JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Chun-Yang Li,Jing-Min Liu,Zhi-Hao Wang,Shi-Wen Lv,Ning Zhao,Shuo Wang
Aflatoxins have been a hot topic in the field related into public health and ecosystem protection, and great effort has been made in developing of adsorptive materials for effective probing the target aflatoxins. Conventional materials, like metal-organic frameworks (MOFs) showed promising application in separation science. However, the cumbersome separation process, competitive adsorption are also major challenges. Regarding this, a novel magnetic micro-composite denoted as Fe 3 O 4 @UiO-66-NH 2 @MON with core-shell structure was constructed. The core of Fe 3 O 4 microspheres was coated with MOFs crystals, and then microporous organic network (MON) was introduced onto the surface of Fe 3 O 4 @UiO-66-NH 2 through a sonogashira coupling reaction. It exhibited good magnetic separation ability, which effectively simplified the pre-treatment steps. The proposed method possessed excellent selectivity and sensitivity, with detection limits in the range of 0.15-0.87 μg L −1 combination with HPLC analysis. More importantly, the MON coating significantly improved the hydro-stability of whole adsorbents, thus enhancing the adsorption efficiency and favoring the practical application of the materials. The developed Fe 3 O 4 @UiO-66-NH 2 @MON-based solid extraction method has been well-applied for real sample analysis, with the recovery of 87.3%–101.8%. We believe the newly-constructed hybrid nano-adsorbents hold great potential in further application in various analytical methods for different target analytes.
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FUEL
·
2019
·
IF 5.128
Lulu Yan,Tingting Duan,Tingting Huang,Bingbing Zhao,Yu Fan
This article proposes a novel strategy for producing highly dispersed H 3 PW 12 O 40 (HPW) on metal-organic frameworks (MOFs) via the anchoring action of amino groups originating from 2-amino terephthalic acid (APTA) in the MOF ligand. Under this method, amino groups are introduced into the linker of UiO-66 materials through a one-pot synthesis to disperse supported HPW, which has a negligible impact on the crystal structure of UiO-66. The acidic densities in the HPW/UiO-66 catalysts are effectively modified by adjusting the molar APTA/PTA (terephthalic acid) ratio in the mixed ligand and HPW loading. Consequently, the dispersion and stability of supported HPW are significantly enhanced, which make the as-prepared catalyst with 40 wt% of HPW present superior sec -butyl acetate (SBAC) yield (38.6 wt%) and selectivity (98 wt%) for the direct esterification of olefins. This strategy provides a new approach for preparing supported HPW with high dispersion and stability to be applied in olefin esterification.
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ACS Applied Materials & Interfaces
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2019
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IF 8.456
Wen Li,Kuncan Wang,Junjie Huang,Xiao Liu,Dun Fu,Jiale Huang,Qingbiao Li,Guowu Zhan
Metal–organic frameworks have been exploited as excellent solid precursors and templates for the preparation integrated nanocatalysts with multicomponent and hierarchical structures. Herein, a novel synthetic protocol has been developed to fabricate versatile Zr-based solid solutions (such as ZnO–ZrO2, Co3O4–ZrO2, and CuO–ZrO2) via pyrolysis of Schiff base-modified UiO-66 octahedrons (size <100 nm), which were then utilized as efficient catalysts for CO2 hydrogenation. The Schiff base serves as an effective bridge to dope secondary metal ions into UiO-66 frameworks with controlled amounts of 0.13–8.8 wt %, which are initially hard to achieve. Interestingly, by simply changing the loading metal ions, the selectivity of C1 hydrogenation products can be facilely tuned. For instance, the maximum CO2 conversion of ZnO–ZrO2, Co3O4–ZrO2, and CuO–ZrO2 solid solutions were 5.8, 11.4, and 22.5%, with the main product selectivity of 70% CH3OH, 92.5% CH4, and 86.7% CO, respectively. Moreover, in situ diffuse reflectance infrared Fourier transform spectra characterization reveals that the significant difference in C1 product selectivity is mainly determined by the balance of *HCOO, *CH3O, and *CO intermediate species over the Zr-based solid solutions.
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SENSORS AND ACTUATORS B-CHEMICAL
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2019
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IF 6.393
Xin Xiong,Yao Zhang,YinFang Wang,HaiFeng Sha,Nengqin Jia
By virtue of the metal organic framework UiO-66-NH 2, an ingenious electrochemiluminescence immunosensor was successfully constructed for subtle exploration of the breast cancer biomarker CA 15-3. In this protocol, Ru(bpy) 3 Cl 2 ·6H 2 O (Ru(bpy) 3 2+ ), as a conventional luminescent reagent, provides a stable and strong luminescent signal. The UiO-66-NH 2 serves as a carrier to provide a large specific surface area for enhancing the electrochemical luminescence signal response of Ru(bpy) 3 2+ . UiO-66-NH 2 , Ru(bpy) 3 2+ are fixed together with Nafion membrane, and CA 15-3 antibody is covalently conjugated onto the membrane through the amide reaction. Ru(bpy) 3 2+ @UiO-66-NH 2 is used as the detection system. The experimental results reveal that the ECL signal decreased obviously after the CA 15-3 antigen molecule is captured on the immunosensor, with the capture of manifesting the principle of electrochemical luminescence quenching detection. Under optimal conditions, the sensor is sensitive and selective for detecting CA 15-3 with the detection range from 5 × 10 −4 to 5 × 10 2 U mL -1 and the low LOD (1.7705 × 10 -5 U mL -1 ). Furthermore, multiple experiments elucidate that the as-prepared sensor could be used for susceptibly detect CA 15-3 in actual samples, which has underlying application prospects in biological analysis.
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CHEMISTRY-A EUROPEAN JOURNAL
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2013
·Vol. 19
·期 42
·14279-14285
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IF 5.831
Dengrong Sun,Yanghe Fu,Wenjun Liu,Lin Ye,Dengke Wang,Lin Yang,Xianzhi Fu,Zhaohui Li
Graphical Higher CO 2 photoreduction activity than previously studied metal–organic framework (MOF) NH 2 -MIL-125(Ti) in the presence of triethanolamine (TEOA) as the sacrificial agent under visible light is exhibited by the amino-functionalized MOF NH 2 -Uio-66(Zr). The photoinduced electron transfer from 2-aminoterephthalate linkers to Zr oxo clusters was revealed for the first time by photoluminescence studies, and the generated Zr III was detected by ESR analysis (see figure). Metal–organic framework (MOF) NH 2 -Uio-66(Zr) exhibits photocatalytic activity for CO 2 reduction in the presence of triethanolamine as sacrificial agent under visible-light irradiation. Photoinduced electron transfer from the excited 2-aminoterephthalate (ATA) to Zr oxo clusters in NH 2 -Uio-66(Zr) was for the first time revealed by photoluminescence studies. Generation of Zr III and its involvement in photocatalytic CO 2 reduction was confirmed by ESR analysis. Moreover, NH 2 -Uio-66(Zr) with mixed ATA and 2,5-diaminoterephthalate (DTA) ligands was prepared and shown to exhibit higher performance for photocatalytic CO 2 reduction due to its enhanced light adsorption and increased adsorption of CO 2 . This study provides a better understanding of photocatalytic CO 2 reduction over MOF-based photocatalysts and also demonstrates the great potential of using MOFs as highly stable, molecularly tunable, and recyclable photocatalysts in CO 2 reduction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yu Yang,Meng Du,Jiaxin Liang,Qian Xu,Wei Liu,Ang Li
The flow-through electroactive membrane adsorption method has been proved to be a promising strategy to enrich low-concentration phosphate. However, the challenges of selective adsorption of phosphate and poor regeneration restrict its industrial application. Here, this study proposed a novel bimetallic Mg-UiO-66@rGO electrode material through the introduction of Mg(II) into UiO-66, which possessed remarkable adsorption selectivity and optimal reproducibility among the reported electrode materials. The maximum phosphate adsorption capacity of Mg-UiO-66(13)@rGO (Zr/Mg = 3:1) was 62.81 mg⋅g −1 at 3.2 V. Furthermore, it maintained the excellent adsorption properties in the presence of all competitive anions and after 30 times of continuous adsorption–desorption. In actual wastewater, Mg-UiO-66(13)@rGO still represented excellent adsorption kinetics of 0.51 mg⋅(g⋅min) −1 and equilibrium adsorption capacity of 61.2 mg⋅g −1 . The superior selectivity of Mg-UiO-66@rGO was attributed to the establishment of coordinative unsaturated metal sites (CUMSs), thus increasing the adsorption sites. The synergic effect of electric field facilitates the breaking and formation of coordination bonds between charged ions and deeper binding sites, boosting the adsorption–desorption ability. Notably, the structural stability is also a key factor in promoting repeated material regeneration. This study advances electrode material to a new level by introducing CUMSs and bimetallic synergies.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Xiao-hu Ma,Si-yuan He,Zhe-rui Zhang,Zhe Meng
Persistent light-emitting materials (PLMs), which have the potential to store and release light energy after light irradiation, are receiving increasing attention for their role in prolonging the lifetime of photogenerated electrons for the development of photocatalysts with round-the-clock applications. In this paper, a double S-scheme Sr 2 MgSi 2 O 7 :Eu 2+ ,Dy 3+ /ZnIn 2 S 4 /UiO-66-NH 2 (SZU) heterojunction with round-the-clock catalytic activity was prepared by hydrothermal self-assembly method. The photocatalytic performance of the SZU heterojunction for RhB(MB) degradation was significantly improved compared with the pristine ZnIn 2 S 4 and UiO-66-NH 2 . The SZU heterojunction has excellent catalytic degradation performance for RhB (MB), and the removal rate of RhB (MB) reaches 72.2 % (81.7 %) after visible light irradiation for 40 (60) minutes. After the end of light, the total removal rate of RhB (MB) reached 86.7 % (96.8 %) when the catalysis continued for several hours under dark conditions, which was 14 % and 15 % higher than that under visible light irradiation, respectively. Based on the characteristics of SMS photoluminescence, combined with a large number of photocatalytic experiments, The sustained photocatalytic activity was enhanced under both daytime and darkness conditions, not only because of the production of SZU complexes, which prolonged the visible light response of ZnIn 2 S 4 , but also because of the construction of double S-scheme heterojunctions, which facilitates the light storage capacity, charge transfer, and the separation of photo-induced charge carriers and effectively promoted the photocatalytic activity of the photocatalysts. This work contributes to a deeper understanding of the design of round-the-clock photocatalysts, and provides a useful exploration for the practical application of photocatalytic technology.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 35
·23940-23947
·
IF 10.7
Kai Chen,Qingqing Liu,Zhiying Qiu,Huan Zhang,Ning Gong,Lihua Zhu
Pt-PMo@UiO-66 catalysts synthesized via a solvothermal method utilizing phosphomolybdic acid as a stabilizing agent exhibit exceptional catalytic performance in the selective hydrogenation of nitroarenes. The nanostructure of the Pt-PMo@UiO-66 catalysts is demonstrated by ICP-OES, XRD, XPS, TEM, HRTEM, STEM-EDS and other characterization studies. The Pt nanoparticles (NPs) or clusters are mainly supported on the surface of UiO-66. There is a synergistic catalytic effect between Pt, phosphomolybdic acid and UiO-66, improving their catalytic hydrogenation performance (activity, selectivity and stability) for nitroarene hydrogenation. It is found that 0.32%Pt-PMo@UiO-66 has the best catalytic properties for nitroacetophenone hydrogenation, with 98.8% conversion and 99.6% selectivity to aminoacetophenone under relatively mild reaction conditions (1.75 h, 40 °C, 3.0 MPa H2). The turnover frequency (TOF) reaches 1498.0 h−1. The catalyst also shows high selectivity for the hydrogenation of halogen-containing nitroarenes without dehalogenation. The appropriate size of the Pt NPs (4.44 nm) and the electronic effect (electron transfer from Pt to Mo) improves the catalytic hydrogenation activity and selectivity of Pt-PMo@UiO-66 for the selective hydrogenation of nitroarenes under moderate reaction conditions.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Guzheng Mao,Qiqi Kan,Zhongyuan Yue,Shengui Ju,Haoli Zhou,Wanqin Jin
Pervaporation (PV) is an energy-efficient membrane technology for separating organic mixtures. Traditional polymer membranes in the PV face limitations due to a trade-off between flux and separation factor. Mixed-matrix membranes (MMMs) fabricated using solution mixing or filler modification often suffer from interfacial defects or require additional complex preparation steps. This study introduces an in situ polymerization method that incorporates UiO-66-NH 2 into the polyamide polymerization process to fabricate UiO-66-NH 2 @polyamide (PA) MMMs for methanol and dimethyl carbonate separation, which effectively resolves the interfacial defect issues while eliminating additional filler modification steps. The trade-off issue is also overcome. Results show that in situ polymerization improves UiO-66-NH 2 dispersion in the polymer matrix and strengthens polymer–filler interactions. MMMs with 5 wt% UiO-66-NH 2 loading achieved a total flux of 11.5 kg/(m 2 ·h) and a separation factor of 12.5 at 30 °C, representing a 2.32-fold and 1.46-fold improvement over pure PA membranes. These findings demonstrate the significant benefits of in situ polymerization in enhancing MMM performance and simplifying fabrication, providing an efficient strategy for industrial PV applications.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Ruirui Li,Wei Zhuang,Yan Gao,Yahan Bai,Keke Zhang,Zhenfu Wang
Herein, UiO-66 was selected as the immobilization carrier of Rhizomucor miehei lipase (RML). After etching and hydrophobic modification, the functionalized UIO-66 (H-UIO-66-OPA) was utilized for RML immobilization and the obtained RML@H-UIO-66-OPA showed about 70 % relative activity after incubation at 60 °C, which was much better than RML (20 %). RML@H-UIO-66-OPA was used in the synthesis of 1,3-dioleic acid glycerol (1,3-DAG) and the effects of reaction conditions (temperature, enzyme addition, substrate molar ratio, and time) on 1,3-DAG yield were investigated. Under the optimal conditions (temperature of 65 °C, enzyme addition of 2 wt%, substrate molar ratio of 2:1, and reaction time of 4 h), 1,3-DAG yield reached 77 %. Finally, Box-Behnken experimental design method was utilized to optimize the process parameters for the preparation of 1,3-DAG, and the final 1,3-DAG content was 79.80 %, which demonstrated that the model could predict the relationship between the factors and be suitable for the process optimization in 1,3-DAG preparation.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Dong Wang,Tinglue Zhang,Mohamed Gamal El-Din,Xuefen Wang
In this work, the 2-fluoroterephthalic acid with asymmetric structure and high electronegative F species was introduced in the assembly of Ce-UiO-66 catalysts to increase the defect density and enlarge pore structure for enhancement in removal efficiency of sulfamethoxazole. Owing to the strong coordination ability from high electronegative F species of 2-fluoroterephthalic acid with Ce-oxo nodes, the designed CUF exhibited improved interfacial properties (accelerated electron transfer rate, available active sites and enhanced interaction with PMS), which was favorable for the exploration and accessibility of active sites with sulfamethoxazole and PMS to decrease the adsorption barrier and accelerate PMS activation. As a result, the CUF catalysts exhibited higher adsorption capacity (173.4 mg/g) than that of CUH (117.8 mg/g), the enhanced degradation efficiency of sulfamethoxazole with a rate constant higher than 2.3 times CUH, good elimination (>95 %) of methylene blue, tetracycline and ibuprofen. In addition, the CUF/PMS system possessed satisfactory stability in wide solution pH, recycling and real water and good potential application in continuous wastewater treatment based on the designed dynamic catalytic reactor. This work provided deep insight into the design of catalysts with high adsorption performance and degradation efficiency based on the structure–activity relationship.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Chao Yang,Hao Chen,Yuankai Li,Zhelin Su,Yeshuang Wang,Xufei Liu,Huiling Fan
The low sulfur selectivity of Fe-based H2S-selective catalytic oxidation catalysts is still a problem, especially at a high O2 content. This is alleviated here through anchoring FeOx nanoclusters on UiO-66 via the formation of Fe–O–Zr bonds. The introduced FeOx species exist in the form of FeIII and FeII. Therein the FeIII–O species are the predominant active sites for H2S-oxidation. The formed Fe–O–Zr bonds strengthen the redox cycle of FeIII/FeII through promoting electron transfer from Fe to Zr. The FeII–O species can activate molecular oxygen to oxidize H2S into elemental S, which accelerates the formation rate of atomic S, hindering its further oxidation into SO2. The combination of these factors empowers the catalysts, enabling 100% H2S conversion and 98.2% sulfur yield. The catalyst also has satisfactory stability with the sulfur selectivity only decreasing from 98.2% to 91.3% after the reaction going on 50 h. The decreased sulfur selectivity might be caused by the deterioration of pores and the deposition of elemental S on the surface. The former hinders the diffusion of sulfur oligomers timely from pores to the gas phase, while the latter is suspected to capture electrons to promote its further reaction with molecular oxygen.
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