APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Yunye Wang,Mengdie Guo,Ya Wang,Xinjie Liu,Xiaopeng Li,Cuong Pham-Huu,Xuemei Liao
Catalytic oxidation of biomass derived 5-Hydroxymethylfurfural (HMF) feedstock is a promising route to produce value-added chemicals 2, 5-diformylfuran (DFF). Here, we find that incorporating monatomic Ru into the crystalline lattice of α-MnO 2 can trigger synergetic catalysis for aerobic oxidation of HMF. Ru species can not only act as active sites for HMF conversion, but also activate surface oxygen species by creating rich oxygen vacancies on the α-MnO 2 . As result, such catalyst delivers much higher DFF productivity than that of Ru located in the tunnel of support (110 °C, 1.5 MPa, 1 h) and state-of-the-art Ru-based catalysts. Furthermore, the direct conversion of fructose into DFF was realized by combination of Amberlyst-15 and Ru-MnO 2 HT catalyst in one-pot via two-step. Characterization and kinetic results indicated that atomically dispersed Ru hosted in the crystalline lattice of support created abundant oxygen vacancies and thus weakened the Mn-O bond, resulting in facile lattice oxygen activation.
研究领域:
化学
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
Waste and Biomass Valorization
·
2016
·Vol. 9
·期 1
·95-101
·
IF 0.915
Ning Liangmin,Liao Shengyun,Sun Yongfa,Yu Linhao,Tong Xinli
Abstract The catalytic synthesis of 2,5-diformylfuran (DFF) from 5-hydroxymethylfurfural (HMF) attracts extensive attention in the research of biomass conversion. However, it is a challenge to achieve high conversion of HMF under mild conditions with a heterogeneous catalyst, which can be easily separated and recycled. Herein, we report a novel cobalt-based catalyst (Co x O y -N@TiO 2 ) for the oxidation of HMF to DFF with 30 % aqueous tert -butyl hydroperoxide as the oxidant. A series of Co-based catalysts were prepared by a typical impregnation method, and detected by XRD, TEM and FT-IR techniques. Based on the experimental results of catalytic test, it is found that a 91 % conversion of HMF and 40 % selectivity of DFF was obtained with the Co x O y -N@TiO 2 catalyst at 80 °C within 5 h. In addition, the Co x O y -N@TiO 2 can be recycled up to five times without significant loss of activity. Graphical Abstract The efficient oxidation of 5-hydroxymethyl furfural, a biomass-derived platform compound, to produce 2,5-diformylfuran is achieved using Co x O y -N@TiO 2 catalyst under mild conditions.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Fu Yang,Jingjing Tang,Rui Ou,Zengjing Guo,Shuying Gao,Yinzhu Wang,Xuyu Wang,Lei Chen,Aihua Yuan
Biomass-derived resources exploited in depth toward the synthesis of high value-added chemicals is very promising, but still limited by the applicable catalyst. In this paper, we report regulated robust multilayer-like polyoxometalates(Niobium molybdate) specific to the catalytic synthesis of promising 5-Ethoxymethylfurfural (EMF). The present solid acid catalysts resulted from precisely-tuned compositions of Nb and Mo toward acquiring controlled Brønsted acid amounts and interlayer space coupling with specific Lewis acid sites are demonstrated to be the determining factors for tuning conversion and selectivity in the synthesis of EMF, respectively. The characterization results indicate that the increment in Nb moiety is beneficial to produce more accessible acid sites and the enlarged interlayer space in the catalyst, thereby promoting the acid-catalyzed conversion. As a result, the full conversion(Conv. 100%) of 5-hydroxymethylfurfural into the 5-Ethoxymethylfurfural (Select. >99%) by etherification with ethanol within only 60 min was realized as the record-high yield under the solvent-free condition, far outperforming several traditional catalysts. In addition, the rational 67% yield of EMF was received when using fructose as an initial reactant. Ulteriorly, the resultant catalyst inherits the superior catalytic activity in the substrate expansion experiments in the presence of different alcohols. More importantly, the resulted catalyst shows durable catalytic activity without any activity-loss during the eight recycling, which reveals the huge potential industrial application prospect.
研究领域:
化学工程
·
催化科学
·
生物质能
✓ 已验证
产品关联
DOI
高影响因子
ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2024
·
IF 3.1
Yu Zhang,Minghui Xiao,Ranran Feng,Hong-Yu Zhang,Yuecheng Zhang,Jiquan Zhao
5-Methyltetrahydrofolate (5-MTHF) is an active form of folic acid (FA) and an essential micronutrient preventing anemia and numerous other adverse health conditions such as cardiovascular disease and cancer. Herein, a continuous flow sequence synthesis of 5-MTHF from FA was developed, involving three elementary steps: catalytic hydrogenation of FA to tetrahydrofolic acid (THFA), methylenation of THFA with formaldehyde, and hydrogenation of the methylenation intermediates to 5-MTHF. This process features an expeditious synthesis of 5-MTHF in an integrated flow platform with water as the sole solvent and without any intermediate purification. The overall yield of this three-step flow process was up to 53.54% in a total residence time of 71.4 min. The separated yield of 5-MTHF reached 49.3%.
研究领域:
生物化学
·
制药工程
·
营养学
✓ 已验证
产品关联
DOI
高影响因子
CRYSTAL GROWTH & DESIGN
·
2016
·
IF 4.425
Xia-Lin Dai,Song Li,Jia-Mei Chen,Tong-Bu Lu
Pharmaceutical cocrystallization is proposed as a new method to enhance membrane permeability of a BCS class III model drug, 5-fluorouracil (5FU). Three cocrystals of 5FU, 5FU/3-hydroxybenzoic acid (1), 5FU/4-aminobenzoic acid (2), and 5FU/cinnamic acid (3), were successfully synthesized by a slurry method or a liquid-assisted grinding process. Spectroscopic methods, thermal analysis, and X-ray diffraction were used to characterize these new forms. The permeability was studied using a Franz diffusion cell and silicone membrane. All of the cocrystals showed improved membrane permeability compared to free 5FU. The cumulative amount per unit area of permeated 5FU in the first 10 h for 1–3 was increased by 41, 70, and 83%, and the steady penetration rates of 1–3 were increased by 38, 66, and 79%, respectively, as compared to the pure drug. Structure–permeability correlation study finds a link between intermolecular interactions and molecular packing in cocrystals and their permeability behavior and has important implications for use of a cocrystallization approach to improve drugs’ permeability in the pharmaceutical field.
研究领域:
药学
·
生物医学工程
·
药物化学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2015
·Vol. 7
·期 9
·1470-1477
·
IF 4.556
Fenghua Xu,Zehui Zhang
Graphical Take baby steps: Polyaniline-grafted vanadyl acetylacetonate shows high catalytic activity for the oxidation of 5-hydroxymethylfurfural (HMF) under atmospheric oxygen pressure. A high HMF conversion of 99 % and a 2,5-diformylfuran (DFF) yield of 86 % are obtained after 12 h. More importantly, the synthesis of DFF directly from fructose is also realized with two binary catalysts: Amberlyst-15 and polyaniline–vanadyl acetylacetonate. Herein, polyaniline-grafted vanadyl acetylacetonate [VO(acac) 2 ] was prepared and used as an effective catalyst for the oxidation of 5-hydroxymethylfurfural (HMF) under atmospheric oxygen pressure. A high HMF conversion of 99.2 % was obtained after 12 h at 110 °C, and 2,5-diformylfuran (DFF) was obtained in 86.2 % yield. More importantly, the one-pot conversion of fructose into DFF was also realized with two binary catalysts: Amberlyst-15 and polyaniline–VO(acac) 2 . Amberlyst-15 was used for the acid-catalyzed dehydration of fructose into HMF, followed by the in situ oxidation of HMF catalyzed by polyaniline–VO(acac) 2 . DFF could be obtained in a yield of 42.1 % from fructose by using the one-pot reaction, whereas two consecutive steps gave a higher DFF yield of 71.1 %. Owing to the facile catalyst preparation and low cost, this method showed a promising potential for the synthesis of DFF from abundant carbohydrates.
研究领域:
化学工程
·
催化反应
✓ 已验证
DOI
高影响因子
ADVANCES IN POLYMER TECHNOLOGY
·
2020
·
IF 1.539
Yunlong Liu,Jie Guo,Zhuobing Xiao,Dazhao Peng,Ke Song
Separation and purification of active components from biomass by inorganic materials during the pretreatment process of hydrothermal conversion are studied in this work. The batch experiment results show that an initial solution pH of 6 favors chelerythrine adsorption, and the optimum adsorbent dosage is 2.0 g. The adsorption mechanism of ZSM-5 for chelerythrine is investigated by adsorption kinetics, isotherm adsorption models, and thermodynamics analysis. The results show that the kinetics data fit the pseudo-second-order model well (R2 = 0.9991), and the intraparticle diffusion model has 3 diffusion stages, preliminarily indicating that chemisorption plays a major role in the adsorption process, and the sorption mechanism includes intraparticle, external, and boundary diffusion. The adsorption isotherms agree well with the Langmuir model, indicating the occurrence of monolayer molecular adsorption during the adsorption process. Meanwhile, the maximum adsorption capacity is 2.327, 2.072, and 1.877 mg/g at different temperatures (288 K, 298 K, and 308 K), respectively. The thermodynamic data demonstrate that the adsorption process is exothermic and spontaneous in nature. These observed results clearly confirm that ZSM-5 has potential superior properties for the enrichment and purification of alkaloids during the pretreatment of biomass.
研究领域:
生物化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Xiuli Shao,Siqi Wang,Youhui Zhou,Xuan Zhang,Haizhou Tian,Zheng Wang,Zhong-Yong Yuan,Huanting Wang
The ZSM-5 zeolite nanosheets are highly desired materials for catalytic reactions and membrane separation . Their synthesis depends on specially designed complex surfactants ; however, the high-cost limits their large-scale industrial production. Herein, the tailored synthesis of coffin-shaped multilamellar ZSM-5 composed of orderly stacked 2D nanosheets is carried out using cetyltrimethylammonium bromide (CTAB) as a structure-directing agent (SDA) in the presence of silicalite-1 seed sol. The morphology and b -axis thickness of nanosheets is controlled by adjusting the amount of silicalite-1 seed sol, CTAB/TEOS ratio, SiO 2 /Al 2 O 3 ratio, and synthesis time. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) analysis indicate that the hydrophobic tail of CTAB acts as an inhibitor, effectively preventing the continuous growth along b -direction with an average thickness of 20–100 nm. This work highlights the role of silicalite-1 seed sol and CTAB in the orderly stacked sheets growth process. This crystallization strategy opens a facile and inexpensive approach for multilamellar ZSM-5 zeolite fabrication with 2D-nanosheets structures, and their practical applications in catalytic conversions of bulky molecules.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2012
·Vol. 38
·期 7
·1421-1429
·
IF 0.697
Li He-ping,Qin Long,Wang Zhou-dong,Li Shan
In order to improve drug loading and achieve a good release effect, this paper adopts the ramose method, choosing chitosan as the carrier and 5-fluorouracil (5-Fu) as a model drug. Ramose chitosan-lysyl-5-Fu(3) and ramose tetralactosyl-lysyl-chitosan-5-Fu(6) were synthesized successfully, then the in vitro release of (6) was researched. The results show that the drug loading of (3) and (6) are 9.17 and 1.63% (w/w), respectively. The in vitro release behavior of (6) in pH 7.4 phosphate buffer solution and pH 1.2 HCl–KCl solution were studied. The zero order release time that (6) maintains in alkaline and acidic media are 64 and 24 h, and the total release by 184 h are 71.97 and 82.34%, respectively. The performance is smooth throughout the whole stage of release, and the concentration of cumulative release is lower in the alkaline environment than in the acidic environment over the same time.
研究领域:
药剂学
·
生物材料学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Guangchuan Tang,Xin Huang,Hui Qin,Chuan Ma,Yunlin Shao,Zhongqing Yang,Changlei Qin,Jingyu Ran
Levoglucosan (LGA), as the main primary anhydrosugar of cellulose pyrolysis , is of great significance for future value-added chemicals production. In this study, effective conversion of LGA to 5-hydroxymethylfurfural (HMF) was investigated in a NaCl–H 2 O/acetone biphasic system over sulfonated resin and AlCl 3 . The results show that the biphasic system could efficiently inhibit the overreaction of HMF compared with pure water, leading to a significant enhancement of HMF production. HMF was obtained with the highest yield of 68.5 % at 96.5 % of LGA conversion at the optimized conditions. The use of cellobiose as substrate produced 61 % of HMF while LGA-rich bio-oil led to a sharp decease of HMF yield to 33 %. Through the respective experiments using LGA, glucose and fructose as the substrates, the reaction network was constructed for kinetic analysis, and satisfactory fitting results are observed in agreement with the experimental results, providing the best conditions for producing glucose and HMF, respectively. In addition, the mechanism of LGA conversion to HMF was calculated by DFT, which needs to overcome the highest free energy barrier of 121 kJ/mol.
研究领域:
化学工程
·
生物质能
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Energy Research
·
2021
·
IF 4.008
Hao Jiawen,Song Xueping,Jia Shaowu,Mao Wei,Yan Yuxiao,Zhou Jinghong
Heteropoly acids containing Brønsted and Lewis acids show excellent catalytic activity. Brønsted acids promote the depolymerization of polysaccharides (such as starch and cellulose) into glucose, while Lewis acids catalyze the conversion of glucose to 5-hydroxymethylfurfural (HMF). Designing stable Brønsted-Lewis acid-containing bifunctional heterogeneous catalysts is crucial for the efficient catalytic conversion of polysaccharides to HMF. In this study, a series of Brønsted -Lewis acid bifunctional catalysts (SnxPW, X = 0.10–0.75) were investigated for the conversion of cassava starch to HMF. The structure of the catalysts was characterized by X-ray diffraction, Fourier transform infrared spectroscopy, Pyridine Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. The acid strength and acid capacity were also investigated. The effects of reaction time, temperature, catalyst concentration, and cassava starch concentration on the selectivity, conversion rate, and yield were examined. The results showed that, among the analyzed catalysts, Sn0.1PW presented the best ability under the test conditions for catalyzing the conversion of starch to HMF. At the optimized conditions of a reaction temperature of 160°C, a catalyst dosage of 0.50 mmol/gstarch, and a 1 h reaction time, the starch conversion rate was 90.61%, and the selectivity and yield of HMF were 59.77 and 54.12%, respectively. Our findings contribute to the development of HMF production by the dehydration of carbohydrates.
研究领域:
化学工程
·
可再生资源转化
✓ 已验证
产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
·
2023
·
IF 4
Lu Yanyu,Lin Changqu,Yang Hao,Ma Peipei,Chen Jishuang,He Zhuang,Wu Hongli,Cao Fei,Chen Kequan,Ouyang Pingkai
Abstract FDCA (2,5-furandicarboxylic acid), produced by oxidizing carbohydrate-derived HMF (5-hydroxymethylfurfural), is a valuable monomer for biopolymers. The difference in the solvent system between the dehydration reaction and oxidation reactions seriously affects the process continuity and production efficiency. Herein, we reported a cascade process for FDCA production from carbohydrates in a single acetic acid system. The fructose conversion was complete and total furan compounds yield reached nearly 90%, which contained 42.8% HMF and 47.1% 5-acetoxymethylfurfural (AMF) in the acetic acid system with NaBr addition. After the azeotropic distillation and vacuum distillation in situ, AMF, a more stable intermediate than HMF, could be easily collected with 90.5% recovery and 99.9% purity. AMF was also oxidized into FDCA with 91.1% yield by Co/Mn/Br catalysts in the acetic acid system. Finally, the cascade process, including fructose dehydration–esterification and HMF/AMF mixture oxidation, was successfully realized in a single acetic acid system. This process is simple to operate, easy to implement, eliminates the use of extra acid or self-made catalysts and expensive solvents, and has the potential for continuous preparation from carbohydrates to FDCA. Graphical Abstract
研究领域:
化学工程
·
生物化工
✓ 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）