MOLECULES
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2022
·Vol. 27
·期 7
·2088
·
IF 4.927
Xue-Li Liu,Yong-Hui Wang,Shu-Yue Ren,Shuang Li,Yu Wang,Dian-Peng Han,Kang Qin,Yuan Peng,Tie Han,Zhi-Xian Gao,Jian-Zhong Cui,Huan-Ying Zhou
The efficient capture of multi-pollutant residues in food is vital for food safety monitoring. In this study, in-situ-fabricated magnetic MIL-53(Al) metal organic frameworks (MOFs), with good magnetic responsiveness, were synthesized and applied for the magnetic solid-phase extraction (MSPE) of chloramphenicol, bisphenol A, estradiol, and diethylstilbestrol. Terephthalic acid (H2BDC) organic ligands were pre-coupled on the surface of amino-Fe3O4composites (H2BDC@Fe3O4). Fe3O4@MIL-53(Al) MOF was fabricated by in-situ hydrothermal polymerization of H2BDC, Al (NO3)3, and H2BDC@Fe3O4. This approach highly increased the stability of the material. The magnetic Fe3O4@MIL-53(Al) MOF-based MSPE was combined with high-performance liquid chromatography-photo diode array detection, to establish a novel sensitive method for analyzing multi-pollutant residues in milk. This method showed good linear correlations, in the range of 0.05–5.00 μg/mL, with good reproducibility. The limit of detection was 0.004–0.108 μg/mL. The presented method was verified using a milk sample, spiked with four pollutants, which enabled high-throughput detection and the accuracies of 88.17–107.58% confirmed its applicability, in real sample analysis.Keywords:magnetic metal organic framework (MMOFs);magnetic solid-phase extraction (MSPE);multi-pollutants;high-performance liquid chromatography (HPLC)
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 36
·17438-17455
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IF 3.925
Qingcan Xiang,Zongxue Yu,Xuyang Li,Pingquan Wang,Niandan He,Yao Pang,Qiuxiang Wang,Yucheng Liu
A g-C3N4/NH2-MIL-88B(Fe)/CD@GO membrane (M2) was prepared by a simple vacuum filtration method. By embedding a Z-scheme heterojunction composite photocatalyst into graphene oxide (GO) nanosheets, not only can the water molecule transport channel be regulated, but the membrane can also be endowed with photocatalytic activity and membrane fouling is effectively alleviated. The pure water permeation flux of M2 (253.26 L m−2 h−1 bar−1) was 13 times that of the original GO membrane (18.83 L m−2 h−1 bar−1). What's more, even after 10 cycles, M2 still maintains excellent separation efficiency and flux. After six cycles, the rejection of Congo Red (CR), Malachite Green (MG) and Rhodamine B (RhB) by M2 was over 95%. At the same time, under the conditions of an extreme pH value and high salt concentration, the rejection of dye remained at the original level after six cycles. Therefore, the novel photocatalytic membrane has excellent separation performance, stability and photocatalytic activity, and can be used as a potential membrane for wastewater purification and environmental protection.
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
·
2022
·
IF 9.463
Huidong Zhao,Bihe Yuan,Yuanyuan Zhan,Fangzhou Yang,Juanjuan Zhou,Congrui Qi,Chunying Lei,Yaoqiang Li
The combustion of polystyrene (PS) releases enormous amounts of toxic fumes and heat, which seriously affects human health and property safety. This research firstly proposes an efficiently feasible surgery to prepare a porous metal–organic framework (P-Fe-MOF) with macroporous based on the microporous MIL-53 and then uses its excellent porous structure to adsorb triethyl phosphate (TEP) as a flame retardant for PS to reduce its fire hazard. Scanning electron microscope images reveal that P-Fe-MOF has a distinct macroporous structure compared with original metal–organic framework (MOF). X-ray photoelectron spectra indicate that TEP has been successfully adsorbed into P-Fe-MOF. The combustion performance of PS composites is analyzed and the results suggest that the prepared PS composite has better flame-retardant performance than pure PS. This research presents a convenient method to fabricating a novel macroporous MOF , which provides a valuable enlightenment for broadening the application field of MOF and improving the comprehensive properties of polymers.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhe Zhao,Wuming Xie,Zijun Huang,Haiming Cai,Yuemeng Ji,Baocong Zhao
The antibiotic florfenicol (FF) discharged into the aquatic environment may cause serious water pollution. Therefore, an effective way to eliminate FF antibiotics from the water bodies should be proposed. Herein, MIL-53(Al)-supported nano zero-valent iron (NZVI@MIL-53(Al)) was synthesized and applied to activate hydrogen peroxide (H 2 O 2 ) to spark the Fenton reaction for FF antibiotics removal. The characterization results demonstrated the successful loading and good dispersion of NZVI onto MIL-53(Al). 100 % FF antibiotics degradation could be achieved under the optimal reaction conditions, including an initial FF antibiotics concentration of 20 mg L −1 , initial solution pH of 3.0, NZVI@MIL-53(Al) dose of 25 mg L −1 , and H 2 O 2 concentration of 0.2 mM. And after four cycles, the FF antibiotic degradation efficiency was still 81.18 %. The lowest tolerance for HCO 3 − was observed while the degradation activity was maintained at the presence of Cl − and HA. EPR measurement and free radical quenching experiment showed that ·OH was the main reactive specie in the NZVI@MIL-53(Al)/H 2 O 2 system. FF antibiotics degradation involved hydroxylation reactions (electrophilic substitution), dehalogenation, hydrolysis, and cleavage based on the UPLC-MS/MS analysis and DFT calculation. Noteworthy, 0.247 mg L −1 of F − and 1.2 mg L −1 of Cl − were detected in the solution after the reaction due to the breakage of the stable C–Cl bond and C–F bond. Finally, this work revealed that the NZVI@MIL-53(Al), with high stability and recyclability, could be a potential heterogeneous catalyst for treating antibiotic wastewater.
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CHEMOSPHERE
·
2021
·
IF 7.086
Peipei Huang,Lili Yao,Qing Chang,Yunhan Sha,Guodong Jiang,Shenghua Zhang,Zhe Li
The slow redox rate of Fe(III)/Fe(II) couples is a rate-limiting step for Fenton-like performance of Fe-MOFs. In this study, a series of catalysts (MIL-101) with various p-phthalic acid/2-aminoterephthalic acid (H 2 BDC/NH 2 –H 2 BDC) molar ratios were prepared using a simple and mild chemical method and applied for catalyzed degradation of bisphenol A (BPA). Interestingly, the –NH 2 modified MIL-101(Fe) can adjust Fe-Oxo node by increasing the electron density of Fe(III) in the presence of –NH 2 group with high electron density, thus forming Fe(II) in situ in MOFs. Meanwhile, the –NH 2 groups used as electron-donors can promote electron transfer , resulting in faster Fe(III)→Fe(II) half-reaction and active H 2 O 2 to continuously generate •OH radical. The BPA degradation and rate constant of Fe-BDC-NH 2 /H 2 O 2 system are 15.4-fold and 86.8-fold higher than that of Fe-BDC/H 2 O 2 system, respectively. The density functional theory (DFT) calculations showed that Fe-BDC-NH 2 possesses higher Fermi level energy (−4.88 eV) and lower activation energy barriers (0.32 eV) compared with Fe-BDC. Moreover, Fe-BDC-NH 2 showed good reusability and stability. This work offers a highly efficient and stable MOFs-based Fenton-like catalyst to rapidly degrade organic pollutants over a wide pH range for potential applications in wastewater treatment .
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Baitong Niu,Biying Yao,Meihua Zhu,Hongxu Guo,Shaoming Ying,Zhangxu Chen
A fern leave-like structure metal-organic frameworks (MOFs), MIL-47(as) has been fabricated by a simple one-pot hydrothermal reaction and characterized by a variety of means, such as X-ray diffraction, Fourier transform infrared spectroscopy, micro-morphology analysis, X-ray photoelectron spectroscopy and specific surface area and pore size distribution. The as-prepared MOFs were found to be an effective material for the selective electrochemical detection of microgram levels of Pb(II), Cu(II) and Hg(II) in aqueous solution performed by differential pulse voltammetry. The electrochemical properties and applications of the modified electrode were also studied, in which operational parameters such as pH, deposition potential, and deposition time, were optimized to detect trace amounts of Pb(II), Cu(II) and Hg(II) ions. The as-prepared electrode not only has good stability and repeatability, but also has good practical detection ability.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Heng Mao,Shen-Hui Li,Ao-Shuai Zhang,Li-Hao Xu,Heng-Xing Lu,Jing Lv,Zhi-Ping Zhao
Furfural is a typical biomass-derived platform chemical. Conventional processes for furfural production are uneconomical and energy-intensive because only about 3–6 wt% of furfural in the hydrolysate needs to be separated. In this study, a series of mixed matrix membranes (MMMs) were prepared by incorporating MIL-53(Al) particles (MAPs) into poly (ether-block-amide) (PEBA 2533) matrix for pervaporation separation of furfural from aqueous solutions. The MAPs with anisotropic morphology and tunable particle size were precisely synthesized by a high-efficiency solvent-controlled microwave synthetic strategy. Effects of MAPs on the microstructures, physicochemical properties of MAPs/PEBA MMMs were investigated in detail through SEM, EDS, XRD, FTIR, TGA, N 2 adsorption and contact angle measurements. The experimental results suggested that compared with the PEBA control membrane, the addition of MAPs notably reduced the permeation energy barrier for furfural, but not for water. The coin-like MAPs-16.7 filled MMMs presented the optimal separation performance, which exceeded other furfural-permselective membranes. Impressively, a high total flux of 3800 g∙m −2 ∙h −1 and an adequate furfural/water separation factor of 50.2 was achieved in PV separation of 1 wt% furfural aqueous solution at 80 °C, which could substantially reduce capital investment and equipment footprint. Furthermore, a continuous testing was operated for 200 h in ternary furfural/acetic acid/water simulated hydrolysate, highlighting the long-term membrane stability in realistic applications. High performance and long-term stability made MAPs/PEBA MMMs potential candidates for industrial furfural production.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Zhoujun He,Ruowen Liang,Chen Zhou,Guiyang Yan,Ling Wu
Industrial sewage often contain metal ions and dyes, and it is difficult to efficiently remove them simultaneously. In this work, novel ternary MIL-53(Fe)/carbon quantum dots/noble metal (MIL-53(Fe)/CQDs/MNPs, MNPs = Ag, Pd, Au) nanocomposites have been rationally constructed and successfully fabricated by a facile two-step strategy with self-assembling and in-situ photoreduction. The resulting MIL-53(Fe)/CQDs/2%Au composite exhibits excellent photoactivity for the Cr(VI) reduction, the reduction ratio is nearly 100% after 20 min of visible light illumination. The rate constant of MIL-53(Fe)/CQDs/2%Au is calculated to be 0.1820 min −1 , which is around 7.4, 2.76, 1.77 and 1.47 times higher than that of as-prepared MIL-53(Fe), MIL-53(Fe)/CQDs, MIL-53(Fe)/CQDs/2%Ag and MIL-53(Fe)/CQDs/2%Pd, respectively. More significantly, MIL-53(Fe)/CQDs/2%Au nanocomposite has been proven to serve as bifunctional photocatalyst for simultaneously removing Cr(VI)/dye mixed system pollutants. The superior photoactivity may be due to the enhanced light absorption intensity, the superior electrical conductivity of Au and CQDs, as well as surface plasmon resonance (SPR) effect of Au. In particular, the possible photocatalytic reaction mechanism has been carefully investigated and proposed.
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ACS Omega
·
2020
·
IF 2.87
Jia Wang,Yansong Liu,Xiuyan Guo,Hongqiang Qu,Ran Chang,Jing Ma
Metal–organic frameworks (MOFs) exhibit highly designable properties and have been used in wide applications. To further improve their performance, the modification of MOFs is an effective method. However, the modification process is usually complicated. Besides, the sustainable use of MOFs is difficult to achieve due to the complicated recycling treatment. Herein, we designed a polyethyleneimine (PEI)-modified NH2-MIL-101(Al) composite (PEI@NH2-MIL-101(Al)). This composite showed excellent dye removal performance of methyl orange (MO, 89.4%) and Direct Red 80 (DR80, 99.8%). Remarkably, the dye removal application of PEI@NH2-MIL-101(Al) also acted as a modification process toward flame retardant application. Thus, the dye-adsorbed PEI@NH2-MIL-101(Al) composite (MO-PEI@NH2-MIL-101(Al) and DR80-PEI@NH2-MIL-101(Al)) was sustainably used as an effective flame retardant for an epoxy resin (EP) at low additions (4.0 wt %). The limiting oxygen values of EP/MO-PEI@NH2-MIL-101(Al) and EP/DR80-PEI@NH2-MIL-101(Al) increased to 26.5 and 26.7%, respectively. The heat release and the smoke production of dyes-PEI@NH2-MIL-101(Al)/EP were greatly reduced compared with those of EP. This strategy provides a simple and effective modification method for MOFs. Meanwhile, the modified MOF composite can achieve sustainable application, giving full play to the advantages of MOFs.
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OPTICAL MATERIALS
·
2020
·
IF 2.779
Lanqing Ling,Yu Tu,Xuanyu Long,Qianwen Li,Jiabao Gu,Nan Liu,Zequan Li
The emission of organic dye wastewater poses a great threat to the ecological environment. Therefore, it is necessary to prepare environment-friendly photocatalytic materials with high photocatalytic performance to degrade organic dyes. In this work, a new composite photocatalyst SnS 2 /NH 2 -MIL-125 (Ti) was formed by loading the multiphase SnS 2 of quantum dots (QDs) and hexagonal nanodiscs (NDs) on the NH 2 -MIL-125 (Ti) through one-step hydrothermal method , then used it to remove 40 mg/L Rhodamine B (RhB) under visible light . Compared with SnS 2 and NH 2 -MIL-125 (Ti), the photocatalytic degradation activity of the 12 wt% SnS 2 /NH 2 -MIL-125 (Ti) was enhanced by 2.4 and 2.1 times respectively, reaching 90.5%, after 80 min of visible light irradiation. The four times recycling test shows that this photocatalyst has outstanding stability and durability. Through analysis, NH 2 -MIL-125 (Ti) modified SnS 2 can improve visible light absorption, provide more active sites and inhibit photoelectron-hole recombination, thus enhancing photocatalytic activity . Superoxide radical (•O 2 − ) and hole (h + ) were determined to be the key active substances in the process by the reaction substance capture experiment. The photodegradation mechanism of RhB is also investigated and studied in detail. This novel multiphase SnS 2 /NH 2 -MIL-125 (Ti) material provides a new perspective for the design of organic-inorganic composite photocatalysts with excellent performance and improved stability, and has potential application in environmental purification.
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TALANTA
·
2020
·
IF 5.339
Yanxiao Jiang,Bo Zhang,Jingkang Li,Ying Sun,Xinghua Wang,Pinyi Ma,Daqian Song
A novel vortex-assisted solid-phase extraction method based on MIL-68(Al)/Chitosan-melamine sponge column (or V-MIL-68(Al)/CS-SC-SPE) is presented in this paper. The MIL-68(Al)/Chitosan-sponge column was prepared by a simple infiltration method and a preparation process that does not consume organic solvents. Scanning electron microscopy was used to characterize the functionalized sponge columns, and the skeleton and pores of the melamine sponge were successfully modified with the coating material (MIL-68(Al) and chitosan). Chitosan was used successfully not only as an adsorption adjuvant material, but also as an adhesive in the preparation of MIL-68(Al)/CS coating sponge materials. The presented method was further combined with high performance liquid chromatography (HPLC) and used in the determination of trace parabens (including methyl-, ethyl-, propyl- and butyl-parabens) in environmental water samples. Several important factors that affect the extraction performance were investigated. Under the optimum conditions, the method was successfully used to detect the four kinds of parabens in different water samples (domestic water, lake water and river water). The limits of detection ranged between 0.21 and 0.50 ng/mL, and the relative standard deviations for all parabens were below 10.8%.
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Nano Research
·
2020
·Vol. 14
·期 7
·2383-2389
·
IF 8.183
Zhang Yuwei,Liu Fei,Yang Zhichao,Qian Jieshu,Pan Bingcai
In the pursuit of heterogeneous catalysts with high reactivity, metal organic framework (MOF) nanomaterials have received tremendous attentions. However, many MOF catalysts especially Fe-based MOFs need to be utilized immediately after synthesis or being activated using high temperature, because of the easy loss of reactivity in humid environments resulting from the occupation of active Fe sites by water molecules. Here, we describe an inspiring strategy of growing MIL-101-Fe nanoparticles inside the three-dimensional confined space of graphene aerogel (GA), generating shapeable GA/MIL-101-Fe nanocomposite convenient for practical use. Compared to MIL-101-Fe, GA/MIL-101-Fe as catalyst demonstrates much higher reactivity in Fenton-like reaction, attributing to smaller MIL-101-Fe particle size, presence of active Fe(II) sites, and abundant defects in GA. Strikingly, the weakly hydrophobic nature of the composite greatly inhibits the loss of catalytic reactivity after being stored in humid air and accelerates the recovery of reactivity in mild temperature, by resisting the entrance of water molecules and helping to exclude water molecules. This work demonstrates that a delicate design of nanocomposite structure could not only improve the reactivity of the catalytic component, but also overcome its intrinsic drawback by taking advantage of the properties of host. We hope this functional nanoconfinement strategy could be extended to more scenarios in other fields.
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