RSC Advances
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2013
·Vol. 3
·期 24
·9201-9205
·
IF 2.562
Zhang Zhang,Bin Du,Li-Jia Zhang,Yu-Xia Da,Zheng-Jun Quan,Liang-Jie Yang,Xi-Cun Wang
52–94% yields of 5-hydroxymethylfurfural (HMF) from carbohydrates such as monosaccharides, disaccharides and polysaccharides were achieved using PEG-OSO3H or PS-PEG-OSO3H as reusable catalysts in a DMSO/H2O reaction system. Using polymer-supported catalysis, corn stover could also be effectively transformed into HMF and furfural.
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Journal of Energy Chemistry
·
2016
·
IF 2.322
Xiaofang Liu,Hu Li,Hu Pan,Heng Zhang,Shan Huang,Kaili Yang,Wei Xue,Song Yang
In this work, a series of MIL-101-SO 3 H( x ) polymeric materials were prepared and further used for the first time as efficient heterogeneous catalysts for the conversion of fructose-based carbohydrates into 5-ethoxymethylfurfural (EMF) in a renewable mixed solvent system consisting of ethanol and tetrahydrofuran (THF). The influence of –SO 3 H content on the acidity as well as on the catalytic activity of the porous coordination polymers in EMF production was also studied. High EMF yields of 67.7% and 54.2% could be successively obtained from fructose and inulin in the presence of MIL-101-SO 3 H (100) at 130 °C for 15 h. The catalyst could be reused for five times without significant loss of its activity and the recovery process was facile and simple. This work provides a new platform by application of porous coordination polymers (PCPs) for the production of the potential liquid fuel molecule EMF from biomass in a sustainable solvent system.
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CHINESE JOURNAL OF CHEMISTRY
·
2014
·Vol. 32
·期 5
·434-442
·
IF 1.04
Changhua Song,Hui Liu,Yuan Li,Shuai Ge,Hongwei Wang,Wenshuai Zhu,Yonghui Chang,Changri Han,Huaming Li
A series of metal-Al 2 O 3 catalysts were prepared simply by the conventional impregnation with Al 2 O 3 and metal chlorides, which were applied to the dehydration of fructose to 5-hydroxymethylfurfural (HMF). An agreeable HMF yield of 93.1% was achieved from fructose at mild conditions (100°C and 40 min) when employing Cr(III)-Al 2 O 3 as catalyst in 1-butyl-3-methylimidazolium chloride ([Bmim]Cl). The Cr(III)-Al 2 O 3 catalyst was characterized via XRD, DRS and Raman spectra and the results clarified the interaction between the Cr(III) and the alumina support. Meanwhile, the reaction solvents ([Bmim]Cl) collected after 1 st reaction run and 5 th reaction run were analyzed by ICP-OES and LC-ITMS and the results confirmed that no Cr(III) ion was dropped off from the alumina support during the fructose dehydration. Notably, Cr(III)-Al 2 O 3 catalyst had an excellent catalytic performance for glucose and sucrose and the HMF yields were reached to 73.7% and 84.1% at 120°C for 60 min, respectively. Furthermore, the system of Cr(III)-Al 2 O 3 and [Bmim]Cl exhibited a constant stability and activity at 100°C for 40 min and a favorable HMF yield was maintained after ten recycles.
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MACROMOLECULAR RAPID COMMUNICATIONS
·
2017
·Vol. 38
·期 17
·1700269
·
IF 4.265
Hui Cao,Zhigang Cui,Pan Gao,Yi Ding,Xuechao Zhu,Xinhua Lu,Yuanli Cai
Easy access to discrete nanoclusters in metal-folded single-chain nanoparticles (metal-SCNPs) and independent ultrafine sudomains in the assemblies via coordination-driven self-assembly of hydrophilic copolymer containing 9% imidazole groups is reported herein. 1 H NMR, dynamic light scattering, and NMR diffusion-ordered spectroscopy results demonstrate self-assembly into metal-SCNPs (>70% imidazole-units folded) by neutralization in the presence of Cu(II) in water to pH 4.6. Further neutralization induces self-assembly of metal-SCNPs (pH 4.6–5.0) and shrinkage (pH 5.0–5.6), with concurrent restraining residual imidazole motifs and hydrophilic segment, which organized into constant nanoparticles over pH 5.6–7.5. Atomic force microscopy results evidence discrete 1.2 nm nanoclusters and sub-5-nm subdomains in metal-SCNP and assembled nanoparticle. Reduction of metal center using sodium ascorbate induces structural rearrangement to one order lower than the precursor. Enzyme mimic catalysis required media-tunable discrete ultrafine interiors in metal-SCNPs and assemblies have hence been achieved.
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JOURNAL OF CHROMATOGRAPHY A
·
2016
·
IF 3.926
Tao Bao,Pingxiu Tang,Deying Kong,Zhenkun Mao,Zilin Chen
Covalent-organic frameworks (COFs) are attractive materials for their fascinating properties, such as rigid structures, exceptional thermal stabilities, low densities, and permanent porosity with specific surface areas, which indicate potential for application in chromatography similar to related metal-organic frameworks (MOFs). However, the utilization of COFs in analytical chemistry is far behind as compared to that of the MOFs due to the challenging work of their immobilization. Here, we have successfully demonstrated the growth of the boron COF-5 on the inner wall of the fused silica capillary by a developed polydopamine-supported method. Combined with the layer-by-layer strategy, multilayer COF-5-coated capillary was obtained. The formation of COF-5 on polydopamine-coated substrate has been confirmed by scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction. A novel stationary phase of COF-5 was developed on the basis of successful growth of COF-5 on polydopamine for open-tubular capillary electrochromatography (OT-CEC). Baseline separation of neutral, acidic and basic analytes was achieved on multilayer COF-5-coated capillary column. The fabricated capillary columns showed high column efficiency (154,060 plates/m for methylbenzene), excellent stability and repeatability. The precision (relative standard deviation (RSD), n = 3) of retention time, peak height, and peak area for tested neutral compounds were in the range of 1.2–1.3%, 1.8–4.2%, and 0.9–2.4%, respectively. To the best of our knowledge, it was the first demonstration that COF-5 was developed as a novel stationary phase.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2017
·Vol. 134
·期 43
·45468
·
IF 1.86
Li Zhang,Lin Chen,Huan Zhang,Yongzhen Yang,Xuguang Liu
Thermosensitive magnetic surface molecularly imprinted polymer microspheres based on thermosensitive monomer n -isopropylacrylamide (NIPAM) are applied for the recognition of 5-fluorouracil (5-FU). A computational analysis is used to predict the interaction sites between 5-FU and NIPAM, the stoichiometry of the synthesis procedure, and the affinity of imprinted cavities toward 5-FU. Due to hydrogen bond interactions, a stable complex configuration of 5-FU and NIPAM shows a binding energy of −46.50 kJ/mol confirming the suitability of imprinting 5-FU into thermosensitive polymer network. After optimization, the appropriate stoichiometry of 5-FU to NIPAM is set to 1:4 during the preparation process. The simulated imprinted cavities show affinity toward 5-FU, with a binding energy of −112.24 kJ/mol. A preliminary experimental evaluation for the drug recognition of thermosensitive magnetic surface molecularly imprinted polymer microspheres is made, obtaining an adsorption capacity of 21.72 mg/g at 25 °C. Pseudo-second-order kinetics well describes the adsorption process. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 45468.
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TALANTA
·
2016
·
IF 4.035
Yueli Hu,Boyue Wu,Qing Jin,Xueyuan Wang,Yan Li,Yuxiu Sun,Jianzhong Huo,Xiaojun Zhao
5 nm intense green emission NaYF 4 :Yb/Er upconversion nanoparticles (UCNPs) with pure β phase was synthesized with a simple “green” strategy for the first time. Traditional organic solvothermal method is often applied to prepare the high-quality and uniform UCNPs, but the preparation of lanthanide-oleate complexes is laborious as heating and multistep post-treatment for purification are often required. The water-alcohols solvothermal method is environmentally friendly, but the fabricated UCNPs have big size, poor biocompatibility and high cytotoxicity, which limited their application for cell imaging. Herein, NaYF 4 :Yb/Er UCNPs were prepared with rare-earth nitrates RE(NO 3 ) 3 (RE=Y 0.80 Yb 0.18 Er 0.02 ) as precursors and diethylene glycol (DEG)/ethylene glycol (EG)/water as the solvent. A facile green solvothermal method with the temperature being controlled at 300 °C was developed. The as-prepared NaYF 4 :Yb/Er UCNPs were characterized and were found to have enhanced UC emission and controllable particle size. The as-prepared UCNPs were further functionalized via folic acid coating for the targeted imaging and improved bio- compatibility. It was made the UCNPs potential for upconversion bioimaging of living cells by the strong upconversion luminescence, the excellent biocompatibility, and the super-small size. The good colloidal stability and low cell cytotoxicity of the as-prepared UCNPs and the developed synthesis protocol might advance both the fields of UCNPs and biomolecule-based nanotechnology for future studies.
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Catalysts
·
2016
·Vol. 6
·期 2
·19
·
IF 2.964
Guozhu Liu,Yunxia Zhao,Jinhua Guo
High selectively catalytic conversion of lignin-based phenols (m-cresol,p-cresol, and guaiacol) intopara-/m-xylene was performed over Pt/HZSM-5 through hydrodeoxygenation andin situmethylation with methanol. It is found that thep-/m-xylene selectivity is uniformly higher than 21%, and even increase up to 33.5% form-cresol (with phenols/methanol molar ratio of 1/8). The improvedp-/m-xylene selectivity in presence of methanol is attributed to the combined reaction pathways: methylation ofm-cresol into xylenols followed by HDO intop-/m-xylene, and HDO ofm-cresol into toluene followed by methylation intop-/m-xylene. Comparison of the product distribution over a series of catalysts indicates that both metals and supporters have distinct effect on thep-/m-xylene selectivity.Keywords:m-cresol;hydrodeoxygenation;methanol;p-/m-xylene;methylation
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SEPARATION SCIENCE AND TECHNOLOGY
·
2016
·
IF 1.083
Cun-Xiang Wang,Dong-Qiang Lin,Tao Liu,Shan-Jing Yao
Hydrophobic charge-induction chromatography (HCIC) is a highly promising technology for antibody separation. HCIC resins ABI-B-6FF were prepared with 5-aminobenzimidazole (ABI) as the functional ligand. The effects of ligand density on the adsorption of human immunoglobulin G (hIgG) and bovine serum albumin were focused. It was found that the adsorption capacity and dynamic binding capacity (DBC) were improved with the increase of ligand density. The adsorption capacity and DBC of hIgG reached 128.07 mg/g gel and 67.63 mg/g gel. The results indicated that ABI-B-6FF resin has a promising potential for the application of antibody purification.
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ACS Sustainable Chemistry & Engineering
·
2016
·
IF 5.267
Ye-Zhi Qin,Min-Hua Zong,Wen-Yong Lou,Ning Li
Valorization of biomass-based platform chemicals into high value-added products has attracted increasing attention recently. In this work, upgrading of 5-hydroxymethylfurfual (HMF) and levulinic acid, two important biomass-based platform chemicals, to HMF levulinate via a green and efficient enzymatic approach was reported. Novozym 435 was found to be the best biocatalyst for the enzymatic esterification. The enzymatic esterification progressed smoothly in t-butanol, 2-methyl-2-butanol, and cyclopentyl methyl ether as well as in the ecofriendly biomass-derived 2-methyltetrahydrofuran (2-MeTHF), while no enzymatic reaction occurred in deep eutectic solvents. When HMF concentration was up to 500 mM, a good conversion of 72% was achieved in 2-MeTHF. The reaction temperature exerted a significant effect on the enzymatic esterification. When the reaction temperature is below 40 °C, high HMF conversions (>85%) were obtained. Besides, significant inactivation of the enzyme was observed at more than 50 °C, resulting in poor conversions.
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CRYSTENGCOMM
·
2017
·Vol. 19
·期 47
·7088-7094
·
IF 3.474
Baoliang Peng,Houbing Zou,Lipeng He,Pingmei Wang,Zhiqiang Shi,Liangkui Zhu,Runwei Wang,Zongtao Zhang
Hierarchical zeolites are promising solid acid catalysts for industrial processes and conversions of bulky molecules because they provide fast mass transfer along with size and shape selectivity; however, their synthesis always involves either complicated post-synthetic modifications or cost-intensive templates. In this work, engineering growth defects has been developed as a new and efficient strategy for preparing hierarchical ZSM-5 zeolite with high specific surface area and abundant uniform intracrystalline mesopores. This route only involved certain energy-efficient conditions, e.g., tender crystallization and mesotemplate-free conditions. Combining tender crystallization conditions with an optimal original Si/Al ratio (150–300) in a colloid synthesis system was found to be the key to successfully engineer the growth defects. Importantly, it even exhibited higher catalytic activities for benzaldehyde–alcohol condensation reactions than mesoporous ZSM-5 zeolite prepared using mesoscale templates.
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JOURNAL OF SEPARATION SCIENCE
·
2016
·Vol. 39
·期 16
·3130-3136
·
IF 2.741
Tao Liu,Dong-Qiang Lin,Cun-Xiang Wang,Shan-Jing Yao
Hydrophobic charge-induction chromatography is a new technology for antibody purification. To improve antibody adsorption capacity of hydrophobic charge-induction resins, new poly(glycidyl methacrylate)-grafted hydrophobic charge-induction resins with 5-aminobenzimidazole as a functional ligand were prepared. Adsorption isotherms, kinetics, and dynamic binding behaviors of the poly(glycidyl methacrylate)-grafted resins prepared were investigated using human immunoglobulin G as a model protein, and the effects of ligand density were discussed. At the moderate ligand density of 330 μmol/g, the saturated adsorption capacity and equilibrium constant reached the maximum of 140 mg/g and 25 mL/mg, respectively, which were both much higher than that of non-grafted resin with same ligand. In addition, effective pore diffusivity and dynamic binding capacity of human immunoglobulin G onto the poly(glycidyl methacrylate)-grafted resins also reached the maximum at the moderate ligand density of 330 μmol/g. Dynamic binding capacity at 10% breakthrough was as high as 76.3 mg/g when the linear velocity was 300 cm/h. The results indicated that the suitable polymer grafting combined with the control of ligand density would be a powerful tool to improve protein adsorption of resins, and new poly(glycidyl methacrylate)-grafted hydrophobic charge-induction resins have a promising potential for antibody purification applications.
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