CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Qiong Wu,Yining Liu,Haochuan Jing,Hongbin Yu,Ying Lu,Mingxin Huo,Hongliang Huo
Special enhanced synergistic effect of ultra-small γ-Fe 2 O 3 and graphene oxide (GO) on MIL-53 (Fe) was achieved for boosting photocatalysis. Compared to traditional methods of surface coverage, the incorporation of γ-Fe 2 O 3 (average size 2–3 nm) inside MOFs particles not only increased the light absorption of catalyst, but also formed numerous micro-heterojunctions with MOFs units and thus effectively facilitated the separation of photogenerated carriers. By supplying attachment sites for MOFs crystal, the functionalized GO reduced the size of MOFs particles to 100–200 nm, meanwhile improved their dispersibility. The active sites and quantum yield of photocatalytic reaction were also intensified benefiting from the large surface area and high electronic conductivity of GO. Therefore, the novel γ-Fe 2 O 3 -MIL-53(Fe)-GO composite exhibited the highest photocatalytic activity towards norfloxacin, with a removal rate of 92.8% in 90 min. The kinetic constant was 4.49-fold higher than that using pure MIL-53 (Fe), and 1.43-time greater than that in the system of MIL-53 (Fe) and hydrogen peroxide, which usually acted as efficient electron acceptors to increase the quantum yield and final photocatalytic performance of MOFs. Based on the identified intermediates, three NOR degradation pathways including the cleavage of piperazine ring, defluorination and decarboxylation, as well as the conversion of quinolones group were proposed. Photocatalytic mechanism investigation revealed the holes and hydroxyl radicals came from the reaction of electrons with oxygen played the important role in γ-Fe 2 O 3 -MIL-53(Fe)-GO photocatalysis. Moreover, the utilization of magnetic nanoparticles improved the recovery and recyclability of ternary catalyst.
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CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Xiaohan Guo,Yanfang Liu,Hongxiang Zhu,Xiaohui Yu,Feng Shi,Qinqin Liu,Qiang Liu,Ying Xu
Asp donates electrons to reprogram Fe O clusters of MIL-53(Fe). • This electronic switch redirects dominant ROS from •OH to •O 2 − . • The mechanism enables neutral-pH POD-like activity of MIL-53(Fe)@Asp. • The Asp-modified nanozyme integrates with GOX for cascade glucose sensing. MIL-53(Fe) exhibits peroxidase-like activity only under acidic conditions, limiting its biosensing applications. We overcome this by using aspartic acid (Asp) as a structure-directing agent to modify MIL-53(Fe) (MIL-53(Fe)@Asp) via hydrothermal synthesis followed by Asp coordination. Unlike conventional pH-reduction strategies, Asp modification does not alter bulk pH but induces intrinsic electronic restructuring of Fe O clusters, as confirmed by increased Fe 3+ /Fe 2+ ratio and introduction of N → Fe coordination (XPS). At pH 6.9, the TMB-based activity of MIL-53(Fe)@Asp is 27-fold higher than that of pristine MIL-53(Fe). Steady-state kinetics show favorable Km values (TMB 0.27 mM, H 2 O 2 1.38 mM) at neutral pH. Mechanistic studies (ROS identification, EPR, band structure, DFT) reveal that Asp exerts an electron-donating effect that reprograms the electron distribution of Fe O clusters, activating the otherwise inactive MIL-53(Fe) framework at neutral pH and diversifying the catalytic pathways to include a less pH-dependent •O 2 − route alongside the partially maintained •OH pathway. This pathway diversification enables efficient neutral-pH peroxidase-like catalysis, with •O 2 − as the dominant pathway. Leveraging this, we construct a cascade nanoplatform (MIL-53(Fe)@Asp@GOX) integrating glucose oxidase, which exhibits excellent cascade activity at neutral pH. The method is applied to glucose detection in blood and saliva, demonstrating good linearity, precision, selectivity, and recovery. The glucose concentrations determined by our sensor correlated well with those obtained using a commercial assay kit. Notably, the limit of detection for glucose in saliva reaches 2.08 μM, offering a promising route toward non-invasive glucose sensing. This work establishes a design principle for creating pH-adaptive catalytic microenvironments in Fe-MOFs through electronic restructuring and pathway diversification, overcoming a long-standing limitation of MIL-53(Fe) for biomedical applications. Download: Download high-res image (111KB) Download: Download full-size image
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FOOD CHEMISTRY
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2023
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IF 8.8
Yu-Han Sun,Liu Yang,Xian-Xian Ji,Yuan-Zhen Wang,Yu-Long Liu,Ying Fu,Fei Ye
Flusilazole is a triazole fungicide with residues that are potentially toxic to humans. It enters the human body mainly through food, although its bactericidal activity is substantial. In this study, an electrochemical sensor Fe/Fe 2 O 3 @C with a core–shell structure was constructed to efficiently detect flusilazole by annealing MIL-53(Fe) which was prepared by a simple solvothermal method. Transmission electron microscopy and scanning electron microscopy were used to characterize the apparent morphology of MIL-53(Fe) and Fe/Fe 2 O 3 @C , and their structures were further characterized by X-ray photoelectron spectroscopy, Raman spectroscopy, powder X-ray diffraction, and the mapping of elements by energy dispersive spectroscopy. The electrochemical behavior of Fe/Fe 2 O 3 @C in the detection of flusilazole was evaluated by differential pulse voltammetry under optimal conditions. The results of the study indicate that the Fe/Fe 2 O 3 @C electrochemical sensor displayed excellent detection capabilities for flusilazole, where the sensor exhibited a wide detection range from 1.00 × 10 −4 to 1.00 × 10 −12 mol/L with an incredibly low LOD of 593 fM, making it highly sensitive to trace amounts of flusilazole. Moreover, Fe/Fe 2 O 3 @C demonstrated superior reproducibility, stability, and resistance to interference, highlighting its reliability in practical applications. The sensor was also successfully utilized to quantitatively detect flusilazole in various real samples, which suggests that Fe/Fe 2 O 3 @C has broad-spectrum environmental resistance and can effectively and rapidly detect flusilazole residues in different types of food items and environmental matrices. The study also delved into the mechanism of Fe/Fe 2 O 3 @C for the detection of flusilazole, providing a deeper understanding of the functionality of this sensor. Overall, these findings emphasize the practical significance of Fe/Fe 2 O 3 @C as an electrochemical sensor, showcasing its potential for real-world applications in food safety and environmental monitoring.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Shiyu Zhang,Mengru Li,Jingwen Wang,Ruonan Zhang,Xiaoyu Ma,Haisheng Tao
Metal-organic frameworks with high porosity have received much attention in environmental pollutant treatment. This study presented a simple single-pot solvent thermal method for the preparation of a bimetal-organic framework MIL-53(Fe,Ni), further used for activated peroxydisulfate to degrade rhodamine B (RhB). The morphology and structure of the sample were characterized by scanning electron microscopy, transmission electron microscopy , x-ray diffraction, photoelectron spectroscopy , fourier transform infrared spectroscopy , and thermogravimetric analysis . The results showed that MIL-53(Fe,Ni) was successfully synthesized by the simple reaction, with high thermal stability and high specific surface area. The effects of pH value, co-existing ions, temperature, humic acid and different real water samples on RhB degradation were systematically investigated. Under optimized conditions, 93.9% of RhB was degraded within 180 min, together with excellent reusability. Quenching experiments and electron paramagnetic resonance showed that both free radicals (∙OH, SO 4 ∙- and O 2 ∙- ) and non-free radicals ( 1 O 2 and direct charge transfer) were responsible for the RhB degradation. In addition, the identification of intermediates by high-resolution mass spectrometer and reaction site prediction calculations (electrostatic potential, Fukui function and molecular orbit analysis), proposing a possible degradation pathway of RhB. The work highlights the broad applications of bimetal-organic frameworks in advanced oxidation processes .
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RSC Advances
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2015
·Vol. 5
·期 50
·40094-40102
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IF 3.84
Zhiming Yan,Wenmin Zhang,Jia Gao,Yifen Lin,Jianrong Li,Zian Lin,Lan Zhang
The application of the metal–organic framework (MOF) MIL-53(Fe) as a novel stationary phase for reverse-phase high performance liquid chromatography (HPLC) separation of positional isomers is described for the first time. Under the optimized conditions, baseline separation of xylene, dichlorobenzene, chlorotoluene and nitroaniline isomers was achieved on the MIL-53(Fe) packed column within a short time. The retention mechanisms of these isomers on the MIL-53(Fe) packed column were discussed in detail, and a typical reverse-phase behavior can describe the results. The thermodynamic characteristics of the HPLC separation of positional isomers were also evaluated. It was confirmed that the HPLC separation of positional isomers was controlled by the Gibbs free energy change (ΔG). In addition, reverse-phase HPLC separation of the tested isomers was also carried on MIL-53(Al, Cr) packed columns to investigate the influence of the metal centre of the MIL-53 framework on their chromatographic behaviors. The results showed that the MIL-53(Fe) packed column exhibited better separation performance than the MIL-53(Al, Cr) packed columns. Moreover, the MIL-53(Fe) packed column also gave efficient HPLC separation of alkylbenzene and naphthalene, aniline compounds and polycyclic aromatic hydrocarbons (PAHs). These successful applications suggest the potential of MIL-53(Fe) as a novel stationary phase for efficient reverse-phase HPLC separation.
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ACS Applied Nano Materials
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2024
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IF 5.3
Baixin Liu,Xuelian Chen,Guojuan Hai,Wenwen Zhao,Kai Li,Zhicong Yuan,Xiaoyong Zhang
The design and synthesis of metal–organic frameworks (MOFs) for direct use as electrode materials are crucial for enhancing the electrocatalytic oxygen evolution reaction (OER). Herein, the ultrathin MIL-53(Fe) nanosheet arrays with enriched coordinatively unsaturated metal sites (denoted as MIL-53(Fe)/NF-B0.2-2) are obtained under the inhibition and modulation of benzoic acid (BA) ligands via a substitution-suppression process. The results confirm that this unique ultrathin structure effectively increases the electrochemical active surface areas (ECSA) and exposes the coordinatively unsaturated metal sites. More importantly, the enriched coordinatively unsaturated metal sites acting as active sites facilitate the adsorption of OH– during the OER process. Additionally, MIL-53(Fe)/NF-B0.2-2, with its optimized energy band structure, exhibits superior charge transfer ability and diffusion processes, significantly improving the reaction kinetics in alkaline electrolytes. As a result, the MIL-53(Fe)/NF-B0.2-2 electrode only requires extremely low overpotentials of 190 and 229 mV to reach current densities of 10 and 100 mA cm–2 for OER, respectively. This research not only proposes a novel strategy for designing efficient electrocatalysts but also provides insights into the structure–activity relationship, advancing the rational design of MOFs as effective electrode materials.
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POLYMER ENGINEERING AND SCIENCE
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2024
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IF 3.2
Wenlong Ma,Tianxu Hao,Xinya Wang,Wei Zhang,Yonggui Li,Mingxing Chen
In this paper, a high-performance composite nanofiber membrane with excellent air filtration and dye degradation properties was prepared by incorporating MIL-53(Fe) nanoparticles into the electrospinning solution. The results showed that the filtration efficiency for PM2.5 of the PP/PVDF-HFP/MIL-53(Fe) composite nanofiber membrane reached up to 99.3% with the addition of 2 wt% MIL-53(Fe). Moreover, the composite nanofiber membrane exhibited steady filtration efficiency across different parameters, including air velocity, PM2.5 concentration, and extended testing time. Furthermore, the incorporation of MIL-53(Fe) significantly enhanced the removal efficiency of the composite nanofiber membrane toward Rh B, resulting in a remarkable 91% removal rate. The polymer/MOF composite nanofiber membranes prepared by simple and cheap electrospinning technology have a wide range of practical applications in the field of environmental protection. Highlights PPM composite nanofiber membrane was prepared via electrospinning method. MIL-53(Fe) nanoparticles were introduced to PPM composite nanofiber membrane. PPM composite nanofiber membrane showed excellent removal efficiency for PM2.5. PPM composite nanofiber showed a good removal performance for RhB in solution.
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JOURNAL OF FOOD ENGINEERING
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2025
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IF 5.8
Sihang Li,Xun Zhou,Jiahao Cui,Xingjian Zou,Zijian Li,Wirote Youravong,Ming Li,Haihua Wang,Zhenyu Li
Residual Alicyclobacillus acidoterrestris severely impacts juice quality. Conventional thermal treatments fail to completely eliminate bacteria and simultaneously cause the loss of heat-sensitive components. Ultrafiltration (UF) has been a nonthermal alternative to conventional thermal process for the sterilization of apple juice. However, membrane fouling, particularly biofouling is an obstacle for deployment of UF in food processing. In order to tackle the challenging issue of membrane biofouling while ensuring food safety, functionalized UF membrane was developed by multi-stage modifications including metal chelator coating and chlorogenic acid-encapsulated MIL-53(Fe) microparticle grafting. The engineered membrane was applied for cold sterilization of apple juice to remove Alicyclobacillus acidoterrestris . Results showed that (i) the engineered membrane could release chlorogenic acid in response to pH stimulation, (ii) the steady state flux of engineered membrane was maintained higher than the pristine membrane after filtration with contaminated apple juice. Only 4.9% viable bacteria were observed on the membrane surface, (iii) the antibacterial mechanism of engineered membrane was mainly due to the disruption of cellular structural integrity and enhanced permeability of cell membranes, which caused the damage to A. acidoterrestris cell, (iv) after filtration, the Fe 3+ concentration in the permeate solution was almost undetectable. The engineered membrane can simultaneously exclude and inactivate A. acidoterrestris in apple juice, while demonstrating excellent anti-adhesion and anti-biofouling properties. Furthermore, the engineered membrane complies with food safety requirements, which verifies that this metal-organic framework modification method has the potential for practical application in food processing.
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CHEMICAL PHYSICS
·
2024
·
IF 2
Qian Liu,Panpan Xu,Qianqian Zhang,Guangming Han,Ling Li,Limin Zhou
A series of novel MIL-53(Fe)/CoWO 4 composites were synthesized by combining MIL-53(Fe) and CoWO 4 nanoparticles via solvothermal method. The structural characterizations showed that CoWO 4 nanoparticles were uniformly distributed on the surface of hexagonal bipyramid MIL-53(Fe). Combining XPS and Mott-Schottky plots, a Z-scheme heterojunction was formed between MIL-53(Fe) and CoWO 4 , resulting in a significant improvement in the electron-hole pair separation efficiency. UV–vis diffused reflectance spectra indicated that the optical arrange of MIL-53(Fe)/CoWO 4 composites were expanded to visible light. The photocatalytic degradation experiments under visible light irradiation showed that MIL/CWO-60 synergistically with PMS degraded 90.5 % of TC-HCl within 50 min. The XRD spectra of used and unused composites were identical, indicating good stability in four consecutive cycles. Electron paramagnetic resonance (EPR) and free radicals trapping experiment revealed that active species included O 2− , SO 4 − , h + , OH and 1 O 2 , and mechanism of the synergistic degradation of TC-HCl by MIL-53(Fe)/CoWO 4 composites and PMS was proposed.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2025
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IF 2.8
Shangsong Han,Yong Wang,Binhong Gan,Jun Cai,Siyi Jiang,Cuiyu Huang,Shanshan Li
MIL-53(Fe), as a typical metal–organic framework (MOFs) material, has shown broad application prospects in the field of membrane separation technology due to its advantages such as high specific surface area and good chemical stability. However, few studies have specifically applied it to the preparation of oil–water separation membranes. Therefore, this study innovatively proposed a self-assembly strategy. By constructing a MOFs composite coating covering the membrane surface and a comprehensive metal polyphenol network (MPN), this approach was designed to form an efficient, comprehensive oil-rejection system while significantly enhancing pure water flux. Then, through a series of characterizations and performance tests, the results showed that the prepared composite membrane exhibited excellent oil–water separation performance: pure water flux was as high as 3641.21 L m −2 h −1 , and at the same time, the rejection rate of oil-in-water emulsion was stably maintained at more than 99.58%. Therefore, this study not only successfully verified the great potential of MIL-53(Fe)-based composite membranes in the field of efficient oil–water separation, providing a new theoretical basis and feasible technical path for its design, but also further expanded the practical application prospects of MOFs materials in the treatment of oily wastewater, opening up new ideas for the development of the next generation of high-performance separation membranes.
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TALANTA
·
2025
·
IF 6.1
Luyang Zhao,Yang Song,Guoyang Xie,Hengyi Xu
A colorimetric assay based on the Fe/Al bimetallic organic framework NH 2 -MIL-53(Fe, Al) was developed for the sensitive detection of Escherichia coli O157:H7 ( E. coli O157:H7), a critical pathogen threatening food safety. The framework’s high specific surface area facilitated efficient antibody immobilization, whereas the incorporation of Al 3+ enhanced electron transfer between Fe 2+ /Fe 3+ , thereby significantly boosting peroxidase activity. The optimized NH 2 -MIL-53(Fe, Al) exhibited 1.4-fold and 4.9-fold higher relative absorbance than NH 2 -MIL-53(Fe) and NH 2 -MIL-53(Al), respectively. And it demonstrated 40-fold and 2-fold greater affinity for TMB and H 2 O 2 , respectively, compared to the natural enzyme. By integrating a dual-recognition system based on antibody and aptamer, the method enabled rapid detection with a limit of detection of 10 1 CFU/mL in colorimetric mode. Its successful application in complex matrices, including lettuce, juice, pool water, and chocolate milk, had yielded satisfactory recovery and precision, confirming its promising potential for food safety monitoring.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Hui Chen,Wengao Zeng,Yutang Liu,Wanyue Dong,Tao Cai,Lin Tang,Juan Li,Wenlu Li
It is important to find an effective way to enhance the photocatalytic efficiency of metal–organic frameworks. In this work, an organic supermolecule perylene diimide (PDI) semiconductor with a carboxyl terminal was added into the synthesis process of MIL-53(Fe) crystals. The PDI/MIL-53(Fe) (PM) composite photocatalyst was first obtained. The TC-H photodegradation rate of the most efficient 5PM was nearly 94.08% within 30 min, whose apparent reaction rate constant (k) is 4 times that of PDI and 33 times that of MIL-53(Fe), respectively. By investigation and characterization, it has been found that PDI nanofibers were dispersed and fixed in MIL-53(Fe) and bonded to each other by covalent bonds. The radical trap experiments and electron spin resonance analysis illustrated that hydroxyl radical (·OH), superoxide radical (·O2–), and photogenerated holes (h+) were active species. Combined with the band structure of PDI and MIL-53(Fe), it is proposed that the PM photocatalyst was a Z-scheme heterojunction mechanism. Therefore, PM photocatalysts showed excellent charge separation and transfer ability. The performance improvement of 5PM is due to enhanced visible light absorption, efficient charge separation, and excellent redox potential. Five cyclic photocatalytic tests and experiments further demonstrate that the 5PM photocatalyst has a promising future for pollutant removal.
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高影响因子
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