NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 29
·13855-13865
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IF 3.3
Yong Cheng,Lin Deng,Dan Wang,Changchun Ji,Ying-Hua Zhou
The development of advanced catalysts is essential for efficient elimination of the emerging organic pollutants in water. Herein, Cu9S5 and Cu9S5@UiO-66-NH2 were prepared and both exhibited high Fenton-like photocatalytic activities for the degradation of organic contaminants. Removal efficiencies of 85% and 92% were achieved for Congo red (CR) and Rhodamine B (Rh B), respectively. It is found from active species trapping experiments and electron spin resonance (ESR) analysis that ˙O2−/h+ and ˙O2−/˙OH played key roles in the oxidation reaction of these two pollutants, respectively. The mechanisms were discussed on the basis of the cycles of Cu+/Cu2+.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 47
·期 5
·2257-2263
·
IF 3.925
Shiyu Nie,Fengfeng Chen,Tianbo Shen,Tingting Wang,Ningyu Di,Junkuo Gao
Adjusting the internal porous environment of MOFs to enhance their adsorption properties is considered an effective strategy to improve their gas separation performance. Herein, 1-ethyl-3-methyl-imidazolium acetate ([Emim][Ac]) was encapsulated in UiO-66 by an impregnation method for the improvement of carbon dioxide (CO2) capture performance. The synthesis and detailed characterizations of the developed [Emim][Ac]@UiO-66 are reported, and the effect of the loading amount of [Emim][Ac] on the CO2 separation performance was also studied. The obtained [Emim][Ac]@UiO-66 could efficiently show the synergistic effect of the adsorption of CO2 between [Emim][Ac] and UiO-66. The optimized [Emim][Ac]@UiO-66 exhibited a much higher CO2 adsorption capacity at 298 K and 1.0 bar, affording 2 times the CO2 uptake than its original UiO-66. In addition, the CO2/N2 selectivity and CO2/CH4 selectivity of [Emim][Ac]@UiO-66-3.5% are significantly higher than those of UiO-66. This study for designing various MOF-encapsulated ionic liquids potentially paves the way for the development of highly efficient absorbents for gas separations.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Shuting Tian,Yang Bai,Shuangshuang Li,Zuoming Chen,Liyun Zhang,Hongjie Li,Peng Zhou,Yi He
Microsphere layers/nanofibrous membranes decorated with UiO-66-NH 2 as a metal-organic framework (MOF) were successfully obtained by one-step coaxial electrospinning. The coaxially spun dense microsphere/wire-like structure and UiO-66-NH 2 hydrophilic components with excellent hydration ability enabled the prepared membrane to have excellent static and dynamic adsorption capacity for dyes and oil-in-water emulsion separation performance (adsorption capacity >247 mg/g; separation efficiency >99%). What's more, the membrane can purify complex wastewater dynamically and efficiently (separation efficiency >99%). After the membrane was desorbed in ethanol and methanol, the reversible recovery rate was as high as 98%, indicating its excellent recyclability. In a word, the as-prepared membrane has broad prospects in the remediation of complex polluted water bodies containing dyes-oil.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wenqing Hou,Chen Chen,Diya Xie,Yiming Xu
Metal–organic frameworks (MOFs) as photocatalysts have received increasing attention. In this work, a dual metal-substituted UiO-66-NH2 (Ti/Ce-MOF) containing different Ti/Ce mole ratios (x = 0–2.46) has been prepared via post-synthetic exchange between Ce-UiO-66 and TiCl4, followed by amination. The solid had a high surface area (828–937 m2/g) and a large pore volume (0.451–0.507 m3/g). Under visible light, Ti/Ce-MOF showed x-dependent activity for H2O reduction and oxidation on a film electrode, respectively. However, such a change for H2 evolution in a Na2S/Na2SO3 aqueous solution was observed only after CdS loading. In combination with the photoluminescence and band parameters, we propose that the photoactivity of Ti/Ce-MOF for redox reaction is determined by its ability for electron transfer. Furthermore, there is an interfacial electron transfer from Ti/Ce-MOF to CdS and a hole transfer from CdS to Ti/Ce-MOF, respectively, significantly improving the efficiency of charge separation for redox reactions. This work offers a new insight that Ti substitution benefits the performance of Ce-based MOF.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 30
·10472-10480
·
IF 4
Pingping Teng,Ying Liu,Zhongqiao Sun,Hao Meng,Yide Han,Xia Zhang
Development of binary MOF-on-MOF heterostructures is a research hotspot in MOFs chemistry due to the advantages elicited by a closely connected interface, which may endow more abundant functionality and even broader applications in interface chemistry. A MOF-on-MOF heterostructure was constructed by in situ growth of MIL-88B on the outer surface of UiO-66. The resultant MIL-88B@UiO-66 produced had an interesting flower-like morphology composed of MIL-88B (petal) on tetrahedral UiO-66 (core). The MIL-88B@UiO-66 heterostructure showed adsorption and Fenton-like oxidation abilities, with distinctly improved structural stability in aqueous solution compared with that of single MIL-88B. Methylene blue (MB) was selected as the target molecule to evaluate the adsorption and Fenton-like oxidation activities. The efficiency of total removal of MB was studied systematically under various operating conditions and the influencing factors were optimized. The kinetics of adsorption and catalytic oxidation were simulated to explore the interactions between MB and MIL-88B@UiO-66. The mechanisms of enhanced adsorption and Fenton-like oxidation were suggested. The cyclic removal performance and structural stability of MIL-88B@UiO-66 were also determined.
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LANGMUIR
·
2022
·
IF 4.331
Lan Ma,Yan Wan,Teng Wang,Yaling Liu,Ying Yin,Liyun Zhang
Developing the high-anti-fouling membrane has kept continuous attention in oil/water emulsion treatment. However, the majority of works on anti-fouling membranes mainly focused on low-viscosity oils, which greatly limited the development and application of a membrane to face the real crude oil wastewater. Inspired by the hydrophilicity of sodium carboxymethyl cellulose (CMC) and zirconium base metal–organic frame (Zr-MOF), an anti-oil-fouling CMC/UiO-66-NH2 composite membrane was constructed by a self-assembly method. Profiting from the hydrophilicity and micro-nanostructure of the CMC/UiO-66-NH2 layer, the obtained CMC/UiO-66-NH2 membranes displayed underwater superoleophobicity and desired oil resistance. It could display the effective separation capability with 1282 ± 62 to 6160 ± 81 L/(m2·h·bar) and above 99.08% toward the different light oil emulsions. More importantly, the CMC/UiO-66-NH2 membrane displayed ultralow crude oil adhesion behaviors toward the crude oil emulsions, which could achieve a considerably high flux (746 ± 60 to 5224 ± 87 L/(m2·h·bar)). Furthermore, electrostatic interaction and physical enwinding–wrapping between CMC and UiO-66-NH2 also endowed the composite membranes with outstanding stability. After immersing the as-prepared membranes into the harsh environments for 24 h, the membranes still maintained high underwater–oil contact angles (UWOCA > 155°) and separation ability (oil rejection was above 99.0%). Therefore, CMC/UiO-66-NH2 composite membranes could demonstrate promising prospects in real oily emulsion treatment.
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Results in Chemistry
·
2022
·
IF 0
Xia Zhang,Lili Sun,Yangang Sun,Meng Zhou,Siqi Wang,Zihao Cao,Xueying Zhang,Yajun Wei,Yuandong Xu
Developing electroactive materials with superior sensitivity, selectivity, and so on is an important issue for target ions detection. Hierarchically heterostructured nanomaterials represent a kind of promising active materials for electrochemical sensors due to the synthetic effect between different components and the high surface area. Herein, heterostructured UIO-66-NH 2 /CNTs nanocomposites have been successfully synthesized via the solvothermal method and investigated for the detection of Pb 2+ ions. The SEM, TEM, XRD and FTIR collectively confirmed that the UIO-66-NH 2 was successfully loaded on the surface of the CNTs. The specific surface areas of the UIO-66-NH 2 /CNTs are 4–7 times higher than that of activated CNTs and more mesoporous structures appear in composite materials. The electrochemical impedance spectroscopy measurements showed that the concentration of CNTs could influence the electron mobility and the UIO-66-NH 2 /CNTs-15 exhibits the lowest charge transfer resistance and the highest capacitive property. The cyclic voltammetry study towards K 3 [Fe(CN) 6 ] further demonstrated that the CNTs can improve the conductivity of the composites especially for the UIO-66-NH 2 /CNTs-15, which was conducive to the sensing behavior confirmed by follow-up performance experiments. Under the optimized condition, UIO-66-NH 2 /CNTs-15 exhibits the best sensing performance towards Pb 2+ . Correspondingly, a high sensitivity of 1.64 μA (μmol/L) −1 and a low detection limitation of 0.206 μmol/L (S/N = 3) are achieved. Meanwhile, a wide detection range, excellent selectivity, repeatability, and stability are also obtained. The recovery experiment by standard addition method is also carried out and a satisfactory result has been attained indicating a promising sensor for practical application.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Rong Shang,Qizhao Zhang,Peng Lin,Bang Gu,Qinghu Tang,Qiue Cao,Wenhao Fang
Direct oxidative coupling of alcohols and amines is an environmental-benign and atomic-economy approach for imine synthesis. We disclosed that UiO-66 framework successfully confined Ru to single-atom scale with assistance of oxophilic Zn 2+ promoter. This RuZn@UiO-66 catalyst showed a highest TOF of 78 h -1 among all Ru catalysts in literature and attained > 99% yield to benzylideneaniline in the model reaction in an O 2 atmosphere at a low temperature without alkaline additives. In addition, this catalyst demonstrated satisfying gram-scale imine synthesis, wide substrate scope and stable reusability. Kinetic investigations and in situ characterizations allowed getting insights to active sites, amphoteric carrier and reaction mechanism. Dynamic interactions between Ru and Zn based on their ratios induced electron-deficient Ru 0 active sites promoted by oxophilic Zn 2+ species. Hence, primary alcohols can be efficiently converted to the corresponding aldehydes using molecular O 2 , i.e. , the rate-determining step. Besides, Zr 4+ -O 2- pairs on UiO-66 provided adequate acidic-basic sites for the tandem catalysis.
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ANALYST
·
2022
·Vol. 147
·期 17
·3867-3875
·
IF 5.227
Fangfang Yu,Yihan Wang,Tengfei Liu,Xiaohui Liu,Hui Jiang,Xuemei Wang
Hypochlorite plays a vital role in biological systems and our daily life. The rapid and convenient detection of hypochlorite is imperative and significant for disease treatment and human health. In this work, EY/UiO-66-NH2 (EY = eosin Y) was prepared through a hydrothermal process and could be applied to the detection and bioimaging of hypochlorite as a self-calibrating sensing nanoprobe. EY/UiO-66-NH2 features two emissions at 432 nm and 533 nm, and the emission intensity of 533 nm is enhanced with increasing ClO− concentration. EY/UiO-66-NH2 could be utilized as a ratiometric fluorescence sensor of ClO−. The linear range of EY/UiO-66-NH2 towards ClO− is 0.1–200 μM and its detection limit is 46.4 nM. In comparison with previously reported probes for ClO−, EY/UiO-66-NH2 has the advantages of a wide linear range, low detection limit, turn-on fluorescence and ratiometric response. This work provides a new method for ClO− detection in living cells.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Xuesheng Liu,Junsu Jin,Hong Meng
In this study, we successfully synthesized a novel composite material UiO-66/polyacrylate (UiO/PA) by suspension polymerization and in situ growth of metal–organic frameworks (MOFs). Due to the control of heterogeneous nucleation and firm growth, nano-UiO-66 with a diameter of only 400 nm has been reduced by about 90%, resulting in lower transfer resistance, effective separation of photogenerated carriers, and more catalytic active sites exposed. Under visible light irradiation, UiO/PA with 48.7% loading can almost completely degrade rhodamine B (RhB) in 120 min and the corresponding degradation rate constant of RhB reached 0.0203 min–1 from 0 min–1. After easy filtration and five cycles, the degradation rate is still above 85%. This study can provide new insights into effectively improving the photocatalytic performance of MOFs.
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TALANTA
·
2022
·
IF 6.556
Yi Wu,Keren Lu,Fubin Pei,Yanghao Yan,Shasha Feng,Qingli Hao,Mingzhu Xia,Wu Lei
The wide clinical application of d -penicillamine (D-PA) makes it inevitably accumulates in the environment, seriously threatening human health and the ecological environment. To better supervisory control D-PA, a highly sensitive and reliable photoelectrochemical (PEC) sensor based on gold nanoparticles (Au NPs) loaded on graphitic carbon nitride sheet and hexagonal NH 2 -UiO-66 composite (g-C 3 N 4 /Au/NH 2 -UiO-66) was synthesized. Tactfully using the strong bonding between D-PA and Au NPs and the effective carrier separation of Z-scheme heterojunction, the designed g-C 3 N 4 /Au/NH 2 -UiO-66 PEC sensor without an extra recognition unit exhibited a selective and sensitive photocurrent to D-PA. With the aid of UV diffuse reflectance spectra (UV-DRs), electron paramagnetic resonance (EPR) characterization, and free radical capture experiments, the electron transfer path of the PEC sensing system was deduced. The proposed g-C 3 N 4 /Au/NH 2 -UiO-66 PEC-based sensor achieved a low detection limit of 0.0046 μM (S/N = 3) with a wide linear response ranging from 10 nM to 400 μM. In addition, its good stability and selectivity also laid a good foundation for practical applications.
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EUROPEAN POLYMER JOURNAL
·
2022
·
IF 5.546
Shuang Han,Yuzhuo Song,Shiwei Liu,Le Zhao,Ruonan Sun
The preparation of synthetic drug delivery systems free of antibody modifications that can effectively recognize tumor sites and control drug delivery is essential for cancer therapy. In this study, UiO-66 metal–organic framework (MOF) modified with amino and phenylboronic acid groups was used as substrate to load the anti-cancer drug doxorubicin (DOX). Then a molecularly imprinted polymer (UiO-66-DOX@MIP) with sialic acid (SA) as the template molecule was further prepared on the surface of the synthesized nanoparticles using surface molecular imprinting technique (MIT). This polymer combines the excellent properties of UiO-66 and molecularly imprinted polymer (MIP). It was simple to prepare, economical and easy to obtain, and had a regular morphology. UiO-66-DOX@MIP containing molecularly imprinted binding sites that match the template molecule SA, could specifically recognize target tumor cells. The imprinted layer prevented drug leakage in normal body fluids while degrading and drug release under tumor microenvironment, with pH and glutathione (GSH) dual-responsive drug release properties. The UiO-66-DOX@MIP showed excellent biocompatibility and great cellular uptake efficiency to cancer cells without influence of interfering substances.
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