JOURNAL OF CHROMATOGRAPHY A
·
2017
·
IF 3.981
Qingxiang Zhou,Man Lei,Yalin Wu,Yongyong Yuan
Metal-organic framework material has been paid more attention because of its good physical and chemical properties. Nanoscale zero valent iron is also in the center of concern recently. Combination of their merits will give impressive results. Present study firstly synthesized a new magnetic nanomaterial nano-scale zero valent iron-functionalized metal-organic framworks MIL-101 (Fe@MIL-101) by co-precipitation method. The morphology and structure of the as-prepared Fe@MIL-101 were characterized by transmission electron microscopy and X-ray diffraction, etc. The experimental results showed that Fe@MIL-101 earned good adsorption ability to polycyclic aromatic hydrocarbons. The limits of detection of developed magnetic solid phase extraction were all below 0.064 μg L −1 and precision can be expressed as relative standard deviation (RSD, %) and which was better than 4.4% (n = 6). The real water analysis indicated that the spiked recoveries were satisfied, and Fe@MIL-101 earned excellent reusability. All these demonstrated that Fe@MIL-101 exhibited excellent adsorption capability to polycyclic aromatic hydrocarbons and would be a good adsorbent for development of new monitoring methods for environmental pollutants.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Chun-Yang Li,Tong Zhai,Wentao Gu,Huan Lv,Xue-Meng Ji,Man-Man Wang,Jing-Min Liu,Shuo Wang
Advanced glycosylation end products (AGEs) are becoming a prominent issue in the biomedical and food safety industries because of their strong relationship to human health. Here, a MIL@PANI@LDH photocatalyst was prepared by in-situ growth method, realizing thorough elimination of AGEs for the first time. The synthesized photocatalysts used MIL-101 holding remarkably specific surface area as the core and PANI with a large number of amino and imine groups as the linker to ensure excellent adsorption capacity. The lamellar LDH structure grown in the outermost layer, on the other hand, introduces a narrower band gap and stronger light absorption ability, capable of activating sodium persulfate (PS) and generating free radicals with powerfully oxidizing ability. They work in concert to achieve the effective degradation. Through the optimization of the reaction conditions, the best photochemical performance could be achieved with a Zn/Al molar ratio of 3:1, and the degradation rates of AGEs were greater than 99.8 % (within 150 min). Additionally, multiple radical synergistic and non-radical action pathways involved in the system were revealed. The precision-engineered catalysts also exhibited high stability, reusability, and desirable biosafety, offering an effective and sustainable solution to the problem of purifying hazardous substances in real application.
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JOURNAL OF HAZARDOUS MATERIALS
·
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.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Zong-Mu Dong,Yaqing Guo,Liming Qin,Peiyi Zhang,Jian-Feng Wu,Guang-Chao Zhao
A multi-step growing and etching method was used to synthesize metal–organic framework materials (MIL-101) with a hollow structure of distinct shell layers. The resorcinol–formaldehyde organic aerogel (RFOA) was embedded in-situ into the triple-shelled hollow MIL-101 (TSHM) to form a novel RFOA@TSHM spherical multilayer shell composite, which was used as a fiber coating material of solid-phase microextraction for the enrichment and determination of six tetracyclines (TCs) by coupling with HPLC-UV–vis detector in aqueous solutions. Due to the embedding of the RFOA and the multilayer shell structure, the RFOA@TSHM composite is characterized by a stable structure with a larger pore size and specific surface area compared with the TSHM alone. Under optimal conditions, limits of detection of 0.13–1.16 μg L −1 and limits of quantification of 0.43–3.83 μg L −1 were obtained for TCs detection. Moreover, the RFOA@TSHM coating fiber was successfully applied to detect TCs in egg and milk real samples.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 21
·9702-9708
·
IF 2.7
An-Xu Ma,Cai-Fang Liu,Yu-Lan Zhu,Zong-Hong Luo,Hong-Mei Zhou,Yue Zhang,Bang-Jin Wang,Jun-Hui Zhang,Sheng-Ming Xie,Li-Ming Yuan
In this work, a chiral core–shell microspheres composite, L-his-MIL-53-NH2@SiO2, was prepared through in situ growth and chiral post-modification strategies. The core–shell microspheres were applied as a novel chiral stationary phase for HPLC enantiomeric separation. Various racemates were separated on the L-his-MIL-53-NH2@SiO2 packed column using n-hexane/isopropanol as the mobile phase. The chiral column showed excellent separation efficiency for fourteen chiral compounds, including alcohols, alkanes, esters, phenols, ketones, and organic acids. The influence of injection mass and temperature on the separation performance of the chiral column were investigated. The relative standard deviations (n = 5) of the retention time and peak area by repeated separation of benzoin are 0.28% and 0.63%, respectively. The results show that the L-his-MIL-53-NH2@SiO2 packed column exhibited good reproducibility and stability. In addition, the chiral resolution ability of the L-his-MIL-53-NH2@SiO2 packed column was compared with that of a commercial chiral column (Chiralpak AD-H). The L-his-MIL-53-NH2@SiO2 packed column exhibits unique advantages in chiral separations that can be complementary to the commercial chiral column. It was demonstrated that the chiral core–shell microspheres composite L-his-MIL-53-NH2@SiO2 prepared based on in situ growth and chiral post-modification strategies has great potential for enantiomeric separation by HPLC.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Hao Du,Rubin Huo,Aoxiang Liu,Yuxin Hui,Bo Shen,Ningyi Li,Yun Ji,Qin Jin,Baobing Zheng,Guoxiang Yang,Zhe Zhang,Qi Wang
Herein, a photo-self-Fenton system of resorcinol-formaldehyde resins/MIL-88A(Fe) (RF/88A) S-scheme heterojunction was successfully established to in-situ generate and activate H 2 O 2 toward tetracycline (TC) degradation and sterilization under visible light illumination. As a result, the 35 %-RF/88A (the mass ratio of RF to 88A was 35 %) can remove most TC and kill approximately 100 % E. coli and S. aureus . Notably, the composites presented superior repeatability and wide pH application range. Fukui index identified the reaction sites of TC molecule and quantitative structure-activity relationship (QSAR) forecasted intermediates toxicity. Density functional theory (DFT) calculations were performed to investigate electron transfer mechanism of the heterojunctions on a molecular scale. Such a S-scheme charge transfer route was also proved by in situ irradiated X-ray photoelectron and electron paramagnetic resonance measurements. In summary, this research innovatively provides deep insights into the in-situ generation and activation of H 2 O 2 and exhibited an environmentally friendly way toward pollutant degradation and sterilization.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 2
·1-9
·
IF 5.833
Senosy Ibrahim Abdelhai,Zhang Xin-Zhong,Lu Zhi-Heng,Guan Xiao-Yu,Yang Zhong-Hua,Li Jian-Hong,Guo Hao-Ming,Abdelrahman Talat Mahmoud,Mmby Mohamed,Gbiliy Asmaa
Fe 3 O 4 @MIL-100 (Fe)/PEI are used for the first time as an adsorbent material for the extraction of pesticide residues (epoxiconazole, flusilazole, tebuconazole, and triadimefon) from food matrices. The adsorbent proposed (Fe 3 O 4 @MIL-100(Fe)/PEI) was characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), field emission scanning electron microscopy (FE-SEM), thermogravimetric (TG) analysis, and vibrating sample magnetometer (VSM) techniques to evaluate the properties of the sorbent. Then, the Fe 3 O 4 @MIL-100 (Fe)/PEI was employed for the quantification of the four triazole fungicides in fruits and vegetables (apple, orange, tomato, cabbage, and cucumber) using HPLC-UV for separation and detection. During the extraction process, the main parameters such as amount of adsorbent, extraction time, pH value, ionic strength, eluting solvent, and eluting volume were optimized. Under the optimum conditions, good linearity of this method was observed for all analytes, with correlation coefficients ( R 2 ) ≥ 0.9908. The limits of detection (LODs) ranged from 0.021–3.04 μg kg −1 . The extraction recoveries of the four triazole fungicides varied from 73.9 to 109.4% with relative standard deviations (RSD) in the range 0.5 to 6.2%. Compared with other MOFs, the modification of Fe 3 O 4 @MIL-100 (Fe) with PEI shows high efficient adsorption due to the combined benefits of MIL-100 (Fe) and PEI. The material is easily synthesized, has good stability, and is of low cost.
Graphical abstract
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Materials
·
2022
·Vol. 15
·期 11
·3761
·
IF 3.748
Lei Wu,Doudou Qin,Fan Fang,Weifeng Wang,Wenying Zhao
Severe environmental pollution is caused by the massive discharge of complex industrial wastewater. The photocatalytic technology has been proved as an effective way to solve the problem, while an efficient photocatalyst is the most critical factor. Herein, a new photocatalyst MIL-68(Ga)_NH2was obtained by hydrothermal synthesis and were characterized by PXRD, FTIR,1H NMR, and TGA systematically. The result demonstrates that MIL-68(Ga)_NH2crystallized in orthorhombic system andCmcmspace group with the unit cell parameters:a= 36.699 Å,b= 21.223 Å,c= 6.75 Å,V= 5257.6 Å3, which sheds light on the maintenance of the crystal structure of the prototype material after amino modification. The conversion of Cr(VI) and binary pollutant Cr(VI)/RhB in wastewater under visible light stimulation was characterized by the UV-vis DRS. Complementary experimental results indicate that MIL-68(Ga)_NH2exhibits remarkable photocatalytic activity for Cr(VI) and the degradation rate reaches as high as 98.5% when pH = 2 and ethanol as hole-trapping agent under visible light irradiation with good reusability and stability. Owing to the synergistic effect between Cr(VI) and RhB in the binary pollutant system, MIL-68(Ga)_NH2exhibits excellent catalytic activity for both the pollutants, the degradation efficiency of Cr(VI) and RhB was up to 95.7% and 94.6% under visible light irradiation for 120 min, respectively. The possible removal mechanism of Cr(VI)/RhB based on MIL-68(Ga)_NH2was explored. In addition, Ga-based MOF was applied in the field of photocatalytic treatment of wastewater for the first time, which broadened the application of MOF materials in the field of photocatalysis.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiamin Wei,Qing Wang,Mian He,Shuai Li,Yunan Zhang,Yang Yang,Shipeng Luo,Lianshe Fu,Xin Wang,Tinghai Yang
The development of highly efficient strategy to facilitate comprehensive charge transmission and effective spatial charge separation is expected as a promising approach to improve photocatalytic performance. Herein, the Fe(III) doping modified AgI/NH 2 -MIL-68(In/Fe) Z-scheme heterojunction (ANM-x composite) with unique internal and interfacial charge transmission performance was fabricated by a facile ion exchange precipitation method. The optimized ANM-50 composite exhibits the maximum photocatalytic activity for the degradation of tetracycline, which is about 9.54, 2.61 and 1.86 times higher than that of pure NH 2 -MIL-68In, NH 2 -MIL-68(In/Fe) and AgI, respectively. The characterization results displayed that Ag nanoparticles (NPs) were generated during the photocatalytic procedure, which not only served as a charge transfer-highway, but also reduced the charge flow energy barrier, thereby accelerating charge transfer efficiency and consolidating the stability of the Z-scheme heterojunction. Mechanism exploration reflected that the superior photocatalytic performance was associated with synergetic effect among the introduced Fe(III), constructed ANM Z-scheme heterojunction and the generated Ag NPs, which significantly expands visible light response range and promotes more effective internal and interfacial charge separation. This research not only designs an efficient photocatalyst for decomposing tetracycline, but also opens a new perspective for rational developing Z-scheme heterojunction with unique internal and interfacial charge flow steering.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Yong Zhang,Jing Wang,Ying Liu,Xuemeng Wu,Lina Gao,Guihua Gao
In this study, a tip foam named as MIL-101(Cr)-NH₂/chitosan (MIL-101(Cr)-NH₂/CS) was prepared by cross-linking chitosan (CS) with MIL-101(Cr)-NH₂ using glutaraldehyde as the cross-linking agent. After freeze-drying, the internal structure of the MIL-101(Cr)-NH₂/CS foam became porous, thereby exposing more MIL-101(Cr)-NH₂, enriching binding sites, ensuring efficient adsorption, and allowing smooth passage of the sample solution. This also facilitates the inhalation and extrusion of the sample solution. Based on the unique advantages of the MIL-101(Cr)-NH₂/CS foam, a method combining pipette tip solid-phase extraction (PT-SPE) with high-performance liquid chromatography equipped with a fluorescence detector (HPLC-FLD) was established for the detection of puerarin and its metabolites (e.g., daidzein and equol) in rat serum. The method exhibited good linearity in the range of 0.5 to 5000 ng/mL, with limits of detection (LOD), lower limits of quantification (LLOQ), and limits of quantification (LOQ) ranging from 0.2 to 15 ng/mL, 0.5 to 50 ng/mL, and 1 to 100 ng/mL, respectively. The relative standard deviations (RSDs) of intra-day and inter-day precision for puerarin, daidzein, and equol were less than 19.8 %, meeting relevant regulatory requirements. The extraction recoveries of puerarin, daidzein, and equol ranged from 80.17 % to 91.70 %, 80.02 % to 87.41 %, and 80.29 % to 85.39 %, with corresponding RSDs of 3.2 % to 10.4 %, 11.2 % to 13.8 %, and 7.9 % to 11.1 %. These results indicate that the developed method meets the methodological requirements for the quantitative analysis of biological samples. The application of MIL-101(Cr)-NH₂/CS foam in PT-SPE further expands the application scope of metal-organic frameworks (MOFs) in solid-phase extraction (SPE) and provides a reference for PT-SPE technology in handling small-volume samples in complex matrices.
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MOLECULES
·
2020
·Vol. 25
·期 4
·897
·
IF 3.267
Qian-Chun Zhang,Guang-Ping Xia,Jun-Yi Liang,Xiao-Lan Zhang,Li Jiang,Yu-Guo Zheng,Xing-Yi Wang
In this study, a novel monolithic capillary column based on a NH2-MIL-53(Al) metal–organic framework (MOF) incorporated in poly (3-acrylamidophenylboronic acid/methacrylic acid-co-ethylene glycol dimethacrylate) (poly (AAPBA/MAA-co-EGDMA)) was prepared using an in situ polymerization method. The characteristics of the MOF-polymer monolithic column were investigated by scanning electron microscopy, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, X-ray diffractometry, Brunauer-Emmett-Teller analysis, and thermogravimetric analysis. The prepared MOF-polymer monolithic column showed good permeability, high extraction efficiency, chemical stability, and good reproducibility. The MOF-polymer monolithic column was used for in-tube solid-phase microextraction (SPME) to efficiently adsorb trace sulfonamides from food samples. A novel method combining MOF-polymer-monolithic-column-based SPME with ultra-high performance liquid chromatography-tandem mass spectrometry (UHPLC-MS/MS) was successfully developed. The linear range was from 0.015 to 25.0 µg/L, with low limits of detection of 1.3–4.7 ng/L and relative standard deviations (RSDs) of < 6.1%. Eight trace sulfonamides in fish and chicken samples were determined, with recoveries of the eight analytes ranging from 85.7% to 113% and acceptable RSDs of < 7.3%. These results demonstrate that the novel MOF-polymer-monolithic-column-based SPME coupled with UHPLC-MS/MS is a highly sensitive, practical, and convenient method for monitoring trace sulfonamides in food samples previously extracted with an adequate solvent.Keywords:monolithic capillary column;metal-organic framework;sulfonamides;solid-phase microextraction;ultra-high performance liquid chromatography-tandem mass spectrometry
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Sustainable Energy & Fuels
·
2024
·Vol. 8
·期 13
·2889-2899
·
IF 5
Jiaqi Wang,Hongyang Huo,Guozhe Sui,Shuang Meng,Dongxuan Guo,Shanshan Fu,Dantong Zhang,Xue Yang,Jinlong Li
The development of visible-light-active photocatalysts with high performance has been regarded as a promising way to address environmental wastewater issues. In this work, a highly efficient g-C3N4/CdS/TiO2 ternary Z-type heterojunction photocatalyst with a hollow structure has been fabricated using a step-by-step self-assembly strategy, which demonstrates excellent photocatalytic performance under visible light and removes various water-soluble organic pollutants effectively. The photocatalytic degradation efficiency of 20-g-C3N4/CdS/TiO2-10 against rhodamine B (RhB) is found to be 29.8 times higher than that of the pristine g-C3N4 within 90 minutes of visible light irradiation attributed to the active species of ˙O2− and h+. Liquid chromatography mass spectrometry results suggest that the degradation pathway of RhB involves main steps such as N-de-ethylation, chromophore cleavage, ring opening, and mineralization. A series of characterization analyses, combined with the observed enhanced photocatalytic performance, indicate that the g-C3N4/CdS/TiO2 ternary heterojunction benefits from the rapid transport and separation of photogenerated carriers facilitated by the formation of a heterointerface. Furthermore, the g-C3N4/CdS/TiO2 ternary heterojunction exhibits favorable stability, with 88.1% degradation efficiency after five cycles of degradation experiments. This work provides novel insights into the preparation and application of ternary heterojunctions with superior photocatalytic performance for eliminating organic pollutants from wastewater.
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