SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Fangfang Li,Jinjin Wang,Ying-Hua Zhou
Metal-organic frameworks (MOFs) possess highly tunable structures, making them promising heterogeneous catalysts for efficient CO 2 conversion reactions. In this work, cerium-modified zirconium-based metal-organic frameworks (ZrCe-UiO-66) were engineered and post-synthetically functionalized with dicationic ionic liquid moieties, enabling the simultaneous introduction of strong Lewis acidic sites and nucleophilic ionic liquid units without the need for external co-catalysts. The resulting ZrCe 0.5 -UiO-66-DIL(n-PyRIm) ( n = 2, 3, 4; R = Et, Pr, Bu, Pe) functionalized MOFs were prepared via a modular grafting approach and exhibited remarkable catalytic performance. Among them, ZrCe 0.5 -UiO-66-DIL(2-PyBuIm) converted epichlorohydrin into the corresponding cyclic carbonate with 96% yield and 98% selectivity under solvent-free conditions at 110 °C and a CO 2 pressure of 0.1 MPa. This outstanding activity arises from a cooperative activation mechanism, in which the mixed Zr 4+ /Ce 4+ activate the epoxide substrate through Lewis acid coordination with the epoxide oxygen, thereby facilitating C O bond activation, while the bromide anions embedded in the ionic liquid moieties promote nucleophilic ring opening. In addition to high catalytic efficiency, the MOF hybrids demonstrated excellent recyclability and broad substrate tolerance. Combined CO 2 adsorption measurements and in situ infrared spectroscopy further revealed key surface intermediates, enabling a plausible mechanistic pathway for the cycloaddition process to be proposed.
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ACS Applied Polymer Materials
·
2026
·
IF 5.2
Ziyi Yuan,Zhihong Lin,Kejing Li,Jian Li,Viatcheslav Freger,Xuezhong He
Polymers of intrinsic microporosity (PIMs) are promising membrane materials for CO2 separation due to their high permeability; however, their limited CO2/N2 selectivity restricts practical application. Herein, mixed-matrix membranes (MMMs) were fabricated by incorporating a CO2-molecularly imprinted UiO-66-NH2 filler (MIP@U) into amidoxime-functionalized PIM-1 (AOPIM-1), followed by thermal treatment at 160 or 250 °C under vacuum to regulate the membrane microstructure. Spectroscopic and porosity analyses (FTIR, XRD, and N2 physisorption) show that thermal treatment at 160 °C promoted oxadiazole-ring formation, leading to enhanced subnanometer microporosity and improved CO2/N2 selectivity. In contrast, treatment at 250 °C partially regenerates nitrile groups and generates larger micropores, resulting in higher CO2 permeability but reduced selectivity. The MIP@U filler introduces CO2-recognition cavities and improves interfacial compatibility, enabling synergistic control of polymer microporosity and interfacial transport pathways. The optimized 3 wt % MIP@U/AOPIM-1-TR160 membrane achieves a CO2 permeability of ∼1600 Barrer and a CO2/N2 selectivity of 50.8. The membrane also demonstrates stable performance under pressures up to 12 bar and during 30 h of continuous operation at 2 bar. This study highlights a dual-approach strategy combining thermally tailored PIM chemistry with molecularly imprinted MOF fillers for designing high-performance MMMs for CO2 capture.
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MICROCHEMICAL JOURNAL
·
2026
·
IF 5.2
Zhaoxia Shi,Zhen Luo,Yilu Liu,Yintang Zhang,Yanli Zhou,Maotian Xu
A synergistic MgO@UiO-66-NH₂ nanocomposite was prepared for CTL sensing. • The proposed CTL sensor enables rapid, non-invasive detection of isopropanol. • The sensor exhibits a wide linear range (0.04–120 mg/L) and good stability. • This method offers a potential approach for preclinical lung cancer screening via exhaled breath analysis. Isopropanol (IPA) has been identified as a potential biomarker for lung cancer, and the rapid detection of IPA in exhaled breath may offer a promising strategy for lung cancer screening. In this study, rod-like MgO, MnO₂, and ZnO, along with natural halloysite nanotubes (HNTs), were synthesized and used as carriers to fabricate nanocomposites with a Zr-based metal–organic framework (UiO-66-NH₂). Their catalytic activities toward IPA were evaluated using cataluminescence (CTL) measurements. MgO@UiO-66-NH₂ exhibited the highest catalytic activity, attributed to the synergistic effect between MgO and UiO-66-NH₂ enhancing the redox capacity in the presence of ozone. Based on this composite, a rapid CTL method was developed for IPA detection in exhaled breath. The intra-sensor precision (nine repeated measurements on the same sensor) gave a relative standard deviation (RSD) of 3.41%; inter-sensor reproducibility (seven different sensors) gave an RSD of 3.81%; and long-term stability over seven weeks showed an RSD of 4.3%. The linear range was 0.04–120 mg/L, with a limit of detection of 0.015 mg/L (S/N = 3). When applied to three healthy human exhaled breath samples, the method achieved spiked recoveries ranging from 90.0% to 105.3%. These results demonstrate that the proposed CTL sensor enables rapid, non-invasive detection of IPA and holds great potential for IPA detection in exhaled breath. Download: Download high-res image (143KB) Download: Download full-size image
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TALANTA
·
2023
·
IF 6.1
Mengyao Mu,Shiping Zhu,Yanmei Gao,Ning Zhang,Youmei Wang,Minghua Lu
Due to widespread application of benzoylurea insecticides (BUs) and its persistence in environment, the effective capture of benzoylurea insecticides residues in environment is an important issue of environmental safety monitoring. To obtain excellent adsorption performance, creating defective structure in metal-organic frameworks (MOFs) can be employed as the method for adjusting its properties. Zirconium(Ⅳ)-based MOF termed as UiO-66-30% was constructed with 2-aminoterephthalic acid (NH 2 -BDC) and terephthalic acid (H 2 BDC) as building blocks. After calcination and removal of thermal-sensitive ligand (NH 2 -BDC), hierarchically porous UiO-66-30% (HP-UiO-66-30%) with multistage pore structure and good stability was obtained. The unique structure of HP-UiO-66-30% endowed it to achieve instantaneous equilibrium (within 2 min) when it was used as a dispersed solid phase extraction (d-SPE) adsorbent to extract BUs from environmental samples, greatly reducing the operation time. A wide linear range (0.05–200 ng mL −1 ), good linearity (R 2 ≥ 0.9980), low detection limits (0.01–0.03 ng mL −1 ) and quantification limits (0.05–0.1 ng mL −1 ) were obtained for BUs. In addition, the HP-UiO-66-30% material possessed the good reusability and the adsorption capacity did not change significantly over 16 adsorption-desorption cycles. Finally, the established dispersed solid phase extraction-high performance liquid chromatography-diode array detector (d-SPE-HPLC-DAD) method was successfully applied to determination of BUs residues in environmental soil samples. The results demonstrated that HP-UiO-66-30% was an excellent sorbent for extraction BUs from environmental samples.
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PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Fangqing Li,Lin Chen,Yufei Wei,Zhiwei Yin,Keying Que
Membrane distillation (MD) is considered an emerging desalination technology. However, the presence of surfactants allows liquid to penetrate the membrane, resulting in membrane wetting, which hinders the commercialization of MD. In this study, we use very few modified materials to prepare novel Janus thin membranes that immobilize modified materials (graphene oxide (GO) and UiO-66-NH 2 ) on polytetrafluoroethylene (PTFE) hydrophobic base membranes via crosslinkers. The composite thin membrane properties with eight different ratios and contents of GO and UiO-66-NH 2 were fabricated and tested by a feed solution of sodium chloride containing a high concentration of sodium dodecyl sulfate. An optimal ratio of Janus membrane with high flux without affecting the effluent water quality was obtained. The Janus membrane exhibited excellent anti-wetting properties compared to the original PTFE membrane. A desalination rate of up to 99.9% was still available even under 48 h of long-term operating conditions by maintaining a flux of approximately 21.2 L/(m 2 ·h). The anti-wetting mechanism of this membrane was further confirmed by the modified XDLVO model. It suggested that the novel Janus membrane could be a highly promising substitute to the MD process for the resource-based treatment of surfactant-containing wastewater, which played an important role in promoting its application.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Yang Li,Xiaohuan Zang,Yahuan Li,Shuaihua Zhang,Chun Wang,Zhi Wang
A defective UiO-66 with rich defect sites was synthesized by a modulator-induced defect formation approach and used as the solid-phase microextraction (SPME) fiber coating material. The extraction experimental results showed that the defective UiO-66 coating can selectively extract the fungicides chlorothalonil, vinclozolin, dimethachlon, procymidone and iprodione with a high adsorption capability. The superior adsorption capability can be attributed to hydrophobic, Lewis acid-base and hydrogen bonding interactions. After optimization, a SPME with the defective UiO-66 as the fiber coating combined with GC–MS detection was established for the sensitive and selective determination of the five fungicides in fruit samples. Under the optimized experimental conditions, the quantitative linear response was in the range of 0.83–300 ng g −1 , with the coefficients of determination in the range from 0.9970 to 0.9986 and the limits of detection between 0.25 and 9.0 ng g −1 for the analytes. The method was successfully applied for the determination of the fungicides in different fruit samples. Satisfactory method recoveries (82.7%-117.7%) and good precisions with the relative standard deviations being from 3.2% to 12% were achieved.
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MOLECULES
·
2023
·Vol. 28
·期 5
·2182
·
IF 4.6
Panpan Liu,Jiafei Lyu,Peng Bai
In this study, a series of Al-doped metal-organic frameworks (AlxZr(1−x)-UiO-66) were synthesized through a one-step solvothermal method. Various characterization techniques, including X-ray diffraction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and N2sorption measurement, suggested that the Al doping was uniform and barely influenced the crystallinity, chemical stability, and thermal stability of the materials. Two cationic dyes, safranine T (ST) and methylene blue (MB), were selected for investigating the adsorption performances of Al-doped UiO-66 materials. Al0.3Zr0.7-UiO-66 exhibited 9.63 and 5.54 times higher adsorption capacities than UiO-66, 498 mg/g and 251 mg/g for ST and MB, respectively. The improved adsorption performance can be attributed to π-π interaction, hydrogen bond, and the coordination between the dye and Al-doped MOF. The pseudo-second-order and Langmuir models explained the adsorption process well, which indicated that the dye adsorption on Al0.3Zr0.7-UiO-66 mostly occurred through chemisorption on homogeneous surfaces. A thermodynamic study indicated the adsorption process was spontaneous and endothermic. The adsorption capacity did not decrease significantly after four cycles.Keywords:metal−organic framework;Al-doped;adsorption;organic dyes;mechanism
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Guozhi Fan,Yi Chen,Yuchan Lu,Qunpeng Cheng,Bo Chai,Guangsen Song
UiO-66-derived H 2 N-UiO-66-SO 3 H with acid-base active sites was used for the co-production of 5-hydroxymethyl furfural (5-HMF) and furfural (FUR) in the direct conversion of holocellulose composed of cellulose and hemicellulose. The prepared catalyst was further characterized by various techniques, confirming its formation, structure, and composition. H 2 N-UiO-66-SO 3 H displayed excellent performance for the selective conversion of holocellulose to 5-HMF and FUR, achieving yields of 39.1 % and 28.2 %, respectively. The reusability of the catalyst was also investigated by direct use after recycling without any pretreatment. The results indicated that H 2 N-UiO-66-SO 3 H had good stability, and after four cycles, the yields of 5-HMF and FUR decreased only slightly to 37.2 % and 27.1 %, respectively. The recyclable catalyst H 2 N-UiO-66-SO 3 H for the effective conversion of holocellulose to 5-HMF and FUR demonstrated application potential for the utilization of lignocellulosic biomass.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Lu Yang,Zhao Wang,HaiJiang Gong,Shili Gai,RuiFang Shen
Chemodynamic therapy (CDT), an emerging oncology treatment, has received considerable attention owing to its high selectivity, less aggressiveness, and endogenous stimulation. However, the complex intra-tumor environment limits the therapeutic effect. In this study, Cu + was directly doped into the structure of the UiO-66 matrix using an in situ one-pot oil bath method. The as-formed UiO-66/Cu possessed a large surface area, making it feasible to modify folic acid (FA) and carry more chemotherapeutic agents like tirapazamine (TPZ), thus forming UiO-66/Cu-FA-TPZ nanoplatforms. For CDT, the nanoplatform catalyzed the cyclic generation of the highly oxidizing hydroxyl radical (·OH) from H 2 O 2 . Particularly, low-frequency ultrasound enhanced the curative effect. Notably, in a tumor, a severe hypoxic environment and ultrasound can activate more TPZ for safe and efficient chemotherapy, achieving synergistic and hypoxia-activated tumor treatment with a low risk of side effects. Moreover, the nanoplatform exhibits computed tomography imaging functions for combined diagnosis and treatment. Our designed nanoplatform overcomes the dilemma of insufficient efficacy from conventional therapy attributed to a hypoxic environment, expecting to guide the design of future treatment regimens for hypoxic tumors.
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PubMed
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Jiarong Wang,Shixiong Chen,Qinghao Zeng,Hong Jiang,Haiqing Chang,Tian C. Zhang,Xiaobao Tian,Yingqi Li,Ying Liang,Kai Wang
A miniaturized point-of-use (POU) water treatment device to achieve convenient and efficient water disinfection for remote and post-disaster areas remains a challenge. Herein, such as POU device consisted of a self-polymerized polydopamine (PDA) layer and UiO-66-NH 2 nanoparticles covered electrospun polyacrylonitrile (PAN) membrane (PAN@PDA@UiO-66-NH 2 ) with bacteria filtration and photothermal antibacterial property is successfully fabricated. The membrane achieves a good interception effect of microorganisms in water because of the synergistic pore interception and adsorption effect. A nearly 100% bacterial retention efficiency was obtained by the PAN@PDA@UiO-66-NH 2 membrane. In addition, the obtained PAN@PDA@UiO-66-NH 2 membrane exhibits nearly 100% photothermal sterilization efficiency against Escherichia coli ( E. coli ) under 6 min of 808 nm infrared irradiation (1.21 W). The great photothermal effect comes from the synergistic effect of good photothermal conversion efficiency and absorption of incident light caused by the PDA layer and rough UiO-66-NH 2 particles, respectively. Through the good filtration performance and photothermal effect of the membrane, the filtration for water containing bacteria and sterilization of membrane can be realized. Meanwhile, the membrane fouling caused by bacterial growth can be inhibited. In this way, this innovative membrane has the ability to maintain great filtration and sterilization ability during long-term operation, and thus, having great potential to be used as an effective, convenient, practical, and safe POU water-treatment device.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xiaoming Xu,Guoyan Hua,Yuxuan Chen,Yanhong Zhang,Zepeng Zhang,Weiben Yang,Fuqiang Liu,Aimin Li
Traditional polyamide nanofiltration membranes suffer from permeability-selectivity trade-off limitation and unsatisfactory rejection for divalent cations. Herein, a novel dually charged membrane was constructed by incorporating positively charged UiO-66-(NH 2 ) 2 into the negatively charged polyamide layer. Thanks to the customizable nanochannels of metal-organic frameworks, the amino-rich nanochannels of UiO-66-(NH 2 ) 2 could be fabricated through a ligand replacement strategy. UiO-66-(NH 2 ) 2 played a crucial role in the enhanced rejection of divalent cations, meanwhile negatively charged polyamide surface guaranteed the efficient Na 2 SO 4 rejection. Satisfactory rejections of CaCl 2 (96.07 %) and Na 2 SO 4 (90.62 %) were achieved simultaneously by optimal TFN-D5. Meanwhile, TFN-D5 owned the greatly-improved water permeance of 19.44 LMH/bar, which was about 1.5 times better than that of the TFC-control. Calculations based on density functional theory further confirmed UiO-66-(NH 2 ) 2 rejected Ca 2+ efficiently since the migration energy barrier across UiO-66-(NH 2 ) 2 was an order of magnitude higher than that of UiO-66-NH 2 and UiO-66. Moreover, the desirable rejections were beyond 94 % towards many divalent cation salts including MgCl 2 , NiCl 2 , PbCl 2 , MnCl 2 , CdCl 2 and ZnCl 2 . Thus, this work provided an efficient way to realize the synergistic removal of both divalent cations and anions.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yuting Qian,Wenrou Tian,Jun Han,Najun Li,Dongyun Chen,Qingfeng Xu,Hua Li,Jianmei Lu
Catalytic oxidation of HCHO is often limited by the serious recombination of carriers in photocatalysts and the high cost of thermal catalysts based on precious metals. Herein, Bi 4 Ti 3 O 12 nanosheets enriched with bismuth vacancies were synthesized and decorated by UiO-66-NH 2 to obtain VBiTO@NU-66 for efficient removal of HCHO via piezocatalytic oxidation. The Bismuth vacancies in VBiTO enhanced the asymmetry of the crystal structure and introduced the atomic-level channels for energy and electron transfer. After loading UiO-66-NH 2 , the adsorption ability was substantially improved by the formation of Schiff-base covalent bonds between HCHO and –NH 2 . Under the joint action of adsorption and piezocatalysis, piezocatalytic oxidation rate of 300 mg/m 3 HCHO by VBiTO@NU-66 was as high as 95.1% within 3 h, which was 6 times of that of pure BiTO nanosheets. This work offers a novel tactics for the efficient purification of gaseous environmental pollutants.
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