures is a major cause of electronic device failure. In this work, with easy installation and good interface adaptability, Phase Change Thermal Interface Materials (PCTIMs) which possess high thermal conductivity were prepared. By incorporating phase change material stearic acid (SA) into the thermal interface material, the instantaneous heat absorption during the solid-liquid phase transition of SA effectively alleviates the problem of instantaneous high heat flux impacting electronic devices. Additionally, the solid-liquid transition reduces the modulus of TIMs, thereby minimizing the contact thermal resistance between the heat source and the heat sink during mechanical installation. To further enhance performance, the thermal interface material utilizes a dynamically cross-linked polyolefin elastomer (POE) with borate bonds, which effectively restricts the flow of SA even at its phase change point due to the three-dimensional cross-linked framework. By constructing a thermal conductive network using carbon fibers and aluminum nitride of different dimensions, the thermal conductivity of the thermal interface material reached 1.82 W∙m −1 K −1 with a filler content of only 30 vol % . At 70 °C, with a force of 50 N applied to a sample area of 400 mm ² , the contact thermal resistance was only 2.39×10 −4 K∙m 2 W −1 . Furthermore, the PCTIMs exhibits excellent self-healing ability under thermal conditions, assuring the permanent encapsulation of small electronic devices.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Han Yin,Yanqing Wang,Dazhi Zhang,Yue Hu,Xiaoqin Si,Xuhai Zhu,Rui Lu,Zhenggang Liu,Xiangtao Kong,Fang Lu
Aromatic poly(carboxylic acid)s, especially terephthalic acid and pyromellitic acid, are extremely important monomers for polyester and polyimide manufacture. Current industrial processes predominantly rely on halogen-promoted oxidation reactions, which require specialized equipment and cause serious environmental pollution. Herein, a novel route was developed to synthesize pyromellitic acid from biomass-derived furanic platform chemicals. The process begins with a Diels–Alder reaction between furan and dimethyl acetylenedicarboxylate, forming an oxygen-bridged cyclohexadiene structure with a yield of 84.4%, and the cycloaddition strategy can also be applied to a variety of substituted furan-based feedstocks. The central diene of dimethyl furan-3,4-dicarboxylate was achieved via a cascade of selective hydrogenation and a retro-Diels–Alder reaction, with an isolated two-step yield of 92.8%. Subsequently, Diels–Alder, deoxy-aromatization, and hydrolysis reactions were integrated to efficiently produce pyromellitic acid, achieving yields higher than 91.3% in each step. Hence, the overall yield of the target product was approximately 65.1%, originating from furan. Preliminary green metrics and life cycle assessment were conducted to calculate the consumption and emissions of the process, thereby indicating its potential environmental friendliness. This work provides an effective methodology for the synthesis of crucial aromatic compounds through the precise design of Diels–Alder and retro-Diels–Alder reactions, paving the way for the production of environmentally friendly polyimide materials from renewable biomass.
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Molecular Catalysis
·
2024
·
IF 3.9
Zhijiao Huang,Yong Liu,Lungang Chen,Xinghua Zhang,Jianguo Liu,Chenguang Wang,Qi Zhang,Longlong Ma
2,5-dimethylfuran (DMF), a promising biomass-derived fuel, is synthesized via the hydrodeoxygenation of 5-hydroxymethylfurfural (HMF). This study focuses on the inherent activity of a 5Pt5Fe/C catalyst for HMF hydrodeoxygenation to DMF. The catalyst exhibited exceptional performance, achieving a remarkable DMF yield of 99.6 %. It displayed specific selectivity for C = O bond hydrogenation and C O bond cleavage in diverse substrates, producing high yield of 2-methylfuran from furfural and furfury alcohol, and high yield of toluene from benzaldehyde, benzyl alcohol. In-depth characterizations unveiled valuable insights into the 5Pt5Fe/C catalyst's properties, emphasizing a harmonious balance between metal and acid sites due to the interactive synergy between Pt and Fe species, enhancing hydrodeoxygenation activity. Additionally, the catalyst demonstrated satisfactory stability, maintaining a commendable DMF yield over five reaction cycles despite observed changes.
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Journal of Future Foods
·
2025
·
IF 7.2
Bowen Guo,Aisha Liu,Xuhan Xie,XueCheng Zhang,Yusen Chen,Tingting Zhou,Huan Zhao,Kairui Zhai,Biao Zhang,Xiaoping Yu,Ying Wang,Xiaodong Lin
The detection of acetamiprid residues is crucial due to its extensive agricultural use and potential health and environmental risks. Traditional methods, hindered by complexity, time consumption, and reliance on advanced equipment, fail to meet the demand for rapid, on-site detection, which is essential for ensuring Chinese herbal medicine safety and regulatory compliance. In this work, we present a triple-modal fluorescence immunochromatographic assay for multi-scenario detection of acetamiprid. Our work pioneers a triple-modal fluorescence immunochromatographic assay (FICA) integrating. The visual screening limit of detection (LOD) of 50.0 ng/mL for acetamiprid on-site assessment during harvesting have been achieved (Mode 1). The cross-scenario detection ranges spanning 5 orders of magnitude (0.1-1000 ng/mL) with LOD of 0.014 ng/mL have been realized via the developed portable immunoanalyzer quantification for regulatory inspection (Mode 2). The smartphone-based quantification detection (Mode 3) enabling consumer self-testing has displayed a good linear relationship towards acetamiprid in the range of 10-1000 ng/mL with LOD of 1.0 ng/mL. Validated in real samples matrices with recovery rates of 87.2-109.3% (RSD <5.0%), the proposed triple-modal fluorescence immunochromatographic assay has an acceptable recovery rate and stability in determination of acetamiprid in real samples. This study introduces the first integrated triple-modal fluorescence immunochromatographic assay platform, offering an effective detection tool compatible with diverse application scenarios across the traditional Chinese herbal medicine supply chain.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Wenpeng Han,Shujuan Wang,Fujiang Geng,Lei Liu,Ruidi Wei,Mingxing Tang
An efficient and selective nickel-molybdenum nitride catalyst has been developed for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to produce 2,5-dimethylfuran (DMF). The results showed that Ni2Mo3N phase of the catalyst exhibited good hydrogenation activity for HMF, while Ni6Mo6C1.06 phase demonstrated effective C-O bond hydrogenolysis activity. By regulating the Ni/Mo molar ratios, the proportions of the Ni2Mo3N and Ni6Mo6C1.06 phases can be adjusted, and the NiMoNx (Ni:Mo=1:2) catalyst with good performance was prepared. Additionally, 2-propanol, as a good solvent, can react with HMF to form ethers, facilitating easier hydrogenolysis. This method leads to full conversion of HMF, achieving a 99% yield of DMF at 160 oC and 2 MPa H2 for 5 h. Furthermore, the catalyst displayed good recyclability, maintaining its activity over 4 cycles, indicating it has the potential application for the industrialization of 5-HMF hydrogenolysis to produce DMF.
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