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FUEL · 2020 · IF 5.578

Synthesis of ionic-liquid-functionalized UiO-66 framework by post-synthetic ligand exchange for the ultra-deep desulfurization

Zhaoyang Qi,Ting Qiu,Hongxing Wang,Changshen Ye

Ionic Liquids (IL) has been recently immobilized into the pores of metal-organic framework materials (MOFs) to prepare heterogeneous catalyst. However, the IL@MOFs composites are generally prepared by impregnation method, which is unstable in polar solvents. So, we design a new strategy to immobilize IL, and a novel Fenton-like catalyst [mim(CH 2 ) 3 COO]FeCl 4 @UiO-66 has been prepared based on the post-synthetic ligand exchange (PSLE) between MOFs and monocarboxylic functional IL. The [mim(CH 2 ) 3 COO]FeCl 4 @UiO-66 was exploited to act as an efficient heterogeneous catalyst for dibenzothiophene (DBT) oxidation in a biphasic system using H 2 O 2 as the oxidant. Based on optimal conditions, the DBT removal efficiency reached up to 99.1%. Moreover, the heterogeneous catalyst had a good thermal and chemical stability, and the DBT removal efficiency still exhibited over 95% after 6 recycle runs. It is worth noting that the high DBT removal efficiency could be attributed to the synergistic effect between adsorptive and oxidative desulfurization, where [mim(CH 2 ) 3 COO]FeCl 4 @UiO-66 is both an adsorbent and a catalyst.

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JOURNAL OF POLYMER RESEARCH · 2020 ·Vol. 27 ·期 3 ·1-12 · IF 2.426

Incorporation of UiO-66-NH2 into modified PAN nanofibers to enhance adsorption capacity and selectivity for oil removal

Chen Yang,Jiang Lanying

In this research, an attempt has been made to prepare a membrane with high adsorption capacity and high separation efficiency for oil water. The composite membrane of UiO-66-NH 2 and polyacrylonitrile (PAN) were fabricated by electrospinning, and hydrophobic modification was carried out to obtain the oil selectivity. UiO-66-NH 2 loaded on fibers significantly enhanced the oil affinity and surface roughness of the composite membrane. The composite membrane was used for colleseed oil, kerosene, methylbenzene, methyl silicone oil and dichloromethane adsorption, and the maximum adsorption capacity were 31.5, 21.9, 19.9, 39.9, 39.7 g·g −1 , respectively, which was 32–96% higher than pure PAN adsorbent. The amount of UiO-66-NH 2 loaded on fibers accelerated the diffusion of oil in membrane and reduced the adsorption time to reach equilibrium. The adsorption process can be well described by pseudo-second-order and intra-particle diffusion model. The composite membrane also showed potential reusability. In addition, the composite membrane has excellent performance in oil/water separation, and the oil can be separated from mixture solution just under gravity. The oil flux is 2286 Lm −2  h −1 and remains 1568 Lm −2  h −1 after ten times continuous filtration. Overall, the composite PAN-MOFs-coated membrane has promising potential in practical application in oil/water separation.

CAS / MDL: 10312-55-7 10026-11-6
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Photodegradation of seven bisphenol analogues by Bi5O7I/UiO-67 heterojunction: Relationship between the chemical structures and removal efficiency

Chun-Shuai Cao,Jingzhen Wang,Xiaoyong Yu,Yinqing Zhang,Lingyan Zhu

Bisphenol analogues have been widely used and displayed adverse effects on human beings. Although many photocatalysts displayed remarkable performance in degrading bisphenol A (BPA) or bisphenol F (BPF), it is not clear if they may also efficiently decompose other bisphenol analogues. In this study, Bi 5 O 7 I with satisfactory photocatalytic activity was doped with metal-organic framework (UiO-67) to build up Bi 5 O 7 I/UiO-67 heterojunctions. The heterojunction enhanced the charge mobility and separation of the electron-hole pairs, which was conducive for improving the photocatalytic activity. Consequently, 4:1-Bi 5 O 7 I/UiO-67 realized highly effective degradation of seven bisphenol analogues in one hour. Density functional theory (DFT) calculations uncovered that the reaction rate constant k displayed a positive correlation with the Hirshfeld charge q (N) of tertiary butyl carbon attached with different substituent groups. This provides a prospective heterojunction catalyst to degrade a group of pollutants with similar structures, and sheds light on the structural relationship of degradation efficiency.

CAS / MDL: 80-05-7
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JOURNAL OF MEMBRANE SCIENCE · 2020 · IF 7.183

Thin-film nanocomposite nanofiltration membrane with an ultrathin polyamide/UIO-66-NH2 active layer for high-performance desalination

Yuqiong Gong,Shoujian Gao,Yangyang Tian,Yuzhang Zhu,Wangxi Fang,Zhenggong Wang,Jian Jin

In this work, ultrasmall metal-organic frameworks (MOFs) nanoparticles , UIO-66-NH 2 nanoparticles were synthesized and embedded in an ultrathin polyamide (PA) active layer via the interfacial polymerization reaction on a polydopamine-wrapped single-walled carbon nanotube film. A thin-film nanocomposite nanofiltration (TFN NF) membrane with a PA/UIO-66-NH 2 active layer as thin as 20 ± 3 nm was thus fabricated. The loading mass of the nanoparticles in the TFN NF membrane could be tuned by controlling the nanoparticles concentration in aqueous phase. Benefiting from the ultrathin thickness of active layer and the high loading mass of the MOFs nanoparticles, water permeability up to 46 L m −2 h −1 bar −1 along with a Na 2 SO 4 rejection of 97.1% was achieved, which is 53% increase of the TFC NF membrane without the addition of UIO-66-NH 2 nanoparticles. Our membrane owns the thinnest active layer in the category of TFN NF membranes reported so far and exhibits outstanding desalination performance.

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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 43 ·期 43 ·16981-16989 · IF 3.069

Ti functionalized hierarchical-pore UiO-66(Zr/Ti) catalyst for the transesterification of phenyl acetate and dimethyl carbonate

Bingying Jia,Miaojiang Wu,Hua Zhang,Yi Zeng,Gongying Wang

Titanates are frequently used as precursors to prepare transesterification catalysts with TiIV species. Unfortunately, it is challenging to control the dispersity of TiIV active sites on supports. Herein, a series of TiIV species is anchored on abundant linker vacancy sites by introducing point and large scale defects in UiO-66(Zr/Ti) with hierarchical-pore structure. The catalyst functionalized by titanium(IV) oxide bis(2,4-pentanedionate) shows excellent catalytic performance in the transesterification of dimethyl carbonate with phenyl acetate. The catalysts are characterized by XRD, FT-IR, N2 adsorption–desorption, XPS, SEM and STEM-HAADF techniques. The results demonstrate that the delicate mesopores in the support can not only exhibit a large surface area for the distribution of the active sites, but also provide better mass transfer performance. Meanwhile, the introduction of octahedral TiIV ions raises the activity of the catalyst via more coordinatively unsaturated ZrIV sites. Furthermore, using titanium(IV) oxide bis(2,4-pentanedionate) as a Ti source can effectively prevent the condensation of tetrahedral TiIV species anchored on the hierarchical-pore UiO-66(Zr/Ti) support.

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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Perovskite-type CsPbBr3 quantum dots/UiO-66(NH2) nanojunction as efficient visible-light-driven photocatalyst for CO2 reduction

Shipeng Wan,Man Ou,Qin Zhong,Xinming Wang

Base-on the excellent optoelectronic properties, perovskite CsPbBr 3 quantum dots (QDs) have been used on perovskite solar cells and LED devices, but little research has been focused on photochemical CO 2 reduction due to their poor moisture stability. Coincidentally, metal-organic frameworks (MOFs) materials have received tremendous attention for sustainable clean energy and environmental remediation. However, the design of excellent performed MOFs is still indispensable. Therefore, the CsPbBr 3 QDs/UiO-66(NH 2 ) nanocomposites that combine the advantages of CsPbBr 3 QDs and UiO-66(NH 2 ) have been successfully designed and fabricated for the first time. Then we employ the nanocomposites as photocatalysts to convert CO 2 to chemical fuels in nonaqueous media. The resultant nanocomposites exhibit significantly improved photocatalytic activity for CO 2 reduction. When CsPbBr 3 QDs content is 15 wt%, the amount of CO can reach 98.57 μmol·g −1 . The remarkable photocatalytic performance could be ascribed to the improved electron extraction and transfer between UiO-66(NH 2 ) and CsPbBr 3 QDs, large accessible specific surface area and enhanced visible light absorption capacity. Moreover, the nanojunction shows excellent reusability for photocatalytic CO 2 reduction. This work might supply new pathway to utilize halide perovskite QDs/MOF nanocomposite in energy conversion and environmental remediation.

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Journal of Cleaner Production · 2019 · IF 6.395

Post-modification of UiO-66-NH2 by resorcyl aldehyde for selective removal of Pb(II) in aqueous media

Likang Fu,Shixing Wang,Guo Lin,Libo Zhang,Qiming Liu,Houhuang Zhou,Chenxia Kang,Shuyun Wan,Hongwei Li,Sheng Wen

A new metal organic framework UiO-66-RSA (UiO-66 with hydroxyl) was prepared by the post-modification of UiO-66-NH 2 (UiO-66 with amino) with resorcyl aldehyde and was employed for the efficient and selective separation and removal of Pb(II) in aqueous media . The maximum adsorption amount of UiO-66-RSA was 189.8 mg/g at an optimal pH of 4. The adsorption isotherm and kinetic were well described by Langmuir/Dubinin-Radushkevich and pseudo-second-order models respectively. Adsorption process was monolayer chemisorption . UiO-66-RSA was regenerated by thiourea/nitric acid and the removal rate was only decreased by 3.7% after five successive cycles. The analysis of X-ray photoelectron spectroscopy suggested the adsorption mechanism lay on the complexation reaction between hydroxyl/nitrogen-containing groups and Pb(II). The UiO-66-RSA bound Pb(II) by forming double/quadri coordinated complexes. Compared with a multitude of usual metal ions , viz., Zn(II), Co(IV), Ni(II), Mg(II), Cd(II), Cu(II) and Ca(II), the Pb(II) could be absorbed selectively by UiO-66-RSA. The results indicated that the UiO-66-RSA sorbent could be of great potential in the removal of Pb(II) from aqueous solutions.

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JOURNAL OF CHROMATOGRAPHY A · 2014 · IF 4.258

Preparation and evaluation of silica-UIO-66 composite as liquid chromatographic stationary phase for fast and efficient separation

Zhiming Yan,Jiangnan Zheng,Jinfeng Chen,Ping Tong,Minghua Lu,Zian Lin,Lan Zhang

A silica-UIO-66 composite was fabricated by a simple hydrothermal method and then applied as liquid chromatographic stationary phase for fast and efficient separation. X-ray diffraction patterns showed the presence of UIO-66 crystals in the silica-UIO-66 composites; while scanning electron microscope (SEM) images revealed that silica-UIO-66 composites were a homogeneous mixture of silica bead and UIO-66 crystals. A variety of substituted aromatics, chlorobenzene compounds and polycyclic aromatic hydrocarbons (PAHs) were used to evaluate the retention properties of the silica-UIO-66 composite packed column. Under the optimized conditions, baseline separation of ethylbenzene (EB) and styrene was obtained with high resolution and short retention time. In addition, the silica-UIO-66 composite packed column also showed some advantages in separation of positional isomers, with which baseline separation of EB and xylene, chlorotoluene and dichlorobenzene isomers was achieved. Moreover, the retention mechanisms of these compounds were also discussed in detail. The relative standard deviations (RSDs) for the separation of EB and xylene, chlorotoluene and dichlorobenzene isomers, as well as EB and styrene were 0.42–0.9%, 1.0–1.9%, 0.75–2.0%, and 0.9–2.1% for the retention time, peak area, peak height, and half peak width, respectively. The column efficiencies for EB, p-chlorotoluene, p-dichlorobenzene and styrene were 8780, 9060, 9990 and 5130 plates/m. The successful applications suggested high potentials of silica-MOFs composite as stationary phase for fast and efficient liquid chromatography separation.

CAS / MDL: 10026-11-6 100-21-0
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2015 ·Vol. 307 ·期 1 ·269-276 · IF 1.034

U(VI) capture from aqueous solution by highly porous and stable MOFs: UiO-66 and its amine derivative

Luo Bai-Cheng,Yuan Li-Yong,Chai Zhi-Fang,Shi Wei-Qun,Tang Quan

Metal–organic frameworks (MOFs) UiO-66 and its amine derivative (UiO-66-NH 2 ) with high surface area and unprecedented chemical stability were synthesized and first explored for U(VI) capture from aqueous solutions. At pH 5.5, U(VI) sorption reach equilibrium in ca. 4 h and the maximum sorption capacity is more than 100 mg g −1 . Moreover, they show desirable selectivity towards U(VI) over a range of competing metal ions. Sorption results demonstrate that introduction of amino groups into MOFs does not enhance U(VI) sorption, probably result from the lower activity of aromatic amines, decrease of surface area and formation of intermolecular hydrogen bonds.

CAS / MDL: 100-21-0
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ELECTROCHIMICA ACTA · 2016 · IF 4.803

Highly dispersed AuPd alloy nanoparticles immobilized on UiO-66-NH2 metal-organic framework for the detection of nitrite

Juan Yang,Lite Yang,Huili Ye,Faqiong Zhao,Baizhao Zeng

In this work, highly dispersed AuPd alloy nanoparticles (NPs, 3–6   nm) decorated amino-functionalized Zr(IV)-based metal–organic framework (i.e. UiO-66-NH 2 ) was prepared via a novel adsorption/reduction method in ethanol-water solution. In this process, the UiO-66-NH 2 acted as both supporting platform and protective agent. The pores of UiO-66-NH 2 could limit the aggregation and migration of AuPd alloy NPs. The resulting AuPd/UiO-66-NH 2 catalyst possessed large specific surface area and excellent stability and dispersity in aqueous media. When it was used to construct a nitrite sensor, the composite material exhibited higher catalytic activity than the metal counterparts (i.e., Au/UiO-66-NH 2 and Pd/UiO-66-NH 2 ) due to the strong metallic synergistic effect. The electrochemical study demonstrated that the AuPd/UiO-66-NH 2 based sensor had an extended linear response concentration range of 0.05–5666   μ M for nitrite detection, with a detection limit of 0.01   μ M. It was successfully applied to determine nitrite in sausage and pickle samples.

CAS / MDL: 10312-55-7 10026-11-6
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MICROCHEMICAL JOURNAL · 2024 · IF 4.9

Determination of the cervical cancer biomarker SCCA using CMK-3@UiO-66@AuNPs composite-modified glassy carbon electrodes

Lixia Luo,Jinglin Shui,Yingying Gu,Dandan Wang,Jiangyang Qin,Yanan Wang,Yong Mei

In order to detect the cervical cancer biomarker squamous cell carcinoma antigen (SCCA) in human serum, an electrochemical immunosensor was constructed. Zirconium 1,4-dicarboxybenzene MOF (UiO-66), with a high specific surface area, was coupled with gold nanoparticles (AuNPs), creating the UiO-66@AuNPs nanomaterial. This coupling increased the sensitivity of the electrochemical immunosensor by providing many biological binding sites for antibodies to bind to Au-S bonds. Then, mesoporous carbon (CMK-3) was added to the UiO-66@AuNPs nanomaterial to obtain a CMK-3@UiO-66@AuNPs nanocomposite. This further increased the electron transfer proficiency of the material and enhanced the electrochemical signal. Finally, the sensitive detection of squamous cell carcinoma antigen (SCCA) was made possible by unique immunological responses between antigens and antibodies. Transmission electron microscopy (TEM) analysis of CMK-3@UiO-66@AuNPs revealed embedded surfaces and voids; cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) confirmed the successful assembly of the electrochemical immunosensor. The developed electrochemical immunosensor demonstrated good linearity (R 1 2  = 0.999) from 0.01 pg/mL to 10,000 pg/mL, which is the concentration range of SCCA in human serum. The limit of detection was 0.0034 pg/mL (at an S/N ratio of 3). The immunosensor exhibited excellent precision, stability and selectivity, with a high rate of recovery (98.26–101.8 %). The experimental validation studies demonstrated that the electrochemical immunosensor was effective for the detection of SCCA in human serum, offering a novel method for the early diagnosis and dynamic surveillance of cervical cancer.

CAS / MDL: 10026-11-6
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ANALYTICA CHIMICA ACTA · 2024 · IF 5.7

Dual-emissive europium doped UiO-66-based ratiometric light-up biosensor for highly sensitive detection of histidinemia biomarker

Li Li,Lin-Lin Zhang,Jin Zou,Jiamin Zou,Lu-Ying Duan,Yansha Gao,Guanwei Peng,Xigen Huang,Limin Lu

Background Lanthanide metal-organic frameworks (Ln-MOFs) are a kind of emerging crystalline porous materials with high fluorescence and easy-to-tunable properties, making them ideal for sensing applications. However, current Ln-MOFs based fluorescent probes are primarily single-emissive or fluorescence-quenched, which greatly limited the detection performances such as sensitivity, accuracy and repeatability, thereby hindering their applications in efficient target monitoring and related disease diagnosis. To address these issues, the reasonable design of Ln-MOFs equipped with dual fluorescence emissions and light-up mode is urgently needed for a high-performance biosensor . Results A dual-emissive europium doped UiO-66 (Eu@UiO-66-NH 2 -PMA)-based ratiometric fluorescent biosensing platform was constructed for highly sensitive and selective detection of the histidinemia biomarker-histidine (His). Eu@UiO-66-NH 2 -PMA (pyromellitic acid abbreviated as PMA) was synthesized utilizing a post-synthetic modification method via coordination interactions between the free –COOH of UiO-66-NH 2 -PMA and Eu 3+ , which exhibited characteristic peaks of broad ligand emission and sharp Eu 3+ emissions simultaneously. Considering that Cu 2+ had the excellent fluorescence quenching ability toward Eu 3+ and superior affinity with His, it was deliberately introduced into the Eu@UiO-66-NH 2 -PMA, acting as active sites for target His responsiveness. The Eu@UiO-66-NH 2 -PMA/Cu 2+ /His ternary competition system demonstrated a low detection limit of 74 nM, excellent selectivity and good anti-interference capability that allowed for sensitive analysis of His levels in milk and human serum samples. Significance Attributing to the superior luminescent properties, good stability and self-calibration capability of Eu@UiO-66-NH 2 -PMA, the developed ratiometric light-up sensing platform enabled sensitive, selective and credible analysis of His in complex practical samples, which might provide an available tool for food nutrition guideline and diagnostic applications of His related diseases.

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