TALANTA
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2014
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IF 3.511
Ning Li,Quanfei Zhu,Yang Yang,Jianlin Huang,Xueping Dang,Huaixia Chen
Metal-organic frameworks (MOFs) have been paid widespread attention in the field of adsorption and separation materials due to its porosity, large specific surface area, unsaturated metal-ligand sites and structural diversity. In this study, the green powder MIL-101 was synthesized and used for the extraction of benzophenone , 2,4-dihydroxybenzophenone and 2-hydroxy-4-methoxy-benzophenone from toner samples for the first time. The synthesized MIL-101 was characterized by X-ray diffraction, scanning electron microscopy, thermogravimetry and nitrogen adsorption porosimetry. The MIL-101 was applied as the dispersive solid phase extraction (DSPE) adsorbent for the extraction and preconcentration of benzophenone, 2,4-dihydroxybenzophenone and 2-hydroxy-4-methoxy-benzophenone from toner samples. The extraction conditions were investigated. Under the optimized conditions, a DSPE-HPLC method for the determination of benzophenone, 2,4-dihydroxybenzophenone and 2-hydroxy-4-methoxy-benzophenone was developed. The method yielded a linear calibration curve in the concentration ranges from 4.0 to 3500 μg L −1 for the three analytes in toner samples with regression coefficients ( r 2 ) of 0.9992, 0.9999 and 0.9990, respectively. Limits of detection were 1.2, 1.2 and 0.9 μg L −1 , respectively. Both the intra-day and inter-day precisions (RSDs) were <10%.
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高影响因子
Journal of Environmental Chemical Engineering
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2014
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IF 0
Tingting Shen,Jinming Luo,Siyu Zhang,Xubiao Luo
Hierarchically mesostructured MIL-101 metal–organic frameworks (MOFs) were synthesized using anhydrous sodium acetate or hydrofluoric acid as a mineralizing agent and cetyltrimethylammonium bromide (CTAB) as a structure-directing agent. These new materials were then used to adsorb and remove the anionic dye methyl orange (MO) and the cationic dye methylene blue (MB) from contaminated water. The adsorption performance was systematically investigated and discussed. Experimental results revealed that the amount of MB adsorbed on MIL-101 that was prepared using sodium acetate is about 3.2 times the amount adsorbed on MIL-101 prepared using hydrofluoric acid, but quantities of adsorbed MO by the two adsorbents were nearly the same. Adsorbents synthesized with higher CTAB content had a higher content of the meso- and macro-scale pores, which favored the MB adsorption but impeded the MO adsorption. Dye adsorption is partially governed by the electrostatic interaction between the dye and the adsorbent, because the mineralizing agent can vary the charge carried by framework in a dye solution. The MB and MO adsorption kinetics followed a pseudo-second-order model, and the equilibrium dye adsorption data provided a good Langmuir model.
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ANALYTICA CHIMICA ACTA
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2017
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IF 4.95
Bin bin Zhang,Yi Shi,Hui Chen,Qing xia Zhu,Feng Lu,Ying wei Li
By coupling surface-enhanced Raman spectroscopy (SERS) with thin-layer chromatography (TLC), a powerful method for detecting complex samples was successfully developed. However, in the TLC-SERS method, metal nanoparticles serving as the SERS-active substrate are likely to disturb the detection of target compounds, particularly in overlapping compounds after TLC development. In addition, the SERS detection of compounds that are invisible under both visible light and UV 254/365 after TLC development is still a significant challenge. In this study, we demonstrated a facile strategy to fabricate a TLC plate with metal-organic framework-modified gold nanoparticles as a separable SERS substrate, on which all separated components, including overlapping and invisible compounds, could be detected by a point-by-point SERS scan along the developing direction. Rhodamine 6G (R6G) was used as a probe to evaluate the performance of the substrate. The results indicated that the substrate provided good sensitivity and reproducibility, and optimal SERS signals could be collected in 5 s. Furthermore, this new substrate exhibited a long shelf life. Thus, our method has great potential for the sensitive and rapid detection of overlapping and invisible compounds in complex samples after TLC development.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Tian Tian,Xuefeng Hu,Yao Huang,Huixian Du,Chao Wang,Mina Yang
The widespread utilization of fossil fuels has resulted in a significant increase in CO 2 emissions, leading to a variety of environmental issues. The photocatalytic conversion of CO 2 into fuel presents an effective solution to both the energy crisis and environmental warming. Therefore, the selection of a suitable catalyst is paramount. However, traditional photocatalysts often encounter challenges such as rapid electron-hole recombination and limited exposure of active sites. To improve these limitations, this study introduces AFM-X, a heterojunction catalyst composed of Au/Fe 3 O 4 /MIL-101(Fe)-X, which facilitates the formation of open metal sites (OMS) that enhance the effective separation of photogenerated carriers. In AFM-X, OMS function as Lewis acid sites, thereby enhancing CO 2 adsorption. The presence of Au nanoparticles (NPs) introduces additional active sites for CO 2 reduction. The synergistic effect between OMS and Au NPs increases the catalyst’s active sites, while the heterojunction construction promotes electron transfer, thereby enhancing CO 2 photocatalytic reduction efficiency. The CO generation rate of AFM-2 reached 98.8 μmol g −1 h −1 , surpassing those of FM, MIL-101(Fe), Fe 3 O 4 , and Au NPs, by 4.1, 6.3, 6.2, and 3.2 times, respectively. Furthermore, AFM-2 maintains stable performance over a 40 h cycle test. In-situ DRIFTS spectroscopy reveals that CO 2 reduction occurs through two parallel pathways. This study offers new insights into the design of composite photocatalytic materials, highlighting the effectiveness of OMS Lewis acid sites in significantly enhancing the photocatalytic reduction of CO 2 .
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Chunlai Liu,Na Wang,Zelin Meng,Mingyang Song,Heming Zhao,Jianglei Hu,Fengwei Shi
The Knoevenagel reaction is one of the most significant reactions in the industrial synthesis of organic materials, pharmaceuticals, and biological compounds. In this study, 2-cyanoethyltriethoxysilane (CTES) was employed as a functionalizing agent to prepare carboxyl-functionalized silica (SBA-16-Cx) using a one-pot method. Subsequently, carboxyl groups served as anchoring points for Cr³⁺, and MOFs-modified SBA-16 (SBA-16-Cx@MIL) was obtained by in situ synthesis. The resulting materials were characterized using FT-IR, XPS, XRD, N 2 adsorption-desorption analysis, SEM, TEM, 13 C MAS NMR, and TG, which confirmed the successful synthesis of MIL-101 on the support. Meanwhile, the pore size of the composite was reduced from 5.1 nm (SBA-16) to 0.6 nm (SBA-16-C1.0@MIL). The condensation reaction of benzaldehyde with malononitrile was selected as a model reaction. The effects of various factors, including solvents, reactants molar ratios, temperature, catalyst dosage, and reaction time, on the reaction were studied. Under optimized conditions, the conversion rate of benzaldehyde reached 100 % and the catalyst demonstrated excellent stability for repeated use. The reaction follows second-order kinetics (R 2 >0.99), and the activation energy of the reaction was 17.18 kJ/mol. Finally, the mechanism of the catalytic process was proposed. This work provides a green catalytic route for the synthesis of α,β-unsaturated carbonyl compounds.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Shu-Huan Chen,Huma Javeria,Xu-Hui Sun,Zhen-Xia Du
With the proliferation of vehicles in households, people are spending more and more time in their cars, so it is important to ensure the air quality and safety of the car. In this research, environmentally friendly, green PET@PDA@MIL-101(Fe) (PPM) was prepared by in-situ solvothermal growth and acid etching methods, which was categorized by SEM, FTIR, XRD, XPS, and BET. PPM was used to adsorb benzene, toluene, and m-xylene at low concentrations. The maximum amount of adsorption of PET@PDA@MIL-101(Fe) (PPM) for benzene, toluene, and m-xylene was 68.72 mg/g, 91.63 mg/g, and 78.47 mg/g respectively. The adsorption process of PPM is well fitted by the pseudo-first-order kinetic model and Langmuir isothermal adsorption model. Furthermore, PPM exhibited excellent toluene removal performance in simulated vehicles and excellent cycling capability in adsorption-desorption experiments. As a result, PPM can be used to treat and manage toluene volatile organic compounds (VOCs) at low concentrations.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yiting Lv,Jinjuan Xue,Zhaoxia Chen,Jianan Qu,Kaiwen Huang,Mingxin Wang,Wei Sun
Photocatalytic production of H 2 O 2 has garnered significant attention, but the use of sacrificial reagents in H 2 O 2 photosynthesis and the subsequent limited H 2 O 2 activation efficiency would impede its practical application in water decontamination. In this work, hydrothermal carbonaceous carbon/NH 2 -MIL-101(Fe) (abbreviated as HTC-cf/NMIL-101(Fe)) heterojunction was fabricated through a solvothermal strategy, and serving as a self-sufficient photo-Fenton-like catalyst to in-situ generate and activate H 2 O 2 . Hydrothermal carbonaceous carbon derived from cost-effective waste coffee grounds, serving as a green and sustainable photocatalyst, demonstrated high H 2 O 2 production rate of 612 μmol/g/h without the need for sacrificial reagents or aeration assistance. Moreover, the excellent self-sufficient photo-Fenton activity for HTC-cf/NMIL-101(Fe) can be obtained, which ascribed to the synergistic effect of self-generated H 2 O 2 production as well as the in-situ catalytic H 2 O 2 decomposition of • OH by Fe species in NMIL-101(Fe) and photogenerated electrons. The optimized HTC-cf/NMIL-101(Fe) photocatalyst showed simultaneous improvements in both H 2 O 2 production and activation capabilities. Impressively, the effective circulation of Fe 3+ /Fe 2+ in NMIL-101(Fe), aided by photogenerated electrons, results in a 5-fold increase toward H 2 O 2 decomposition rate constant (K d ) compared to HTC-cf alone under light irradiation in open-air conditions. The enhanced charge separation and appropriate band structure of HTC-cf/NMIL-101(Fe) photocatalyst assured the high selectivity of two-electron O 2 -reduction to H 2 O 2 . HTC-cf/NMIL-101(Fe) displayed excellent photocatalytic sterilization efficiency against E. coli and S. aureus under visible light, and its sterilization application in actual water was also demonstrated. Notably, the adaptability of this system to ambient conditions, including open-air atmosphere, non-sacrificial reagents, and low leaching of Fe ions, highlights the promising practical utility of the HTC-cf/NMIL-101(Fe) photocatalyst.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yingjie Guo,Jiayi Yan,Zan Chen,Cuijia Duan,Claudia Li,Yinhui Li,Sibudjing Kawi
The tendency of small-sized covalent organic framework (COF) nanoparticles to easily agglomerate, and the propensity of photo-generated carriers in α -Fe 2 O 3 to recombine pose challenges in the efficient removal of tetracycline (TC) through adsorption-photocatalysis synergy. This study addresses these challenges by introducing MIL-101, known for its excellent chemical stability and large specific surface area. The amino functional group facilitates the in-situ growth of acyl chloride-covalent organic framework (AC-COF) on the surface of MIL-101, resulting in the fabrication of AC-COF@MIL-101 with a core-shell structure. Loading α -Fe 2 O 3 through structural regulation leads to the preparation of the final α -Fe 2 O 3 /AC-COF@MIL-101 ternary nanocomposite. In α -Fe 2 O 3 /AC-COF@MIL-101 composites, the high surface energy of AC-COF is mitigated by the strong chemical energy of N C-N, reducing AC-COF aggregation and decreasing the recombination rate of photogenerated carriers in α -Fe 2 O 3 . The heterojunction structure between AC-COF@MIL-101 and α -Fe 2 O 3 enhances the degradation of TC, attributed to the synergistic effect of adsorption and photocatalysis. Experimental results demonstrate that α -Fe 2 O 3 /AC-COF@MIL-101 has a maximum adsorption capacity of 135.14 mg/g, achieving a 100% TC removal rate within 30 min. Compared to AC-COF, MIL-101, and α -Fe 2 O 3 , α -Fe 2 O 3 /AC-COF@MIL-101 exhibits higher adsorption capacity and photocatalytic activity. Specifically, its adsorption capacity is 2.1 times that of AC-COF, 1.8 times that of MIL-101, and 10.6 times that of α -Fe 2 O 3 . Additionally, its degradation ability is 8.6 times that of α -Fe 2 O 3 . The adsorption of TC by α -Fe 2 O 3 /AC-COF@MIL-101 occurs through monolayer chemical adsorption, and the process is exothermic. The main active species involved in the photocatalytic degradation process are h + and ·OH. This study introduces a new ternary composite multifunctional material with high adsorption and photocatalytic performance for TC, offering a potential strategy for enhancing the synergistically adsorption-photocatalytic effect in ternary composite systems.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zhiqiang Guo,Xinmiao Wu,Juanjuan Meng,Xinxin Li,Yuan Li,Liangliang Hu
MIL-101(Fe) has received more and more attention in wastewater treatment, and how to further improve its stability and sorption capacity has become a research focus. In this study, metal Mg was used to dope MIL-101(Fe) to construct Mg@MIL-101(Fe) with bimetallic sites, which was then mixed with NH 2 -MIL-125(Ti) to successfully fabricate Mg@MIL-101(Fe)/NH 2 -MIL-125(Ti) (MOM) bis-MIL composites. MOM not only contains a large number of sorption sites but also exhibits excellent stability and reusability, realizing efficient sorption of Pb(II) from aqueous solution. In addition, the sorption performance and mechanism of Pb(II) on MOM were investigated by the characterizations of SEM, BET, TG, XRD, FTIR and XPS, as well as the kinetic and thermodynamic analyses. The sorption of Pb(II) on MOM is in accordance with the Langmuir isothermal model and pseudo-second-order kinetic model. The maximum sorption capacity of Pb(II) on MOM derived from the Langmuir model fitting is 320.941 mg·g −1 . The sorption of Pb(II) on MOM is strongly affected by pH, but not by ionic strength, which indicates that MOM has good resistance to salt interferences. The strong complexation of carboxyl, hydroxyl and amino functional groups with Pb(II) is the main sorption mechanism of Pb(II) on MOM, and electrostatic interaction and ion exchange also contribute to the sorption. In conclusion, MOM has strong practical application prospects in the treatment of Pb(II)-containing wastewater.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Zhengtao Zhu,Xi Deng,Yongqiang Ye,Na He,Bihe Yuan,Fei Xiao,Kaiyuan Li
To address the challenge of balancing fire safety and mechanical properties in thermoplastic polyurethanes (TPU), this study developed a CP@MIL-101 hybrid by confining liquid cyclic phosphates within the pore structure of MIL-101 using a hierarchical design strategy. The results demonstrated that the introduction of CP@MIL-101 slightly improved the thermal stability of TPU. Notably, the residual char yield increased significantly from 0.1 % to 9.3 % with only 0.5 % loading. With just 2 wt% loading of CP@MIL-101, the TPU composite achieved a UL-94 V-0 rating (3 mm) and exhibited a 20.4 % increase in the limiting oxygen index (LOI), reaching 26.0 %. Furthermore, significant reductions in peak heat release rate, total heat release, and fire growth rate index were observed, indicating enhanced fire safety of the TPU composites. Characterization analyses suggested that the improved fire retardancy resulted from the synergistic effects of MIL-101 and cyclic phosphates in both the condensed and gas phases, through the formation of a protective char layer and free radical quenching. Additionally, incorporating 2 wt% CP@MIL-101 endowed the TPU matrix with exceptional ultraviolet shielding properties due to unique electron transitions absorption. Simultaneously, the tensile strength of the TPU increased by 15.85 % compared to neat TPU, demonstrating mechanical reinforcement. This work establishes a strategic approach for developing multifunctional flame retardants and fire-safe TPU composites, paving the way for their application in high fire-safety environments.
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LANGMUIR
·
2025
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IF 3.9
Changhua Li,Wei Liu,Yuquan Jing,Hao Yang,Qiuping Tang,Yongxu Cui,Chao Zhang,Wei Ren,Jing Zhang,Yi He
Metal–organic framework materials with large specific surface areas are ideal choices for storing corrosion inhibitors in organic coatings. Existing reports focus on materials such as ZIF-8 and ZIF-67, which release corrosion inhibitors by disintegrating themselves upon external stimuli. This release mechanism may lead to the formation of holes within the coating, providing channels for penetration into corrosive media. In this study, NH2-MIL 101 (Cr), which is stable under acidic/alkaline conditions, was grown on Ti3C2Tx surface via a hydrothermal method. Its porous structure was utilized to load environmentally friendly MoO42– corrosion inhibitors, and a stimulus-responsive TEOS shell was wrapped as a valve to control the release of the corrosion inhibitors. The synthesis of the Ti3C2Tx-MIL 101-MoO42–-TEOS (TMIT) composite material was verified by FT-IR spectroscopy and XPS, respectively. The TMIT-epoxy (TMITP) composite coating was prepared through a solid–liquid mixing method. The surface-active groups of NH2-MIL 101 (Cr) (−NH2) enhanced the interfacial strength with the resin and the crosslinking density, significantly increasing the tensile strength and adhesion strength of the composite coating. Due to the improved interfacial strength, the low-frequency impedance value remained at 4.14 × 108 Ω cm2 after 6 cycles of accelerated cyclic electrochemical tests (−4.0 V, 30 min), which greatly shortening the evaluation period of the coating performance. Additionally, the stimulus-responsive release mechanism of the TMIT filler endowed the coating with self-healing effects, achieving corrosion inhibition in damaged areas. Notably, the acid/alkali stability of NH2-MIL 101 (Cr) ensured that few holes would form within the coating after the release of corrosion inhibitors, preventing the penetration of corrosive media. This study utilized the pores of NH2-MIL 101 (Cr) to load corrosion inhibitors and prepare self-healing composite coatings, achieving intelligent release and enhancing the corrosion resistance of coatings, thus broadening the application strategy of MOF materials in corrosion protection coatings.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2020
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IF 7.1
Jingjing Guo,Shu Wu,Yan Wang,Min Zhao
A label-free and high sensitive fluorescence biosensor for the detection of choline and acetylcholine (ACh) was developed based on the MIL-101(Fe) nanozyme with dual functions of mimetic peroxidase and fluorescent emission. This fluorescence sensing strategy involves the reaction of acetylcholinesterase (AChE) catalyzing the hydrolysis of ACh into choline that is in turn oxidized by choline oxidase (ChOx) to generate H 2 O 2 , and the as-produced H 2 O 2 is decomposed into highly reactive hydroxyl radicals under the catalysis of MIL-101(Fe) nanozyme, thereby the non-fluorescent organic ligand terephthalic acid of MIL-101(Fe) is oxidized by hydroxyl radicals to form a highly fluorescent 2-hydroxy terephthalic acid. By virtue of this finding, the label-free detection of choline and ACh via multienzyme cascade reaction was realized with low detection limits of 20.0 nM and 8.9 nM, respectively. Moreover, the practicality of the developed bifunctional MIL-101(Fe)-based sensing strategy was successfully validated through the detection of choline in milk and ACh in human plasma. This proposed assay not only exhibited high sensitivity and selectivity towards choline and ACh, but also simplified the sensing systems, reduced the detection cost, and avoided the potential risks caused by the fluorescent reagents, which opened a green avenue for the analysis of complex biological samples.
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