CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Zhen Zhong,Min Li,Jinghao Fu,Yuexin Wang,Yaseen Muhammad,Sihan Li,Jiaxing Wang,Zhongxing Zhao,Zhenxia Zhao
Cu 2 O/MIL(Fe/Cu) composite was fabricated via an in-situ Cu-bridging strategy to enhance interfacial synergistic effect of photo-Fenton catalysis for thiacloprid (TCL) degradation. Characterization results showed that: (1) Cu 2 O was proved to grow on the surface of MIL(Fe/Cu) in Cu 2 O/MIL(Fe/Cu) composite and display a high BET surface area of 1553 m 2 /g; (2) Cu 2 O/MIL(Fe/Cu) reduced band gap from 2.5 to 1.3 eV and extended absorption from UV to visible region; (3) Cu-bridge was proved to promote the intimate interface between Cu 2 O and MIL(Fe/Cu), which accelerated charge transferred and shortened the binding gap and the reaction pathway from photo-induced electrons to Fenton-generated radicals. As a result, this boosted the redox reaction of Fe 2+ /Fe 3+ and promoted the reversible degree of this catalytic redox ability of MIL(Fe). Catalytic performance exhibited that (1) Cu 2 O/MIL(Fe/Cu) showed a fast kinetics (2–40 times faster than the state-of-the-art catalysts) and ultra-high mineralization (82.3% within 80 min) for TCL degradation; (2) Cu 2 O/MIL(Fe/Cu) showed a promising cycling stability due to improved charge transfer ability that could protect Cu 2 O from photo-corrosion during photo-Fenton reaction; (3) The catalytic performance of Cu 2 O/MIL(Fe/Cu) was characterized and seven photocatalytic intermediates were identified by both HPLC/MS and Surface Enhanced Raman Spectroscopy. The cyanoimino group in TCL was proved for the first time to be attacked primarily. Moreover, among all the detected intermediates, thiazolidin-2-amine (P6) was found to be the most stable intermediate to be degraded, and it can directly influence the TOC determination during photodegradation process.
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CRYSTENGCOMM
·
2019
·Vol. 21
·期 38
·5824-5833
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IF 3.382
Ji-Min Yang,Run-Zhi Zhang,Ying-Yan Liu
We herein report that the adsorption driving forces (i.e., electrostatic interactions, hydrogen bonding, and π–π interactions) of MIL-101-COOH microcrystals toward dyes can be tuned by varying the molar ratio of H2BDC : H2BDC–COOH in the reaction system. More specifically, the adsorption capacities of MIL-101-COOH-1 were determined to be 2835.7 (Congo red, CR), 473.9 (methyl orange, MO), and 240.8 (acid chrome blue K, AC) mg g−1, exceeding those reported for pristine MIL-101 by 107.5, 16.7, and −25.8%, respectively. The above-mentioned adsorption behavior was rationalized based on the dye molecular structure, zeta potential, BET surface area and dye adsorption investigations, which revealed that free –COOH groups increase the electrostatic and hydrogen bonding interactions between the adsorbent and linear dyes, thereby improving the adsorption capacity for linear anionic dyes and overriding the effect of pore volume, whereas an increased steric hindrance effect between the adsorbent and a nonlinear dye decreases the adsorption capacity for the nonlinear anionic dye and overrides the effects of the electrostatic and hydrogen bonding interactions. The adsorption capacity of MIL-101-COOH-1 toward the anionic organic dyes (CR, MO, and AC) was found to be significantly higher than those of the other MIL-101-COOH adsorbents examined herein. The adsorption capacity of MIL-101-COOH is determined by the synergetic interplay between the electrostatic, hydrogen bonding, and π–π interactions, steric hindrance effect, and pore volume of the adsorbent. The results shed light on the adsorption mechanism of metal–organic frameworks toward organic dyes.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Wanlin Qin,Lufang He,Yuchi Zhang,Bohan Li,Le Han,Yan Xu
Construction of heterocompositional hybrid metal–organic frameworks (MOFs) by integration of more than two MOFs is a smart strategy for fine-tuning MOF properties. In this work, a novel yolk-shell MIL-88A@NiFe-PB heterostructure, in which MIL stands for Materials from Institute Lavoisier, and PB represents the coordination network of Prussian Blue, was fabricated through a fast wrapping and then inward-etching growth synthetic strategy under mild stirring condition. The thickness of the outmost layer of NiFe-PB and the internal core structure of MIL-88A can be controlled by tuning the concentration of K 4 [Fe(CN) 6 ]·3H 2 O in the assembly system. A rational growth mechanism for the yolk-shell MIL-88A@NiFe-PB heterostructure was proposed. The as-prepared yolk-shell MIL-88A@Ni 10 Fe PB-50 architectures were then explored for non-enzymatic glucose sensing. The results show that the designed glucose sensor exhibits a high sensitivity of 1963.2 μA mM −1 cm −2 over a wide linear range of 0.005–1.0 mM, a low detection limit (0.12 μM), as well as a fast reaction time (<2 s) and long-term stability for non-enzymatic glucose detection. Also, it shows good applicability in real serum samples. This work provides a “wrapping-inward-etching” synthetic strategy for construction of hybrid MOFs with exceptional outstanding non-enzymatic glucose sensing performance, providing a reasonable guide for construction of other MOF on MOF intriguing structures for electrochemical sensing applications.
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JOURNAL OF SOLID STATE CHEMISTRY
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2023
·
IF 3.3
Rui Zhao,Cheng Cheng,Xiurong Wu,Xueyan Bai,Fenghuan Wang
Due to the excellent pore structure , MOFs as the stationary phase was playing an important part in chromatography . In this work, the shell-core MIL-101(Al)@SiO 2 composites post-synthetic modified by ligands with different polarities were fabricated for separation of estrogens. The structure and morphology of these materials were characterized by X-ray diffraction (XRD), Fourier transform infrared spectrum (FTIR), scanning electron microscope (SEM) and Brunauer-Emmett-Teller (BET). In order to investigate the influence of the ligand polarity on chromatographic separation performance of estrogens, alkyl molecules with different chain length were introduced as the ligands. With the hydrophobicity and chain length of the ligands increasing, the resolutions of the MIL-101(Al)@SiO 2 columns for the separation of estrogens exhibited the tendency of a parabola. Best result was achieved on the C4-MIL-101(Al)@SiO 2 column. On that basis, the possible retention mechanism on C4-MIL-101(Al)@SiO 2 column was elucidated by studying the mobile phase effect on separation behavior.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Kunpeng Liu,Nan Wang,Jianhua Li,Fanglin Du,Baorong Hou,Ruiyong Zhang
Electrochemical two-electron water oxidation reaction (2e − WOR) to produce H 2 O 2 has been widely concerned. However, four-electron competition reaction causes the large overpotential and low production rates of 2e − WOR, which restrict its’ development and application. Herein, we prepared N-TiO 2 derived from NH 2 -MIL-125 by the hydrothermal combined with calcination method. We found that N-TiO 2 as photoanode exhibited the well properties of photoelectrocatalysis water oxidation, which gave an overpotential of 630 mV at 1 mA cm −2 . The overpotentials of N-TiO 2 was approximately 130 mV (at 1 mA cm −2 ) lower than NH 2 -MIL-125, and even lower than the previous reported TiO 2 , which may attribute to the increased oxygen vacancy with the calcination process and N doping. In addition, we investigated the degradation performance of the prepared catalysts to degrade methylene blue by photoelctrocatalysis on-site the preparation of H 2 O 2 . It was shown that N-TiO 2 performed high degradation efficiency (∼91%) and excellent stability. The possible mechanism was speculated due to the increased oxygen vacancy and N doping. This work provides a new idea for photoelectrocatalysis water oxidation materials and points out a new way for on-site H 2 O 2 production for direct use.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2023
·Vol. 24
·期 14
·11480
·
IF 5.6
Wei Mao,Jiawen Hao,Lingyu Zeng,Hao Wang,Hao Xu,Jinghong Zhou
Herein, we report the synthesis of bimetal–organic frameworks (BMOFs) with both Brønsted and Lewis acidities, in which phosphotungstic acid (PTA) was encapsulated in BMOFs. It is efficient in converting starch to 5-hydroxymethyl-furfural (HMF) in deep eutectic solvents (DESs) such as choline chloride and formic acid. The highest yield of HMF (37.94%) was obtained using P0.5/BMOFs1.0to catalyze starch in a mixed solvent system comprising DESs and ethyl acetate (EAC) (v/v; 2:3) at 180 °C and a reaction time of 10 min. Employing a DES as a cocatalyst and solvent reduced the use of organic solvents. The catalyst showed adequate reusability, and the HMF yield only decreased by 2.88% after six cycles of reuse compared with that of the initial catalyst. This study demonstrates the application potential of BMOFs in the conversion of biomass to useful molecules with commercial and/or research value.Keywords:bimetal–organic frameworks;phosphotungstic acid;loading;cassava starch;catalysis
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高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Chunyan Hu,Jinke He,Jianjun Liang,Tao Lin,Qiuliang Liu
A novel photo-Fenton catalyst α-Fe 2 O 3 @g-C 3 N 4 @NH 2 -MIL-101(Fe) (FGN) with dual Z-scheme heterojunction was successfully prepared by hydrothermal method to degrade tetracycline (TC). The preparation conditions were optimized by orthogonal test, and the successful synthesis was confirmed by characterization analyses. The prepared FGN showed better light absorption performance, higher photoelectrons-holes separation efficiency, lower photoelectrons transfer resistance, and higher specific surface area and pore capacity compared with α-Fe 2 O 3 @g-C 3 N 4 and α-Fe 2 O 3 . The effects of experimental conditions on the catalytic degradation of TC were investigated. The degradation rate of 10 mg/L TC could reach 98.33% within 2 h when the dosage of FGN was 200 mg/L, and the degradation rate could remain 92.27% after 5 times of reuse. Furthermore, the XRD spectra and XPS spectra of FGN before and after reuse were compared to explore the structural stability and catalytic active sites of FGN, respectively. According to the identification of oxidation intermediates, three degradation pathways of TC were proposed. Through H 2 O 2 consumption experiment, radical-scavenging experiments, EPR results, the mechanism of the dual Z-scheme heterojunction was proved. The improved performance of FGN was attributed to the dual Z-Scheme heterojunction effectively promoting the separation of photogenerated electrons from the holes and accelerating the electrons transfer , and the increase of the specific surface area.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Dianfa Zhao,Jie Liu,Yunshan Zhou,Lijuan Zhang,Yuxu Zhong,Yang Yang,Baoquan Zhao,Mengru Yang,Yong’an Wang
It is very important to establish a sustained-release pralidoxime chloride (2-PAM) drug system with brain targeting function for the treatment of neurotoxicant poisoning. Herein, Vitamin B1 (VB1), also known as thiamine, which can specifically bind to the thiamine transporter on the surface of the blood–brain barrier, was incorporated onto the surface of MIL-101-NH2(Fe) nanoparticles with a size of ∼100 nm. Pralidoxime chloride was further loaded within the interior of the above resulted composite by soaking, and a resulting composite drug (denoted as 2-PAM@VB1-MIL-101-NH2(Fe)) with a loading capacity of 14.8% (wt) was obtained. The results showed that the drug release rate of the composite drug was increased in PBS solution with the increase of pH (2–7.4) and a maximum drug release rate of 77.5% at pH 4. Experiments on the treatment of poisoning by gavage with the nerve agent sarin in mice combined with atropine revealed that sustained release of 2-PAM from the composite drug was achieved for more than 72 h. Sustained and stable reactivation of poisoned acetylcholinesterase (AChE) was observed with an enzyme reactivation rate of 42.7% in the ocular blood samples at 72 h. By using both zebrafish brain and mouse brain as models, we found that the composite drug could effectively cross the blood–brain barrier and restore the AChE activity in the brain of poisoned mice. The composite drug is expected to be a stable therapeutic drug with brain targeting and prolonged drug release properties for nerve agent intoxication in the middle and late stages of treatment.
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RSC Advances
·
2019
·Vol. 9
·期 41
·23711-23717
·
IF 3.049
Shu-Hui Huo,Chen-Xu Liu,Peng-Xin Zhou,Jing Yu,Lei Bai,Zhen-Gang Han,Xiao-Quan Lu
Development of novel porous materials for efficient adsorption and removal of environmental pollutants from aqueous solution is of great importance and interest in environmental science and chemistry. Herein, we reported a facile synthesis of recyclable magnetic carbonaceous porous composite derived from iron-based metal–organic framework MIL-100(Fe) for superior adsorption and removal of malachite green (MG) from aqueous solution. Because of large surface area and high porosity, the synthesized magnetic carbonaceous porous material presented a superior adsorption capacity of 2090 mg g−1 for MG. The adsorption of MG on magnetic carbonaceous porous composite is endothermic and spontaneous. The prepared magnetic carbonaceous porous composite could be separated easily and rapidly from the solution matrix by an external magnet. The rapid adsorption, large adsorption capacity and good reusability make it attractive for practical use in the adsorption and removal of dyes from aqueous solutions.
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Analytical Methods
·
2019
·Vol. 11
·期 27
·3467-3473
·
IF 2.378
Zhiyang Lv,Cheng Yang,Yuehong Pang,Weiying Xie,Xiaofang Shen
Dispersive solid phase extraction (d-SPE) is a preponderant methodology featuring direct contact and interaction between adsorbents and analytes. Herein, we used the porous metal–organic framework (MOF) MIL-101(Cr) as a d-SPE adsorbent for pretreatment of edible oil samples and determination of benzo[a]pyrene (BaP). The samples after treatment are applied to determination by high performance liquid chromatography coupled with a fluorescence detector (HPLC-FLD). We optimized the type and dosage of the MOF, diluent and eluent. Under the optimized conditions, this method gave a linear calibration curve for the determination of BaP in the range of 1–30 ng mL−1 (R2 = 0.9958) and the relative standard deviation (RSD) ranged from 1.07 to 8.14% (n = 6). The limit of detection was 0.19 ng mL−1 (S/N = 3) and the recoveries from different types of spiked oil samples were between 88.8 and 118.8%. Compared with conventional methods, the MOF-based d-SPE reduces organic solvent consumption and simplifies operation, which provides potential for application in extraction of hydrophobic targets from oil complexes.
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JOURNAL OF SEPARATION SCIENCE
·
2018
·Vol. 41
·期 9
·2046-2055
·
IF 2.415
Yulan Deng,Ruiqi Zhang,Di Li,Peng Sun,Ping Su,Yi Yang
Here, we describe a simple one-pot solvothermal method for synthesizing MIL-101(Fe)@polydopamine@Fe 3 O 4 composites from polydopamine-modified Fe 3 O 4 particles. The composite was used as a magnetic adsorbent to rapidly extract sulfonylurea herbicides. The herbicides were then analyzed by high-performance liquid chromatography. The best possible extraction efficiencies were achieved by optimizing the most important extraction parameters, including desorption conditions, extraction time, adsorbent dose, salt concentration, and the pH of the solution. Good linearity was found (correlation coefficients >0.9991) over the herbicide concentration range 1–150 μg/L using the optimal conditions. The limits of detection (the concentrations giving signal/noise ratios of 3) were low, at 0.12–0.34 μg/L, and repeatability was good (the relative standard deviations were <4.8%, n = 6). The method was used successfully to determine four sulfonylurea herbicides in environmental water and vegetable samples, giving satisfactory recoveries of 87.1–108.9%. The extraction efficiency achieved using MIL-101(Fe)@polydopamine@Fe 3 O 4 was compared with the extraction efficiencies achieved using other magnetic composites (polydopamine@Fe 3 O 4 , Hong Kong University of Science and Technology (HKUST)-1@polydopamine@Fe 3 O 4 , and MIL-100(Fe)@polydopamine@Fe 3 O 4 ). The results showed that the magnetic MIL-101(Fe)@polydopamine@Fe 3 O 4 composites have great potential for the extraction of trace sulfonylurea herbicides from various sample types.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2018
·
IF 2.829
Mingjuan Han,Ying Li,Zheng Gu,Huali Shi,Chong Chen,Qiang Wang,Hui Wan,Guofeng Guan
A novel functionalized MOF heterogeneous catalyst (MIL-101(Cr) @MBIAILs), 2-Mercaptobenzimidazole ILs with electron-rich SH groups immobilized onto the surface of the well-defined MIL-101(Cr) frameworks, was constructed and fabricated by the S Cr coordination bond on the basis of the facile post-synthetic modification strategy. The heterogeneous catalyst was measured by XRD , FTIR, SEM, TEM , TGA , EA and N 2 adsorption–desorption, and the catalytic behavior of the catalyst was assessed by the esterification about oleic acid and methanol as a model reaction. The results showed that MBIAILs have been successfully immobilized onto the surface of MIL-101(Cr) frameworks by S Cr coordinate bonds. More importantly, the conversion of oleic acid just decreased from 91.0% to 82.1% when the catalyst had been reused six times. This exhibited the prepared catalyst had superior catalytic behavior and excellent reusability.
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