CHEMICAL ENGINEERING SCIENCE
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2020
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IF 3.871
Sa Wang,Yufan Zhang,Yuning Tang,Yijing Wen,Zhenqiang Lv,Sihao Liu,Xiang Li,Xin Zhou
Separating propane from propylene is a significant challenge in petrochemical industry. Rational chemistry design of the propane-selective adsorbent has not been reported. This work demonstrates the first design of propane-selective adsorbents. Two strategies based on surface chemistry tuning, namely compositing 2D g-C 3 N 4 and replacing ligand, have been proposed to yield the propane-selective g-C 3 N 4 @Zr-BPDC (BPDC = biphenyl-4,4′-dicarboxylate) and Zr-BPYDC (2,2′-bipyridine 5,5′-dicarboxylate). Whereas g-C 3 N 4 @Zr-BPDC has a high propane capacity of 8.79 mmol/g at room temperature and ambient pressure, Zr-BPYDC exhibits superior propane/propylene selectivity. The isosteric heat of propane and propylene adsorption on both adsorbents is lower than that of most reported adsorbents, indicating facile regeneration of the adsorbents. DFT calculations suggest the propane-selectivity comes from multiple C H δ+ ⋯N δ− interactions between propane and nitrogen atoms of the adsorbents. Moreover, both adsorbents produce polymer-grade propylene through a one-step separation using a packed column, facilitating the energy-effective production of polymer grade propylene under ambient conditions.
研究领域:
化学工程
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材料科学
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吸附技术
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石油化学
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2018
·Vol. 28
·期 16
·1707356
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IF 13.325
Zhe Wang,Shuanggang Hu,Jian Yang,Ajuan Liang,Yongsheng Li,Qixin Zhuang,Jinlou Gu
Introduction of large pore in the primitive microporous metal–organic frameworks (MOFs) with tailorable particle size can endow them with desired properties for potential applications in the intracellular delivery of membrane-impermeable proteins. However, no research is found to focus on this topic until now. Herein, a monocarboxylic acid (MA) and organic base comodulation strategy is developed to synthesize the hierarchically porous UiO-66 nanoparticles. MA of dodecanoic acid is utilized to control the pore size while trimethylamine (TEA) plays a key role in modulating the nucleation of crystallization to regulate the particle size. In comparison with microporous UiO-66, a model protein of cytochrome c (Cyt c) could be efficiently loaded into the mesoporous MOFs (mesoMOFs). The size-dependent cellular uptake is also evaluated, and it is verified that mesoMOFs with particle size of 90 nm could be endocytosed into living cells with highest efficiency. These outstanding merits enable the current mesoMOFs not only to exhibit efficient encapsulation of Cyt c but also facilitate the protein delivery into the cytosol and subsequent endosomal escape. Given the exceptional chemical stability, hierarchically porous structure as well as tunable particle size, the elaborated mesoUiO-66 nanoparticles might offer a promising platform for a variety of biomedical applications.
研究领域:
材料科学
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纳米技术
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生物医学工程
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药物递送系统
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产品关联
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2024
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IF 3.7
Zhaorui Qi,Xurui Li,Yueming Zhu,Li Li,Yu Liu
Metal–organic framework (MOF) is a porous material composed of metal ions/clusters and organic ligands. It has attracted much attention due to its high specific surface area, good biocompatibility, chemical modifiability, and diversity of components. Among many MOFs, zirconium-based MOFs are particularly suitable for biological applications due to their optimal stability and low toxicity to hydrolysis. However, due to the weak coordination bonds between many metal clusters and organic ligands, most MOFs are prone to collapse in acidic environments, and the stability of MOFs as drug carriers cannot be guaranteed so that they cannot be widely used as oral drug carriers. This study synthesized the three MOFs using metal Zr ion clusters as the center and different nitrogen-containing organic ligands, which are stable in gastric acid, namely, UiO-66-PDC, UiO-66-NH 2 , and UiO-66-NO 2 . The anionic drug loxoprofen (LOX) was loaded and characterized using scanning electron microscopy, infrared spectroscopy, thermogravimetric analysis, differential scanning calorimetry, and x-ray diffraction. The adsorption and release behaviors of LOX and the three MOFs were studied from the molecular point of view by computer simulation. A series of behaviors and mechanisms of pH-responsive nitrogen-containing MOFs as oral drug carriers were further explored through rat pharmacokinetic experiments, the everted gut sac experiments, and intestinal absorption mechanism experiments. The experimental results show that there is a strong electrostatic interaction between anionic drug LOX and UiO-66-PDC under simulated gastric acid environment, which prolongs the half-life of the drug, proving that LOX@UiO-66-PDC is a promising new oral drug delivery system.
研究领域:
材料科学
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药学
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生物医学工程
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Jinshan Xie,Xiaoxiang He,Kexin Liu,Wulong Li,Zhanxiong Li
In this paper, carboxylated cotton fabric (CF-Ph-COOH) were obtained as active substrate by diazonium radical polymerization modification of cotton fibers. Then the MOF fabric composites were prepared by in situ growth of metal zirconium ions (Zr) and organic ligands on the surface of carboxylated cotton fabrics under carboxylic acid modifier. MOF fabric composites with controllable morphologies structures were achieved by regulating organic ligands, reaction time the type and dosage of regulator (formic acid and acetic acid). The prepared acetic acid regulated MOF fabric composites were designated as CF-HAc1-UiO-66, CF-HAc2-UiO-66, CF-HAc1-UiO-66-NH 2 , and CF-HAc2-UiO-66-NH 2 , respectively, and the formic acid regulated as CF-FA-UiO-66 and CF-FA-UiO-66-NH 2 . The fabricated carboxylic acid modulated MOF fabric composites were well characterized using SEM, TGA, XRD, FTIR, and XPS spectra. The adsorption experiment results show that carboxylic acid modulated Zr based MOF fabric composites can serve as adsorbent for effective removal of Cr(VI) from water, in which the CF-FA-UiO-66-NH 2 was prepared under the ratio of ZrCl 4 and BDC-NH 2 is 1.006 and with 5.47 M formic acid regulator exhibits that the optimal adsorption efficiency and the removal efficiency is 79.5 %. In addition, the adsorption of Cr(VI) in water by CFA-UiO-66-NH 2 showed a quasi-secondary kinetic model following the Langmuir adsorption model, showing a a typical of chemisorption. What’s more, the Cr(VI) removal efficiency and saturated adsorption capacity of CF-FA-UiO-66-NH 2 was up to 80 % and 318.85 mg/g, respectively. The prepared CF-FA-UiO-66-NH 2 MOF fabric composite was recyclable for removal of Cr(VI), and could be used as the potential adsorbent membrane for waste water treatment.
研究领域:
材料科学
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环境工程
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化学工程
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产品关联
DOI
高影响因子
FOOD CHEMISTRY
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2024
·
IF 8.5
Wei Man,Shuo Zhang,Yunlong Wang,Mengjun Wang,Chongjiang Cao,Linyu Nian
The metabolic processes of fruits induce water vapor condensation in packaging, creating a high-humidity microenvironment that exacerbates the proliferation of microorganisms and causes food spoilage. Therefore, a Fe/Zr bimetallic organic framework (Fe-MOF-801) packaging (i.e., FeMGCF) with high binding stability to transpiration water was prepared based on transition metal Fe doping strategy, and the mechanism of its enhanced binding stability towards transpiration water was investigated. The results indicate that Fe enhances the interaction between MOFs and H 2 O by promoting the charge depletion at the O sites coordinated with Zr, thereby increasing the aggregation tendency of H 2 O in the T 1 and T 2 cavities (characterized by strong hydrogen bonding) of Fe-MOF-801, which increased the binding energy of MOFs to H 2 O by 29.6 %. Accordingly, the application of FeMGCF packaging extended the shelf life of tomatoes by 6 days and delayed the degradation of lycopene and anthocyanins during postharvest tomato preservation.
研究领域:
材料科学
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食品科学
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化学
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农业
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Lei Shi,Fan Xiang,Kexin Liu,Wulong Li,Zhanxiong Li
Metal-organic frameworks (MOFs) show great potential applications in dealing with heavy metal pollution due to their unique large specific surface area, tunable pore size, and diverse active groups. However, the powder form of MOFs has suffered from the disadvantages of difficult recycling and secondary contamination after adsorption of heavy metals, which seriously limits their practical application. Therefore, in this work, we prepared a series of bifunctional zirconium-based MOFs cotton fabric composites (MCFC) via in situ growth of MOFs on carboxylated cotton fabric, exhibiting large specific surface area, adjustable pore size, and effective adsorption ability. The prepared CF-UiO-66-(OH) 2 -FA shows an excellent adsorption efficiency of Au(III) more than 99.990 %, and the saturated adsorption amount is up to 190.98 mg·g −1 at 25 °C. Meanwhile, the kinetic experiment analysis demonstrated that the Au(III) adsorption behavior of MCFC follows pseudo-second-order (PSO) kinetic model. More importantly, it also exhibits great selectivity in adsorbing Au(III) from the mixture of multiple metal ions coexisted solution. The results of adsorption thermodynamics and adsorption isotherms indicate that adsorption is monolayer and a spontaneous, exothermic process. And the ideal adsorption and separation process could be finished by quickly filtrating with a single or multi-layer MCFC. Excellent adsorption performance even after four cycles of adsorption. Therefore, the fabricated MCFC shows great processability, flexibility, collectability and reusability in adsorbing and recycling precious metal ion from wastewater.
研究领域:
环境科学
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材料科学
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化学工程
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废水处理
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产品关联
DOI
高影响因子