SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yeshuang Wang,Mingxian Duan,Zhelin Su,Chao Yang,Bingning Wang,Jiawei Kou,Huiling Fan
The abundant Fe 3+ Lewis acidic sites and well-developed pore structure endow the Fe-MOFs with great potential for H 2 S catalytic oxidation at room temperature, but their performance is inferior owing to the insufficient redox ability of the Fe 3+ species inherent in frameworks. Herein, an effective protocol was proposed for the first time to remarkably improve the catalytic oxidation performance of MIL-100(Fe) under ambient conditions through the introduction of Fe 2+ coordinatively unsaturated site (CUS) species into the framework. As expected, the sample after modification had a superior H 2 S breakthrough capacity of 267.3 mg S/g, an 18.4-fold increase compared with that without Fe 2+ CUS (14.5 mg S/g). The introduced Fe 2+ species triggered the Fe 3+ /Fe 2+ redox cycle for H 2 S catalytic oxidation by enhancing the oxidative ability of the Fe 3+ CUS intrinsic to the framework. Moreover, the Fe 2+ CUS was also found act as an active site for O 2 activation into O 2 ∙– , which not only provides an additional pathway for H 2 S catalytic oxidation but also accelerates the redox cycling of Fe 3+ /Fe 2+ during the catalytic oxidation process. On the basis of the experimental findings, a plausible catalytic mechanism involving mixed-valence iron sites in MIL-100(Fe) was proposed.
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
Inorganics
·
2022
·Vol. 10
·期 3
·33
·
IF 3.149
Tian Zhao,Hexin Zhu,Ming Dong,Minmin Zou,Songfan Tang,Mingliang Luo,Xianggang Li
The chromium-benzenedicarboxylate metal–organic framework (MOF), MIL-101(Cr), is one of the most well-investigated and widely used prototypical MOFs. Regarding its synthesis, the use of a toxic modulator (usually HF) and high reaction temperature (220 °C) are the main factors hindering its further expansion of production and utilization. In fact, high quality MIL-101(Cr) crystals can be prepared at a much lower temperature (160 °C) with spherical morphology via an additive-free approach. Compared to traditional octahedral MIL-101(Cr), the spherical MIL-101(Cr) possesses higher adsorption performance toward dye molecules, including methyl orange (MO) and rhodamine B (RB). The results suggest that toxic additives and high reaction temperatures are not essential in the synthesis of MIL-101(Cr), and the fabrication of spherical MIL-101(Cr) may offer a facile and effective pathway for the large-scale industrial application of MIL-101(Cr).
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
Catalysts
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2018
·Vol. 8
·期 9
·394
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IF 3.465
Tian Zhao,Ming Dong,Ling Yang,Yuejun Liu
Nowadays, the controllable synthesis of stable hierarchical metal–organic frameworks (MOFs) is very important for practical applications, especially in catalysis. Herein, a well-known chromium–benzenedicarboxylate metal–organic framework, MIL-101(Cr), with a stable hierarchical structure, was produced by using phenylphosphonic acid (PPOA) as a modulator via the hydrothermal method. The presence of phenylphosphonic acid could create structural defects and generate larger mesopores. The synthesized hierarchical MIL-101(Cr) possesses relatively good porosity, and the larger mesopores had widths of 4–10 nm. The hierarchical MIL-101(Cr) showed significant improvement for catalytic activity in the oxidation of indene. Further, the presence of a hierarchical structure could largely enhance large dye molecule uptake properties by impregnating.Keywords:MIL-101(Cr);phenylphosphonic acid;hierarchical;enhanced catalytic activity;large molecule uptake
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Chemical Engineering Journal Advances
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2023
·
IF 0
Mengsi Cheng,Ying Fang,Zhaoguang Yang,Xinghao Liu,Bo Qiu,Tong Zhang,Haipu Li,Wenbo Zhao
MIL-100(Fe) was modified by amino groups (MIL - 100(Fe) - NH 2 ) to enhance the removal of antimonate (Sb(V)) with low concentration (50−200 μg/L) from natural water through batch adsorption experiments. With the initial Sb(V) concentration up to 200 μg/L, the residual Sb(V) concentration after treated by MIL - 100(Fe) - NH 2 was only 3.52 ± 0.131 μg/L, lower than the drinking water standards (5 μg/L) in China, while that was much higher (94.2 ± 3.52 μg/L) after pristine MIL-100(Fe) treatment. Based on results of XPS analysis, and adsorption kinetics and isotherms, we concluded that Sb(V) substituted the terminal −OH groups of MIL-100(Fe) to form inner-sphere complexes by coordination reactions with Fe nodes and be adsorbed by hydrogen bonding as well. The grafted amino groups (−NH 2 ) adsorbed Sb(V) by hydrogen bonding and facilitated the coordination reactions between Sb(V) and Fe nodes. The higher K L value (0.0116 ± 0.00,118 L/μg) obtained by fitting with the Langmuir isotherm model, while that of unmodified MIL-100(Fe) was 4.74 × 10 −4 ± 5.85 × 10 −5 L/μg, also confirmed that the −NH 2 groups greatly enhanced the affinity between MIL-100(Fe) and Sb(V). Furthermore, MIL - 100(Fe) - NH 2 still worked nicely in a wide pH range (2 − 12), with varied ionic strength (0.05 µmol/ L −1.5 mol/L), coexisting ions (CO 3 2− , NO 3 − , SO 4 2− , Cl − , H 2 PO 4 − ), and even in the real water bodies. Additionally, MIL - 100(Fe) - NH 2 exhibited good reusability and low Fe leaching (99.92 μg/L). We hope MIL - 100(Fe) - NH 2 become a candidate for effective removal of Sb(V), even other heavy metals from natural waterbodies.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
DALTON TRANSACTIONS
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2018
·Vol. 47
·期 18
·6394-6403
·
IF 4.099
Yanqin Li,Qi Gao,Lijuan Zhang,Yunshan Zhou,Yuxu Zhong,Ying Ying,Mingcai Zhang,Chunqian Huang,Yong'an Wang
Currently extensive effort is compulsively expended to decontaminate efficiently banned chemical war agents. In this work, H5PV2Mo10O40 molecules have been encapsulated in mesoporous MIL-101(Cr), which features two types of mesoporous cages (internal diameters of 29 Å and 34 Å) and microporous windows (diameters of 12 Å and 16 Å), leading to the formation of a new composite H5PV2Mo10O40@MIL-101(Cr) through a simple impregnation method. The composite was characterized thoroughly by elemental analysis, FT-IR spectroscopy, powder X-ray diffraction, scanning electron microscopy, energy dispersive X-ray spectroscopy, TG/DTA, and textural analysis thereby confirming the encapsulation of the H5PV2Mo10O40 into MIL-101(Cr). The decontamination efficiency of sulfur mustard (4 μL HD in 40 μL of petroleum ether) by 20 mg of the composite is found to be 97.39% in 120 min under ambient conditions. GC-MS analysis on the decontaminated products using 2-chloroethyl ethyl sulfide (CEES), which has been widely used as a simulant of sulfur mustard, showed that MIL-101(Cr) just decontaminates CEES by adsorption, while CEES can be decontaminated under ambient conditions by a synergetic combination of adsorption of MIL-101(Cr) and subsequent chemical oxidation degradation to nontoxic 2-chloroethyl ethyl sulfoxide (CEESO) due to the presence of highly dispersed H5PV2Mo10O40 within the composites.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
DOI
高影响因子
Frontiers in Chemistry
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2021
·
IF 5.221
Zhang Hui,Zhou Liang,Li Jing,Rong Sijia,Jiang Jianping,Liu Shengquan
Herein, we report a novel carboxymethyl cellulose (CMC)/MIL-101 (Fe)/poly(β-cyclodextrin) (β-CDP) hydrogel with high photocatalytic activity. β-CDP can significantly enhance the photoactivity of MIL-101(Fe) in the hydrogel prepared by a simple solvothermal method. The structure and property of this composite hydrogel were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. Tetracycline was selected as a model pharmaceutical antibiotic to evaluate the photocatalytic activity of the composite hydrogel under visible light irradiation and darkness, respectively. This composite hydrogel shows excellent activity for degrading pharmaceutical antibiotics under visible light irradiation. The increased photocatalytic activity can be attributed to β-CDP, which acts as a promoter and affords an efficient separation of photogenerated electron-hole pairs of MIL-101(Fe). Moreover, the composite hydrogel is shown to have good water retainability. The hydrogel is inexpensive and shows high photocatalytic activity. Hence, it can be used as an efficient photocatalytic material.
研究领域:
环境科学
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材料科学
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药学
✓ 已验证
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
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2024
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IF 4.3
Yuhao Che,Wenhui Li,Chunqi Wang,Xuemin Zhang,Zilei Guo,Aziz Bakhtiyarovich Ibragimov,Junkuo Gao
The development of materials with superior thermal insulation and flame retardancy is critical for industrial applications and daily life. Metal–organic framework (MOF)@poly(vinyl alcohol) (PVA) (MOF@PVA) aerogel composites have demonstrated remarkable thermal insulation and flame retardancy properties. In this work, MIL-53(Al) was directly mixed with PVA and formed by freeze-drying, and the influence of the pore structure on the thermal insulation and flame retardancy properties of the materials was investigated. The incorporated MIL-53(Al) nanoparticles introduced abundant micro- and mesopores, enhancing the complexity of the pore structure and improving the thermal insulation and flame retardancy properties of the aerogels. The directionally freeze-cast aerogel achieved a thermal conductivity of 0.040 W·mK–1, and maintained excellent thermal insulation ability even at 220 °C. Furthermore, the aerogel exhibited nonflammable and self-extinguishing characteristics. This environmentally friendly manufacturing method provides new ideas for the design of MOF-based composites, thereby expanding their application areas.
研究领域:
材料科学
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化学工程
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热能工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
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2017
·
IF 3.981
Shu-Hui Huo,Hai-Yan An,Jing Yu,Xue-Feng Mao,Zhe Zhang,Lei Bai,Yan-Feng Huang,Peng-Xin Zhou
In this study, we report a facile, environmental friendly fabrication of a type of magnetic metal-organic framework (MOF) MIL-100 that can be used for magnetic solid-phase extraction (MSPE). The magnetic MOF composites were fabricated using in situ calcination method. The as-synthesized materials exhibited both high porosity and magnetic characteristics. They used for the MSPE of polycyclic aromatic hydrocarbons (PAHs) from water samples. Such MOF-based magnetic solid-phase extraction in combination with gas chromatography equipped with a flame ionization detector (GC-FID), exhibited wide linearity (0.02–250 μ g L −1 ), low detection limits (4.6-8.9 ng L −1 ), and high enrichment factors (452–907) for PAHs. The relative standard deviations (RSDs) for intra- and inter-day extractions of PAHs were ranging from 1.7% to 9.8% and 3.8% to 9.2%, respectively. The recoveries for spiked PAHs (1 μ g L −1 ) in water samples were in the range of 88.5% to 106.6%. The results showed that the special anion-π orbital (electron donor-acceptor) interaction and π-π stacking between magnetic MIL-100 and PAHs play an important role in the adsorption of PAHs.
研究领域:
分析化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
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2024
·
IF 14
Jinzhi Jia,Jinhua Zhang,Kailu Guo,Lanyue Zhang,Gening Du,Hao You,Junfeng Huang,Mudong Tu,Hua Li,Yong Peng,Wei Dou,Cailing Xu
Designing highly active and stable electrocatalysts of oxygen evolution reaction (OER) is one of the crucial challenges. In this study, a novel OER electrocatalyst, NiFe-MIL-53 modified with ultra-low rhodium (Rh@NiFe-MIL-53), is successfully prepared via the hydrothermal method. In-situ Raman spectroscopy and electrochemical impedance spectroscopy reveal that the doped Rh accelerates the phase transformation of NiFe-MIL-53 and the in-situ formed Rh@NiFeOOH is the actual active species. More importantly, the enhanced reversibility of electrochemical reconstruction between NiFeOOH and NiFe(OH) 2 after doping Rh is beneficial for improving the electrochemical stability of the catalyst. X-ray photoelectron spectroscopy spectra show the strong electronic interaction between single-atom Rh and Ni/Fe in Rh@NiFeOOH. Furthermore, theoretical calculations confirm that the integration of single-atom Rh into the NiFeOOH successfully reduces the band gap, regulates the d -band center ( ε d ), accelerates the charge transfer, and optimizes the adsorption behavior of oxygen-containing intermediates, thereby lowering the energy barrier of rate-determining steps. Consequently, the optimized Rh@NiFe-MIL-53 exhibits excellent OER activity (240 mV) with a small Tafel slope of 48.2 mV dec −1 and long-term durability (over 1270 h at 10 mA cm −2 and 110 h at 200 mA cm −2 ). This work presents a new perspective on designing highly efficient OER electrocatalysts.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Mingyu Li,Chaoqun Li,Zhao Chunrui,Tianren Li,Jingjing Jiang,Zhonghui Han,Chongjun Zhang,Haoran Sun,Shuangshi Dong
Fe-based metal organic framework with high active site exposure, wide light absorption and fast H 2 O 2 activation are pivotal for photo-Fenton degradation of contaminants. However, insufficient active site exposure, weak visible light adsorption and low charge transfer efficiency in iron-oxo clusters usually lead to the slow Fe(II)/Fe(III) cycle. In this study, we develop a novel citric acid (CA)-modified MIL-88A(Fe) strategy to boost photo-Fenton efficiency by accelerating Fe(II)/Fe(III) cycle for emerging contaminants removal. Relationship between CA coordination mode and photo-Fenton performance was studied by using methylene blue (MB) and carbamazepine (CBZ) as model contaminants. It was found that the degradation rate constants of MIL-88A(Fe)-CA-3 were 6.5 and 2.6 times higher than those in the pristine MIL-88A(Fe) for MB and CBZ degradation, respectively. The optimized MIL-88A(Fe)-CA-3 also exhibited good recyclability, enabling multiple cycles in photo-Fenton reaction. The results of experimental characterizations and density functional theory calculations demonstrated that ligand substitution was conductive to active site exposure, visible light absorption, charge carrier transfer and Fe 2+ /Fe 3+ redox cycle, which are responsible for an improved photo-Fenton performance.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
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2025
·
IF 2.3
Xiaoli Ding,Qiankun Zhang,Hongyong Zhao,Qingping Xin,Yuzhong Zhang
Two series of mixed matrix membranes (MMMs) have been synthesized via in situ UV polymerization for the removal of N2 from CH4. MIL-100(Cr) particles activated at different temperatures were used as fillers. MIL-100(Cr) activated at 150°C with CH4-selective adsorption was incorporated with poly(ethylene oxide)-based polymer to improve the CH4/N2 separation performance, and that activated at 250°C with N2-selective adsorption and diffusion was incorporated with fluoropolymer to improve the N2/CH4 separation performance. The effects of the filler loadings on the gas permeation and separation performances were investigated. The optimum MMMs with 5 wt.% loading of MIL-100(Cr) activated at 150°C exhibited a 70% increased CH4/N2 permselectivity of 5.0 with a 37% increased CH4 permeability of 11.2 Barrer (tested at 0.2 MPa and 35°C). The optimum MMMs with 5 wt.% loading of MIL-100(Cr) activated at 250°C exhibited a 106% increased N2 permeability of 71.5 Barrer with an 89% increased N2/CH4 permselectivity of 1.9.
研究领域:
化学工程
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材料科学
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膜技术
·
气体分离
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2024
·
IF 5.9
Fuhao Gan,Chunmei Gao,Shifeng Ji,Yunqing Xing,Tianming Gong,Lihui Tian,Yiming Bai,Zhuolong Wu
In this study, the iron-based metal–organic framework MIL-53(Fe) was successfully prepared by a solvent method and used as a photocatalyst for the efficient degradation of DDBAC under visible light. The morphology, structure and photocatalytic properties of MIL-53(Fe) were investigated by SEM, XRD, XPS and UV–vis DRS characterization methods. The optimum conditions for the degradation of DD pathways of DDBAC were analyzed in combination with DFT calculations. Based on molecular orbital theory and free radical quenching experiments, it was demonstrated that hydroxyl radicals were the main contributors in the oxidative degradation of DDBAC. The toxicity of DDBAC and its intermediates was evaluated by culturing Chlorella vulgaris, and the results showed that the Vis/MIL-53(Fe)/H 2 O 2 system was capable of solution detoxification.
研究领域:
环境科学
·
材料科学
✓ 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）