JOURNAL OF APPLIED POLYMER SCIENCE
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2018
·Vol. 135
·期 46
·46759
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IF 1.901
Mingmin Jia,Yi Feng,Jianhao Qiu,Xiaocheng Lin,Jianfeng Yao
UiO-66-NH 2 nanocrystals were synthesized and embedded into bromomethylated poly(phenylene oxide)/polyethersulfone (BPPO/PES) polymer matrix to form UiO-66-NH 2 /BPPO/PES mixed matrix membranes (MMMs). The crystalline structure, interaction between UiO-66-NH 2 and BPPO, and dispersion of UiO-66-NH 2 were characterized by FTIR, XRD, and SEM. Nanoparticle dispersion was drastically enhanced with the assistance of BPPO, giving an improved adhesion between the polymer and filler particles. Owing to the intrinsic adsorption property of UiO-66-NH 2 and BPPO to CO 2 , the CO 2 permeability was significantly increased. As a result, the UiO-66-NH 2 /BPPO/PES membrane exhibited enhanced gas separation performance, where CO 2 /N 2 and H 2 /N 2 ideal selectivities were increased to 50.2 and 302.4 with a CO 2 permeability of 125.6 Barrer. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135 , 46759.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2024
·
IF 4
Tianyu Wang,Wenyan Guo,Yonghui Xia,Yuefang Zhu,Li Chen,Yafeng Zhang,Guangli Li
The abuse and persistent use of Lomefloxacin (LOM) produces residues that deteriorate the ecological environment and endanger human health. Therefore, it is highly urgent to establish a simple and reliable method for the determination of LOM to guarantee food safety. Herein, a sensitive voltametric sensor based on bimetallic UiO-66(Zr/Ce) MOF/reduced graphene oxide (UiO-66 (Zr/Ce)/rGO) was fabricated for the determination of trace LOM residues in milk. The UiO-66(Zr/Ce)/rGO increased the electroactive surface area and lowered the charge transfer resistance. Due to the synergistic interactions between UiO-66(Zr/Ce) MOFs with good electrocatalytic activity and rGO nanosheets with high electrical conductivity, the UiO-66(Zr/Ce)/rGO/GCE exhibited the highest peak current response of LOM, 4.2-fold higher than the bare GCE. Consequently, the UiO-66(Zr/Ce)/rGO showed remarkably electrocatalytic activity for LOM oxidation with two broad linear detection ranges (0.03 – 2.0 μM and 2.0 – 30 μM), high sensitivities (5.1254 and 0.2198 μM μA −1 ), and a low detection limit (5.0 nM). The UiO-66(Zr/Ce)/rGO exhibited strong anti-interfering ability against potential interfering species even at high concentration, and maintained robust voltametric responses up to 25 days. Moreover, the UiO-66(Zr/Ce)/rGO/GCE achieved accurate determination of trace LOM residues in liquid milk with good recovery (96.11 − 103.2 %) and highly consistent sensitivity with that in PBS.
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
·
IF 8
Gangbing Zhu,Diyan Liao,Nian Hu,Jing Li,Yong He,Yinhui Yi
Herein, we proposed a novel bioenzyme-free dual-mode sensing strategy for the rapid and accurate monitoring of organophosphorus pesticides (OPs) by preparing tris(2,2′-bipyridyl) ruthenium(II) (Ru(bpy) 3 2+ ) encapsulated with UiO-66-NH 2 MOFs as nanozyme (Ru@Zr-MOFs). The as-prepared Ru@Zr-MOFs nanozyme not only exhibits superior peroxidase-like activity which can catalyze O-phenylenediamine (OPD) oxidation to generate yellow 2,3-diaminophenazinc, but also exhibits dual-fluorescence feature (at 442 and 612 nm respectively) and specific interaction capacity with OPs. However, in the existence of OPs, the peroxidase-like activity of Ru@Zr-MOFs nanozyme is restricted and the oxidation process of OPD is stopped; meanwhile, the fluorescence of Ru@Zr-MOFs at 442 nm increases rapidly (< 10 s) while that at 612 nm is apathetic, thus a colorimetric and ratiometric fluorescent sensing strategy was first designed to detect OPs by using glyphosate (Gly) as a typical model of OPs. Then, in consideration of the benefits of smartphone which can make the sensing process more convenient, stable, rapid and sensitive feedback, a smartphone coupled with hydrogel detection platform was proposed also for OPs determination. In addition, the designed sensing strategy offers superior selectivity , stability and real application capabilities. It’s thus expected the as-designed Ru@Zr-MOFs nanozyme based dual-mode sensing strategy possesses important real application for the low-cost, rapid, sensitive and accurate determination of OPs.
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CRYSTENGCOMM
·
2015
·Vol. 17
·期 33
·6434-6440
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IF 4.034
Yitong Han,Min Liu,Keyan Li,Yi Zuo,Yingxu Wei,Shutao Xu,Guoliang Zhang,Chunshan Song,Zongchao Zhang,Xinwen Guo
UiO-66 with crystal size ranging from hundreds of nanometers to a few micrometers and with cubic and cuboctahedral morphologies were synthesized. Crystal size and morphology varied with the additive amount of hydrofluoric acid and the concentration of reactants (ZrCl4 and H2BDC) during solvothermal synthesis. According to energy dispersive spectrometry (EDS) and 19F MAS NMR measurements, the fluorine ions directly bonded to Zr in the SBUs (secondary building units) in the MOF framework due to their strongest electronegativity. The bonding of the fluorine ions and Zr not only compensated for the charge imbalance of the framework caused by missing linkers but also competed with the linkers to coordinate with the Zr metal centers, thereby controlling the processes of nucleation and growth of the UiO-66 crystals. The samples were further characterized by scanning electron microscopy (SEM), powder X-ray diffraction (XRD), Fourier transform-infrared (FT-IR) spectroscopy, thermogravimetric analysis (TGA) and Ar sorption isotherms, showing that the introduction of fluorine enhanced the thermostability and porosity of UiO-66.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·Vol. 38
·期 6
·e7500
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IF 3.7
Yu Zhang,Pei Wang,Gaiying Han,Zhaoyang Wang,Haitao Yu,Zhenzi Li,Xuepeng Wang,Ying Xie,Wei Zhou
Defects engineering is significant for photocatalytic environment remediation. To this end, visible-light-driven α-Fe 2 O 3 /ZrO 2-x S-scheme heterojunction photocatalysts with optimal oxygen vacancy (O v ) defects are successfully synthesized via a two-step method. Compared with pristine UiO-66-NH 2 -derived ZrO 2-x and α-Fe 2 O 3 , the heterojunction photocatalysts exhibit a wider range of visible light response and higher efficiency in separating photogenerated electron–hole pairs. Among them, the 5% α-Fe 2 O 3 /ZrO 2-x sample shows the best photocatalytic performance to the degradation of tetracycline (TC) (89.3%), in which the pseudo-first-order kinetic rate constants are 8.20 and 16.75 times that of pristine ZrO 2-x and α-Fe 2 O 3 , respectively. The outstanding photocatalytic degradation efficiency can be attributed to both the narrow-bandgap ZrO 2-x with visible light response and the formation of α-Fe 2 O 3 /ZrO 2-x S-scheme heterojunctions. During the formation of heterojunctions, the concentration of oxygen vacancies (O v ) at the interface of α-Fe 2 O 3 /ZrO 2-x decreases monotonically with the increasing loading of α-Fe 2 O 3 , thereby altering the electronic structure of the photocatalyst and forming the heterojunction firmly. In addition, the high stability implies the potential applications in fields of environment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Xiaoyu Mao,Changhua Li,Xiaofeng Zhang,Hao Chen,Chao Zhang,Rui Gou,Yi He
In this study, we developed a composite material comprising UIO-66-NH 2 encapsulated tannic acid (TA) loaded on Ti 3 C 2 Tx to improve the corrosion resistance of water borne epoxy (WEP) coatings. The successful synthesis of the material was determined by FT-IR, XRD, XPS, EDS, TGA, SEM and TEM characterization. Furthermore, ultraviolet (UV)tests were conducted to evaluate the release rate of TA at varying pH levels, revealing a release rate of approximately 95 % at pH 2. Electrochemical impedance spectroscopy (EIS) results over 60 d indicated that the R c value of TU-T/WEP remained unchanged at 3.934 × 10 8 , demonstrating a two-order magnitude increase compared to those of pure epoxy coatings, attributed to the synergistic active and passive protection of TU-T materials. The self-healing ability of the TU-T/WEP coating was validated through manual scratch experiments. Additionally, the EIS test showed that the R c value of TU-T/WEP coating increased to 3.5 × 10 5 after 72 h, representing a two-order magnitude increase over that of the WEP coating alone. This study introduces a novel approach using green tannic acid as a corrosion inhibitor and amino-functionalized Ti 3 C 2 Tx with UIO-66-NH 2 to enhance corrosion resistance and self-healing aproperties of coatings.
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PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
·
IF 15.7
Rushuo Li,Linmeng Wang,Peiyun Zhou,Jing Lin,Zhiyuan Liu,Juan Chen,Danfeng Zhao,Xiubing Huang,Zhiping Tao,Ge Wang
Developing catalysts for dicyclopentadiene (DCPD) hydrogenation to tetrahydrodicyclopentadiene (THDCPD) at low temperature is crucial and challenging for the green and energy-saving production of high energy density aviation fuel. Herein, hierarchically porous UiO-66(Ce) encapsulate Ru nanoclusters (NCs) was successfully customized by soft template method and in-situ reduction. The mesoporous UiO-66(Ce) promoted the high dispersion of Ru NCs, and the transfer of substrate molecules. By controlling the synthesis conditions, the electronic state, abundance, and microenvironment of Ru NCs were precisely regulated. Theory calculation and experimental results revealed that metallic Ru as the main active sites greatly promoted the adsorption and activation of substrate molecules. Therefore, mesoporous UiO-66(Ce) encapsulated Ru NCs showed remarkable catalytic DCPD hydrogenation performance with DCPD conversion of 100% and THDCPD selectivity of ~100% (60 °C, only 35 min). This study has brought new inspiration and guidance to the rational design of function materials for various catalytic applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Yuanyuan Cui,Jianmin Sun
Developing a highly efficient catalyst for the conversion of CO 2 into cyclic carbonate is crucial for achieving carbon neutrality. Incorporating target-specific active sites into solid catalysts represents a novel and promising strategy for enhancing the chemical conversion of CO 2 . In this study, the original UiO-66-NH 2 was post-synthetically modified by replacing the H atom of –NH 2 functional group in UiO-66-NH 2 with the Br group in 1-bromobutylimidazole (BIm) under alkaline conditions. Subsequently, the imidazole group in UiO-66-NH 2 -BIm was quaternized with bromoalkyls (including 3-bromopropionic acid, 2-bromoethanol, and 2-bromoethylamine hydrobromide), resulting in the synthesis of UiO-66-NH 2 modified by ionic liquids (ILs) containing hydrogen bond donors, denoted as IL-R@UiO-66-NH 2 (where R OH, NH 2 , COOH). The catalytic performance was assessed in the absence of cocatalyst and solvent at 100 °C, 5 h and 1.0 MPa CO 2 . Notably, IL-COOH@UiO-66-NH 2 exhibited the highest catalytic performance, achieving propylene carbonate yield of 96.1 %. This outstanding performance was attributed to the synergistic interactions between the Lewis acidity of the MOF node, the strong nucleophilicity provided by the Br − of the IL, and the hydrogen bonding interaction facilitated by the carboxyl group, Lewis basic N site from the IL cation. Additionally, IL-COOH@UiO-66-NH 2 demonstrated compatibility with a wide range of epoxy substrates and exhibited good recyclability.
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JOURNAL OF MOLECULAR LIQUIDS
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2024
·
IF 5.3
Jiawei Zheng,Xiaoyi Zhang,Zhuowa Li,Nanjing Zhong
Immobilization of acid ionic liquid (AIL) for heterogeneous catalysis is benificial for products separation and recycling the AIL for continuing reuse. In this study, AIL was grafted onto the amino group functionalized zirconium-based metal organic framework (NH 2 -UiO-66) to catalyze esterification for short chain fatty acid glycerides synthesis. AIL of 1-(4-Sulfobutyl)-3-Methylimidazolium Hydrogen Sulfate ([HSO 3 -BMIM][HSO 4 ]) was found suitable for short chain fatty acid glycerides after screening varied fatty acids with chain length from 4 to 18. [HSO 3 -BMIM][HSO 4 ] was therefore grafted and butyric acid glyceride was synthesized. Reaction conditions were optimized by means of single factor study and orthogonal experiment. The reusability of the AIL@NH 2 -UiO-66 was evaluated. The AIL@NH 2 -UiO-66 showed good esterificaiton performance and fine reusability. Butyric acid conversion (converted into the glycerides of mono-, di- and tributyrin) at 62.16% was obtained under the optimum conditions. In addition, the present AIL@NH 2 -UiO-66 was quite stable, and 67.39% of its initial esterification activity was retained after 11 cycles of reuse, suggesting it was potential in the esterification reaction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Yuanyuan Cui,Jianmin Sun
The direct oxidative carboxylation of olefins and CO 2 to synthesize cyclic carbonates involves a tandem process of epoxidation and CO 2 cycloaddition reactions. However, designing a multifunctional catalyst for this reaction remains challenging. Herein, a composite catalyst ImBr@UiO-66-Br(Co) was synthesized by post-metallization of Co 2+ and subsequent functionalization with an imidazole ionic liquid (IL), which was used effectively for this reaction. The effects of temperature, CO 2 pressure, catalyst dosage, and reaction time on the direct oxidative carboxylation of olefins to cyclic carbonates were investigated. The results showed that ImBr@UiO-66-Br(Co) exhibited optimal performance in the solvent-free reaction system with styrene (3 mmol), tert -butyl hydroperoxide (6 mmol), and tetrabutylammonium bromide (TBAB, 50 mg) at 80 ℃ under 1 MPa CO 2 for 24 h, achieving a styrene conversion of 90.3 % and styrene carbonate selectivity of 80.7 %. The excellent catalytic activity of ImBr@UiO-66-Br(Co) was attributed to the synergistic interactions of the Lewis acidity Zr 4+ sites, the strong nucleophilicity provided by Br - , the weak base sites from tertiary amine and quaternary ammonium groups in imidazole IL, and the redox-active Co 2+ sites. Additionally, the catalyst was easy to separate and maintained stable activity and selectivity over at least five cycles. Finally, the potential catalytic mechanism for the direct oxidative carboxylation of olefins to cyclic carbonates was proposed.
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APPLIED ORGANOMETALLIC CHEMISTRY
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2024
·
IF 3.7
Fangfang Li,Xiaofang Hou,Ying-Hua Zhou
CO 2 chemical fixation offers a feasible approach for carbon mitigation and high-value utilization, but it is still challenging to develop an efficient catalyst for CO 2 conversion into cyclic carbonate. Herein, the triethylenediamine-derived dicationic ionic liquids (DIL-X, X = Cl, Br, and I) were grafted into UiO-66 linkers through self-assembly of Zr 4+ ions and the mixed ligands of terephthalic acid and DIL-bearing dicarboxylic acid, resulting in UiO-66-DIL-X n , ( n designated as molar amount of the feeding DIL-X). Their catalytic performance was evaluated by the epoxide cycloaddition reaction in the absence of solvent and cocatalyst. Among them, the UiO-66-DIL-Cl 0.4 catalyst exhibited outstanding performance, with a chloropropene carbonate yield of 92% and a high selectivity of 99% under 0.1 MPa CO 2 at 110 °C for 16 h. Its high activity could be ascribed to the cooperativity among Lewis acidity of MOF nodes, the enhanced CO 2 absorption, and the strong nucleophilicity offered by halogen ions of ionic liquid-modified MOF. Moreover, UiO-66-DIL-Cl 0.4 presented excellent recyclability and substrate extension. A potential catalytic mechanism for the epoxide-CO 2 cycloaddition into cyclic carbonate has been proposed. This work will shed light on the rational design of functionalized MOFs-based catalysts for CO₂ utilization.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·
IF 3.7
Yan Gao,Shumin Zhao,Jingwen Huang,Tao Han,Jianshe Zhao
Venturello-structured polyoxometalates (POMs) are effective homogeneous catalysts and confining POMs to size-matched metal-organic frameworks (MOFs) as heterogeneous catalyst is an effective way to improve their practical application. The appropriate pore and narrow window of pristine UiO-67 can not only enclose POMs in single molecule but also limit their leaching and can provide a suitable platform for the oxidation of most sulfur-containing organic compound. The composite (CTA) 3 PW 4 @UiO-67 was prepared by a facile in situ synthesis method, characterized by a variety of means and tested for desulfurization of multicomponent simulated diesel. The results prove that the active component (CTA) 3 PW 4 is effectively encapsulated, and the composite (CTA) 3 PW 4 @UiO-67 show remarkable desulfurization activity and excellent reusability. In addition, the kinetics and possible mechanism of the reaction were investigated. This work opens up a new idea for the design of “host-guest adapted” catalyst suitable for fuel desulfurization technology.
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