JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Hang Liu,Hua Yin,Xiaolong Yu,Minghan Zhu,Zhi Dang
In this work, the amino-functionalized metal-organic frameworks (MIL-88B-NH 2 ) was synthesized, characterized and used as heterogeneous photo-Fenton catalyst for tris-(2-chloroisopropyl) phosphate (TCPP) degradation. The photo-Fenton activity of MIL-88B-NH 2 was investigated on the basis of influence factors, such as initial pH and TCPP concentration, and coexisting impurities. The results revealed that MIL-88B-NH 2 +H 2 O 2 +Vis system exhibited a satisfactory degradation efficiency of TCPP (almost 100%) within 60 min accompanied by a good reusability. Noticeably, the degradation kinetics constant of TCPP by MIL-88B-NH 2 +H 2 O 2 +Vis system was 0.086 min −1 , which was visibly higher than that of MIL-88B+H 2 O 2 +Vis system (0.021 min −1 ) since the addition of amino-functionalized organic linker inhibiting the recombination rate of the photo-generated electron-hole pairs and improving the visible light response. Combined with the characterization, the conversion of Fe III to Fe II could be accelerated by the photo-generated electron from the excitation of Fe-O clusters and NH 2 functionalities, which strengthened the decomposition of H 2 O 2 and formed plenty •OH. Simultaneously, six steady products were validated and potential degradation pathways of TCPP were proposed. It was anticipated that MIL-88B-NH 2 could be considered as a desirable and alternative candidate in the application of heterogeneous photo-Fenton reaction to control the environmental risks caused by organophosphate flame retardants (OPFRs).
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JOURNAL OF CHROMATOGRAPHY A
·
2026
·
IF 4
Shijie Xing,Zhikun Li,Jiaxiang Liu,Wei Zhang,Fuqiang Sun,Shu-Xuan Liang
To address the ongoing issue of quinolones (QNs) residues in aquatic products, accurate and sensitive detection of trace QNs has always been necessary and urgent. In this work, a composite material of NH 2 −MIL-125(Ti)@TpBD(SO 3 H) 2 consisting of metal organic frameworks and based on bisulfonic acid-based covalent organic frameworks was synthesized and applied as a dispersive solid-phase extraction (dSPE) adsorbent. Combining with liquid chromatography-tandem mass spectrometry, a simple and effective method for simultaneous detection of 18 QNs in aquatic products was established. Meanwhile, the selective adsorption mechanism was thoroughly investigated through material characterization combined with density functional theory calculations. The results showed that the method had a good linear relationship ( r ≥ 0.9981), low limits of detection of 0.0019–0.0641 μg kg⁻¹, along with high recovery rates in the range of 80.6–113.2 %, and good precision with relative standard deviations less than 8.8 %. The selective adsorption mechanism revealed the synergistic adsorption mechanism of electrostatic interactions, hydrogen bonding, and π-π interactions. The material had good reusability and excellent stability. In summary, the dSPE method based on NH 2 −MIL-125(Ti)@TpBD(SO 3 H) 2 composites provided a practical sample pretreatment solution for the determination of trace QNs in complex matrixes.
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ELECTROPHORESIS
·
2016
·Vol. 37
·期 19
·2478-2486
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IF 2.482
Yue Liu,Jia Hu,Yan Li,Xiao-Shuang Li,Zhong-Liang Wang
A novel method with high sensitivity for the rapid determination of chrysin, apigenin and luteolin in environment water samples was developed by double-pumps controlled on-line solid-phase extraction (SPE) coupled with high-performance liquid chromatography (HPLC). In the developed technique, metal organic framework MIL-101 was synthesized and applied as a sorbent for SPE. The as-synthesized MIL-101 was characterized by scanning electron microscope, X-ray diffraction spectrometry, thermal gravimetric analysis and micropore physisorption analysis. The MIL-101 behaved as a fast kinetics in the adsorption of chrysin, apigenin and luteolin. On-line SPE of chrysin, apigenin and luteolin was processed by loading a sample solution at a flow rate of 1.0 mL/min for 10 min. The extracted analytes were subsequently eluted into a ZORBAX Bonus-RP analytical column (25 cm long × 4.6 mm i.d.) for HPLC separation under isocratic condition with a mobile phase (MeOH: ACN: 0.02 M H 3 PO 4 = 35:35:30) at a flow rate of 1.0 mL/min. Experimental conditions, including ionic strength, sample pH, sample loading rates, sample loading time and desorption analytes time, were further optimized to obtain efficient preconcentration and high-precision determination of the analytes mentioned above. The method achieved the merits of simplicity, rapidity, sensitivity, wide linear range and high sample throughput. The possible mechanism for the adsorption of flavonoids on MIL-101 was proposed. The developed method has been applied to determine trace chrysin, apigenin and luteolin in a variety of environmental water samples.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Qing Jin,Kai Ma,Guilong Gao,Xinyu Zhou,Lijie Xu,Ying Zhang,Jiangtao Shi,Lu Gan
In this study, a series of carbon nanofiber (CNF) based one-dimensional catalysts were prepared by pyrolyzing MIL-88B(Fe) anchored PAN/lignin electrospun nanofibers, which were then employed to activate peroxymonosulfate (PMS) for bisphenol A (BPA) degradation. The results indicated that adjusting the lignin content in nanofiber precursor could engineer the crystalline phase of iron compounds in the catalysts, as well as their catalytic activity and stability. Specifically, the precursor with lower lignin content was converted into Fe 3 O 4 loaded CNF (P2L1-Fe-C), whereas Fe 3 C loaded CNF was obtained (P1L1-Fe-C) by increasing lignin content to 50 wt% in the nanofiber precursor. Having multiple Fe valence states within Fe 3 C which facilitated internal electron transfer, P1L1-Fe-C exhibited high catalytic activity with high stability and low iron ion leaching when activating PMS for BPA degradation. P1L1-Fe-C/PMS system could produce more kinds of active species including hydroxyl radical (•OH) and multiple non-radical species like singlet oxygen ( 1 O 2 ), high-valent iron-oxo species, and electron transfer process. Comparatively, P2L1-Fe-C/PMS system was only able to produce •OH and 1 O 2 . The existence of more BPA degradation pathways resulted in enhanced resistance of P1L1-Fe-C/PMS system towards various environmental interferences. This study inspires a new thinking of developing iron based Fenton-like catalyst with tunable crystalline phases through precursor recipe regulation, achieving both high activity and stability. Download: Download high-res image (225KB) Download: Download full-size image
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TALANTA
·
2016
·
IF 4.035
Xiuna Jia,Pan Zhao,Xiu Ye,Lianjun Zhang,Ting Wang,Qinyu Chen,Xiaohong Hou
As a novel material, metal-organic framework/graphite oxide (MIL-101(Cr)@GO) has great potential for the pretreatment of trace analytes. In the present study, MIL-101(Cr)@GO was synthesized using a solvothermal synthesis method at the nanoscale and was applied as sorbent in the dispersive micro-solid phase extraction (DMSPE) for the enrichment of the trace sulfonamides (SAs) from milk samples for the first time. Several experimental parameters including kinds of sorbents, the effect of pH, the amount of MIL-101(Cr)@GO, ionic strength , adsorption time, desorption solvent and desorption time were investigated. Under the optimal conditions, the linear ranges were from 0.1 to 10 μg/L, 0.2–20 μg/L or 0.5–50 μg/L for the analytes with regression coefficients ( r ) from 0.9942 to 0.9999. The limits of detection were between 0.012 and 0.145 μg/L. The recoveries ranged from 79.83% to 103.8% with relative standard deviations (RSDs)<10% ( n =3). MIL-101(Cr)@GO exhibited remarkable advantages compared to MIL-101(Cr), MIL-100(Fe), activated carbon and other sorbent materials used in pretreatment methods. A simple, rapid, sensitive, inexpensive and less solvent consuming method of DMSPE-ultra-high performance liquid chromatography-tandem mass spectrometry (DMSPE-UHPLC-MS/MS) was successfully applied to the pre-concentration and determination of twelve SAs in milk samples.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Junxue Liu,Yufei Wang,Mingqin He,Xiaohong Chen,Chenyu Zhou,Jiyang Li
Determination of glucose and maltose is crucial for food production and human health. Herein, a novel Au/CD@MIL-53(Fe)-NH 2 self-cascade nanozyme was constructed via host–guest assembly with “three-in-one” features, including blue fluorescence, H 2 O 2 production as an oxidase mimic, and •OH generation as a peroxidase mimic. Theoretical and experimental results proved that the incorporation of carbon dots renders the composite with high peroxidase-like activity and extremely high affinity for H 2 O 2 (K m : 0.011 mM), 336 times higher than that of the natural enzyme. The self-cascade catalytic process could oxidize colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue ox-TMB, which further quenched the fluorescence and produced a photothermal effect. Consequently, colorimetric/fluorescence/photothermal-based multimodal detection of glucose and maltose was first achieved, obtaining low detection limits of 12/7.5/1.1 and 18/11.3/1.4 μM, respectively. This study offers a promising strategy for designing efficient nanozyme-based cascade systems that help enhance food quality determination.
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Ying Wang,Tengfei He,Jingguo Cao,Ke Li,Chengqian Wang,Qun Liu,Yu Zhang
This study demonstrates a sustainable strategy for synthesizing MIL-53(Al) and ZSM-5 zeolite through dual-waste synergy using coal fly ash (CFA) and waste polyethylene terephthalate (PET). A sequential alkaline fusion-acid leaching protocol selectively fractionated CFA into aluminum-rich solutions and silica residues, while alkaline hydrolysis of PET liberated terephthalic acid (PTA) as organic ligands. The Al 3+ -PTA coordination under solvothermal conditions produced MIL-53(Al)(CFA-PET) exhibiting well-defined 1D rhombic channels with a high BET surface area (1303 m 2 ·g −1 ), whereas hydrothermal crystallization of silica residues yielded ZSM-5(CFA), which formed spherical aggregates composed of 100 nm nanosheets with 89.9 % yield and a surface area of 311 m 2 ·g −1 . Structural advantages were evidenced by exceptional adsorption performance: MIL-53(Al)(CFA-PET) achieved 96.24 % methylene blue removal at pH 7 (250 mg·L −1 ), outperforming rhodamine B (30.8 %) and methyl orange (66.4 %), as well as reagent-synthesized MIL-53(Al) Che (91.99 %). Both materials demonstrated exceptional CO 2 capture capacities (4.23 mmol·g −1 for MIL-53(Al)(CFA-PET) vs. 2.37 mmol·g −1 for ZSM-5(CFA) at 273 K/1 bar), attributable to MIL-53′s flexible framework enabling dynamic pore adjustment and ZSM-5′s rigid microporous channels favoring molecular sieving. This work establishes a closed-loop strategy for converting industrial and plastic wastes into functionally differentiated porous materials through element-targeted process design.
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ANALYST
·
2015
·Vol. 140
·期 15
·5308-5316
·
IF 4.107
Ting Wang,Jian Wang,Conglu Zhang,Zhao Yang,Xinpeng Dai,Maosheng Cheng,Xiaohong Hou
An attractive metal–organic framework (MOF) MIL-101(Cr) material was synthesized at the nanoscale and applied as a sorbent in the porous membrane-protected micro-solid-phase extraction (μ-SPE) device for the pre-concentration of phthalate esters (PAEs) in drinking water samples for the first time. Parameters influencing the extraction efficiency, such as the selection of sorbent materials, pH adjustment, the effect of salt, magnetic-stirring extraction time, the desorption solvent and the desorption time, were investigated. Under the optimum conditions, the limits of detection from gas chromatography-mass spectrometric analysis for PAEs varied from 0.004 to 0.02 μg L−1. The linear ranges were from 0.1 to 50 μg L−1 or from 0.2 to 50 μg L−1 for the analytes with the relative standard deviations fluctuating from 0.8 to 10.9% (n = 5). The enrichment factors (EFs) for the target PAEs were varied from 143 to 187. MIL-101(Cr) exhibited remarkable advantages compared to activated carbon and MIL-100(Fe). On the other hand, the computational method was first used to predict the adsorption of MIL-101(Cr) towards PAEs. The molecular interactions and the free binding energies between MIL-101(Cr) and PAEs were observed and calculated in terms of the molecular modeling method. MIL-101(Cr) showed high potential in the analysis of PAEs at trace levels in drinking water. The computational result was consistent with the detected enrichment factors. The computational modeling accurately predicted the extraction efficiency of MOF-based material towards the target analytes. Therefore, the combination of experimental and computational study provided a new strategy on the trace contaminant analysis.
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MICROCHIMICA ACTA
·
2018
·Vol. 186
·期 1
·1-10
·
IF 5.705
Zhang Li,Li Shaobin,Xin Jianjiao,Ma Huiyuan,Pang Haijun,Tan Lichao,Wang Xinming
A Cr-based metal-organic framework MIL-101(Cr) was used to load platinum nanoparticles (PtNPs) that were placed on a glassy carbon electrode (GCE). The modified GCE was used as a non-enzymatic xanthine sensor. Compared to bare GCE, it requires a strongly decreased working potential and an increased signal current for xanthine oxidation. This is due to the crystalline ordered structure and large specific surface of the MIL-101(Cr), and to the high conductivity of the Pt NPs. Differential pulse voltammetry (DPV) shows the sensor to have a wide linear range (0.5 – 162 μM), a low detection limit (0.42 μM), and high selectivity. It was applied to the simultaneous determination of dopamine, uric acid, xanthine and hypoxanthine at working potentials of 0.13, 0.28, 0.68 and 1.05 V, respectively (vs. Ag/AgCl) and to quantify xanthine in spiked serum samples.
This is the first report of non-enzymatic xanthine electrochemical sensor based on metal-organic framework loaded with nanoparticles.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2016
·Vol. 408
·期 29
·8515-8528
·
IF 3.125
Lu Nan,Wang Ting,Zhao Pan,Zhang Lianjun,Lun Xiaowen,Zhang Xueli,Hou Xiaohong
In the presented work, metal-organic framework (MOF) material MIL-101(Cr) (MIL, Matérial Institute Lavoisier) was used as a sorbent for vortex assisted dispersive micro-solid-phase extraction (VA-D-μ-SPE) of trace amount of metronidazole (MNZ), ronidazole (RNZ), secnidazole (SNZ), dimetridazole (DMZ), tinidazole (TNZ), and ornidazole (ONZ) in different environmental water samples. Ultra-high-performance liquid chromatography coupled with tandem mass spectrometry (UPLC-MS/MS) was used to quantify the target analytes. The extraction conditions, including type of sorbents, amount of MIL-101(Cr), solution pH, extraction method, extraction time, effect of salt, and elution conditions were investigated. Upon the optimal conditions, the developed method showed an excellent extraction performance with the average recovery ranging from 75.2 to 98.8 %. Good sensitivity levels were achieved with the detection limits of 0.03∼0.06 μg/L and the quantitation limits of 0.09∼0.20 μg/L. The linear ranges were varied from 0.1 to 20 for SNZ and ONZ and from 0.2 to 40 μg/L for MNZ, RNZ, DMZ, and TNZ ( r
2 > 0.992), and repeatability of the method was satisfactory with the relative standard deviations (RSD) <8 %. Ultimately, the applicability of the method was successfully confirmed by the extraction and determination of 5-nitroimidazoles (5-NDZs) in 12 real water samples, showing the positive findings of MNZ and TNZ ranging from 0.3 to 1.0 μg/L. Furthermore, molecular docking was applied to explain the molecular interactions and free binding energies between MIL-101(Cr) and 5-NDZs, providing a deep insight into the adsorption mechanism. The proposed method exhibited the advantages of simplicity, rapidly, less solvent consumption, ease of operation, higher sensitivity, and lower matrix effect.
Schematic diagram of the extraction process and molecular docking investigation
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TALANTA
·
2017
·
IF 4.162
Guihua Gao,Sijia Li,Shuo Li,Yudan Wang,Pan Zhao,Xiangyu Zhang,Xiaohong Hou
In this work, computational and experimental methods were used to study the adsorption of estrogens and glucocorticoids on metal–organic frameworks (MOFs). Computer-aided molecular simulation was applied to predict the adsorption of eight analytes on four MOFs (MIL-101(Cr), MIL-100(Fe), MIL-53(Al), and UiO-66(Zr)) by examining molecular interactions and calculating free binding energies. Subsequently, the four water-stable MOFs were synthesized and evaluated as adsorbents for the target hormones in aqueous solution. As the MOF exhibiting the highest adsorption capacity in both computations and experiments, MIL-53(Al) was chosen as a sorbent to develop a dispersive micro-solid-phase extraction procedure coupled to ultra-performance liquid chromatography tandem mass spectrometry for simultaneous determination of the target analytes in water and human urine samples. Experimental parameters affecting the extraction recoveries, including pH, ionic strength , MIL-53(Al) amount, extraction time, desorption time, and desorption solvent, were optimized. The optimized method provided a linear range of 0.005025–368.6 μg/L with good correlation coefficients (0.9982 ≤ r 2 ≤ 0.9992), and limits of detection (S/N = 3) and quantification (S/N = 10) of 0.0015–1.0 μg/L and 0.005–1.8 μg/L, respectively. The analyte recoveries were in the range of 80.6–98.4% in water samples and 88.4–93.2% in urine samples. Furthermore, MIL-53(Al) showed good stability over 10 extraction cycles (RSD < 10.0%). Good agreement between experimental measurements and computational results showed the potential of this approach for elucidating adsorption mechanisms and predicating extraction efficiencies for MOFs and targets, providing new directions for the development and utilization of MOFs.
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
·
2019
·
IF 2.983
Qianqian Cai,Tianyu Zhao,Lianjun Zhang,Pan Zhao,Yajie Zhu,Haiyan Xu,Xiaohong Hou
Dispersive micro-solid-phase extraction (DMSPE) combined with dispersive liquid–liquid microextraction based on the solidification of a floating organic droplet (DLLME-SFO) was successfully developed for extraction and depuration of pantoprazole in rat plasma. The remarkable metal organic framework (MOF), MIL-101(Cr) was used as DMSPE adsorbent. The detection of pantoprazole was performed by convenient HPLC-UV. In the extraction of pantoprazole from plasma samples, small molecule compounds, including the target and abundant impurities, were easily admitted into the porous structure of MIL-101 (Cr) material in DMSPE; while, macromolecular compounds were handily excluded from the adsorbent. Next, the depuration process was achieved by removal of small polar impurities in DLLME-SFO. Influential factors were systematically optimized for ideal enrichment and depuration efficiency. Under the optimal conditions, a satisfactory linearity range from the lower limit of quantification (LLOQ, 100 ng/L) to 10 000 ng/L with the correlation coefficients ( r ) of 0.9934 was obtained. The LLOQ was 100 ng/mL and the relative recoveries were ≧ 73.2 ± 4.8%. The approving reproducibility, acceptable accuracy, and stability were all within the acceptance limits. This proposed method presented the advantages of environment-friendly, low-cost, recyclable, low impurity, and preferable applicability. It could offer a new idea for the pretreatment and pharmacokinetic study of pantoprazole in rat plasma.
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