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
✓ 已验证
产品关联
DOI
高影响因子
Chemical Engineering Journal Advances
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2023
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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
FUEL
·
2022
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IF 8.035
Hui Li,Tianyu Wang,Yangyang Wang,Fengsheng Liu,Yan Li,Yunpu Wang,Min Guo,Guoning Li,Xiaoling Ma
Sulfated metal oxides are widely used in catalyzing esterification for biodiesel production due to their low corrosivity and easy separation. While, the catalytic stability is still a challenge on account of active site leaching during successive batch experiments. To this end, the typical metal organic frameworks, MIL-100(Fe) doped with Co was adopted to load ammonium sulfate ((NH 4 ) 2 SO 4 ) for stable heterogeneous acid preparation, which was employed to catalyze the esterification of methanol and oleic acid. Influence of preparation factors of (NH 4 ) 2 SO 4 loading amount and activation temperature on catalytic activity were initially evaluated. Furthermore, to elucidate the effect of Co doping, catalysts were characterized by TG, XRD, FTIR, nitrogen adsorption–desorption, Py-FTIR, XPS, SEM and NH 3 -TPD. Results indicated that the maximum esterification conversion of 92.56 % was achieved by MS(Fe/Co) with molar ratio of methanol to oleic acid of 8:1 and catalyst amount of 8 wt% at 70 °C in 2 h. In comparison to MS(Fe), Co doping significantly improved the stability, where the catalytic activity of MS(Fe/Co) was increased by 20 % at the fifth cycle. The activation energy and pre-exponential factor of esterification catalyzed by MS(Fe/Co) were also calculated as 42.06 kJ/mol and 5.24 × 10 5 min −1 . This study provides a feasible way to enhance the catalytic stability of heterogeneous acid for biodiesel production.
研究领域:
催化化学
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材料科学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
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2017
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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
ACS Applied Nano Materials
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2021
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IF 5.097
Mingqi Xu,Dingzhou Liu,Jinghua Yang,Qian Zhu,Yunliang Wang,Jingquan Sha
Study and application of MIL-100(Fe)-based two-dimensional graphene oxide (GO) nanocomposite was limited because the nucleation of the spherical structure of MIL-100(Fe) on GO along different directions hindered the formation of MOF-100(Fe). To address this issue, MIL-100(Fe)/three-dimensional graphene (3DG) nanocomposites (abbreviated as MIL-3DG-n, n = 25, 50, 75, and 100) were successfully fabricated via in situ growth of MIL-100(Fe) on 3DG matrixes in this work because the unique structure of 3DG can avoid the attachment with MIL-100(Fe) on nucleation sites along multiple directions, resulting in their ideal combination. The prepared MIL-3DG nanocomposites exhibited higher peroxidase-like catalytic activities than pure MIL-100(Fe), and MIL-3DG-75 exhibited the best peroxidase-like activities for detecting xanthine with the detection limit of 0.0014 μM in the linear range of 0–200 μM to date, to the best of our knowledge, which is attributed to the higher affinity of MIL-3DG-75 nanocomposite to peroxidase substrates o-phenylenediamine (OPD) and H2O2, confirmed by the Michaelis–Menten kinetics (Vm: 49.5 × 10–8 M s–1 for H2O2, 18 × 10–8 M s–1 for OPD, Km: 0.029 mM for H2O2, 0.011 mM for OPD). Owing to the high catalytic efficiency of the MIL-3DG-75 nanocomposite, a rapid and efficient strategy for the sensitive colorimetric detection of xanthine was established.
研究领域:
材料科学
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生物医学工程
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
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2025
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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
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气体分离
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Hongbing Mao,Huijun Wang,Yanyan Xing,Deyong Wang,Xiujun Cao,Jie Yu,Junya Yan
In this work, a boronic acid decorated mesoporous iron-based metal-organic framework (MIL-100(Fe)-B) nanozyme as an efficient immobilization matrix for glucose oxidase (GOx) was designed and prepared through a facile microwave-assisted metal-ligand-fragment co-assembly strategy. Compared with the unboric acid-modified MIL-100(Fe), boron-doped MIL-100(Fe) exhibited enhanced peroxidase-like activity, which was mainly due to the introduced B causing MIL-100(Fe) defects, accelerating mass transfer, facilitating more active sites for H2O2 decomposition. Besides, the MIL-100(Fe)-B nanozyme possessed sufficient recognition sites for immobilizing glucose oxidase with little enzyme leakage to form a cascade nanozyme with both peroxidase-like and cascade catalytic activities. A colormetric biosensor based on the integrated nanozyme reactor (GOx@MIL-100(Fe)-B) was developed for glucose detection. The proposed cascade biosensor had a linear range of 5-150 μM and a limit of detection (LOD) of 0.97 μM (3.3 δ/S). Interestingly, a portable microfluidic paper-based analytic device (μPAD) biosensor based on the cascade nanoplatform was further fabricated for visualized detection of glucose combined with a ColorPicker App on smartphone. It indicated that the integrated nanozyme GOx@MIL-100(Fe)-B was a promising candidate for glucose detection and provided a potentially analytical avenue for biosensing and other applications.
研究领域:
生物化学
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分析化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
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IF 3.171
Tao Zhao,Dazhong Zhong,Genyan Hao,Guang Liu,Jinping Li,Qiang Zhao
Metal-organic frameworks (MOFs) exhibit excellent application potential in the field of electrocatalysis. In this study, we first prepare MIL-100 nanosheets on nickel foam (MIL-100/NF) and then successfully anchor Ag nanoparticles (NPs) on the nanosheets (Ag@MIL-100/NF) for oxygen evolution reaction (OER) catalysis. This strategy dramatically improves the conductivity of MIL-100 and the Ag NPs are uniformly dispersed on the nanosheets. The Ag@MIL-100/NF catalyst has excellent electrocatalytic performance and long-term corrosion resistance, with a low overpotential of 207 mV and a long-term stability of at least 100 h at a current density of 50 mA·cm −2 . The experimental results demonstrate that this high OER catalytic performance is due to the improved charge transfer after loading Ag NPs, the combination of nanosheets and highly dispersed Ag NPs that expose more active sites and the adjusted chemical valence states of Fe and Ni in MIL-100. This work provides a surface decoration approach for the preparation of excellent catalysts directly used in the OER.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Munir Ahmad,Shuo Chen,Fei Ye,Xie Quan,Shahzad Afzal,Hongtao Yu,Xueyang Zhao
Metal-organic frameworks (MOFs) have received significant interest as a promising photocatalyst for environmental remediation due to its high surface area and porous nature. The small pores (<2 nm) in microporous MOFs help the adsorption of small molecules but limits diffusion and accessing of bigger molecules from MOF cavities, thus preventing their applications in some situation. The aim of this work is to fabricate mesoporous MOF composite with larger pore sizes (>2 nm) and open pore cavities that can provide right pathways for ingoing and outgoing of molecules during catalysis. Herein, we successfully report stable mesoporous MIL-100(Fe) loaded with ZnO NS by an in situ self-assembly method. The prepared samples were characterized by Brunauer–Emmett–Teller (BET) and N 2 adsorption-desorption isotherm to study their surface area and porosity. The catalytic performance of mesoporous MIL-100(Fe) was approximately 2–3 order of magnitude more than that of microporous MIL-100(Fe). Such higher catalytic activity in mesoporous MIL-100(Fe) can be ascribed to its mesocellular structure which can improve the molecular diffusion and accessibility inside MOF channels. The charge separation efficiency and photo-Fenton activity of mesoporous MIL-100(Fe) can further be increased by introduction of certain amount of ZnO NS and H 2 O 2 . Moreover, the as synthesized sample shows higher photo-Fenton degradation efficiency at lower pH value with certain amount of H 2 O 2 . Lastly, the possible catalytic mechanism has been tentatively proposed. This study not only used for the pollutants degradation but also provide useful platform for the application of mesoporous MOFs as an efficient photo-Fenton activity to various other fields.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Sijia Li,Jianan Cui,Xia Wu,Xuan Zhang,Qi Hu,Xiaohong Hou
Metal-Organic Frameworks (MOFs) are efficient adsorbent and catalyst, however, the prepare of MOFs can be extremely time consuming. The rapid in situ microwave synthesis process offers the possibility of MOFs to a large-scale application. In this study, Fe 3 O 4 @MIL-100(Fe) was rapidly prepared via microwave in 30 min using Fe 3 O 4 as metal precursor and applied as the adsorbent and photocatalyst to remove diclofenac sodium (DCF) from water. Fe 3 O 4 @MIL-100(Fe) exhibited an excellent adsorption effect to DCF with the maximum adsorption capacities of 400 mg/L. The presence of H 2 O 2 could promote the removal of DCF during photocatalytic process. Approximately 99.4% of the DCF was removed in Fe 3 O 4 @MIL-100(Fe)/vis/H 2 O 2 system via adsorption removal and consequent photocatalytic degradation . The high efficiency was attributed to the large BET surface area (1244.62 m 2 /g) and abundant iron metal sites (Fe(III) and Fe(II)) of Fe 3 O 4 @MIL-100(Fe). The adsorptive, photocatalytic property of Fe 3 O 4 @MIL-100(Fe) and the Fenton-like reaction were the main mechanisms for DCF removal. TOC analyzer was served to assess the mineralization of solutions treated by Fe 3 O 4 @MIL-100(Fe)/vis/H 2 O 2 in 12 h. High elimination of TOC (87.8%) was observed during the DCF mineralization process. In addition, the major products were illuminated using HPLC-Q-TOF-MS and DCF degradation pathways were also proposed.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
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IF 6.361
Haibo Zhang,Jia Wen,Ying Fang,Siyu Zhang,Guangming Zeng
Hypothesis Modification of MIL-100(Fe) with ethanediamine (ED) is expected to improve the removal percentage of Pb(II) ions from aqueous solution. Nevertheless, the adsorption performance of ED-MIL-100(Fe) in natural waters will be affected by natural organic matter such as fulvic acids (FA). Hence, it is necessary to study the influence of FA on the physicochemical property, adsorption behavior and mechanisms of ED-MIL-100(Fe) towards the removal of Pb(II) from water. Experiments Batch adsorption experiments were conducted to compare adsorption capacity of MIL-100(Fe) and ED-MIL-100(Fe) for Pb(II). In addition, XRD , FTIR, SEM and XPS techniques were applied to investigate the characteristics, adsorption isotherms , and kinetics in the presence and absence of FA. Findings ED-MIL-100(Fe) enabled 99% removal of Pb(II) from water at or below 60 mg L −1 , whereas the MIL-100(Fe) hardly adsorbed any Pb(II). Additionally, the adsorption percentage of the Pb(II) ions (76%) outcompeted that of other metal ions (i.e. Co, Cu, Ni, Zn, and Cd) (each ≤ 25%) in the mixed solution. The negative surface charge of ED-MIL-100(Fe) was not affected by FA. Increasing FA concentration steadily increased the functional groups surrounding the ED-MIL-100(Fe) via electrical interaction, thus facilitating the Pb(II) ions adsorption.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2025
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IF 5.3
Zhuo Chen,Ze Zhang,Rongxin Xia,Junhu Zhou,Jun Cheng
To improve the conversion rate of carbon dioxide (CO2) to methane (CH4) in a microbial electrochemical system (MES), the zeolitic imidazolate framework ZIF-67(Co) with electron storage properties was first grown in situ on MIL-100(Fe) with excellent CO2 adsorption properties by a hydrothermal method. The obtained binary core–shell MIL@ZIF material was then adsorbed by carbon felt on a cathode to grow biofilms composed of electroactive microorganisms for characterization and testing in an MES. This system exhibited a CH4 production rate of 0.42 mmol LR–1 d–1, along with an impressive faradaic efficiency of 96.4%. Three-dimensional excitation–emission matrix spectra of extracellular polymeric substances indicated that those containing higher contents of humic acid shifted electron pairs and converted redox states to facilitate electron transfer. MIL@ZIF enriched hydrogenotrophic methanogens and electrogenic bacteria in microbial communities with enhanced gene expression of electrically conductive pili and cytochrome C to strengthen interspecies electron transfer. MIL@ZIF enhanced CO2 adsorption and electron storage, reinforcing electron transfer chains and boosting CH4 yield by a factor of 10.7.
研究领域:
环境科学
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微生物学
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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）