RSC Advances
·
2021
·Vol. 11
·期 60
·38016-38025
·
IF 3.361
Yuxin Zhang,Xinluo Song,Shicong Li,Bangyao Zhao,Liangliang Tong,Yuanrui Wang,Yafeng Li
A polyoxometalate acid can be encapsulated into a metal–organic framework to construct a novel kind of solid-acid catalyst. In this work, the two-step method —high-temperature preparation of Zr6O4(OH)4(CH3COO)12 and low-temperature self-assembly—has been adopted to synthesize the PW12@UIO-66 composite (PW12 = H3PW12O40; UIO-66 = Zr6O4(OH)4(OOC–C6H4–COO)12). The as-synthesized PW12@UIO-66 composite exhibits highly crystalline, good octahedron morphology, large specific surface area (1960 m2 g−1) and high thermal stability (>500 °C), which clearly demonstrates the potential as a solid-acid catalyst. Additionally, the PW12@UIO-66 composite may be accomplished with 85% utilization of H3PW12O40 and 95% yield through this synthetic procedure. The performances of the PW12@UIO-66 composite are investigated by catalyzing the simultaneous transesterification and esterification of soybean oil into biodiesel. Under the optimal conditions, the conversion of the soybean oil into biodiesel would exceed 90% over the as-synthesized PW12@UIO-66 composite. As the crucial indexes for industrial prospects, the recycling and life experiments were surveyed. After 10 times recycling and 4 weeks, the structure and performance of the PW12@UIO-66 composite remained unchanged and in the meantime the PW12@UIO-66 composite still maintained a high activity to convert soybean oil into biodiesel.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Sihan Li,Yanqi Gan,Syed Jalil Shah,Ruimeng Wang,Wenxue Gong,Rule Wei,Hongbing Ji,Zhongxing Zhao,Zhenxia Zhao
Competitive adsorption of complex nonsteroidal anti-inflammatory drugs (NSAIDs) from wastewater often reduces the adsorption capacity of object pollutants on most porous materials. To address this issue, NSAIDs molecules were proposed for engineering imprinted pores in UiO-66s to boost their adsorption capacity towards diclofenac sodium (DCF) and Cu(II) in a complex solution. Naproxen (NAP) with proper chemical structure was proved to introduce more imprinted pores (at ~19 Å) with enhanced mesoporous volume, abundant unsaturated metal sites, and terminal hydroxyl groups in UiO-66@NAP. These new intriguing properties awarded high adsorption affinity to UiO-66@NAP for DCF and Cu(II), and their adsorption capacities reached up to 385 and 52 mg/g for single DCF and Cu(II) components, respectively. When DCF and Cu(II) simultaneously appeared in an aqueous solution, DCF was proved to preferentially occupy adsorption sites on UiO-66@NAP with higher adsorption kinetics compared to Cu(II). Afterwards, these pre-adsorbed DCF acted as new adsorption sites to bridge more Cu(II) in the solution. Similarly, the adsorbed Cu(II) on UiO-66@NAP had the same reciprocal bridging effect towards DCF, which realized the synergistic adsorption of DCF and Cu(II) over UiO-66@NAP. Notably, DCF was found to greatly boost the synergistic effect of the Cu(II) adsorption. As a result, UiO-66@NAP exhibited 1.5 and 2.6 times higher uptakes for DCF (573 mg/g) and Cu(II) (135 mg/g) in the binary system compared to their single pollutant system, and its equilibrium adsorption capacity was much higher compared to several state-of-the-art adsorbents. The current work set out a new strategy to modify MOFs for enhanced adsorption of complex NSAID contaminants and revealed a deep understanding of the interactions between NSAIDs and heavy metals ions .
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MOLECULES
·
2020
·Vol. 25
·期 19
·4557
·
IF 3.267
Qian Wang,Chunmeng Gu,Yafen Fu,Liangliang Liu,Yixi Xie
Luteolin is a kind of natural flavonoid with many bioactivities purified from a variety of natural herbs, fruits and vegetables. Electrochemical sensing has become an outstanding technology for the detection of luteolin in low concentration due to its fast response, easy operation and low cost. In this study, electroreduced graphene oxide (ErGO) and UiO-66 were successively modified onto a glassy carbon electrode (UiO-66/ErGO/GCE) and applied to the detection of luteolin. A combination of UiO-66 and ErGO showed the highest promotion in the oxidation peak current for luteolin compared with those of a single component. The factors affecting the electrochemical behavior of UiO-66/ErGO/GCE were evaluated and optimized including pH, accumulation potential, accumulation time and scan rate. Under optimum conditions, UiO-66/ErGO/GCE showed satisfactory linearity (from 0.001 μM to 20 μM), reproducibility and storage stability. The detection limit of UiO-66/ErGO/GCE reached 0.75 nM of luteolin and was suitable for testing real samples. Stable detection could be provided at least eight times by one modified electrode, which guaranteed the practicability of the proposed sensor. The fabricated UiO-66/ErGO/GCE showed a rapid electrochemical response and low consumption of materials in the detection of luteolin. It also showed satisfactory accuracy for real samples with good recovery. In conclusion, the modification using MOFs and graphene materials made the electrode advanced property in electrochemical sensing of natural active compounds.Keywords:electrochemical;glass carbon electrode;luteolin;reduced graphene oxide;UiO-66
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Polymers
·
2020
·Vol. 12
·期 2
·281
·
IF 3.426
Chi-Xuan Yao,Ning Zhao,Jing-Min Liu,Guo-Zhen Fang,Shuo Wang
A rapid method was developed to determine the content of tyramine in food on the basis of the combination of molecular imprinting technique and the metal-organic frameworks. We developed the new molecular imprinted polymers based on metal-organic frameworks UiO-66 (named UiO-66@MIPs) as the sensing recognition element, the non-molecular imprinted polymers based on UiO-66 (named UiO-66@NIPs) was synthesized according the same steps without tyramine for comparison. The characterization of obtained UiO-66@MIPs was investigated through a series of characterization experiments. The results indicated that the octahedral shaped UiO-66 was encapsulated in the sol-gel polymer film, with a desirable thermal stability and possessed a specific surface area (SSA) of 994.3 m2·g−1. The imprinting factor of the UiO-66@MIPs for tyramine was 1.956 in static experiment. This indicates the synthesized UiO-66@MIPs have outstanding performance compered to UiO-66@NIPs on the static adsorption quantity and selective adsorption affinity. It’s to make use of advantages of the synthetic materials to develop a quartz crystal microbalance (QCM) sensor for the sensitive detection of tyramine. The detection limit of the system was 61.65 μg·L−1within measurable concentration range from 80 to 500 μg·L−1. The prepared QCM sensor was verified in selectivity and application. The UiO-66@MIPs possess good behavior on selectivity, absorptivity, and chemical stability, so the UiO-66@MIPs achieve accurate and rapid trace detection of biogenic amines in food combining with the quartz crystal microbalance.Keywords:metal–organic frameworks;UiO-66;molecularly imprinted polymers;quartz crystal microbalance;tyramine
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Haojie Zeng,Zongxue Yu,Liangyan Shao,Xiuhui Li,Meng Zhu,Yuchuan Liu,Xiaofang Feng,Ximei Zhu
A composite membrane based on a novel strategy was prepared which using graphene oxide (GO), UiO-66-NH 2 and polyacrylic acid (PAA) as basic materials on the surface of nylon membrane by vacuum filtration self-assembly. The structure of the composite membrane was made of graphene oxide as vertical separation layer, the PAA@UiO-66-NH 2 (PAA@UiO) embedding between GO as horizontal capture material. The PAA@UiO-66-NH 2 /GO (PAA@UiO/GO) membrane was characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and atomic force microscopy (AFM). Compared with the GO membrane, PAA@UiO/GO membrane combined the effects of GO, UiO-66-NH 2 and PAA, which significantly enhances the separation performance of dye wastewater. In particular, the PAA@UiO/GO membrane can achieve complete removal of MB , RB and CR while the fluxes during filtration process can reach about 100 L ∙ m - 2 ∙ h - 1 . At the same time, PAA@UiO/GO membrane almost retained stable removal rate on all dyes under extreme pH and ionic strength conditions. In addition, after 10 cycles of experiments, PAA@UiO/GO membrane retained a removal rate and a flux more than 95% and 85 L ∙ m - 2 ∙ h - 1 for all dyes, respectively. Compared to a composite membrane based on intercalation, the unique structure of PAA@UiO/GO membrane with a large number of adsorption sites and screening structures, resulting a better removal rate for dyes. Furthermore, PAA@UiO/GO membrane has a great potential in practical applications and a solution to balance trade-off effect.
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Nanomaterials
·
2019
·Vol. 9
·期 12
·1698
·
IF 4.034
Yanliang Yang,Dongsheng Deng,Dong Sui,Yanfu Xie,Dongmi Li,Ying Duan
The hydrogenation of furan ring in the biomass-derived furans is of great importance for the conversion of biomass to valuable chemicals. Fabrication of high activity and selectivity catalyst for this hydrogenation under mild conditions was one of the focuses of this research. In this manuscript, UiO-66-v, in which vinyl bonded to the benzene ring, was first prepared. Then, the uniformly distributed vinyl was used as the reductant for the preparation of Pd/UiO-66-v. The catalyst was characterized by X-ray diffraction, thermogravimetric, N2physical adsorption/desorption, X-ray photoelectron spectroscopy, scanning electron microscope, transmission electron microscopy, energy dispersive spectrometer elemental mappings, and inductively coupled plasma atomic emission spectroscopy to find the Pd/UiO-66-v had a narrow palladium nanoparticles size of 3–5 nm and maintained the structure and thermal stability of UiO-66-v. The Pd/UiO-66-v was used for the hydrogenation of furfuryl alcohol to tetrahydrofurfuryl alcohol in water. 99% conversion of furfuryl alcohol was obtained with 90% selectivity to tetrahydrofurfuryl alcohol after reacted at 0.5 MPa H2, 303 K for 12 h. The Pd/UiO-66-v was proved to be effective for the hydrogenation of furan ring in furans and could be used for at least five times.Keywords:furfuryl alcohol;hydrogenation;tetrahydrofurfuryl alcohol;Pd/UiO-66-v;water solvent
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 11
·1-11
·
IF 5.7
Li Dan,Gao Yanmei,Mu Mengyao,Zhu Shiping,Zhang Ning,Lu Minghua
Ionic liquid (IL)-modified UiO-66-NH 2 composite was prepared and used as sorbent of dispersed solid-phase extraction (dSPE) for extracting trace benzoylurea insecticides (BUs) from complex environmental matrices. The IL in framework endowed the prepared material had electropositive characteristics, which can produce interaction with electron rich guest molecules, such as BUs. The high thermal and chemical stability of UiO-66-NH 2 /IL enabled it to be reused for 16 times without significant reduction in adsorption performance. Due to the multiple forces including π-π, hydrogen bonding, and fluorine-fluorine interaction, UiO-66-NH 2 /IL showed good adsorption performance, short adsorption time (20 s) and rapid desorption ability (60 s) for BUs. Under the optimal conditions, the method exhibited wide linear range (0.02–500 ng mL -1 ) with correlation coefficient ( R 2 ) not worse than 0.9928, high enrichment factor (252–300), and low detection limit (0.005–0.4 ng mL -1 ). The dispersed solid phase extraction coupling with high-performance liquid chromatography-diode array detector (dSPE-HPLC-DAD) was successfully used to detection of BUs in real environmental samples and satisfactory recoveries were obtained (80.5%±2.4–118%±3.2). The results indicated that UiO-66-NH 2 /IL composite can be a potential sorbent for the preconcentration of trace insecticides in environmental samples. Graphical abstract
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2023
·
IF 5.8
Ke Cai,Wei Pi,Jiangyang Qin,Chenxi Peng,Dandan Wang,Yingying Gu,Yong Mei
In this study, an electrochemical immunosensor was constructed to detect the cytokeratin 19 fragment antigen 21-1 (CYFRA 21-1) in human serum. CYFRA 21-1 is the most sensitive tumor marker of non-small cell lung cancer (NSCLC), its content in normal human serum should be less than 3.3 ng/mL. When lung cancer cells dissolve or die, a myriad of CYFRA 21-1 is released into a tumor patient’s blood circulation , and its serum content elevates strikingly. Consequently, detecting CYFRA 21-1 by an electrochemical biosensor is expected to provide a new method for the early detection and prevention of lung cancer. In this study, a composite of UiO-66-NH 2 and carboxylated multi-walled carbon nanotubes (CMWCNTs) was used as the substrate material of a sensor; the resulting sensor had a large specific surface area and strong electrical conductivity . Moreover, gold nanoparticles (AuNPs) were used to bind to antibodies through an Au-S bonds. Also, a supersensitive detection of CYFRA 21-1 was achieved through the specific bindings of antigens and antibodies. Under optimal detection conditions, the change of current signal intensity of the immunosensor was proportional to the logarithm of CYFRA 21-1 concentration and had a linear relation in the range of 0.005–400 ng/mL, while the detection limit was 1.15 pg/mL (S/N = 3). The proposed immunosensor had high precision, stability, and selectivity . More importantly, the sensor was been successfully applied to detect CYFRA 21-1 in human serum with high recovery, providing a new method for early screening and dynamic monitoring of lung cancer.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Zhihong Lin,Ziyi Yuan,Kaifang Wang,Xuezhong He
Novel mixed matrix membranes (MMMs) with superior CO 2 /N 2 separation properties are of great importance for post-combustion CO 2 capture from flue gas . Metal-organic frameworks (MOFs) as one of the most attractive porous fillers for MMMs fabrication, are considered to provide a solid molecular sieving mechanism for enhancing CO 2 /N 2 selectivity. However, it causes the reduction in gas permeability and limits its further industrialization. Herein, we proposed a new strategy for filler functionalization by doping silver ions (Ag + ) into UiO-66-NH 2 nanoparticles through the double-solvent method and used for the preparation of advanced MMMs. The double-solvent method is benefits for the enrichment of Ag + in the hydrophilic pores of UiO-66-NH 2 . As a result, the prepared novel MMMs called Ag + @UiO@PIM-1 with the polymers of intrinsic microporosity (PIMs) as polymer matrix , show outstanding CO 2 permeability. According to the mixed gases (CO 2 /N 2 = 10:90) permeation experiments under 25 °C and 2 bar, the membrane with 30%Ag + @10%UiO loading achieves more than 65% increase in CO 2 /N 2 selectivity (∼30) and 120% in CO 2 permeability (>15,000 Barrer) compared to the pristine PIM-1 membrane. By optimizing the Ag + doping amount and Ag + @UiO loading content, the separation performance exceeds the 2019 CO 2 /N 2 upper bound. To figure out the separation mechanism, the pore texture properties and CO 2 affinity of the functional filler (Ag + @UiO) together with the membrane structure were characterized by XPS , PXRD , SEM, gas sorption , etc. The synergistic mechanisms by combing CO 2 facilitated transport and molecular sieving from pore regulation were identified to enable advanced CO 2 /N 2 membrane separation .
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Qiang Le,Zan Liu,Zhilin Cheng
In this work, a novel core-shell nanostructured coaxial nanofiber membranes (CFMs) were successfully produced by the coaxial electrospinning . The structure and composition of CFMs were probed by a series of characterizations. The results demonstrated that the CFMs were comprised of the versatile core-shell structure nanofibers, therein Cu(I)/UIO-66 scattered in the shell layer and HNTs dispersed in the core layer. As applied in the selective adsorption desulfurization , the Cu(I)/UIO-66 embedded on the surface of the nanofiber undertook the adsorption active sites, while HNTs in core layer served as enhancing the mechanical performance of PAN nanofibers. The CFMs had the superior adsorption performance in the batch adsorption (maximum:40.14 mg·g −1 ) and fixed-bed adsorption (maximum: 47.43 mg·g −1 ) capacities for benzothiophene (BT) from fuel oil, respectively. Furthermore, due to having the robust mechanical performance, the CFMs exhibited the preferable recycling adsorption and mechanical stability . The adsorption mechanism of BT molecules on CFMs was explored by the kinetics, isotherms and thermodynamic models , indicating the existence of the synergistic effect of physical adsorption and chemical adsorption.
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ChemNanoMat
·
2023
·Vol. 9
·期 5
·e202300051
·
IF 3.8
Qiankun Xu,Yaru Li,Wen Ji,Jun Mei,Xianbiao Wang
Graphical TiO 2 hollow sphere/UiO-66-NH 2 heterostructures were successfully synthesized by an adsorption-induced in-situ solvothermal growth strategy. The integration of TiO 2 and UiO-66-NH 2 could construct a type-II heterojunction to broaden the absorption range of light and suppress the recombination of photoproduced electrons and holes, thus boosting the photoreduction activity toward Cr(VI) of TiO 2 /UiO-66-NH 2 . Water contamination caused by highly toxic Cr(VI) should be resolved imminently with a more efficient photocatalytic approach. The interaction between photocatalyst heterostructure is critical for charge separation which largely affects the photocatalytic efficiency. Herein, TiO 2 hollow sphere/UiO-66-NH 2 (TiO 2 /UiO-66-NH 2 ) heterostructures were successfully synthesized by an adsorption-induced in-situ solvothermal growth strategy. The UiO-66-NH 2 particles were well dispersed on TiO 2 hollow spheres by solvothermal treatment of Zr 4+ adsorbed TiO 2 hollow spheres with NH 2 -BDC ligand. The photocatalytic activities of TiO 2 /UiO-66-NH 2 heterostructures were investigated by reduction of Cr(VI) with visible light irradiation. With the introduction of UiO-66-NH 2 , the reduction efficiency toward Cr(VI) by TiO 2 /UiO-66-NH 2 heterostructures reached 89% after 180 min of irradiation, which is much higher than those of TiO 2 hollow spheres (10%) and UiO-66-NH 2 crystals (29%). Moreover, the TiO 2 /UiO-66-NH 2 heterostructures display good regeneration ability and can still maintain 70% of Cr(VI) removal ability after four cycles. The integration of TiO 2 and UiO-66-NH 2 could construct a type-II heterojunction to broaden the absorption range of light and suppress the recombination of photoproduced electrons and holes. As a result, such unique composite structure significantly enhance the photocatalytic performance towards Cr(VI) reduction. This work not only inspires a new approach for in-situ solvothermal synthesis of semiconductor@MOFs composites, but provides a novel photocatalyst for highly efficient removal of Cr(VI) from wastewater.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Jing Wang,Yakun Teng,Shushu Jia,Wenyan Li,Tianyi Yang,Ya Cheng,Hao Zhang,Xiang Li,Lijuan Li,Ce Wang
The successful development of a cost-effective and efficient adsorbent is crucial for the optimal treatment of pharmaceutical sewage. In this study, a UiO-66(Hf)–NH 2 nanocrystal modified composite nanofiber membrane (HfPNFM) was synthesized through electrospinning and solvothermal techniques, for the removal of salicylic acid (SA). The in-situ growth of UiO-66(Hf)–NH 2 on the nanofibers led to a significant increase in the specific surface area of the composite nanofiber membrane. Furthermore, HfPNFM demonstrated exceptional flexibility and reusability, with the removal efficiency of SA still at 96.85 % even after ten cycles. The adsorption process of SA onto HfPNFM was well described by the pseudo-second-order kinetic model and Langmuir isotherm model, with a maximum adsorption capacity of 128.21 mg/g. In dynamic adsorption experiments, HfPNFM effectively removed 100 % of SA at a concentration of 50 mg/L. The chemical oxygen demand (COD) concentration of SA was reduced from 165.89 mg/L to 41.47 mg/L by two layers of HfPNFM filtration, below the standard for pharmaceutical wastewater discharge (GB: 21904-2008). X-ray photoelectron spectroscopy (XPS) revealed that electrostatic interactions, π-π interactions, hydrogen bond interactions, and metal complexation interactions between SA and HfPNFM were responsible for the adsorption. This highly effective composite nanofiber membrane has promising potential for pharmaceutical wastewater treatment.
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