APPLIED CATALYSIS A-GENERAL
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2013
·
IF 3.41
Zhiguo Sun,Gang Li,Hai-ou Liu,Liping Liu
A series of MOF-based catalysts, metal-salen complexes incorporated into amino-functionalized MIL-101 matrices by salicylaldehyde condensing to amino group and coordinating metal ion through one pot method, have been prepared and characterized. The successful preparation of catalysts demonstrates that postsynthetic modification (PSM) is a practical and powerful route to generate MOF-based catalyst with multiple active sites. The catalytic performances of prepared catalysts were investigated via selective oxidation of cyclohexane to cyclohexanone and cyclohexanol (KA-oil) by molecular oxygen in the absence of solvent. It was found that NH 2 -MIL-101(Cr)-Sal-Co, as a typical case, behaves as cooperative catalyst for cyclohexane selective oxidation. That is, salen-Co(II) attached to framework of MOF is able to assist in the generation of new radicals from peroxides via a Haber–Weiss catalytic cycle to promote conversion of cyclohexane while framework Cr ion is able to catalyze the dehydration of intermediate product cyclohexyl hydroperoxide (CHHP) to improve KA-oil selectivity. Furthermore, this catalyst exhibits good recyclability and behaves as truely heterogeneous catalyst.
研究领域:
材料化学
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催化化学
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产品关联
DOI
高影响因子
Journal of Inorganic and Organometallic Polymers and Materials
·
2023
·Vol. 34
·期 4
·1751-1764
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IF 4
Zhou Zhuyou,Zou Congyang,Wang Yong,Liu Menghe,Ji Yufeng
A one-step solvothermal synthesis technique was employed to fabricate C 60 /MIL-101(Fe) composites. The C 60 /MIL-101(Fe) composites showed a better performance in the degradation of methylene blue (MB) and tetracycline hydrochloride (TCH) when compared to MIL-101(Fe) in the photo-Fenton system, which can be credited to the charge transfer and separation facilitated by the addition of C 60 . Results showed that C 60 /MIL-101(Fe) had the capacity to nearly completely eliminate TCH and MB over a broad pH range. The catalysts demonstrated remarkable catalytic degradation on various organic pollutants and water samples. Through active substance quenching experiments and EPR, it was determined that hydroxyl radical (·OH) is the main factor in the photocatalytic reaction process.
研究领域:
环境科学
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材料科学
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化学工程
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纳米技术
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DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
·
IF 5.4
Rui Zhang,Lingqiao Hu,Zixi Li,Jingjing Hao
The special layered structure and narrow band gap of BiOI semiconductors lead to a high recombination rate of photogenerated electrons and holes. Therefore, it is compounded with the porous structure of the metal–organic backbone NH 2 -MIL-101(Fe) to form heterojunctions and provide more active sites. In this paper, NH 2 -MIL-101(Fe)/BiOI composites were successfully prepared by solvothermal method, which has a high specific surface area and adjustable pore size, which is conducive to the effective separation and transport of photogenerated electrons and holes, thereby improving the photocatalytic efficiency. The results of XRD, SEM, XPS and other characterization experiments show that NH 2 -MIL-101(Fe)/BiOI composites have been successfully prepared. Secondly, ultraviolet diffuse reflectance spectroscopy (UV–vis DRS) was used to test the light absorption performance of the composites, which confirmed that the materials had a larger visible light range. Through PL, EIS confirmed that the efficiency of photogenerated electron and hole separation was further improved. In addition, the M–S curves of NH 2 -MIL-101(Fe) and BiOI were tested to calculate the valence and conduction band values of the material. Combined with the results of free radical trapping experiments, O 2 − and h + play a major role in the degradation of tetracyclines and can be degraded into CO 2 and H 2 O. The Z-type electron transfer mechanism of the composites is deduced, which can improve the separation rate of electrons and holes. In addition, the cyclic test verified that the composite material has good stability. When the tetracycline concentration was 30 mg/L, the degradation rate of the 10 % NH 2 -MIL-101(Fe)/BiOI composite reached 93.3 %. Its materials also have certain potential application value in environmental treatment, energy conversion and other fields, especially for the treatment of pollutants in water bodies.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Food Science & Nutrition
·
2022
·Vol. 10
·期 7
·2224-2235
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IF 3.553
Zhentao Tang,Qingrong Han,Gang Yu,Fei Liu,Yuzhu Tan,Cheng Peng
Magnetic solid-phase extraction (MSPE) strategy based on the Fe 3 O 4 @PDA/MIL-101(Cr) has been proposed to separate and purify five common mycotoxins in licorice, including aflatoxin B 1 , aflatoxin G 1 , sterigmatocystin, zearalenone, and ochratoxin A. Integrating the MSPE and solid–liquid extraction/partitioning, a modified QuEChERS was established to adapt to the complex licorice samples. The Fe 3 O 4 @PDA/MIL-101(Cr) was successfully synthesized and characterized by Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and nitrogen adsorption–desorption isotherms. Sorbents with superior advantages for exclusion of matrix interference and extraction of target analytes in a short time were obtained, according to their ability of magnetic separation, high surface area (287.75 m 2 /g), large pore volume (0.61 cm 3 /g), and nanosized structure with mesopores. Prior to analysis with ultrahigh-performance liquid chromatography-tandem mass spectrometry (UHPLC-MS/MS), several key parameters that would affect the sorbents’ extraction efficiency were extensively investigated. Under the optimized conditions, the practicality of the developed method for analysis of mycotoxins in licorice samples was confirmed by adequate linearity ( R 2 ≥ 0.9967), high sensitivity (LODs and LOQs, respectively, in the ranges 0.01–0.09 and 0.02–0.30 μg/kg), acceptable recovery (78.53%–116.28%), satisfactory reusability, and good interbatch precision of the sorbents (RSDs in the ranges 6.70%–11.20% and 6.02%–10.35%, respectively). The results indicated that the established method was feasible and reliable for the environment-friendly and rapid screening of mycotoxins in complex licorice samples.
研究领域:
分析化学
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食品安全
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中药学
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DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Yue Cao,Yanping Wang,Lirong Guo,Zhiyue Han,Haining Liu,Kaipeng Zhong,Shaoju Bian,Naicai Xu
A novel composite adsorbent, AMP@MIL-101(Cr), has been successfully synthesized by integrating ammonium phosphomolybdate (AMP) with the metal–organic framework MIL-101(Cr) for the efficient adsorption of rubidium ions (Rb+) from aqueous solutions. The results of structural characterizations confirmed that the crystalline framework of the adsorbent remained intact after Rb+ adsorption, indicating excellent structural stability. Adsorption kinetics, isotherm, and thermodynamics studies revealed that the adsorption process followed a single-layer chemisorption mechanism and was an endothermic reaction and spontaneous adsorption process with negligible influence from solution pH. The adsorbent exhibited a remarkable Rb+ adsorption capacity, reaching 69.4 mg·g–1 within 5 min in a solution containing 250 mg·L–1 Rb+ at 45 °C. In the Nanyi Mountain Oilfield, the adsorption rate of adsorbent for Rb+ (10.69%) exceeded that of other ions (Li+: 0.75%; Na+: 0; K+: 0.95%; Mg2+: 0.67%). Furthermore, the adsorbent still maintained 86.72% of its initial adsorption capacity after 5 consecutive adsorption–desorption cycles. These findings highlighted the great potential of AMP@MIL-101(Cr) as an efficient and stable adsorbent for the selective recovery of rubidium from aqueous environments.
研究领域:
环境科学
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材料科学
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化学工程
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吸附技术
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无机化学
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产品关联
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2017
·Vol. 184
·期 8
·2981-2990
·
IF 4.58
Wang Ting,Liu Siyu,Gao Guihua,Zhao Pan,Lu Nan,Lun Xiaowen,Hou Xiaohong
The authors describe a method for magnetic solid phase extraction (MSPE) combined with ultra-high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) for the quantitation of eight non-steroidal anti-inflammatory drugs (NSAIDs) in wastewater and environmental water samples. Specifically, the NSAIDs were directly extracted by using a magnetic nanocomposite of type Fe 3 O 4 /MIL-101(Cr) (Matérial Institute Lavoisier, MIL) from 50 mL water samples without any further cleanup. The effects of the amount of adsorbent, pH value, salt concentration, ultrasonic extraction time, desorption solvent nature and volume and desorption time were investigated. Under the optimal conditions, UPLC-MS/MS based detection resulted in the following figures of merit: (a) Linear calibration plots that typically extend from 0.1 (0.2, 0.05, 0.02) to 50 μg·L −1 , depending on the compound; (b) detection limits between 3 to 60 ng·L −1 ; and (c), recoveries varying from 81.2% to 116.8% with relative standard deviations between 0.4% and 10.8%. The adsorption of NSAIDs on Fe 3 O 4 /MIL-101(Cr) was characterized by adsorption isotherms, kinetics and thermodynamics studies and provides a deeper insight into the adsorption mechanism. Compared to other method for pretreatment and preconcentration of NSAIDs, the new method is more rapid, sensitive, accurate and eco-friendly. The method was successfully applied to the determination of the NSAID residues in a variety of real environmental and wastewater samples.
Schematic of a method for determination of non-steroidal anti-inflammatory drugs (NSAIDs) in environmental water by magnetic solid phase extraction based on Fe 3 O 4 /MIL-101(Cr) combined with UPLC-MS/MS. The adsorption mechanism of NSAIDs on Fe 3 O 4 /MIL-101(Cr) was studied.
研究领域:
环境科学
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分析化学
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产品关联
DOI
高影响因子
FOOD CHEMISTRY
·
2025
·
IF 9.8
Zhiyang Qin,Tianyue Peng,Xinguang Qin,Gang Liu,Haizhi Zhang
Accurate detection of tetracycline residue is of great significance for ensuring product quality and protecting human health. Here, a colorimetric/fluorescent dual-mode biosensor was developed for the detection of tetracycline in honey by using metalloporphyrin [TCPP(Fe)] covalently modified NH 2 -MIL-101(Fe) [named NH 2 -MIL-101(Fe)@TCPP(Fe)]. The morphology, chemical structure and peroxidas-like activity of this hybrid nanozyme were comprehensively studied. Based on excellent catalytic activity and intrinsic fluorescence of NH 2 -MIL-101(Fe)@TCPP(Fe), a colorimetric/fluorescent dual-mode biosensor was developed for the detection of tetracycline. The primary mechanism for this dual mode biosensor was the inhibitory effect of tetracycline on on NH 2 -MIL-101(Fe)@TCPP(Fe) catalyzed chromatic reaction between H 2 O 2 and 3,3′,5,5′-tetramethylbenzidine (TMB)/ o -phenylenediamine (OPD), which was ascribed to the consumption of · OH by tetracycline and the adsorption of tetracycline on the surface of NH 2 -MIL-101(Fe)@TCPP(Fe). After effective validation, this colorimetric/fluorescent dual mode method was applied to detect tetracycline residues in three actual honey samples.
研究领域:
生物化学
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分析化学
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食品安全检测
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2025
·
IF 11.3
Renjie Pan,Zongchen Li,Tian-Yang Zhang,Qi Fu,Zheng-Xiong Zheng,Jun Shi,Jian Lu,Chen-Yan Hu,Yu-Lin Tang,Mohamed Gamal El-Din,Bin Xu
Peracetic acid-based advanced oxidation processes (PAA–AOPs), which generate various reactive radicals, have garnered substantial attention for degradation emerging contaminants (ECs). However, nonselective radical-based PAA–AOPs often suffer from interference by water matrix components, causing low contaminants removal efficiency. This study explores the use of amino-(NH 2 )-functionalized metal–organic frameworks (MIL-101(Fe)-NH 2 ) as heterogeneous catalysts for PAA activation, enabling the generation of high-valent iron- (Fe)–oxo species (Fe(IV)) capable of efficiently degrading ECs (80 −100 %, within 30 min). The Fe(II) clusters in MIL-101(Fe)-NH 2 , modulated by electron-donating −NH 2 groups, play a pivotal role in Fe(IV) generation. Scavenger and probe experiments confirmed Fe(IV) as the primary reactive species responsible for ECs degradation. Density functional theory calculations demonstrated that the four-electron transfer to generate Fe(IV) has lower free energy than the two-electron transfer to generate organic radicals (e.g., CH 3 COO • and CH 3 C(O)OO • ). Furthermore, thermodynamically unfavorable CH 3 COO • desorption further promotes Fe(IV) generation. The PAA/MIL-101(Fe)-NH 2 system efficiently degraded SMX ( k app = 121.2 −287.2 M −1 s −1 ) and other ECs ( k app = 40 −432 M −1 s −1 ) with minimal interference from water matrix components and excellent reusability. This study demonstrates that MIL-101(Fe)-NH 2 is a robust catalyst for PAA activation and provides a novel approach for selectively generating Fe(IV) for ECs degradation.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
CRYSTAL GROWTH & DESIGN
·
2018
·
IF 3.972
Wei Zhang,Run-Zhi Zhang,Yong-Qing Huang,Ji-Min Yang
Herein, we report that the surface charge status and size of the metal–organic framework (MOF) MIL-101(Cr) can be tailored by varying the concentration of tetramethylammonium hydroxide. The adsorption capacity of MIL-101(Cr)-2 toward the anionic dye Congo red (CR) was found to be significantly higher than that of other MIL-101(Cr) adsorbents, although MIL-101(Cr)-3 microcrystals exhibited the highest adsorption capacity toward the anionic dye methyl orange (MO) due to the different adsorption mechanisms involved. This is the first demonstration of the synergetic interplay between the electrostatic and π–π interactions, adsorption spaces and sites, and size of the dye molecules, in terms of the uptake capacity of an adsorbent. In addition, the obtained results shed new light on the adsorption mechanism toward organic dyes over MOFs. Moreover, the MIL-101(Cr) microparticles exhibited excellent adsorption capabilities toward CR, achieving a maximum capacity of 1367.1 mg g–1, which is higher than the majority of reported values for other materials. Therefore, these results indicate that the MIL-101(Cr) nanostructure exhibits potential for application in the treatment of anionic dye-containing wastewater.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
ELECTROPHORESIS
·
2016
·Vol. 37
·期 19
·2478-2486
·
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.
研究领域:
分析化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Tongtong Wang,Xuedan Song,Qunxing Luo,Xiaodong Yang,Siying Chong,Jie Zhang,Min Ji
In terms of ‘green chemistry’ and ‘atom economy’, the cycloaddition of CO 2 to yield cyclic carbonate without any additive is an eco-friendly way to utilize CO 2 . Unfortunately, the low CO 2 capture quantity of common catalysts limited its catalytic efficiency. Herein, a novel acid-base bifunctional catalyst was successfully prepared by immobilizing ionic liquid on MIL-101-NH 2 (IL/MIL-101-NH 2 ) and tested for propylene carbonate (PC) rapid and facile synthesis from CO 2 and propylene oxide (PO). The synergetic interaction between Lewis base with strong CO 2 chemical capture capacity and Brønsted acid with strong hydrogen bond donor leads to the high catalytic efficiency of IL/MIL-101-NH 2 for carbonate synthesis from CO 2 and PO without any additive. The immobilization mode between MIL-101-NH 2 and IL is energetically supported by the density functional theory (DFT) calculations. This design idea of specific catalyst and the acid-base synergetic strategy provides new insights into the design of powerful catalyst systems for the CO 2 conversion.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Linlin Zheng,Xuechuan Lv,Yanan Chen,Bingyu Wei,Wanqing Hao,Ziyi Zhang,Jingru Yang,Ruiyu Liu,Xu Zhu,Yanli Zhou,Maotian Xu,Xiaohan Gao,Hui Dong
The iron-based metal–organic framework (NH2-MIL-101(Fe)) nanoparticles exhibited excellent conductivity, exceptional catalytic effect, sturdy stability flexible structure, etc. Consequently, it has been exploited in various applications. Herein, NH2-MIL-101(Fe) nanoparticles were successfully synthesized via the hydrothermal method and were grown in situ onto the pencil core electrode (PCE) for simultaneous determination of caffeic acid (CA) and acetaminophen (AP). The PCE decorated by NH2-MIL-101(Fe) as electrode substrate, combined with the dual effects of the excellent electrocatalytic activity of NH2-MIL-101(Fe) and the commendable electrical conductivity of PCE, the constructed sensor exhibits superior electrochemical sensing activity. The electrochemical behavior of CA and AP at the electrodes were investigated mainly by differential pulse voltammetry (DPV) and cyclic voltammetry (CV), exhibiting broad linear responses from 0.1 to 500 μM, and 0.08 to 800 μM for simultaneous detection of CA and AP, with detection limits of 29 nM and 24 nM, respectively. Moreover, the results of CA and AP in drug and human urine using this sensor were satisfactory, which proved that the sensor is feasible to simultaneously detect CA and AP.
研究领域:
分析化学
·
电化学
·
纳米材料
✓ 已验证
产品关联
DOI
高影响因子