ANALYST
·
2022
·Vol. 147
·期 24
·5655-5662
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IF 5.227
Ying Zhou,Ruichun Li,Guomei Zhang,Yan Zhang,Caihong Zhang,Shaomin Shuang
Metal–organic frameworks (MOFs) have emerged as interesting nanomaterials owing to their large surface area, high porosity, tunable pore architecture and easy functionalization. However, an inferior electrical conductivity hinders their application in electrochemical sensing. In this paper, gold–palladium alloy/UiO-66-NH2/graphene (AuPd/UiO-66-NH2/GN) composites were synthesized by loading alloys on the surfaces of MOFs and then attaching them to the graphene surface. The addition of metal nanoparticles and graphene enhanced the electron transfer ability of MOFs. Then, composites were used to modify a glassy carbon electrode (GCE) to construct a sensitive dopamine (DA) electrochemical sensor. The developed sensor manifested two linear relationships in lower concentration ranges and in higher concentration ranges with a 0.21 × 10−6 mol L−1 low detection limit (3σ/k) under optimal conditions. The results certified that the constructed sensor had high selectivity, excellent reproducibility and good stability, and had been used successfully for DA detection in actual human serum samples.
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高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Di Zhang,Hao Tang,Bing Zhao,Lijie Liu,Hongwei Pang,Xiangxue Wang,Shujun Yu
Radioactive uranium removal plays a key role in energy development and environmental security. Sulfide nanoscale zero-valent iron (S-NZVI) has good antioxidant capacity, dispersibility and activity to eliminate U(VI) from wastewater, but the removal efficiency is limited. To improve the reduction and adsorption capacity of S-NZVI, through treating Fe 3+ solution by nitro-functionalized UiO-66 (UiO-66-NO 2 ) with high porosity, UiO-66-NO 2 enhanced S-NZVI adsorbent (S-NZVI/UiO-66) was prepared by liquid phase reduction method. The smaller size and larger specific surface area of S-NZVI/UiO-66 were confirmed by a variety of characterization techniques. Based on the excellent surface structure and reactivity, the U(VI) removal capacity of S-NZVI/UiO-66 (895 mg g −1 ) was much better than S-NZVI (434 mg g −1 ) and UiO-66-NO 2 (267 mg g −1 ). The impacts of pH, background ion strength, coexisting ions and different water environments on adsorption were studied via macroscopic batch experiments. The results showed that S-NZVI/UiO-66 could remove U(VI) adequately in a wide pH range. The removal rate was basically not affected by the concentration of NaNO 3 , demonstrating that the adsorption process of U(VI) on S-NZVI/UiO-66 tended to inner surface complexation. From XPS technique combined with the results of batch adsorption experiments, it was clear that the elimination mechanisms of U(VI) by S-NZVI/UiO-66 were mainly the physical adsorption, electrostatic attraction and complexation of UiO-66-NO 2 , and the reduction and complexation of S-NZVI. Therefore, it is believed that S-NZVI/UiO-66 has a great potential to be an excellent adsorbent in the field of the environment remediation. Moreover, S-NZVI/UiO-66 promises to be a novel nanomaterial for solving the problem of radionuclide contamination in practical environments.
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TALANTA
·
2022
·
IF 6.556
Pengfei Zhao,Sisi Tang,Xiaodan Wu,Yu Chen,Kangling Tang,Jinli Fu,Huibin Lei,ZhaoXia Yang,Zhaohui Zhang
Development of method with micro-volume reagent usage and high selectivity for rapid determination of valuable disease-related biomarkers is of great importance for disease surveillance. Herein, a novel ratiometric fluorescence capillary imprinted sensor was developed for highly selective fluorescence determination of sialic acid (SA) based on luminescent metal-organic framework (UiO-66-NH 2 ). In this strategy, the imprinted pre-polymer with double emissions was sucked into the capillary to grow imprinted layer on the inner wall of the capillary. In presence of SA, the blue fluorescence (440 nm) served as fluorescence response signal was quenched due to the electron transfer mechanism between metal organic framework and SA while the red fluorescence (655 nm) served as the reference signal was remained. Within SA concentration linear range of 1.0 × 10 −7 –3.0 × 10 −4 M, the ratiometric fluorescence capillary imprinted sensor was applied to detect SA in human serum and saliva samples successfully with a detection limit of 2.5 × 10 −8 M. A sensitive and selective fluorescence method with micro-volume sample consumption (15 μl) for determination of SA in practical samples was established.
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CARBOHYDRATE POLYMERS
·
2022
·
IF 10.723
Zhi Chen,Zhi-Bo Zhang,Jun Zeng,Zhi-Jie Zhang,Shan Ma,Cong-Ming Tang,Jun-Qiang Xu
In this work, a polyethyleneimine-modified chitosan/Ce-UIO-66 composite hydrogel (PEI-CS/Ce-UIO-66) was prepared using the ex-situ blend method. The synthesized composite hydrogel was characterized by SEM, EDS , XRD, FTIR, BET, XPS, and TG techniques, while the zeta potential was recorded for sample analysis. The adsorbent performance was studied by conducting adsorption experiments using methyl orange (MO), which showed that PEI-CS/Ce-UIO-66 exhibited excellent MO adsorption properties (900.5 ± 19.09 mg/g). The adsorption kinetics of PEI-CS/Ce-UIO-66 could be explained by the pseudo-second-order kinetic model , and its isothermal adsorption followed the Langmuir model. Thermodynamics showed that the adsorption was spontaneous and exothermic at low temperatures. MO could interact with PEI-CS/Ce-UIO-66 via electrostatic interaction , π–π stacking, and hydrogen bonding . The results indicated that the PEI-CS/Ce-UIO-66 composite hydrogel could potentially be used for the adsorption of anionic dyes.
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高影响因子
PLoS One
·
2022
·Vol. 17
·期 8
·e0271075
·
IF 3.752
Bicun Jiang,Fuqiang Liu,Yang Pan,Yan Tan,Chendong Shuang,Aimin Li
Tetracycline (TC) is widely-used antibiotic pollutant with high toxicity, refractory, persistence and bacteriostasis, and its removal from water needs to be enhanced. In this work, a novel Graphite-UiO-66(Zr)/Ti electrode was successfully prepared and evaluated for electrochemical oxidation degradation of TC. The electrochemical performance tests indicate the Graphite-UiO-66(Zr)/Ti electrode had higher electrochemical oxidation activity, which achieved higher TC removal efficiency (98.1% ± 1.5%) than Ti plate (65.2% ± 3.5%), Graphite-MIL-53(Al)/Ti electrode (79.5% ± 2.9%) and Graphite-MIL-100(Fe)/Ti electrode (89.0% ± 2.6%). The influence of operating condition was also systematically studied, and the optimized condition was pH 5.0, 20 mA/cm 2 current density and 0.1 M electrolyte (Na 2 SO 4 ). Through the liquid chromatography mass spectrometry (LC-MS), the TC degradation pathway by Graphite-UiO-66(Zr)/Ti electrode oxidation was proposed. Under the •OH free radical oxidative decomposition effect, the double bond, phenolic group and amine group of TC were attacked. TC was transformed into intermediate product ① (m/z = 447), then was further degraded to intermediates ② (m/z = 401) and ③ (m/z = 417). The latter was fragmented into small fractions ④ (m/z = 194), ⑤but-2-enedioic acid (m/z = 116) and ⑥oxalic acid (m/z = 90, the proposed intermediate). In addition, TC removal remained at 89.6% ± 2.7% in the sixth cycle of operation, which confirmed the efficient reusability and stability for antibiotics removal from water.
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高影响因子
FUEL
·
2021
·
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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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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Applied Materials Today
·
2021
·
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 MATERIALS SCIENCE
·
2020
·Vol. 56
·期 2
·1577-1589
·
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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MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
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 Environmental Chemical Engineering
·
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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Arabian Journal of Chemistry
·
2020
·
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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