Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Baiyu Chen,Man Zhang,Kaili Yao,Churu Zhang,Qi Wu,Tianding Hu,Shaoyun Shan
Metal-organic frameworks (MOFs) have attracted exciting application prospects in photocatalytic hydrogen (H 2 ) evolution due to the diversity of organic ligands and metal ions . However, the inappropriate conduction band position of pristine MOFs and corresponding large overpotential for H 2 evolution restrict the H 2 production under visible light. Herein, a dye-sensitized NH 2 -UiO-66 anchored with copper ions (EY-6Cu-NU-66) was synthesized by in-situ Cu anchoring followed by Eosin Y sensitization. The H 2 production activity showed that EY-6Cu-NU-66 reached 3579.82 μmol·g −1 ·h −1 under visible light, which was four times higher than that of dye-sensitized pristine NU-66 (EY-NU-66) and 99-fold higher than that of 6Cu-NU-66 free of dye sensitization. A series of characterizations and theoretical computations indicated that photo-generated electrons first transfer from the excited Eosin Y to the lowest unoccupied molecular orbital (LUMO) of the NU-66, then further transfer to the transition Cu II /Cu I metal center that is formed by Cu anchored on -NH 2 . This tandem mechanism not only improves the visible-light absorption ability of NU-66 but also promotes its separation efficiency of photo-generated carriers, thus greatly reducing the overpotential for H 2 evolution. This work provides a new strategy for visible-light-driven H 2 production by dye-sensitized MOF-based materials without noble metal loading.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Yongtong Lei,Lijing Zhu,Jilong Xu,Shuan Liu,Zhixiang Zeng,Xiaocheng Li,Gang Wang
Metal organic framework (MOF) with fine pore structures, ultra-high porosity and large specific surface area can provide more water transport channels while achieving precise sieving of different sizes of ions, which is a promising material for high efficiency desalination. However, particle agglomeration, interface incompatibilities and interface defects severely restrict the performance of MOF-based membranes. It is still a challenge to construct MOF-based desalination membranes with both high water permeability and high ion sieving. Herein, the UiO-66-NH 2 based nanofiltration membrane was fabricated by in-situ growth of UiO-66-NH 2 on Nylon membrane and composed with polyamide (PA) layer by interfacial polymerization (IP). With 12 h solvothermal reaction, the UiO-66-NH 2 nanoparticles are found uniformly loaded on the Nylon substrate. Therefore, the water molecule transport channels provided by UiO-66-NH 2 nanoparticles reduce the transport resistance, which can improve the water permeability. More importantly, UiO-66-NH 2 nanoparticles are found to be involved in the IP process, which can reduce the interfacial defects and thus enhance the bonding force between the PA layer and base film. The synergistic effect of the UiO-66-NH 2 and PA layer improves the nanofiltration performance of the membrane with rejection rate of 92.97% for Na 2 SO 4 and the pure water permeance (PWP) of 11.55 L m −2 h −1 bar −1 . The N-UN12 @PA membrane also has excellent antifouling performance (flux recovery ratio (FRR) of 95.86%, reversible fouling ratio (Rr) of 33.93%, irreversible fouling ratio (Rir) of 4.14%). Unlike the mixed-matrix membrane (MMM) and polycrystalline MOF membrane, this strategy provides a promising method to prepare high-performance nanofiltration membrane for desalination.
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高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Xuan Wan,Haohao Du,Du Tuo,Xiaoman Qi,Tianyu Wang,Jingtao Wu,Guangli Li
The excessive use of gatifloxacin (GAT) can seriously pollute the environment and damage human health. Therefore, reliable detection of its concentration is essential for environmental protection and physical health. Herein, an efficient and stable voltammetric sensor based on zirconium-based metal–organic framework/carboxylated multiwalled nanotube nanocomposites (UiO-66/MWCNT-COOH) was constructed for the determination of GAT. The morphologies, microstructures, and electrochemical properties of UiO-66/MWCNT-COOH were investigated by using various microscopic, spectroscopic, and electrochemical techniques. UiO-66/MWCNT-COOH showed good electrocatalytic activity for GAT oxidation with remarkable voltammetric response signals, which was primarily attributed to the synergistic effect from UiO-66 and MWCNT-COOH. Electrochemical kinetics studies revealed that the electrocatalytic oxidation of GAT is an irreversible and diffusion-limited reaction involving two protons and two electrons. The anodic peak current of GAT is linearly correlated with GAT concentration in the range from 0.05 to 10 μM with a low detection limit of 0.0075 μM. Moreover, UiO-66/MWCNT-COOH demonstrated high selectivity, reproducibility, and repeatability as well as extraordinary long-term stability (at least 7 weeks). The proposed UiO-66/MWCNT-COOH reliably detected trace GAT in the effluent, milk, human serum, and eye drops with satisfactory recoveries. Together with its outstanding merits such as low cost, robust response, short assay time, and good sensitivity, the proposed sensor shows enormous prospects for in situ determination of multiple antibiotics.
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高影响因子
Water
·
2023
·Vol. 16
·期 1
·145
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IF 3.4
Yanqiu Zhang,Yang Lu,Minrui Sun,Dechang Zeng
In recent years, the excessive use and disordered discharge of antibiotics have had sustained adverse effects on ecological balance and human health. The convenient and effective detection of these “emerging pollutants” has become one of the research hotspots in the environmental field. In this study, a defective UiO-66 material, namely UiO-66-D, was constructed for the sensitive and selective sensing of tetracycline (TC) and moxifloxacin (MXF) in water. By utilizing a modulated synthesis approach with concentrated HCl, stable blue fluorescence at 400 nm was achieved for UiO-66-D. The as-prepared UiO-66-D could conduct the inner filter effect (IFE) within a short time (10 s) when sensing TC and MXF, and the fluorescence of the UiO-66-D was quenched. In particular, when sensing MXF, a ratiometric signal response was generated due to the combined effect of the IFE and the fluorescence of MXF itself. The sensitive and selective detection of TC and MXF using UiO-66-D was free from the interference of common anions and cations in water samples. The detection limit (LOD) for TC was determined to be 70.9 nM (0–115 μM), while for MXF, it was found to be 33.1 nM (0–24 μM). Additionally, UiO-66-D was successfully used to recognize TC and MXF in lake water with good recoveries, demonstrating that UiO-66-D exhibits substantial potential in the recognition of pollutants in environmental waters.
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Applied Materials Today
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2021
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IF 10.041
Minghao Ni,Ming Gong,Xiang Li,Jinlou Gu,Bo Li,Ye Chen
Metal-organic frameworks (MOFs) have attracted significant attention thanks to their excellent physical and chemical properties. Metal-organic frames are widely used in optics. For example, metal-organic frameworks can be used in fluorescent probes to detect and treat diseases, and can also be used to make solid-state light-emitting devices. Considering the high stability and easy synthesis of Zr-based UiO-66 MOF as well as the strong fluorescent emission of porphyrin molecules, the TCPP-incorporated UiO frameworks would inherit these advantages and exhibit intriguing optical performance. Therefore, in this paper, TCPP was doped into UiO-66, and the optical properties of the resulting MOF structure were observed. To obtain the optimal doping condition, three doping concentrations of TCPP were used. Besides the structural and morphological characterization by X-ray diffraction and scanning electron microscopy, more attentions have paid on the optical testing based on absorption and fluorescence spectroscopy, two-photon fluorescence spectroscopy and time-resolved spectroscopy. As a result, the TCPP-doped MOFs exhibited good fluorescence properties and satisfied our previous expectations of nonlinear optical properties and two-photon absorption. This work would pave a new way in constructing various MOFs-based solid-state devices with widespread optical applications.
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Journal of Environmental Chemical Engineering
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2020
·
IF 4.3
Yi Cheng,Jilin Zhang
Excessive phosphate in wastewater can cause eutrophication of water body, which will worsen the ecological environment and threaten human health and biological life safety. Adsorption of phosphate is the most effective way to remove phosphate, and efficient adsorbent is the key. Amorphous La(OH) 3 has been deemed as a potential phosphate adsorbent on account of high adsorption capacity and environmentally friendly property. However, it also shows some disadvantages such as easy agglomeration, poor water dispersion. In this study, UiO-66-NH 2 was used as carrier to load amorphous lanthanum hydroxide as an adsorbent for phosphate removal. The adsorbent (UiO-66-NH 2 @La(OH) 3 , ULCs) has good water dispersibility and it is easy to be separated and recovered. At the same time, the maximum phosphate adsorption capacity can reach 140.7 mg P/g. The adsorption process accords with pseudo second order kinetic model and Freundlich isotherm model. The thermodynamic results showed that the adsorption process was spontaneous and endothermic. In addition, in the presence of coexisting anions (such as Cl − , SO 4 2− , NO 3 − ), it also exhibited high selectivity and phosphate removal efficiency. Meanwhile, the adsorption capacity keeps at a high level in the range of pH 3–11. By the merit of above-mentioned properties, the prepared material is expected to be an ideal candidate for phosphate removal from contaminated water.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2020
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IF 4.551
Zongjian Liu,Zhicong Sun,Zhao Zhang,Lifei Xu,Lin Zhang,Qun Cui,Haiyan Wang
UiO-66-Z with uniform mesopores using 2-aminoterephthalic acid and terephthalic acid as mixed ligands was synthesized by hydrothermal method in this paper. Thermodynamic and dynamic properties of UiO-66-Z were discussed. Dynamic separation performance and adsorption selectivity of UiO-66-Z for the equimolar n-heptane/methylcyclohexane (nHEP/MCH) binary mixture were investigated. Results show that UiO-66-Z has complete tetrahedral cages with uniform mesopores of 38 Å. Adsorption rate constant of MCH on UiO-66-Z (14.5 × 10 −3 S −1 ) is twice that of UiO-66 (6.7 × 10 −3 S −1 ), while nHEP does not significantly change at 323K with the pressure of 0.05–0.1 kPa. Effective adsorption diffusion coefficient of nHEP and MCH on the UiO-66-Z is about 25 times higher than that on the UiO-66. Compared with UiO-66, the desorption activation energy (Ed 1 ) of the first desorption peak of nHEP and MCH on the UiO-66-Z is reduced by 53.75% and 76.66%, respectively. The separation selectivity of MCH to nHEP on the UiO-66-Z reaches up to 3.13 at 473 K. Results indicate that the introduction of mesopores in the UiO-66-Z can enhance mass transfer of nHEP and MCH in the pores, especially which is more obvious mass transfer effect for MCH with a larger molecular dynamics diameter under low partial pressure. The retention of most tetrahedral cages in the UiO-66-Z is conducive to improving its inverse shape separation selectivity for MCH/nHEP. Compared with UiO-66, nHEP and MCH have higher desorption efficiency on UiO-66-Z at the same temperature and time.
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JOURNAL OF MATERIALS SCIENCE
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2020
·Vol. 56
·期 2
·1577-1589
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IF 3.553
Li Zhaohua,Hu Rui,Ye Shuai,Song Jun,Liu Liwei,Qu Junle
Abstract We report herein a versatile new approach for improving the photodegradation performance of UiO-66 by introducing 2-methylimidazole through a straightforward in situ one-pot solvothermal method. The resultant complex UiO-66-M-0.7 has demonstrated a reaction rate constant of 0.0183 min −1 in the photodegradation of rhodamine B under visible light, which is 69.4% higher than that with unmodulated UiO-66. Further investigation has confirmed that the improved activity can be attributed to enhanced adsorption of the dye by the photocatalyst during the adsorption–desorption equilibrium. The main active species involved in the photodegradation process have been identified as h + and O 2 − ·. In addition, the complex has shown ideal stability in recycling tests and excellent activity in the degradation of methylene blue. This study provides a novel perspective for the future design of various photocatalysts with superior performance. Graphic abstract 2-Methylimidazole-modulated UiO-66 exhibits increased catalytic performance in the photodegradation of rhodamine B (RhB) under visible light because of enhanced adsorption of RhB on the catalyst during the adsorption-desorption equilibrium.
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Arabian Journal of Chemistry
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2020
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IF 4.762
Zhen Huang,Chen Wang,Jiling Zhao,Shixing Wang,Yang Zhou,Libo Zhang
A new adsorbent was successfully fabricated by chemically linking pyromellitic acid onto a zirconium-based metal-organic framework composite for selective adsorption of Pd(II) from an aqueous solution. The adsorbent was characterized by Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller equation and scanning electron microscope. The adsorption capacity, selectivity and repeatability of the adsorbent were tested by batch experiments. The optimum pH was 2.0, and the maximum adsorption capacity at room temperature was 226.1 mg/g. In the kinetic experiments, the adsorption process achieved equilibrium within 5 h and generally conformed to the quasi-second kinetics and Freundlich isotherm model. The N-H and O H groups on the adsorbent interacted with Pd(II) by electrostatic and coordination action. The adsorbent maintained excellent adsorption capacity after at least 5 cycles. At the same time, the selectivity of the adsorbent in aqueous solution is excellent from interfering ions. Therefore, the new adsorbent will have an obvious application prospect on the recovery of palladium.
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Membranes
·
2021
·Vol. 11
·期 9
·693
·
IF 4.106
Fei Guo,Bingzhang Li,Rui Ding,Dongsheng Li,Xiaobin Jiang,Gaohong He,Wu Xiao
Mixing a polymer matrix and nanofiller to prepare a mixed matrix membrane (MMM) is an effective method for enhancing gas separation performance. In this work, a unique UiO-66-decorated halloysite nanotubes composite material (UiO-66@HNT) was successfully synthesized via a solvothermal method and dispersed into the Pebax-1657 matrix to prepare MMMs for CO2/N2separation. A remarkable characteristic of this MMM was that the HNT lumen provided the highway for CO2diffusion due to the unique affinity of UiO-66 for CO2. Simultaneously, the close connection of the UiO-66 layer on the external surface of HNTs created relatively continuous pathways for gas permeation. A suite of microscopy, diffraction, and thermal techniques was used to characterize the morphology and structure of UiO-66@HNT and the membranes. As expected, the embedding UiO-66@HNT composite materials significantly improved the separation performances of the membranes. Impressively, the as-obtained membrane acquired a high CO2permeability of 119.08 Barrer and CO2/N2selectivity of 76.26. Additionally, the presence of UiO-66@HNT conferred good long-term stability and excellent interfacial compatibility on the MMMs. The results demonstrated that the composite filler with fast transport pathways designed in this study was an effective strategy to enhance gas separation performance of MMMs, verifying its application potential in the gas purification industry.Keywords:composite material;UiO-66;HNT;mixed matrix membrane;CO2/N2separation
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PubMed
高影响因子
FUEL
·
2021
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IF 6.609
Mengchang Zhou,Changsong Zhou,Dong Chen,Hao Wu,Zhen Zhang,Hongmin Yang,Wei Ruan,Yaming Zhou,Zengqiang Tan
Gaseous toluene, one of the volatile organic compounds, has aroused wide concerns in China due to its growing emissions and harmfulness. Herein, novel manganese decorated UIO-66 catalysts (Mn/UIO-66) were prepared by hydrothermal synthesis and applied to the vaporized hydrogen peroxide system for toluene removal. TEM, BET, XRD, ICP, and XPS were used to analyze the chemical and physical characteristics of Mn/UIO-66. A toluene removal efficiency of 82% with the 3-Mn/UIO-66 catalyst in the vaporized hydrogen peroxide system could achieved. The effects of different reaction conditions (reaction temperature, hydrogen peroxide concentration, and initial toluene concentration) on toluene removal were determined. The yield of hydroxyl radical in the Mn/UIO-66 catalyst combined with the hydrogen peroxide system was positively correlated with the Mn decorated ratio. Results suggested that the catalytic performance is related not only to the yield of hydroxyl radical but also to the catalyst specific surface. The intermediate products during toluene removal were analyzed by gas chromatography-mass spectrometry (GC–MS), and the possible reaction pathway of toluene removal was proposed.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Qian Chen,Yi Feng,Rongrong Tian,Jinghang Chen,Anqing Wang,Jianfeng Yao
Photosensitization is a promising way to make UiO-66 visible light responsive. In this work, zirconium (Zr) precursors and synthetic methods (solvent-assisted or nonsolvent-assisted) were found to significantly affect the electric charge and the defect sites of UiO-66. UiO-66 with enhanced adsorption and photosensitized photocatalytic ability was then obtained. When ZrOCl2·8H2O was applied as Zr-precursor in a nonsolvent method, defect rich UiO-66 (UiO–OCl–N) was achieved with higher Cr(VI) adsorbing ability and improved photosensitized photocatalytic ability. Moreover, with the coexistence of Rhodamine B in Cr(VI) solution, photocatalytic performance of UiO-66 can be further enhanced.
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危险品化学品经营许可证（带存储）