Petroleum Science
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2023
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IF 5.6
Bo-Long Jiang,Dong-Xu Zhang,Dan-Dan Yuan,Yan-Guang Chen,Tian-Zhen Hao,Hua Song
Oxidative desulfurization from fuel oil is one of the important methods for deep desulfurization. The development of efficient oxidative desulfurization catalysts is crucial for improving the desulfurization performance. Successful encapsulation of phosphotungstic acid (HPW) and ionic liquid (BMImBr) inside the mesoporous cages of MIL-101(Cr) was accomplished through a combination of “bottle around ship” and “ship in bottle” methods. The obtained BMImPW@MIL-101(Cr) composite was characterized by XRD, FTIR, BET, SEM, XPS and ICP methods. Results indicated that the BMImPW@MIL-101(Cr) composites with PW 3− loading of 23.1–50.7 wt% were obtained, demonstrating that the “bottle around ship” method is beneficial to make full use of nanocages of MIL-101(Cr) to obtain expected high loading of active PW 3 − . The BMImPW@MIL-101(Cr) exhibits excellent reusability with no evidence of leaching of active PW 3 − and BMIm + , and well-preserved structure after successive cycles of regeneration and reuse. The significantly improved stability of BMImPW@MIL-101(Cr) as compared to HPW@MIL-101(Cr) is possibly because the leaching of the active PW 3 − − sites can be greatly suppressed by forming large size of BMImPW owing to introduction of BMIm + cation. The BMImPW@MIL-101(Cr) exhibited excellent catalytic activity for solvent free oxidative desulfurization of refractory sulfides. The enhanced oxidative desulfurization activity as compared to HPW@MIL-101(Cr) can be explained by the intimate contact of sulfides with active PW 3 − sites owing the strong attraction of BMIm + cation with the sulfides.
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JOURNAL OF CHROMATOGRAPHY A
·
2017
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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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高影响因子
MICROCHEMICAL JOURNAL
·
2025
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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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MICROCHEMICAL JOURNAL
·
2026
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IF 5.2
Xu Xu,Yumeng Liu,Jia Lv,Baocheng Ji,Junguang Li,Ke Li,Dianbo Zhao,Yanhong Bai
A modified QuEChERS method was developed in analysis of 52 veterinary drugs. • A novel MIL-101(Cr)–rGO@melamine sponge composite was fabricated. • The fast matrix purification could be achieved within several seconds. • Matrix cleanup was achieved through simple soaking and squeezing. • The method showed low matrix effects, good recoveries, and high precision. Herein, we report the fabrication of an elastic, quick, easy, cheap, effective, rugged, and safe adsorbent using a functionalized melamine sponge (MLS) and used it for the high-throughput analysis of 52 veterinary drugs in beef liver samples via ultraperformance liquid chromatography–tandem mass spectrometry. The as-prepared adsorbent was obtained by successive loading of Matérial Institut Lavoisier-101 (Chromium) [MIL-101(Cr)] and reduced graphene oxide (rGO) on melamine sponge skeletons. Excellent linearity with determination coefficients of ≥0.9942 was obtained across a range of 0.25–200 μg·kg −1 . Relatively low limits of detection (0.1–4.9 μg·kg −1 ) and limit of quantitation (LOQ; 0.3–16.2 μg·kg −1 ) were obtained. When fortified at three levels (1×, 5×, and 10× LOQ), spiked recoveries varied between 63.5% and 115.4%, with the intraday and interday relative standard deviations of ≤12.9%. Through direct infiltration and compression, efficient matrix purification was accomplished within seconds, yielding negligible matrix effects (from −18.4% to +19.1%). Thus, the MIL-101(Cr)–rGO@MLS adsorbent possesses high potential for fast, convenient, and efficient matrix purification in complex sample analysis. Download: Download high-res image (179KB) Download: Download full-size image
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TALANTA
·
2022
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IF 6.556
Lin Li,Yingying Li,Sijia Zhang,Ting Wang,Xiaohong Hou
In this study, MIL-101(Cr)/cellulose aerogel/melamine sponge composite was fabricated through a simple soaking method. The composite was packed in the syringe barrel and used as the sorbent for microextraction in packed syringe. Coupled to UPLC-MS/MS, the proposed method was employed for the analysis of trace nitroimidazoles in water samples. The parameters affecting the extraction efficiency, including sorbent type, pH value of sample solution, sample solution volume and elution solvent were optimized. Under the optimal conditions, good linearity (r > 0.99 for five analytes), high sensitivity (limit of detection: 8.250–16.33 ng L −1 ), ideal precision (intra-day precision: 1.1%–5.3%, inter-day precision: 1.8%–6.7%) and satisfactory accuracy (recovery: 70.4%–96.7%) were achieved. The proposed method was proved to be efficient, easily operative and environmentally friendly.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Liping Liang,Fenfen Xi,Jinhui Zhao,Gunel Imanova,Sridhar Komarneni,Jianfeng Ma
nZVI was immobilized on MIL-101(Cr), a metal–organic framework (MOF), and subsequently utilized for the removal of U(VI) from aqueous solution. This composite was also tested for its toxicity to Escherichia coli ( E. coli ). The results demonstrated that MIL-101(Cr) and nZVI had a significant synergistic effect. This composite material is excellent for removing U(VI) and the optimal ratio of MIL-101(Cr) to nZVI was found to be 1.2:1 on mass basis. Adsorption data exhibited excellent fitting to the Freundlich and pseudo-second-order kinetic models, and a maximum removal capacity of 526.32 mg/g of U(VI) was achieved by M-Fe at 298 K (pH = 6.0). The removal mechanisms were clarified by the X-ray absorption near edge structure (XANES), X-ray photoelectron spectroscopy (XPS), and extended X-ray absorption fine structure (EXAFS). Results reveled that U(VI) was mainly removed through chemisorption, forming a bidentate mononuclear edge-sharing linkage between UO 3 pyramid and iron(hydro)oxide. Through free radical quenching experiments and EPR analysis, it was indicated that the existence of reactive oxygen species (ROS) accelerates the oxidation of nZVI, generating more iron oxides or hydroxides for U(VI) adsorption, while inhibiting the reduction of U(VI) to U(IV). Furthermore, immobilized nZVI on MIL-101(Cr) mitigated the biotoxicity of Escherichia coli ( E. coli ). Direct contact played a crucial role in inactivating E. coli cells by nZVI/ E. coli system. Extracellular reactive oxygen species (ROS) played a vital role in inactivating E. coli in the M-Fe/ E. coli system where OH is the main ROS. These findings enhance our understanding of the mechanism of U(VI) removal and bactericidal effect on organisms using ZVI-based composites, which will broaden the application scope of the two materials in pollution removal, especially in radioactive decontamination.
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JOURNAL OF CHROMATOGRAPHY A
·
2024
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IF 3.8
Tianci Lv,Fubin Liu,Mengqian Xiao,Ying Liu,Litao Wang,Guihua Gao
In this study, a novel hierarchical pore MIL-101(Cr) foam (HPF-MIL-101) was designed and prepared using the sacrificial template method with NaCl as the sacrificial template. This method involved grinding, heating, and washing the NaCl template to produce HPF-MIL-101, with PVDF as the binder and MIL-101(Cr) as the adsorbent. This preparation process is both straightforward and cost-effective, avoiding the use or generation of any organic reagents, thereby offering an environmentally sustainable approach for producing metal-organic framework (MOF) composites. The prepared HPF-MIL-101 exhibited excellent adsorption capabilities for both anionic dye (methyl orange, MO) and cationic dye (methylene blue, MB). The adsorption process followed a pseudo-second-order kinetic model and Friedrich isotherm model, indicating a multilayer adsorption. This is further supported by the Weber-Morris intraparticle diffusion model, which divided the adsorption process into three stages. Furthermore, the adsorption process was consistent with the Freundlich isotherm model, with a correlation coefficient ( r ) greater than 0.96. HPF-MIL-101 can also be used as an adsorbent for solid phase extraction (SPE). Therefore, an SPE method combined with high-performance liquid chromatography (HPLC) was developed using HPF-MIL-101 as the adsorbent to analyze five fluoroquinolones (FQs) in water samples. This analytical method showed good linearity in the range of 30–2000 ng·mL −1 , with excellent linear correlation coefficient ( r = 0.9991–0.9999), reasonable extraction recoveries ranging from 80.39 to 112.7 % (RSD ≤ 7.9 %), and low limits of detection (8–30 ng·mL −1 ). Overall, the results indicated that HPF-MIL-101 not only had a simple, environment-friendly, and pollution-free preparation process but also can be reused for enrichment and detection of trace FQs in water. Thus, HPF-MIL-101 exhibits immense application potential in environmental pollutant removal and also provides a valuable reference for the preparation and application of other MOF composites.
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MICROCHEMICAL JOURNAL
·
2022
·
IF 5.304
Li Yang,Shuang Wang,Zhongshui Xie,Rongrong Xing,Runqin Wang,Xuan Chen,Shuang Hu
A novel deep eutectic solvent - loaded magnetic solid phase extraction (DES-L-MSPE) method was proposed, which was based on the direct loading of a hydrophobic DES composed of L-menthol and lactic acid (1:2) into the pores of core–shell magnetic Fe 3 O 4 @MIL-101(Cr) nanoparticles. The function of DES was to condition the Fe 3 O 4 @MIL-101(Cr) and promote liquid phase microextraction for the analytes. Through coupling with HPLC-UV analysis, this method was utilized for the determination of six non-steroidal anti-inflammatory drugs (NSAIDs), including ketoprofen, naproxen, flurbiprofen, diclofenac sodium, ibuprofen, and mefenamic acid in environmental water samples. The influencing parameters such as type and ratio of DES, amount of adsorbent, sample solution pH, salt concentration, extraction time, elution solvent and time were investigated and optimized in detail. Under the optimal conditions, the method exhibited good linearity (5.0–1000 μg/L for ketoprofen, ibuprofen, 1.5–600 μg/L for flurbiprofen, mefenamic acid, 2.5–1000 μg/L for naproxen and 3.0–600 μg/L for diclofenac sodium with the correlation coefficients ranging from 0.9972 to 0.9993), low limits of detection (0.20–1.1 μg/L), and high precision (RSD < 8.2 %). Besides, the recoveries in spiked lake and river water samples were 89.8 %–110.4 % and 83.8 %–109.0 %, respectively. Taken together, the established method was proved to be simple, fast, highly sensitive and accurate for the determination of NSAIDs from aqueous matrices.
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FOOD CONTROL
·
2022
·
IF 6.652
Dakai Guo,Qingwen Huang,Rui Zhao,Wenbo Guo,Kai Fan,Zheng Han,Zhihui Zhao,Dongxia Nie
An efficient and fast magnetic solid phase extraction (MSPE) method was developed using MIL-101(Cr)@Fe 3 O 4 nanocomposites as adsorbent for purification and enrichment of 9 mycotoxins in agricultural products. The successful synthesis of MIL-101(Cr)@Fe 3 O 4 was confirmed via various characterization methods. Several key parameters affecting the performance of the MSPE procedure were extensively investigated including loading solution, elution solution and dosage of adsorbents. Under the optimal sample pretreatment conditions, the complex matrix effects from different agricultural products could be efficiently eliminated and the calibration curves constructed in neat solvent were directly used for the accurate quantification of these mycotoxins. Coupled with the analysis by ultra-high-performance liquid chromatography-tandem mass spectrometry, good linearity (R 2 ≥ 0.991), high sensitivity (limit of quantification in the range of 0.08–0.20 μg kg −1 ), satisfactory recovery (83.5–108.5%) and acceptable precision (RSD, 1.6–10.4%) were obtained. The applicability of the validated method was further verified in real maize, wheat, watermelon and melon samples.
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TALANTA
·
2024
·
IF 5.6
Xueyun Wei,Zhuomin Zhang,Gongke Li
Aromatic disinfection by-products (DBPs) have garnered considerable interest in recent years for their potential carcinogenicity. However, efficient separation and enrichment of DBPs in complex samples is a challenge due to the extremely low content of aromatic DBPs and the complexity of sample matrices. In this study, a MIL-101(Cr)–NH 2 @TAPB-DVA-COF hybrid material was prepared as the enrichment medium of membrane solid-phase extraction (M-SPE) to efficiently determine trace emerging aromatic DBPs. This medium exhibited excellent enrichment capacity and selectivity for aromatic DBPs because of the strong hydrogen bonding, π-π stacking and hydrophobic interactions. An efficient analytical method for five aromatic DBPs in juice drinks was successfully established by use of this hybrid material as the enrichment medium for M-SPE in combination with liquid chromatography tandem mass spectrometry (LC-MS/MS). The limits of detection of the established method were from 0.50 to 3.00 ng/L. Moreover, the method had been successfully used in real juice drinks to determine trace five aromatic DBPs with the spiked recoveries ranging from 84.1% to 125%. The method possessed high analytical sensitivity and accuracy for these five aromatic DBPs in juice drinks with the aid of the efficient M-SPE technology proposed.
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CRYSTAL GROWTH & DESIGN
·
2018
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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.
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TALANTA
·
2016
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IF 4.035
Xinpeng Dai,Xiuna Jia,Pan Zhao,Ting Wang,Jian Wang,Peiting Huang,Lu He,Xiaohong Hou
As a novel kind of materials, metal-organic frameworks (MOFs) have great potential for the preconcentration of trace analytes. In our work, MIL-101(Cr) was prepared and applied as a solid phase extraction (SPE) sorbent for the pretreatment of sulfadiazine (SDA), sulfamethazine (SMZ), sulfachloropyridazine (SCP) and sulfamethoxazole (SMX) in different environmental water samples coupling with ultra-high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) detection. Experimental parameters, such as SPE materials, pH of water sample, volume of sample, flow rate , and type and volume of elution solvent, were properly optimized. Under the optimum conditions, good sensitivity levels were achieved with the detection limits of 0.03–0.08 μg/L and the quantitation limits of 0.11–0.27 μg/L. The linear ranges were from 0.2–40 or 0.5–100 μg/L ( r 2 >0.996) for the analytes, and the relative recoveries were in the range from 83.5% to 107.3% with the relative standard deviations (RSD) between 0.2% and 8.0% ( n =6). In addition, computational simulation was primarily used to predict the adsorption of MIL-101(Cr) toward sulphonamides (SAs), and also demonstrated the molecular interactions and free binding energies with the molecular modeling method. The results revealed that the combination of experimental and computational study not only accurately recognized the adsorption of MIL-101(Cr) on SAs, but also provided a new strategy on the trace contaminant analysis.
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