ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Chunyan Hu,Jinke He,Jianjun Liang,Tao Lin,Qiuliang Liu
A novel photo-Fenton catalyst α-Fe 2 O 3 @g-C 3 N 4 @NH 2 -MIL-101(Fe) (FGN) with dual Z-scheme heterojunction was successfully prepared by hydrothermal method to degrade tetracycline (TC). The preparation conditions were optimized by orthogonal test, and the successful synthesis was confirmed by characterization analyses. The prepared FGN showed better light absorption performance, higher photoelectrons-holes separation efficiency, lower photoelectrons transfer resistance, and higher specific surface area and pore capacity compared with α-Fe 2 O 3 @g-C 3 N 4 and α-Fe 2 O 3 . The effects of experimental conditions on the catalytic degradation of TC were investigated. The degradation rate of 10 mg/L TC could reach 98.33% within 2 h when the dosage of FGN was 200 mg/L, and the degradation rate could remain 92.27% after 5 times of reuse. Furthermore, the XRD spectra and XPS spectra of FGN before and after reuse were compared to explore the structural stability and catalytic active sites of FGN, respectively. According to the identification of oxidation intermediates, three degradation pathways of TC were proposed. Through H 2 O 2 consumption experiment, radical-scavenging experiments, EPR results, the mechanism of the dual Z-scheme heterojunction was proved. The improved performance of FGN was attributed to the dual Z-Scheme heterojunction effectively promoting the separation of photogenerated electrons from the holes and accelerating the electrons transfer , and the increase of the specific surface area.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2023
·
IF 3.3
Rui Zhao,Cheng Cheng,Xiurong Wu,Xueyan Bai,Fenghuan Wang
Due to the excellent pore structure , MOFs as the stationary phase was playing an important part in chromatography . In this work, the shell-core MIL-101(Al)@SiO 2 composites post-synthetic modified by ligands with different polarities were fabricated for separation of estrogens. The structure and morphology of these materials were characterized by X-ray diffraction (XRD), Fourier transform infrared spectrum (FTIR), scanning electron microscope (SEM) and Brunauer-Emmett-Teller (BET). In order to investigate the influence of the ligand polarity on chromatographic separation performance of estrogens, alkyl molecules with different chain length were introduced as the ligands. With the hydrophobicity and chain length of the ligands increasing, the resolutions of the MIL-101(Al)@SiO 2 columns for the separation of estrogens exhibited the tendency of a parabola. Best result was achieved on the C4-MIL-101(Al)@SiO 2 column. On that basis, the possible retention mechanism on C4-MIL-101(Al)@SiO 2 column was elucidated by studying the mobile phase effect on separation behavior.
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Energy & Environmental Materials
·
2021
·Vol. 6
·期 1
·e12254
·
IF 15.122
Ailin Li,Jian Xiong,Ye Liu,Liming Wang,Xiaohong Qin,Jianyong Yu
MIL-101(Cr) is a promising moisture absorbent for solar-driven water harvesting from moisture to tackle the worldwide water shortage issue. However, the MIL-101(Cr) powder suffers from a long ab/desorption cycle due to the crystal aggregation caused by its inherent powder properties. Here, we demonstrate a MIL-101(Cr) nanofibrous composite membrane with a nanofibrous matrix where MIL-101(Cr) is monodisperse in the 3D porous nanofibrous matrix through a simple spray-electrospinning strategy. The continuous porous nanofibrous matrix not only offers sufficient sites for MIL-101(Cr) loading but also provides rapid moisture transport channels, resulting in a super-rapid ab/desorption duration of 50 min (including an absorption process for 40 min and a desorption process for 10 min) and multicycle daily water production of 15.9 L kg −1 d −1 . Besides, the MIL-101(Cr) nanofibrous composite membrane establishes a high solar absorption of 92.8%, and excellent photothermal conversion with the surface temperature of 70.7 °C under one-sun irradiation. In addition, the MIL-101(Cr) nanofibrous composite membrane shows excellent potential for practical application due to its flexibility, portability, and use stability. This work provides a new perspective of shortening MOF ab/desorption duration by introducing a porous nanofibrous matrix to improve the specific water production for the solar-driven ab/desorption water harvesting technique.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Chan Zhou,Lei Zhu,Lin Deng,Haojie Zhang,Hanxuan Zeng,Zhou Shi
For improving the catalytic activity and recyclability of CuS in Fenton-like reaction processes, novel sulfur vacancies-enriched CuS@MIL-101(Fe) was constructed, characterized, and examined as heterogeneous catalysts for activating peroxymonosulfate (PMS) to degrade coumarin (COU). Thanks to the redox pairs of Fe 3+ /Fe 2+ , Cu + /Cu 2+ , S 2− /S 2 2− /S 0 /sulfate species, copper-iron synergistic effect and sulfur vacancies, the CuS@MIL-101(Fe) realized a complete removal of COU (30 μM) in 10 min with reaction rate constant of 0.577 min −1 , which was 11.1 and 17.0 times of CuS and MIL-101(Fe), respectively. The effect of various experimental conditions (i.e., initial pH, CuS@MIL-101(Fe) dosage, PMS concentration, and background anions) on COU degradation was discussed, and the stability and versatility of CuS@MIL-101(Fe) was studied as well. Radical scavenging experiments and electron paramagnetic resonance (EPR) spectroscopy identified • OH and 1 O 2 as the main reactive oxygen species (ROS). Finally, the possible mechanism of higher COU degradation efficiency in the CuS@MIL-101(Fe) activated PMS system and the degradation pathways were also deeply explored. Consequently, this work provided a novel insight into construction of sulfur vacancies-enriched heterogeneous catalysts for efficiently activating PMS for refractory organic pollutants elimination.
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INTERNATIONAL JOURNAL OF ENVIRONMENTAL ANALYTICAL CHEMISTRY
·
2020
·
IF 1.431
Jiahui Yang,Kaixuan Ma,Nan Li,Xinyue Gu,Shengchao Miao,Meixing Zhang,Jing Yang,Shihai Cui
Novel magnetic CoFe2O4-embedded MIL-101(Cr) with tetramethylammonium hydroxide (CoFe2O4/MIL-101T) was prepared through the facile hydrothermal method. Tetramethylammonium hydroxide acts as a template molecule and avoids the recrystallisation of terephthalic acid. The material was applied as the adsorbent in the magnetic solid-phase extraction (MSPE) process coupled with high-performance liquid chromatography to detect the five flame retardants in environmental water samples. Several parameters affecting MSPE efficiency were systematically investigated, such as MIL-101T content, material amount, desorption solvents, adsorption time, solution pH, theoretical maximum enrichment factor (EFmax) and the reusability. Under optimised conditions, good linearities were achieved for five flame retardants with correlation coefficients R2 > 0.9961. The limits of detections for analytes at the signal-to-noise ratio of three were 0.013–0.071 μg·L−1. This method was applied to the analysis of tap, pond, lake and river waters. The recoveries were in the range of 81.5 ± 3.2–107.0 ± 2.3% with the relative standard deviations ranging from 0.11% to 8.66% in four real water samples. The adsorption mechanism was the hydrophobic interaction between the material and the analytes besides pore adsorption action of the material.
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CRYSTENGCOMM
·
2019
·Vol. 21
·期 38
·5824-5833
·
IF 3.382
Ji-Min Yang,Run-Zhi Zhang,Ying-Yan Liu
We herein report that the adsorption driving forces (i.e., electrostatic interactions, hydrogen bonding, and π–π interactions) of MIL-101-COOH microcrystals toward dyes can be tuned by varying the molar ratio of H2BDC : H2BDC–COOH in the reaction system. More specifically, the adsorption capacities of MIL-101-COOH-1 were determined to be 2835.7 (Congo red, CR), 473.9 (methyl orange, MO), and 240.8 (acid chrome blue K, AC) mg g−1, exceeding those reported for pristine MIL-101 by 107.5, 16.7, and −25.8%, respectively. The above-mentioned adsorption behavior was rationalized based on the dye molecular structure, zeta potential, BET surface area and dye adsorption investigations, which revealed that free –COOH groups increase the electrostatic and hydrogen bonding interactions between the adsorbent and linear dyes, thereby improving the adsorption capacity for linear anionic dyes and overriding the effect of pore volume, whereas an increased steric hindrance effect between the adsorbent and a nonlinear dye decreases the adsorption capacity for the nonlinear anionic dye and overrides the effects of the electrostatic and hydrogen bonding interactions. The adsorption capacity of MIL-101-COOH-1 toward the anionic organic dyes (CR, MO, and AC) was found to be significantly higher than those of the other MIL-101-COOH adsorbents examined herein. The adsorption capacity of MIL-101-COOH is determined by the synergetic interplay between the electrostatic, hydrogen bonding, and π–π interactions, steric hindrance effect, and pore volume of the adsorbent. The results shed light on the adsorption mechanism of metal–organic frameworks toward organic dyes.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Jingjing Zhu,Huaqiang Chen,Lan Wang,Engang Fu,Jianping Wu,Qilei Zhang,Lirong Yang,Gang Xu
A composite hollow mesoporous MIL-101@Pd@ZIF-8-30min (HM-MIL@Pd@ZIF-30min) nanocatalyst with hollow core and stable shell was developed in this study. Hollow mesoporous MIL-101(HM-MIL) was hydrothermally synthesized and employed as the supports of Pd nanoparticles by adopting a facile HM-MIL-template strategy to make ZIF-8 crystals uniformly overgrew on HM-MIL-101@Pd microcrystal cores. The obtained core-shell catalyst possessed hollow mesoporous structure, and the shell layer of ZIF-8 had additional advantages of abundant Lewis basic sites for heterogeneous racemization reaction. Compared with unmodified HM-MIL@Pd and solid MIL-101(Cr)@Pd@ZIF-8 (S-MIL@Pd@ZIF-8), HM-MIL@Pd@ZIF-8-30min had higher racemic chemical activity (conv. 99%) and selectivity (sel. R-amide 94%) in one-pot dynamic kinetic resolution (DKR) reaction system of rac -1-phenethylamine. The catalyst showed excellent stability, and the conversion and selectivity reached 95% and 93% respectively after ten catalytic cycles.
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Analytical Methods
·
2019
·Vol. 11
·期 27
·3467-3473
·
IF 2.378
Zhiyang Lv,Cheng Yang,Yuehong Pang,Weiying Xie,Xiaofang Shen
Dispersive solid phase extraction (d-SPE) is a preponderant methodology featuring direct contact and interaction between adsorbents and analytes. Herein, we used the porous metal–organic framework (MOF) MIL-101(Cr) as a d-SPE adsorbent for pretreatment of edible oil samples and determination of benzo[a]pyrene (BaP). The samples after treatment are applied to determination by high performance liquid chromatography coupled with a fluorescence detector (HPLC-FLD). We optimized the type and dosage of the MOF, diluent and eluent. Under the optimized conditions, this method gave a linear calibration curve for the determination of BaP in the range of 1–30 ng mL−1 (R2 = 0.9958) and the relative standard deviation (RSD) ranged from 1.07 to 8.14% (n = 6). The limit of detection was 0.19 ng mL−1 (S/N = 3) and the recoveries from different types of spiked oil samples were between 88.8 and 118.8%. Compared with conventional methods, the MOF-based d-SPE reduces organic solvent consumption and simplifies operation, which provides potential for application in extraction of hydrophobic targets from oil complexes.
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Polymers
·
2018
·Vol. 10
·期 7
·750
·
IF 2.935
Nan Wang,Li-Ye Yang,Yang-guang Wang,Xiao-kun Ouyang
In this work, a tetraethylenepentamine (TEPA)-grafted metal-organic framework material (MIL-101) was synthesized. The introduction of TEPA increased the abundance of functional groups on the MIL-101. As a powdery adsorbent, MIL-101-TEPA can be difficult to separate. In order to solve this problem, we combined MIL-101-TEPA with sodium alginate (SA) and injected the mixture into a CaCl2solution to solidify the powder into beads with a particle size of 3 mm. The easily recovered adsorbent was applied to the adsorption of Pb(II) from water. The structure and characterization of the adsorbent were investigated through scanning electron microscope (SEM), Fourier-transform infrared spectroscopy (FTIR), X-Ray diffraction (XRD), thermogravimetric analysis (TGA), and X-ray photoelectron spectroscopy (XPS). We also optimized the adsorption conditions. The results of the study showed that the adsorption process was chemisorptive and endothermic in nature. The maximum adsorption capacity of the composite beads was 558.6 mg/g. Meanwhile MIL-101-TEPA@CA showed good repeatable utilization.Keywords:sodium alginate;functional MIL-101;composite beads;adsorption;Pb(II)
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2018
·
IF 2.829
Mingjuan Han,Ying Li,Zheng Gu,Huali Shi,Chong Chen,Qiang Wang,Hui Wan,Guofeng Guan
A novel functionalized MOF heterogeneous catalyst (MIL-101(Cr) @MBIAILs), 2-Mercaptobenzimidazole ILs with electron-rich SH groups immobilized onto the surface of the well-defined MIL-101(Cr) frameworks, was constructed and fabricated by the S Cr coordination bond on the basis of the facile post-synthetic modification strategy. The heterogeneous catalyst was measured by XRD , FTIR, SEM, TEM , TGA , EA and N 2 adsorption–desorption, and the catalytic behavior of the catalyst was assessed by the esterification about oleic acid and methanol as a model reaction. The results showed that MBIAILs have been successfully immobilized onto the surface of MIL-101(Cr) frameworks by S Cr coordinate bonds. More importantly, the conversion of oleic acid just decreased from 91.0% to 82.1% when the catalyst had been reused six times. This exhibited the prepared catalyst had superior catalytic behavior and excellent reusability.
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RSC Advances
·
2015
·Vol. 5
·期 57
·46301-46306
·
IF 3.84
Jing Fang Guo,Rong Mei Fang,Cheng Zhi Huang,Yuan Fang Li
In order to eliminate the scattered light induced by the signal amplifier in fluorescence anisotropy (FA) assays, a nanosized metal–organic framework MIL-101, ranging from 80–500 nm, has been synthesized through a hydrothermal method with the addition of glycerol. We chose the 100 nm MIL-101 to enhance FA for label-free detection of the respiratory syncytial virus (RSV) gene sequence and the DNA-intercalating dye SYBR Green I (SGI) as the fluorophore, based on the different affinities of MIL-101 toward ssDNA and dsDNA. The nanosized MIL-101 has a negligible scattering effect owing to its smaller particle size, so all of the experimental data of FA values were smaller than the maximum initial anisotropy of 0.4. As a specific advantage, a dual amplification result of not only an increase in the FA value of SGI/ssDNA (r1) but also a decrease in the FA value of SGI/dsDNA (r2) was presented at the same time. Consequently, a larger FA value change Δr (Δr, Δr = r1 − r2) was obtained and contributed to improve the sensitivity. In addition, the quantitative detection of the target DNA (T) was achieved according to the relationship between Δr and the concentration of T. In the presence of MIL-101, the Δr is 7-fold higher than that without MIL-101 and achieved the sensitive and selective detection of RSV DNA.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Yu Zou,Wanshan Wang,Fengyin Duan,Wen Yun,Hong Chen,Yiping Li,Lizhu Yang
An ultrasensitive fluorescence detection strategy of chloramphenicol (CAP) was developed based on product catalysis of tetrahedral DNA framework (TDF) and fluorescent quenching of MIL-101(Fe). The product was used to catalyze the reaction. As the concentration of catalyst increased, the reaction time was significantly shorted to 21 min which was much shorter than other isothermal amplification technologies. Moreover, the multiple fluorophores of TDF and high efficient quenching ability of MIL-101(Fe) provided better performance with a linear range for CAP detecting from 1.6 pM to 80 pM and the limit of detection (LOD) as low as 0.67 pM. In addition, it also demonstrated good specificity and resistance to interference from other related antibiotics. Importantly, this strategy exhibited satisfactory relative standard deviation and recovery results for practical application, exhibiting a favorable application prospect in CAP analysis.
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