ANALYTICA CHIMICA ACTA
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2021
·
IF 6.558
Tiantian Si,Shuai Wang,Haixia Zhang,Xiaofeng Lu,Licheng Wang,Xiaojing Liang,Yong Guo
The preparation of the metal-organic frameworks (MOFs)@silica core-shell microspheres as the stationary phases mainly relied on the method of electrostatic interaction between the metal ions of MOFs and the silanol groups. Herein, the ligands of MOFs were preferentially modified to the surface of silica as connection points and seed crystals to connect or form the MOFs. In this way, the evenness of the MOFs particles on the silica surface was effectively improved, and the prepared composites possessed excellent reproducibility and stability, including acid-base stability. The relative standard deviation of the retention time for repeatability ranged from 0.1% to 0.26% and for stability retention time from 0.3% to 0.6%. Compared with commercial columns, the prepared stationary phase showed enhanced separation selectivity for separation of both hydrophilic and hydrophobic compounds containing alkaloids, nucleosides , antibiotics and alkylbenzenes , etc. The obtained column was used as a matrix for fast separation and analysis of antibiotics in actual samples. In short, the composites showed superior reproducibility, stability and satisfactory separation performance towards a variety of compounds in the studied conditions. It also provided another way to improve the evenness of MOFs particles on the surface of silica and enhance the stability of them under polar conditions.
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高影响因子
JOURNAL OF MATERIALS RESEARCH
·
2021
·Vol. 36
·期 14
·2961-2972
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IF 3.089
Zhu Lijun,Zhu Xinxin,Zhang Chao,Huo Tian,Hou Xinlan,Guo Dandan,Zhang Huiming,Xia Daohong
The zirconium-based porphyrin MOFs sensitized TiO 2 (PCN224–TiO 2 ) was synthesized in situ by self-assembly of porphyrin, ZrCl 4 with nano TiO 2 . The composite catalyst was determined by detailed structural and photoelectrochemical characterization. The UV–Vis absorption and fluorescence spectrum confirm that PCN224 and TiO 2 are coupled. The PCN224–TiO 2 had significant absorption of visible light and the PCN224–TiO 2 had the largest photo-generated current, which proved the porphyrin MOFs material has good internal conductivity and has a close combination with TiO 2 . Compared with carboxyphenyl porphyrin sensitized TiO 2 (HTCPP–TiO 2 ), mixture of TCPP and TiO 2 (TCPP/TiO 2 ) and PCN224, the PCN224–TiO 2 showed better removal performance of methylene blue under visible light. Under low-power xenon lamp irradiation, the removal rate of PCN224–TiO 2 (1:3) on methylene blue reached 93.2% in 4 h. And PCN224–TiO 2 had stable cycling catalytic performance. The PCN224–TiO 2 promoted the degradation process by strengthening the adsorption of organic pollutants, thus improving the removal performance. Graphic abstract
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TALANTA
·
2018
·
IF 4.244
Nuanfei Zhu,Yanmin Zou,Menglu Huang,Shuaibing Dong,Xiangyang Wu,Guoxi Liang,Zhixiang Han,Zhen Zhang
A sensitive and artful colorimetric immunosensor based on horseradish peroxidase (HRP) was designed by labelling metal–organic frameworks (Cu-MOFs) on the second antibody (Cu-MOFs@Ab 2 ) as signal amplification for the detection of trace dibutyl phthalate (DBP). In this system, when Cu-MOFs@Ab 2 was captured by antigen- primary antibody (Ab 1 ) complex, tremendous Cu(II) will be released from Cu-MOFs in the presence of nitric acid (HNO 3 ), and Cu(II) will be further reduced to Cu(I) after the addition of sodium ascorbate (SA), consequently, inhibiting the HRP to catalyse the colorless 3,3′,5,5′-tetramethylbenzidine (TMB) into blue oxidized TMB (ox TMB). Under the optimized conditions, the limit of detection (LOD) was 1 μg L −1 , which was almost 60 times lower than that using a conventional ELISA with the same antibody. In addition, our method showed good accuracy and reproducibility (recoveries of 87.73–103.4%; CV values of 1.46–5.95%) through a spike-recovery analysis. The proposed immunosensor indicated great potential for trace DBP determination from environmental and food samples.
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DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 32
·11253-11263
·
IF 4.099
Yana Liu,Cheng Zhang,Chen Xu,Caixue Lin,Keke Sun,Jie Wang,Xueli Chen,Ling Li,Andrew K. Whittaker,Hai-Bing Xu
Using a facile one-step hydrothermal method, a series of metal–organic frameworks containing Gd/Tm (Gd/Tm-MOFs) were prepared successfully. Through the mutual activation of Gd3+ and Tm3+, Gd/Tm-MOFs showed unexpected excellent up-conversion luminescence (UCL) and a superior positive magnetic resonance image (MRI). Using doxorubicin hydrochloride (DOX) as a drug model, the feasibility of Gd/Tm-MOFs as a multifunctional drug carrier was demonstrated. Through modifying Gd/Tm-MOFs with uniform mesoporous silica (mSiO2) shells and folic acid (FA), the drug loading was improved up to 41.5 mg g−1, and pH responsive drug release increased to 64% from 12% by regulating the pH from 5.8 to 7.4. Also, the particles were tracked by MRI, and the second highest longitudinal relaxivity (r1) among the reported gadolinium complexes of 225.86 mM−1 s−1 was achieved. The cell imaging shows obvious blue and red luminescence under 980 nm laser excitation, and the up-conversion luminescence is unique because there is no autofluorescence from cells under 980 nm excitation. This indicates their promising application in the biological field. All the experiments indicate the promising application of Gd/Tm-MOFs in diagnosis and treatment.
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Chemical Engineering and Processing-Process Intensification
·
2018
·
IF 2.826
Ding Chen,Peng-fei Feng,Fu-hua Wei
Fe-based metal-organic frameworks(Fe(III)-MOFs)were synthesized by Fe 2 (SO 4 ) 3 and trimesic acid using microwave-assisted ball milling method. The structure of the Fe(III)-MOFs was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and Fourier transform infrared spectrometry (FTIR). The thermostability of the MOFs was analyzed by thermogravimetric analysis (TGA). Fe(III)-MOFs were added in aqueous solutions to remove organic dyes. The removal efficiencies of Orange II, CR and MB reached 95.9%, 98.7%, 95.7% respectively at 10℃ and reached 97.7%, 99.7%, 97.5% respectively at 35℃ in 300 min.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2015
·
IF 7.435
Wei Zhu,Peijue Liu,Shuning Xiao,Wenchao Wang,Dieqing Zhang,Hexing Li
A novel Ag-doped MOF-like organotitanium polymer (Ag@NH 2 -MOP(Ti)) was synthesized via a microwave-assisted coordination and polymerization reaction with 2-aminoterephthalic acid (H 2 ATA) and tetra- n -butyl titanate (Ti(OC 4 H 9 ) 4 ), followed by the crystal growth and assembly onto Ag nanoparticles (NPs). This Ag@NH 2 -MOP(Ti) exhibited excellent activity in visible-light driven photocatalytic NO oxidization, much higher than N -doped TiO 2 by two times. The NH 2 -MOP(Ti) absorbed visible lights to generate photoelectrons and holes, accompanied by producing HO and O 2 − active sites for the subsequent NO oxidation into NO 3 − . The Ag NPs allowed assembly of NH 2 -MOP(Ti) polymer favoring light absorbance via multiple reflections and also facilitated photoelectrons transfer to reduce photoelectron–hole recombination, leading to the enhanced photocatalytic activity for NO oxidation and inactivating bacteria. Moreover, it could be used repetitively owing to the high stability.
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2015
·
IF 2.679
Qi Yang,Xiaxia Song,Jing Ge,Guowei Zhao,Wendou Zhang,Gang Xie,Sanping Chen,Shengli Gao
A new energetic MOFs , {[Ni 2 (C 2 H 5 N 5 ) 2 (C 3 H 2 O 4 ) 2 (H 2 O)]·3H 2 O} n (Hdatrz (C 2 H 5 N 5 ) = 3,5-diamino-1,2,4-triazole, H 2 mal (C 3 H 4 O 4 ) = malonic acid), has been synthesized and characterized by element analysis, chemical analysis, IR spectroscopy, single-crystal X-ray diffraction and thermal analysis. X-ray diffraction analysis confirmed that the compound featured a 2D layer structure with dinuclear Ni(II) unit. Thermal analysis demonstrated that the compound after dehydration have good thermostability with decomposition temperature up to 633 K. The non-isothermal kinetics for the compound was studied by Kissinger’s and Ozawa’s methods. The Arrhenius equation of initial thermal decomposition process of compound can be expressed as ln k = 55.89 − 332.01 × 10 3 / RT . Furthermore, a reasonable thermochemical cycle was designed based on the preparation reaction of the compound, and standard molar enthalpy of dissolution of reactants and products were measured by RD496-2000 calorimeter. Finally, the standard molar enthalpy of formation of the compound was determined to be −(2766.3 ± 2.3) kJ · mol −1 in accordance with Hess’s law. In addition, the specific heat capacity of the compound at T = 298.15 K was determined to be 1.42 ± 0.11 J · K −1 · g −1 by RD496-2000 calorimeter.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Tian Lan,Yue Chang,Jiaran Song,Lingxin Meng,Pengyun Zhao,Jinxuan Lei,Jingmei Xu
In this paper, amino monomer (4Am-PH) and the sulfonated poly (arylene ether ketone sulfone) involving amino groups (Am-SPAEKS) were successfully prepared by diazotization reaction and direct polycondensation, respectively. The polyethyleneimine-modified UiO-66-NH 2 (P-MOFs) were prepared as fillers. Composite membranes were fabricated by incorporating different contents of P-MOFs into Am-SPAEKS polymer matrix using non-solvent-induced phase separation. The morphology, chemical structure and properties of the polymers, fillers and composite membranes were proved by FT-IR, 1 H NMR, FE-SEM, XPS and etc. The final experimental results showed that the introduction of hydrophilic fillers, P-MOFs, substantially improved the hydrophilicity, water flux and antifouling capabilities of the membranes. The water contact angle decreased from 78.5° to 56.4°. The flux of water from a pure membrane was 333.68 L/m 2 h. When the content of P-MOFs was 0.1 %, the water flux could attain to 830.23 L/m 2 h, the retention rate of bovine serum albumin (BSA) solution could attain to 98.6 % and the flux recovery rate (FRR) values of the composite membrane remained high (86.1 %) for BSA solution. In addition, after three cycles, the pure water flux of the composite membrane could still attain 595.49 L/m 2 h. The results demonstrated that P-MOFs have significant potential for utilization in the preparation of composite ultrafiltration membranes and provided an effective idea for the modification and design of other hydrophilic MOFs applied in the study area of ultrafiltration membranes.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Hang Ruan,Yuwen Zhong,Huining Ding,Zehui He,Jiaqi Li,Meng Long,Zhi Wang,Qing Xia,Teng Guo,Chunyun Zhu,Tao Yang,Nianping Feng,Yongtai Zhang
Licorzinc is a commonly used immunomodulator, but faces poor water solubility, high oral dose, and side effects of zinc accumulation by long-term administration. Herein, a new licorzincform was developed by adsorbing glycyrrhizic acid (GA) into zeolitic imidazolate framework-8 (GA@ZIF-8) with superior solubility and acid-responsive drug release properties. Then, a dual-continuous microneedle patch was developed for simultaneous transdermal delivery of GA@ZIF-8 and monitoring Zn 2+ in local tissues, where dissolving microneedles as a drug delivery unit were fabricated from hyaluronic acid. In contrast, swollen hydrogel microneedles as a diagnostic unit were prepared from double cross-linking of N-acryloyl-glycinamide and α-methylacrylic acid and hybridized with Eu 3+ and terpyridine (TPy). The microneedles for transdermal GA@ZIF-8 delivery were completely dissolved in 2 min, which improved the cyclophosphamide-induced hair follicle recession in mice by reducing CD8 + NKG2D + T cells infiltration, inhibiting Jak receptor activation, and decreasing IL-15 and IFN-γ. Additionally, as a sensor unit, the microneedles rapidly absorbed water swelled when stabbed into the skin, and fluoresced red when exposed to 365 nm light. Zn 2+ in the inter tissue fluid competes with Eu 3+ in the TPy-Eu 3+ complex and coordinates with Tpy, which triggers a change in fluorescence. Notably, the detection Zn 2+ concentration range was 10 –8 M–10 –1 M, and it was not disturbed by metal ions including Na + , K + , Mg 2+ , and Ca 2+ , suggesting that it is competent to be applied as a real-time chemosensor of Zn 2+ . Collectively, this newly designed system with both therapeutic and diagnostic functions provides a new strategy for treating zinc-related diseases.
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CHEMOSPHERE
·
2024
·
IF 8.1
Yang Zhang,Wenqian Zhao,Xiaodong Zhang,Shuguang Wang
Given the presence of emerging pollutants at low concentrations in water bodies, which are inevitably affected by background substances during the removal process. In this study, we synthesized molecularly imprinted catalysts (Cu/Ni-MOFs@MIP) based on bimetallic metal-organic frameworks for the targeted degradation of ciprofloxacin (CIP) in advanced oxidation processes (AOPs). The electrostatic interaction and functional group binding of CIP with specific recognition sites on Cu/Ni-MOFs@MIP produced excellent selective recognition (Q max was 14.82 mg g −1 ), which enabled the active radicals to approach and remove the contaminants faster. Electron paramagnetic resonance (EPR) analysis and quenching experiments revealed the coexistence of ∙OH, SO 4 2− , and 1 O 2 , with ∙OH dominating the system. Based on experimental and theoretical calculations, the reaction sites of CIP were predicted and the possible degradation pathways and mechanisms of Cu/Ni-MOFs@MIP/PMS systems were proposed. This study opens up a new platform for the targeted removal of target pollutants in AOPs.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Lingyan Ma,Di Wu,Lianzhe Hu,Rui Xiao,Kanglin Pei,Wenjing Qi
Phenylglyoxylic acid (PGA) as styrene metabolite is an indicator of styrene occupational exposure. In this work, a novel anodic and cathodic dual-emitting electrochemiluminescence (ECL) ratiometric method for PGA detection is developed using persulfate (S 2 O 8 2- ) and silver metal organic frameworks (Ag-MOFs) amplification strategy. PGA can enhance anodic ECL intensity of Ru(bpy) 3 2+ /PGA system nearly 2 times and cathodic ECL intensity nearly 16 times. S 2 O 8 2- and Ag-MOFs as co-reactant accelerators promote redox reaction of PGA and enhance ECL intensity. Ag + can catalyze S 2 O 8 2- to produce SO 4 ·- , which can convert Ag + to Ag 2+ . Furthermore, SO 4 ·- can accelerate the transformation of Ag + generating more Ag 2+ . Compared with Ru(bpy) 3 2+ system, cathodic ECL intensity of Ru(bpy) 3 2+ /K 2 S 2 O 8 /Ag-MOFs/PGA system gets enhanced nearly 170 times and anodic ECL intensity gets enhanced nearly 6 times. First electro-reduction and then electro-oxidation using scanning potential direction of 0→− 1.3 V→1.4 V→0 also simultaneously enhanced cathodic and anodic ECL nearly 2 times. Thus this ECL ratiometric method for PGA detection has high sensitivity with LOD of 0.8 nM and rapid response once PGA is added in an instant (several seconds). More importantly, anodic and cathodic dual-emitting improves selectivity and avoid interference in complex detection.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Elia Gadallah,Mohamed N. Khalil,Sami Karam,Wael Ali,Jinchao Chen,Xiangmin Xu,Yuan Jing,Fang Li
Designing and fabricating ultrafiltration membranes that possess relatively high permeability while simultaneously maintaining high rejection and improved antifouling properties continues to be a challenge. In this study, we investigated the integration of novel melamine modified Zr-based metal organic frameworks (Zr-MOFs) with nanosheets of graphene oxide (GO) and sulfonated graphene oxide (SGO). These composite materials were synthesized using the solvothermal process and subsequently coated onto the PES membrane surface using the vacuum-assisted dip-coating method. The stability enhancement of the topmost MOF composite layer adhering to the membrane surface is attributed to hydrogen bonding, π-π stacking, and van der Waals interactions. These effects are augmented by the incorporation of polar functional groups such as hydroxyl, carboxyl, sulfonate, and amine groups. The optimized composite membranes incorporating MOFs exhibit enhanced performance, with a permeability of 80.2 L/m 2 h bar, achieving a bovine serum albumin (BSA) rejection of ≥97.8 % and a humic acid (HA) rejection of 98.9 %. Moreover, a flux recovery ratio (FRR) of 89.5 %. To investigate the interactions among the incorporated components, molecular dynamics (MD) simulations were employed in a computational study. The simulations validated hydrogen bond formation and reinforced prior studies, demonstrating the potential of Zr-MOF compositions as effective hydrophilic nanoparticles. The overall results indicate a substantial enhancement in membrane performance and underscore the high potential for practical applications.
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