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.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Zhujun Huang,Zhan Lai,Dongying Zhu,Haiyan Wang,Chenxi Zhao,Guihua Ruan,Fuyou Du
The electrospun graphene oxide/MIL-101(Fe)/poly(acrylonitrile- co -maleic acid) nanofibers (E-spun GO/MIL-101(Fe)/PANCMA NFs) were fabricated by a facile electrospinning method and used as integrated photocatalytic adsorbents (IPAs) to remove dye pollutant from water samples. Compared with E-spun GO/PANCMA and E-spun MIL-101(Fe)/PANCMA NFs, the fabricated E-spun GO/MIL-101(Fe)/PANCMA NFs exhibited higher adsorption ability and excellent photocatalytic activity towards a model pollutant Rhodamine B (RhB). Under the optimized conditions, the as-prepared IPAs achieved almost complete adsorption of RhB within 15 min with the maximum adsorption capacity of 10.46 mg/g. Under visible-light irradiation, 93.7% of RhB in 20 mL water sample was degraded within 20 min, and the degradation kinetics of RhB fitted well with the first-order kinetic model. In addition, LC-MS analysis of the RhB degradation products confirmed the degradation pathways, and the generated •OH radicals played important roles in the degradation process. Importantly, the E-spun GO/MIL-101(Fe)/PANCMA NFs exhibited good reusability and could be reused for consecutive 20 cycles, which make them promising candidate materials in the field of industrial applications and environmental remediation.
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CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Shihui Zhang,Xu Zhang,Wanting Shi,Weiyan He,Caihong Li,Xiaojing Wang
Slow charge transfer and a weak built-in electric field (BIEF) at the heterojunction interface critically hinder the construction of efficient S-scheme heterojunctions. Secondary calcination and ultrasonic treatment of g-C 3 N 4 enhance interfacial contact with MIL-101, shortening carrier migration paths. P and Mn doping increases the Fermi-level difference between g-C 3 N 4(C,S) and MIL-101, strengthening the BIEF to drive directional carrier migration. This facilitates the recombination of carriers with low-redox-potential at the heterojunction interface while spatially separating carriers with high-redox-potential, successfully constructing an S-scheme P-Mn-MCN (C,S) heterojunction. The optimized system delivers remarkable photocatalytic performance, achieving 98 % tetracycline hydrochloride degradation under visible light within 60 min.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shuang Luo,Chenghua Zhang,Xingyan Liu,Yue Li,Lei Tang,Min Fu,Song Wang,Jie Wu,Mengmeng Xu,Xiaoping Wang,Youzhou He
A novel protonated NH 2 -MIL-125 was fabricated to introduce the moiety with charge and ample hydrogen (–NH 3 + Cl - group) into NH 2 -MIL-125 using HCl vapor obtained by natural volatilization of hydrochloric acid as a protonating reagent, which could exhibit excellent photocatalytic activity in both hydrogen production and NO purification under visible light irradiation. The hydrogen production and NO purification rate of the best protonated NH 2 -MIL-125 were 6762.80 μmol g −1 and 49.17%, respectively, which were 20.53 and 1.84 times as that of the original NH 2 -MIL-125. A series of characterizations, such as Mott-Schottky, PL, FT-IR and in situ DRIFTS , etc. were used to characterize the photoelectrochemical properties of the optimal catalyst, which demonstrated the protonation effect can not only enhance the electron migration rate, but also effectively accelerate photo-generated electron-hole pairs separation in the photocatalytic reaction process. This research believed that using HCl vapor as a facile protonation reagent to introduce the moiety with charge and ample hydrogen (–NH 3 + Cl - ) was a very effective method to decorate MOFs for hydrogen evolution and NO removal.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Tingting Zhang,Xing Liu,Yanqiu Jiang,Xiaowei Zheng,Jian Zhang,Yudong Li,Defeng Li,Kaifeng Lin
Photo-Fenton reaction has received increasing attention in removing antibiotics in water. Herein, Fe 2 O 3 -on-ZrO 2 polypods were designed and synthesized via metal organic frameworks (MOFs) derivation strategy combined with reflux heating and baking. The experimental results showed that under Ultraviolet–visible (UV–vis) light irradiation, more than 95 % tetracycline hydrochloride (TC-HCl) was degraded by Fe 2 O 3 -on-ZrO 2 with Fe/Zr mole ratio of 1.3 in 25 min within full pH range. Mainly due to the following points, there were abundant Fe 2 O 3 -on-ZrO 2 heterojunctions, which conduced to transfer photo-induced electrons (e − ) from ZrO 2 to Fe 2 O 3 , thus accelerating the iron cycle. Besides, OH – adsorbed was oxidized to hydroxyl radicals (·OH) by holes (h + ) in the valence band (VB) of ZrO 2 , and ZrO 2 also enhanced the stability of the catalyst and reduced the leaching of iron ions. Finally, the reasonable degradation pathway and degradation mechanism were speculated by high performance liquid chromatography-mass spectrometry (HPLC-MS), electron spin resonance technology (ESR), scanning Kelvin probe (SKP), the conduction band (CB) and VB positions of Fe 2 O 3 -on-ZrO 2 , etc. This work exhibited a new structure and degradation mechanism, which would further encourage researchers to study the rational regulation of materials with special morphology and structure.
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JOURNAL OF RAMAN SPECTROSCOPY
·
2022
·Vol. 53
·期 4
·682-693
·
IF 2.727
Hongbin Pu,Haofan Zhu,Fang Xu,Da-Wen Sun
Malachite green (MG) abuse in aquaculture has caused food safety issues and surface-enhanced Raman scattering (SERS) can be utilized to monitor MG residues in aquatic products. However, the sensitivity and accuracy of SERS detection are limited by food matrix interference. Therefore, in this study, SERS active MNP@Au@MIL-100(Fe) substrates were developed by utilizing magnetic nanoparticle (MNP) as the core, which was evenly decorated with Au nanoparticles (AuNPs), and then coated with metal–organic frameworks (MOFs) shell of MIL-100(Fe), which acted as a filter to only allow molecules with appropriate sizes to approach the inner AuNPs, thus avoiding food matrix interference and improving the identification ability to analytes. Experiments in detecting MG residues in prawns was realized with the limit of detection (LOD) of 1.32 × 10 −10 M, showing great potential for its use as a reliable SERS substrate for monitoring food contaminants.
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FOOD CHEMISTRY
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2022
·
IF 9.231
Meng Wang,Jingjing Wang,Kangkang Wang,Liugen Zhang,Xianglei Cao,Cheng Guo,Jide Wang,Bin Wu
More and more attention has been paid to the improved QuEChERS (quick, easy, cheap, effective, rugged and safe) method in dealing complex sample matrices, especially for the study of QuEChERS adsorbents. In this study, a magnetic mesoporous material, which was derived from MIL-88B modified by l -alanine, was synthesized as modified QuEChERS adsorbents for the simultaneous determination of multiple pesticides (Methomyl, Isoprocarb, Carbofuran, 3-Hydroxycarbofuran, Acetamiprid, Imidacloprid) in Chinese cabbage, celery, long bean and leek. The prepared magnetic adsorbents can effectively remove interfering substances from the sample, and the proposed modified QuEChERS method can reduce sample pretreatment time via an external magnetic field. To achieve the best performance of QuEChERS method, the clean-up time and amount of QuEChERS adsorbents were investigated. Under the optimized conditions, a simple, rapid and sensitive method for the determination of 6 pesticide residues in vegetables was established by coupling the modified QuEChERS to ultrahigh-performance liquid chromatography-tandem mass spectrometry. Excellent sensitivity (The limit of detection for the 6 pesticides ranged from 0.001 to 0.020 µg kg −1 ), satisfactory linearity (r 2 ≥ 0.9952), good recovery (73.9–107.7%) and good precision (3.6–16.9% for intraday relative standard deviation, 0.5–15.0% for interday relative standard deviation) were obtained. Compared with traditional QuEChERS method, the proposed method is simple, cost-effective, and efficient, which indicates that the method can be used to detect carbamate and neonicotinoid pesticides in real samples and provide an excellent pretreatment technique for the detection of trace multi-analytes from complex substrates.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 30
·5998-6005
·
IF 6.331
Pan Li,Lixiang Zhang,Sheng Zhang,Chenchen Xu,Yinuo Li,Juan Qu,Shuai Li,Guojiang Mao,Hua Wang
A high-throughput and selective fluorimetric platform has been constructed for the analysis of ammonia in blood by using a polymer-stabilized metal–organic framework (MOF) of porous NH2-MIL-125, which was coated onto a wettable microwells array constructed on an indium tin oxide (ITO) substrate. It was found that the nitrogen plasma treatment for the ITO substrate could create a super-hydrophilic interface that combined with the hydrophobic pattern yielded a wettable microwells array, enabling the condensation-based enrichment of targets from the sample droplets. Moreover, the NH2-MIL-125 MOF encapsulated using polymers could be firmly coated onto the microwells to act as fluorescent probes for sensing NH3 with enhanced responses. In addition, the use of the polymer polyvinyl pyrrolidone could protect and stabilize the crystals of NH2-MIL-125 probe in aqueous media, revealing the improved hydrophilicity and significantly depressed signal background. The as-developed fluorimetric platform, containing a MOF-coated microwells array, can enable the detection of ammonia in blood, with concentrations ranging linearly from 0.10 to 300 μM. More importantly, this plasma treatment-based fabrication route may hold promise for designing different wettable microwells arrays for the high-throughput detection of multiple targets in the fields of biomedical analysis and environmental monitoring.
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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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zhenfei Yang,Longlu Wang,Ming Fang,Xinnian Xia,Yutang Liu
The key to achieve an efficient cooperative photoredox reaction system is to elaborately construct high-efficiency multifunctional photocatalysts with the maximum carrier utilization. Herein, a well-design S-scheme MIL-88B (Fe)/ZIS heterojunction modified with amorphous CoS 1+x cocatalyst (CMZIS) was firstly successfully constructed. The CMZIS heterojunctions show a high H 2 evolution rate of 3164.9 μmol g −1 h −1 coupling with a benzaldehyde generation rate of 3417.8 μmol g −1 h −1 , which are 7.9 and 8.1 times higher than those of pure ZIS. The excellent performance of CMZIS heterojunctions benefits from the synergistic effect of S-Scheme heterojunction and CoS 1+x cocatalysts. This synergy realized the directional transfer and spatial separation of photogenerated carriers in CMZIS, thus inhibiting charge recombination and and maximizing the redox ability of charge carriers. Moreover, CoS 1+x cocatalyst offer more active sites and further enhance the H 2 evolution efficiency. This work will offer fresh insights to the construction and mechanism study of advanced multifunctional photocatalysts for the highly efficient cooperative photoredox reaction system.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Ting Wang,Jie Cheng,Jinmao You,Zhiwei Sun
A selective and rapid high-performance liquid chromatography with fluorescence detection (HPLC-FLD) method for determining fumonisins was established and validated, which based on dispersed microsolid-phase extraction (D-μ-SPE) and precolumn derivatization. The MIL-101 was prepared as sorbents to selectively enrich two fumonisins from feed samples. The obtained extracts were labeled by a novel derivatization reagent 2,5-dioxopyrrolidin-1-yl 4-(1-methyl-1H-phenanthro[9,10-d]imidazol-2-yl)benzoate (MPIBA-Su). There was no fluorescence from fumonisins itself, while their derivatives exhibited considerable fluorescence with a maximum excitation at λex 255 nm and a maximum emission at λem 457 nm. Key factors affecting extraction efficiency and derivatization efficiency were fully optimized. Excellent linearity was achieved with correlation coefficients > 0.9935 under optimal conditions. The detection limits (LODs) were between 2.4 and 3.5 ng·mL −1 , and the quantitation limits (LOQs) were between 8.1 and 11.7 ng·mL −1 . With recoveries in the range of 83.8% − 94.3%, the established method has successfully been applied to the quantitative analysis of fumonisins in feed samples.
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ANALYST
·
2012
·Vol. 137
·期 22
·5411-5419
·
IF 4.23
Xiang-Feng Chen,Hao Zang,Xia Wang,Jian-Guang Cheng,Ru-Song Zhao,Chuan-Ge Cheng,Xiao-Qing Lu
In this paper, the potential applications of metal–organic framework (MOF) materials as fiber coatings for the solid-phase microextraction (SPME) of polycyclic aromatic hydrocarbons (PAHs) in water samples were explored. Fibers coated with MIL-53(Al, Cr, Fe) materials were fabricated by an adhesive method for SPME. The quantitation was performed by gas chromatography–tandem mass spectrometry (GC–MS/MS) using the multiple reaction monitoring mode. Among the three MIL-53(M) coatings, MIL-53(Al) showed the highest extraction efficiency towards PAHs under the current fabrication procedure. Under optimized conditions, the MIL-53(Al)-coated fiber showed good precision (relative standard deviation <12.5%), low detection limits (0.10 ng L−1 to 0.73 ng L−1, S/N = 3), and good linearity (R2 > 0.98) for aqueous solutions containing 16 PAH . The fiber also offered high thermal and chemical stability. The method developed based on MIL-53(Al) SPME–GC–MS/MS was successfully applied in the analysis of real water samples. Based on the simulation results, the PAHs were adsorbed on MIL-53(Al) primarily through the hydrophobic and π–π interactions between PAHs and the organic linker of the material. The results presented in this paper indicate that water-stable MOF materials have great potential for the SPME of aromatic compounds in water samples.
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