FUEL
·
2024
·
IF 6.7
Renjie Ji,Defu Yin,Yao Chen,Like Ma,Fanglin Lv,Yuhao Zhang,Zhen Jia,Jingyun Zhang,Mingya Liu,Shitao Yu,Yue Liu
A core–shell catalyst mZSM-5@SO 4 2- /mSiO 2 composed of mZSM-5 core and SO 4 2- /mSiO 2 shell was prepared by the soft template method. Core-shell structure could promote the building of Brønsted -Lewis (B-L) acids interface and significantly improve the synergistic effect of B-L. In this paper, the Brønsted/Lewis (B/L) of mZSM-5@SO 4 2- /mSiO 2 was targeted regulating by innovatively introducing Brønsted acid (BA) sites into the shell. The optimal mZSM-5@SO 4 2- /mSiO 2 catalyst (B/L = 0.142) could achieve 72.1 % furfural yield at 140 ℃ for 1 h. In addition, 70.2 % furfural yield could be obtained after the catalyst was recycled and regenerated for 5 times. Combining In-situ IR and 13 C NMR, the reaction path was revealed in detail: xylose was first isomerized to xylulose and then dehydrated to furfural. This paper provides a research idea for the directional regulation of dual active sites of cascade reaction catalysts.
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2024
·Vol. 26
·期 12
·7140-7155
·
IF 9.3
Yunhan Bai,Jianqi Tang,Xiaoshu Ding,Xinqiang Zhao,Yanji Wang
Given the enormous safety risks and environmental pollution that restrict the green development of isocyanate produced by phosgene reactions, we propose a new green and intrinsically safe route for synthesizing diisocyanates containing the furan ring from 5-hydroxymethylfurfural. In this work, the following novel reactions have been systematically investigated, including synthesizing a new compound methyl furan-2,5-dimethylene dicarbamate (FDC) using 2,5-bis(aminomethyl)furan (BAF) and dimethyl carbonate (DMC), the selective hydrogenation of FDC to a new compound methyl tetrahydrofuran-2,5-dimethylene dicarbamate (THFDC), and FDC and THFDC catalytic decomposition to produce corresponding furan-2,5-dimethylene diisocyanate (FDI) and tetrahydrofuran-2,5-dimethylene diisocyanate (THFDI). The results showed that CH3ONa could effectively catalyze the synthesis of FDC from BAF and DMC, and the separation yield of FDC was 98.1% under mild conditions including a nBAF : nDMC ratio of 1 : 10 at 70 °C for 4 h. CH3ONa can be recycled up to four times with high stability. A 0.5% Pd/γ-Al2O3 catalyst with low Pd loading was prepared, and it showed high catalytic activity and stability for FDC hydrogenation to THFDC, with a THFDC yield of 99.9% at 100 °C, 2 MPa H2 and 1 h, and the catalyst could be reused after simple treatment with ethanol. The structure–activity relationship of supported Pd catalysts was studied. The conditions for the thermal decomposition reactions of FDC and THFDC were optimized, resulting in FDI and THFDI yields as high as 89.6% and 92.8%, respectively. Owing to the urgent need for raw materials sustainability and environmental friendliness, the brand-new safe pathway for synthesizing FDI and THFDI was constructed, significantly improving the competitiveness of the non-phosgene method in preparing bio-based isocyanate.
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2024
·
IF 3.4
Chenan Yang,Yi Liu,Ying Hu,Peng Wang,Yuling Yang,Shangxing Chen,Zongde Wang,Xiang Li
Catalytic valorization of biomass into high energy density fuels plays a vital role in order to achieve future carbon neutrality. Herein, a class of H-MZ-5 catalysts with different mesoporous pore structures and acid site properties were synthesized. Among them, HMZ-5 prepared with tetrapropylammonium bromide (TPABr) and hexadecyltrimethylammonium bromide (CTAB) as templating agents showed the most excellent catalytic activity and selectivity of α-pinene dimerization. Under optimal catalytic conditions, 100% α-pinene was converted with 89.6% selectivity to dimers. The efficient catalytic activity and affordability of the catalysts in this system make it promising for industrial applications.
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2024
·Vol. 14
·期 4
·248
·
IF 3.8
Xinyi Xing,Wanni Liu,Siquan Xu,Jianxiu Hao
H-Beta zeolite is a solid acid catalyst commonly utilized in the catalytic conversion of biomass resources. In this study, H-Beta zeolite was calcined at different temperatures (350, 550, 750, and 1000 °C) to explore the effects of high temperature-induced dealumination on its physicochemical properties and its catalytic ability to convert glucose into 5-hydroxymethylfurfural (HMF). It was shown that as the calcination temperature increased, the Si-O-Al bond of H-Beta zeolite was broken and its dealumination effect was enhanced. Dealumination led to the collapse of the framework of H-Beta zeolite and a reduction in the number of acid sites, which in turn reduced its catalytic performance and the efficiency of HMF formation from glucose. Furthermore, H-Beta zeolite exhibited an extraordinary catalytic ability for the production of HMF from carbohydrates. Using glucose and cellulose as substrates, superior HMF yields of 91% and 46%, respectively, were achieved under optimal reaction conditions. Further, calcination removes carbon deposits in the recovered H-Beta zeolite, but it affects the cycling stability of the catalyst. Meanwhile, the by-products formed during the synthesis of HMF from glucose catalyzed by H-Beta zeolite catalyst were also clearly detected.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Xingyilong Zhang,Houfang Lu,Kejing Wu,Yingying Liu,Yingming Zhu,Bin Liang
Fructose dehydration produces 5-hydroxymethylfurfural (HMF), which is a versatile precursor for clean fuels, advanced biofuels and fuel additives. Hierarchical porous carbon-based solid acid (HPCSA) was applied to catalyze fructose dehydration to produce HMF in dimethyl sulfoxide (DMSO). The active sulfonic acid groups were grafted onto the hierarchical porous carbon prepared from waste alkali lignin in paper industry using SiO 2 and CaCl 2 dual templates. The interconnected macropores and large specific areas benefit to loading S content and improve accessibility of active acid sites to fructose molecules. The results show that HPCSA achieves the HMF yield of 90 % at 110 °C for 90 min with 1 wt% catalyst loading. Under same numbers of acids, the yield of HMF with HPCSA as catalyst is 6.7 and 1.4 times higher than that of sulfonated activated carbon and sulfonated nonporous carbon, respectively. Macropores promote accessibility of fructose to active sites and avoid the local concentration of HMF in catalyst, and high acid loading are also the key factors to improve the catalytic activity of HPCSA. The activity of reused HPCSA can be easily recovered via sulfonation.
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Nanomedicine
·
2025
·
IF 6.5
Jia Zhang,Xiaotuan Zhang,Zhuocheng Yao,Juan Pan,Jianzhong Ye,Ping Xia,Tieli Zhou,Jianming Cao
Introduction Carbapenem-resistant gram-negative bacteria (CR-GNB) pose a significant threat to public health and require immediate attention. The development of novel antibacterial agents against CR-GNB has become an urgent priority, and nanomaterials offer promising solutions due to their unique properties. This study introduces 5-amino-2-mercaptobenzimidazole (5-A-2MBI) functionalized gold nanoparticles (5-A-2MBI_Au NPs) and evaluates their antibacterial activity against CR-GNB.Methods The 5-A-2MBI_Au NPs was synthesized using a one-pot method. Its biocompatibility, bactericidal properties, and mechanisms of action were systematically characterized through in vivo and in vitro toxicity tests, antimicrobial susceptibility testing, live/dead staining, membrane permeability and reactive oxygen species (ROS) generation assays, as well as transcriptomic analysis.Results The results of this study demonstrate that 5-A-2MBI_Au NPs exhibit excellent antibacterial efficacy against carbapenem-resistant gram-negative bacteria with various resistance mechanisms, with a minimum inhibitory concentration (MIC) of 2 μg/mL. In vivo experiments further confirmed that 5-A-2MBI_Au NPs not only possess effective bactericidal activity but also exhibit satisfactory biocompatibility. Mechanistic studies revealed that 5-A-2MBI_Au NPs enhance bacterial membrane permeability, increase the generation of reactive oxygen species, and disrupt intracellular oxidative stress and succinate synthesis, thereby conferring potent antibacterial activity. This study results demonstrate that 5-A-2MBI_Au NPs exhibit notable antibacterial efficacy against CR-GNB, with a minimum inhibitory concentration of 2 μg/mL. The antibacterial mechanism involves enhanced membrane permeability, increased reactive oxygen species production, and interference with intracellular oxidative stress and succinate synthesis. These mechanisms collectively contribute to the potent antibacterial activity of 5-A-2MBI_Au NPs against CR-GNB.Discussion 5-A-2MBI_Au NPs are a novel and highly effective antibacterial agent prepared through a simple process using benzimidazole and HAuCl4•3H2O. They efficiently eradicate the most challenging multidrug-resistant GNB both in vitro and in vivo while demonstrating excellent biocompatibility. This highlights their potential as a promising antibacterial agent to combat multidrug-resistant GNB.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RENEWABLE ENERGY
·
2025
·
IF 9.1
Feipeng Wang,Huiting Zhao,Yuan Zhang,Feng Song,Hongzi Tan,Fangyong Yu,Hongyou Cui,Yujiao Xie
Cellulose, one of the most abundant renewable biomass resources, can be converted into valuable chemicals like 5-hydroxymethylfurfural (HMF). This study explores an efficient strategy using mixed metal salts for the conversion of cellulose to HMF. The catalytic performance of both single and mixed metal salts was examined, showing CrCl 3 –SnCl 4 to be highly effective, achieving a maximum HMF yield of 54.8% under optimal conditions (CrCl 3 :SnCl 4 = 2:3, 180 °C). Ultraviolet-visible spectroscopy (UV) and electrospray ionization-mass spectrometry (ESI-MS) analyses revealed that the mixed solution generates multiple catalytic active species, which enhance the conversion of substrates to HMF. The developed kinetic model indicates that the conversion process is highly temperature-sensitive, and the production of HMF from glucose is more favored compared to the hydrolysis of cellulose. The findings from this study provide a deeper understanding of the catalytic process, offering a promising approach for efficient biomass conversion, which is crucial for advancing sustainable chemical production technologies.
✓ 已验证
产品关联
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2024
·Vol. 137
·期 4
·1911-1925
·
IF 1.7
Song Linyan,Nie Genkuo,Chen Xiulei,Wang Hongyu,Liu Shiwei,Yu Hailong,Liu Xuguang,Yang Guihua,Yu Shitao
The multifunctional groups of 5-hydroxymethylfurfural (5-HMF) make it could extend carbon chain by different C–C coupling reactions and extensively applied in the bio-jet fuel synthesis. Herein, one-pot reaction of lignocellulose derived chemicals with 5-HMF was studied by experimental and density functional theory (DFT) methods. The kinetic models of products were established and the apparent activation energies of the products by C–C coupling reaction of phenol, anisole, guaiacol, cyclohexanone and acetone with 5-HMF on Hβ were 95.3 kJ/mol, 104.8 kJ/mol, 90.4 kJ/mol, 90.0 kJ/mol and 112.2 kJ/mol, indicating these reactions centering on 5-HMF competitive intensively. Then the effects of the catalysis were analyzed by applying commercial catalysis to the mixed coupling reaction of 5-HMF. It was found that Brønsted acid is more favorable to alkylation reaction, and Lewis acid is more beneficial to aldol condensation reaction. By Fukui function, due to the nucleophilic index of cyclohexanone (2.74 eV) is higher than that (2.48 eV) of acetone, and the Mulliken electronegativity (3.43 eV) is weaker than that (3.55 eV) of acetone, cyclohexanone is more conducive than acetone to the aldol condensation reaction. This work provides data reference for product regulation in the bio-jet fuel synthesis.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Huan Wang,Weitao Wang,Yihong Ma,Jiaqi Zhu,Zhen-Hong He,Zhao-Tie Liu,Buxing Han
5-Hydroxymethylfurfural (HMF) can be upgraded to ether as fuel or fuel additives through conversion of the hydroxyl and aldehyde groups. The two groups are always involved in different catalytic reactions, such as etherification, acetalization, hydrogen transfer reduction, and even ring-opening reactions. This makes the etherification upgrading of HMF with high selectivity to desired product a great challenge. In the present wok, transformation of HMF in isopropanol was systematically investigated over different catalysts with Brønsted acid and Lewis acid sites. The effect of catalytic sites on product distribution and selectivity was studied. Moreover, several products, such as 5-isopropoxymethylfurfural, 5-isopropoxymethylfurfuryl alcohol, 5-isopropoxymethylfurfuryl alcohol, and 2,5-furandimethanol, were obtained with high selectivity, and the conversion pathway of HMF with alcohols on different catalytic sites was revealed under different catalytic conditions. The transformation of HMF to furan triether products over multi-site catalyst was realized for the first time based on the proposed reaction pathway with excellent activity and selectivity.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jinxiu Qian,Fan Yang,Hongchen Liu,Guohua Li,Siyuan Sun,Xiaoyun Zhang,Guang Ma,Jiating Cheng,Mingjie Li,Ni Wu,Xi Li,Yongfeng Li
Achieving efficient production of hydrogen and obtaining high value-added products can maximize energy efficiency, but challenging. Herein, a nanoarray-structured heterojunction catalyst (CoP-MoO 2 /NF) was proposed as a potent bifunctional electrocatalyst for hydrogen evolution reaction (HER) and 5-hydroxymethylfuran oxidation reaction (HMFOR). Density Functional Theory (DFT) showed that heterojunction enhanced the adsorption of reactants on the electrocatalyst surface, the CoP-MoO 2 /NF exhibits excellent HER activity with an overpotential of 37 mV and a Tafel slope of 43 mV·dec −1 at 10 mA·cm −2 . Also, nearly 100% HMF conversion and 98.6% FDCA selectivity demonstrate the favorable performance of the material toward HMFOR. The work here shows a way for producing hydrogen in the future that is low-cost, efficient, reliable and also adds value to the final product.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Ke-Juan Meng,Kunyu Xiong,Iftikhar Hussain,Momang Tian,Xinwen Ma,Yuxiang Li,Qi-Long Yan,Kaili Zhang
Advanced energetic composites possess promising properties and wide-ranging applications in explosives and propellants. Nonetheless, most metal-based energetic composites present significant challenges due to surface oxidation and low-pressure output. This study introduces a facile in situ method to develop energetic composites Cutztr@AP through the intermolecular assembly of nitrogen-rich energetic coordination polymers and high-energy oxidant ammonium perchlorate (AP). Morphological analysis reveals the unique structure of Cutztr@AP, where Cutztr is distributed throughout the interior and surface of the AP particles. The nonisothermal thermodynamic analysis reveals a heat release of 2378.2 J g–1 for Cutztr@AP2, outperforming the Cutztr/AP2 achieved through ultrasonic mixing (2000 J g–1). Notably, Cutztr@AP2 exhibits promising combustion and pressure output performances, including a significantly shorter duration, a larger flame area, and higher pressure values. This novel and facile preparation technique and microstructure design approach holds significant promise for high-performance propellants, gas generators, and other related applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Mengjiao Yu,Xiong-Fei Zhang,Siting Yang,Yunhua Bai,Zhongguo Wang,Jianfeng Yao
Developing functional catalysts with both Lewis and Brønsted acid sites is an essential task for achieving the direct conversion of glucose to 5-hydroxymethylfurfural (5-HMF), a process that is crucial for the sustainable production of renewable fuels and chemicals. In this work, a mixed-linker strategy is proposed to prepare defective MIL-53(Al)-NH 2 by introducing trifluoroacetic acid into the MIL-53(Al)-NH 2 synthesis process. The creation of defects facilitates the exposure and accessibility of Al 3+ centers, as well as changes the coordination environment within the MIL-53(Al)-NH 2 skeleton. Both the number of Lewis and Brønsted acid sites are boosted, which is beneficial for glucose activation and 5-HMF generation. Through optimizing the reaction conditions, a glucose conversion of 98.3 % with a 5-HMF yield of 59.3 % was achieved by using defective 6d-MIL-53(Al)-NH 2 in a biphasic tetrahydrofuran/H 2 O NaCl system. Moreover, the 6d-MIL-53(Al)-NH 2 catalyst showed excellent recyclability and reusability, with its catalytic efficiency maintained almost unchanged for consecutive 10 cycles. The catalytic mechanism was elucidated and the acidity of the Lewis and Brønsted acid was modulated by defect engineering to achieve exceptional performance.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）