CRYSTENGCOMM
·
2020
·Vol. 22
·期 21
·3670-3682
·
IF 3.117
Xia-Lin Dai,Chao Wu,Jin-Hui Li,Lian-Chao Liu,Xin He,Tong-Bu Lu,Jia-Mei Chen
5-Fluorouracil (5FU) is a classical anti-metabolic drug with broad-spectrum antitumor effects. However, the oral absorption of 5FU is incomplete with a short biological half-life and an obvious peak-valley phenomenon, leading to the frequent administration requirement and severe side effects. Herein, a pharmaceutical cocrystallization approach based on crystal engineering was employed to modulate the pharmacokinetic properties of 5FU by changing its aqueous solubility. Four cocrystals of 5FU with a group of dihydroxybenzoic acids were synthesized and characterized. The powder dissolution experiments showed that all the cocrystals exhibited different aqueous solubilities and dissolution rates in comparison with pure 5FU. As compared to pure 5FU, the apparent solubility values of two cocrystals were increased by 34% and 11% while those of the other two cocrystals were reduced by 27% and 51%, respectively. The pharmacokinetic parameters of all the cocrystals, including Cmax, tmax, MRT0–t, t1/2 and AUC0–t, as well as the shape of the pharmacokinetic curves, were accordingly altered in the in vivo pharmacokinetic study. This study has important implications for using cocrystallization techniques to modulate the pharmacokinetic properties of drugs with undesirable oral absorption, especially to avoid the in vivo peak-valley effect and reduce side effects in clinical practice.
研究领域:
药物化学
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药理学
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晶体工程
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DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 26
·19823-19829
·
IF 3.84
Zhenzhen Miao,Tianxiao Wu,Jingwei Li,Ting Yi,Yibo Zhang,Xiangguang Yang
The oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) was efficiently catalyzed when Pt nanoparticles (NPs) were supported onto a Ce0.8Bi0.2O2−δ solid solution. 98% yield of FDCA was achieved within 30 min at room temperature and the catalyst was reused five times without much loss of FDCA selectivity. It is the first report on the oxidation of HMF, an alcohol and an aldehyde, effectively catalyzed by a ceria-based material supported Pt catalyst. The individual properties of the Pt NPs and the ceria-based support were retained and not affected after their combination. The superior oxygen activation ability of the Bi-doped ceria thoroughly changed the performance of the ceria supported Pt catalyst. Pt NPs were responsible for the formation of the Pt–alkoxide intermediate, followed by β-H elimination with the help of hydroxide ions. Bi-containing ceria accelerated the oxygen reduction process because of the presence of a large amount of oxygen vacancies and the cleavage of the peroxide intermediate promoted by bismuth. These specific functions were well incorporated during the catalytic oxidation cycle, leading to the generation of the highly efficient Pt/Ce0.8Bi0.2O2−δ catalyst for HMF oxidation at room temperature.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 4
·e202404857
·
IF 2
Wei Jiang,Chenkang Zhao,Yanfeng Liu,Yu Zu,Hongyu Guo,Guanghui Zhao,Weizhong Wang,Yong Sun
Graphical In this study, a straightforward coprecipitation method was employed to synthesize the bimetallic catalyst MnO@Co-CN, which demonstrates high efficiency in catalyzing the direct oxidative esterification of HMF to produce FDMC with a yield reaching 90.3%. The synergistic interactions between the dual metals during the reaction significantly enhance the catalytic performance for optimal oxidative esterification. As a versatile platform molecule derived from biomass, 5-hydroxymethylfurfural (HMF) has the potential to be transformed into a variety of chemicals. Of these, furan-2,5-dimethylcarboxylate (FDMC) stands out as an excellent precursor for the synthesis of poly(ethylene furandicarboxylate) (PEF), a polymer with broad applications in the production of various polymeric materials. However, a majority of studies have focused on the use of noble metal catalysts to achieve the direct oxidative esterification of HMF for the production of FDMC. Given the scarcity and high cost of noble metal catalysts, there is a pressing need to develop non-noble metal catalysts to efficiently facilitate the direct oxidative esterification of HMF. Accordingly, a bimetallic catalyst, MnO@Co-CN, was prepared in this paper by a simple coprecipitation method, and a 90.3% FDMC yield was obtained under optimal conditions. The findings revealed that in the oxidative esterification of HMF, MnO x predominantly adsorbs the reactants onto the catalyst surface, whereas CoO x is primarily responsible for the oxidation. The synergistic interaction between Mn and Co enhances the catalytic performance, leading to the superior oxidative esterification outcomes. This work offers a cost-effective, scalable method for FDMC synthesis, highlighting potential for industrial applications.
研究领域:
化学工程
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催化材料
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可再生资源转化
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuan Bao,Weijia Pu,Yiwei Zhang,Yahui Xiao,Yong Liu
Ni-Co nano-alloys confined by in-situ formed N-doped porous carbon overlayer have been prepared through chelation of metal cations with citric acid and urea followed by carbonization for hydrodeoxygenation of 5-hydroxymethylfurfural (HMF) into 2, 5-dimethylfuran (DMF). The results indicated that the Ni-Co nano-alloys were formed and homogeneously distributed within the N-doped porous carbon overlayer. The electronic effect of the Ni-Co nano-alloys significantly boosted hydrodeoxygenation activity of the Co 2 Ni 1 @NC catalyst and simultaneously inhibited further hydrogenation and opening of furan ring. The N-doped porous carbon overlayer around Ni-Co nano-alloys not only facilitated to disperse and stable Ni-Co nano-alloys through strong metal-support interaction, but also protected the Ni-Co nano-alloys from aggregation. Therefore, the Co 2 Ni 1 @NC catalyst offered superior catalytic performance with the HMF conversion of 100 % and DMF selectivity of 93.0 %. Moreover, the Co 2 Ni 1 @NC catalyst displayed excellent stability without significant activity loss after five recycles due to the spatial confinement of N-doped carbon overlayer.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 2
·1-18
·
IF 2.4
Xu Lingling,Pan Xiaomei,Gao Lijing,Wei Ruiping,Li Jihang,Wen Xiu,Li Yuanzhuang,Xiao Guomin
UiO–66–NH 2 (Ti/Zr) modified by Ti metal oxide (TiO 2 ) was used to catalyze the hydrolysis of cellulose to prepare 5-HMF. Under the optimal reaction conditions of H 2 O(NaCl)/THF(1/4 mL), 190 °C, 2 h and 50 mg UNT-3(Ti/Zr) (TiO 2 and UiO–66–NH 2 with mass of 1.5 and 0.1 g, respectively), the yield of 5-hydroxymethylfurfural reached 59.88%. UiO–66–NH 2 (Ti/Zr) nanocomposites with different mass ratios were successfully prepared by simple solvent evaporation method. SEM and TEM have shown that the modified UiO–66–NH 2 (Ti/Zr) are wrapped into sphere by TiO 2 densely attached to the surface of UiO–66–NH 2 , which provides favorable conditions for the uniform dispersion of TiO 2 and coordination of the Lewis acidic site of UiO–66–NH 2 . NH 3 –TPD results confirmed the existence of super-strong, strong, middle and weak acid sites in UiO–66–NH 2 (Ti/Zr), and Py-FTIR confirmed the existence of Brønsted and Lewis acids. After four cycles, the yield of 5-HMF and FUR decreased slightly from 59.88 to 51.89% and 9.11 to 7.66%, respectively, and the yield of 5-HMF could still remain above 50%. The results showed that the modified composite treatment of TiO 2 with rich Lewis acid/base and UiO–66–NH 2 could provide a certain idea for the extensive application of biomass research in the future. Graphic
研究领域:
材料科学
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催化化学
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生物质能研究
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 5
·2754-2759
·
IF 3.591
Long Cao,Han-Ling Guo,Rui-Lian Lin,Zhi-Hua Zhang,Li-Fei Tian,Jing-Xin Liu,Zhu Tao
Using multiple techniques, this work studied the binding behaviors of decamethylcucurbit[5]uril (Me10Q[5]) with o-, m- and p-phenylenediamine (PDA) isomers both in the solid state and in aqueous solution. Experimental data indicate that Me10Q[5] forms exclusion complexes with the three PDA isomers, but their binding affinities are significantly different. Their different binding interactions provided an effective method to separate the three PDA isomers by using Me10Q[5]: when p-phenylenediamine interacts with Me10Q[5] in acidic medium (3.0 mol L−1 HCl), they precipitated immediately and quantitatively; m-phenylenediamine can continuously form microcrystals with Me10Q[5] after a period of time; however, o-phenylenediamine cannot form solid substances with Me10Q[5] under the same conditions.
研究领域:
化学
·
材料科学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2024
·
IF 4.7
Junfan Zhang,Peiya Chen,Huai Liu,Rui Zhang,Wenlong Jia,Junhua Zhang,Lincai Peng
Modulating the electronic structure of metal nanoparticles (NPs) demonstrates to be useful for the optimization of the catalytic performance. Herein, electron-sufficient ruthenium NPs were successfully constructed on a nitrogen-doped carbon support (Ru x -NC), which displayed excellent catalytic activity for the oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA). Especially, a high FDCA yield of 97% was implemented over Ru 2.0 /NC catalyst in water. The FDCA productivity in this case is also as high as 4.8 mol FDCA ‧mol Ru −1 ‧h −1 , which value exceeds most of the previous reported Ru-based catalysts for the production of FDCA. It has been disclosed that the Ru 2.0 /NC was endowed with high N content and abundant electron-rich Ru 0 NPs evoked by the electronic interactions between the NC support the Ru NPs. These facts greatly contribute to the activation of O 2 , and accelerate the oxidation both of the hydroxymethyl and aldehyde groups of HMF to the carboxyl one. This work provides new understanding for the development of effective Ru-based catalysts for the catalytic oxidation reactions by the electronic structure regulation strategy.
研究领域:
化学
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材料科学
·
催化反应
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Dongmei Hao,Yanbin Sun,Dezhong Xie,Fuhao Chu,Weiguang Wang,Anran Zhou,Chen Chen,Yong Wang,Hongying Lü
The oxidation of 5-hydroxymethylfurfural (HMF) to produce high value-added 5-formyl-2-furancarboxylic acid (FFCA) represents a promising biomass conversion reaction that holds potential for biomass-based material for the drug synthesis and polyester industry. The present study presents a metal-free and alkali-free catalytic system consisting of N-hydroxyphthalimide (NHPI) as an organic molecule and a deep eutectic solvent (DES). This system was successfully employed for the aerobic oxidation process of HMF to FFCA, demonstrating exceptional catalytic activity with 100% conversion and 96% FFCA yield in the absence of any alkali. Multiple hydrogen bond interactions were found to be indispensable and play a crucial role in promoting the catalytic process. These H-bond interactions serve three essential purposes: facilitating the formation of deep eutectic solvents (DESs) between polyethylene glycol and tetrabutylammonium chloride, accelerating the dissolution and activation of HMF, and aiding in the generation of active free radicals for NHPI. This work demonstrated the predominant oxidation ability of the NHPI-DESs system for the oxidation of HMF to FFCA through hydrogen bond interaction, thereby offering invaluable insights into the aerobic oxidation processes involving hydrocarbons or alcohols.
研究领域:
有机化学
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生物质转化
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催化化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF ANTIMICROBIAL AGENTS
·
2024
·
IF 4.9
Muchen Zhang,Siyuan Yang,Yongqing Liu,Zhiyu Zou,Yan Zhang,Yunrui Tian,Rong Zhang,Dejun Liu,Congming Wu,Jianzhong Shen,Huangwei Song,Yang Wang
The global increasing incidence of clinical infections caused by carbapenem-resistant Gram-negative pathogens demands urgent and effective treatment strategies. Antibiotic adjuvants represent a promising approach to enhance the efficacy of meropenem against carbapenem-resistant bacteria. Herein, we identified the anticancer agent 5-fluorouracil (5-FU, 50 µM) significantly reduced the minimal inhibitory concentration of meropenem against bla NDM-5 positive Escherichia coli by 32-fold through cell-based high-throughput screening. Further pharmacological studies indicated that 5-FU exhibited the potentiation effects on carbapenem antibiotics against 42 Gram-negative bacteria producing either metallo-β-lactamases (MBLs), such as NDM and IMP, or serine β-lactamases (Ser-BLs), like KPC and OXA. These bacteria included E. coli, Klebsiella pneumoniae, Pseudomonas aeruginosa and Acinetobacter spp. , with 32 of them obtained from human clinical samples. Mechanistic investigations revealed that 5-FU inhibited the transcriptional and expressional level of the bla NDM-5 gene. Additionally, the 5-FU combined with meropenem can enhance bacterial metabolism, and stimulate the production of Reactive Oxygen Species (ROS), thereby rendering bacteria more susceptible to meropenem. This drug combination could effectively elevate the survival rate from 16.7% to 83.3% compared to meropenem monotherapy, and reduce bacteria loads in tissues in a mouse systemic infection model. Collectively, these findings reveal that the potential of 5-FU as a novel meropenem adjuvant to improve treatment outcomes against carbapenem-resistant bacteria infections.
研究领域:
微生物学
·
药理学
·
感染病学
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DOI
高影响因子
CHEMBIOCHEM
·
2018
·Vol. 19
·期 7
·654-659
·
IF 2.774
Ke-Feng Wang,Chun-lei Liu,Kun-yan Sui,Chen Guo,Chun-Zhao Liu
Graphical Cleaning up catalysis : There is a great need for the eco-efficient and sustainable oxidation of bio-based chemicals by using clean catalysts. In this study, magnetic laccase catalyst with TEMPO as the mediator showed high activity in the oxidation of 5-hydroxymethylfurfural (HMF). Interesting and promising results were obtained, with 90.2 % yield of 2,5-furandicarboxylic acid (FDCA) and complete HMF conversion. 2,5-Furandicarboxylic acid (FDCA) is a bio-based platform chemical for the production of polyethylene furanoate (PEF) and other valuable furanic chemicals. A magnetic laccase catalyst with (2,2,6,6-tetramethyl-piperidin-1-yl)oxyl (TEMPO) as the mediator has the remarkable capability of oxidizing 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA). Under optimal reaction conditions, a quantitative yield (90.2 %) of FDCA with complete HMF conversion was obtained after 96 h of reaction. More importantly, the magnetic laccase catalyst exhibited good recyclability and stability, maintaining 84.8 % of its original activity following six reuse cycles. This is the first report on the efficient catalytic oxidation of HMF to FDCA by using an immobilized enzyme catalyst.
研究领域:
催化
·
生物技术
·
绿色化学
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生物基化学品
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产品关联
DOI
PubMed
高影响因子
Frontiers of Chemical Science and Engineering
·
2021
·Vol. 15
·期 6
·1514-1523
·
IF 4.204
Qu Huaxin,Deng Jie,Wang Bei,Ouyang Lezi,Tang Yong,Yu Kai,Lou Lan-Lan,Liu Shuangxi
A base-free catalytic system for the aerobic oxidation of 5-hydroxymethyl-2-furfural was exploited by using Pt nanoparticles immobilized onto a thermoresponsive poly(acrylamide- co -acrylonitrile)- b -poly( N -vinylimidazole) block copolymer, with an upper critical solution temperature of about 45 °C. The Pt nanocatalysts were well-dispersed and highly active for the base-free oxidation of 5-hydroxymethyl-2-furfural by molecular oxygen in water, affording high yields of 2,5-furandicarboxylic acid (up to >99.9%). The imidazole groups in the block copolymer were conducive to the improvement of catalytic performance. Moreover, the catalysts could be easily separated and recovered based on their thermosensitivity by cooling the reaction system below the upper critical solution temperature. Good stability and reusability were observed over these copolymer-immobilized catalysts with no obvious decrease in catalytic activity in the five consecutive cycles.
研究领域:
化学工程
·
材料科学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Zhijian Li,Changhui Zhu,Haiyong Wang,Yuan Liang,Haosheng Xin,Song Li,Xiaohong Hu,Chenguang Wang,Qi Zhang,Qiying Liu,Longlong Ma
For the biomass catalytic valorization in the presence of a H2 atmosphere, large amounts of H2O and H2 are necessary to improve the processing efficiency, which resulted in the waste of such generous inputs. As a model reaction, the traditional hydrodeoxygenation of 5-hydroxymethylfurfural (5-HMF) selectively produces 2,5-dimethylfuran (2,5-DMF) under high pressure H2. Meanwhile, the water-gas shift reaction (WGSR) can counteract the harmful CO by simultaneously producing H2 from H2O. The hydrogenolysis of 5-HMF to 2,5-DMF produces H2O because of the hydroxyl group removal. Therefore, adding a trace amount of H2O to initiate 5-HMF hydrodeoxygenation coupled with WGSR to achieve H2O recycling in the reaction process is of great significance but extremely challenging. Herein, we reported a new process for the selective hydrodeoxygenation of 5-HMF to 2,5-DMF coupled with WGSR using a single catalyst, Au/ZrO2. A detailed study showed that the hydrogen species produced in situ by WGSR was used for 5-HMF hydrodeoxygenation to obtain 78.5% of 2,5-DMF yield. The H/H2O cycle in the coupling reactions exhibited a H2 utilization efficiency of 88.2%. Without using external H2, this work provided a new method for 5-HMF hydrodeoxygenation to 2,5-DMF triggered by WGSR and also showed the potential for application in H2O-saving conversion of cellulosic biomass with C–OH or C═O groups to value-added chemicals and fuels.
研究领域:
生物质催化转化
·
绿色化学
·
可再生资源利用
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DOI
高影响因子
危险品化学品经营许可证（带存储）