A facile approach to the preparation of a novel magnetically separable H_5PMo_（10）V_2O_（40）/Fe_3O_4/g-C_3N_4（PMoV/Fe_3O_4/g-C_3N_4） nanocomposite by chemical impregnation is demonstrated.The prepared nanocomposi...A facile approach to the preparation of a novel magnetically separable H_5PMo_（10）V_2O_（40）/Fe_3O_4/g-C_3N_4（PMoV/Fe_3O_4/g-C_3N_4） nanocomposite by chemical impregnation is demonstrated.The prepared nanocomposite was characterized and its acidity was measured by potentiometric titration.PMoV/Fe_3O_4/g-C_3N_4 showed high catalytic activity in the selective oxidative desulfurization of sulfides to their corresponding sulfoxides or sulfones.The catalytic oxidation of a dibenzothiophene（DBT）-containing model oil and that of real oil were also studied under optimized conditions.In addition,the effects of various nitrogen compounds,as well as the use of one- and two-ring aromatic hydrocarbons as co-solvents,on the catalytic removal of sulfur from DBT were investigated.The catalyst was easily separated and could be recovered from the reaction mixture by using an external magnetic field.Additionally,the remaining reactants could be separated from the products by simple decantation if an appropriate solvent was chosen for the extraction.The advantages of this nanocatalyst are its high catalytic activity and reusability;it can be used at least four times without considerable loss of activity.展开更多
The development of heterogeneous catalytic processes is crucial for the synthesis of chiral compounds for both academic and industrial applications.However,thus far,such achievements have remained elusive.Herein,we re...The development of heterogeneous catalytic processes is crucial for the synthesis of chiral compounds for both academic and industrial applications.However,thus far,such achievements have remained elusive.Herein,we report the heterogeneous asymmetric hydrogenation of 2-methylquinoline over solid chiral catalysts,which were prepared by the one-pot polymerization of(1R,2R)-N-(4-vinyl-benzenesulfonyl)-1,2-diphenylethane-1,2-diamine(VDPEN)and divinylbenzene(DVB)in the presence or absence of activated carbon(C)or carbon nanotubes(CNTs),followed by Ru coordination and anion exchange.The solid chiral catalysts were fully characterized by N2 sorption analysis,elemental analysis,TEM,FT-IR spectroscopy,and 13C CP-MAS NMR.All the solid chiral catalysts could efficiently catalyze the asymmetric hydrogenation of 2-methylquinoline to afford 2-methyl-1,2,3,4-tetrahydroquinoline with 90%ee.Studies have shown that polymer/C and polymer/CNTs composites are more active than pure polymers.The polymer/CNTs composite exhibited the highest activity among all the solid chiral catalysts under identical conditions,owing to the unique morphology of CNTs.The recycling stabilities of the solid chiral catalysts were greatly improved when ionic liquids(ILs)were employed as solvents;this is mainly attributed to the decreased leaching amount of anions owing to the confinement effect of ILs on ionic compounds.展开更多
Nitrogen-doped carbon nanotubes (N-CNTs)/polyaniline (PANI) composites are developed as an electrode material for biosensors. The morphology, composition, and optical properties of the resulting products were characte...Nitrogen-doped carbon nanotubes (N-CNTs)/polyaniline (PANI) composites are developed as an electrode material for biosensors. The morphology, composition, and optical properties of the resulting products were characterized by transmission electron microscopy (TEM), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FT-IR), and ultraviolet-visible absorption spectra (UV-vis). Furthermore, N-CNTs/PANI composite was immobilized on the surface of a glassy carbon electrode (GCE) and applied to construct a sensor. The obtained N-CNTs/PANI-modified GCE showed one pair of redox peaks and high catalytic activity for the oxidation of dopamine (DA) in a neutral environment. Differential pulse voltam-mograms results illustrate that the fabricated DA biosensor has high anti-interference ability towards ascorbic acid (AA). In addition, the fabricated biosensor showed superior performances with two wide linear ranges from 1 to 80 μM and from 1.5 to 3.5 mM and a low detection limit of 0.01 μM.展开更多
Based on the noncovalent functionalization of ferrocene-grafted polyethylenimine （PEI-Fc） and carbon nanotubes （CNTs）, CNT bundles are exfoliated by PEI-Fc solution and thus form stable compounds PEI-Fc@CNTs, whic...Based on the noncovalent functionalization of ferrocene-grafted polyethylenimine （PEI-Fc） and carbon nanotubes （CNTs）, CNT bundles are exfoliated by PEI-Fc solution and thus form stable compounds PEI-Fc@CNTs, which is used to construct the PEI-Fc@CNTs/DNA multilayers through layer-by-layer assembly. The multilayers show a highly uniform and homogeneous characteristic, which significantly improve the electrical property of the multilayers. Upon the oxidation electrical potential, the ferrocene groups are switched from reduction state （[Fe（C5H5）2]） to oxidation state （[Fe（C5H5）2]^＋）, leading to change of microenvironments＇ charge density, resulting in swelling of the multilayers and a final degree of swelling of 37 % and the decrease of multilayer stiffness. We maintain that electrochemical control over the swelling behavior of multilayers could have important implications for responsive coatings of nanoscale devices, including mechanically tunable surfaces which are used to modulate cellular activities and control drug delivery.展开更多
基金the Razi University Research Council for support of this work
文摘A facile approach to the preparation of a novel magnetically separable H_5PMo_（10）V_2O_（40）/Fe_3O_4/g-C_3N_4（PMoV/Fe_3O_4/g-C_3N_4） nanocomposite by chemical impregnation is demonstrated.The prepared nanocomposite was characterized and its acidity was measured by potentiometric titration.PMoV/Fe_3O_4/g-C_3N_4 showed high catalytic activity in the selective oxidative desulfurization of sulfides to their corresponding sulfoxides or sulfones.The catalytic oxidation of a dibenzothiophene（DBT）-containing model oil and that of real oil were also studied under optimized conditions.In addition,the effects of various nitrogen compounds,as well as the use of one- and two-ring aromatic hydrocarbons as co-solvents,on the catalytic removal of sulfur from DBT were investigated.The catalyst was easily separated and could be recovered from the reaction mixture by using an external magnetic field.Additionally,the remaining reactants could be separated from the products by simple decantation if an appropriate solvent was chosen for the extraction.The advantages of this nanocatalyst are its high catalytic activity and reusability;it can be used at least four times without considerable loss of activity.
基金supported by the National Natural Science Foundation of China (21733009, 21621063)the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17020200)~~
文摘The development of heterogeneous catalytic processes is crucial for the synthesis of chiral compounds for both academic and industrial applications.However,thus far,such achievements have remained elusive.Herein,we report the heterogeneous asymmetric hydrogenation of 2-methylquinoline over solid chiral catalysts,which were prepared by the one-pot polymerization of(1R,2R)-N-(4-vinyl-benzenesulfonyl)-1,2-diphenylethane-1,2-diamine(VDPEN)and divinylbenzene(DVB)in the presence or absence of activated carbon(C)or carbon nanotubes(CNTs),followed by Ru coordination and anion exchange.The solid chiral catalysts were fully characterized by N2 sorption analysis,elemental analysis,TEM,FT-IR spectroscopy,and 13C CP-MAS NMR.All the solid chiral catalysts could efficiently catalyze the asymmetric hydrogenation of 2-methylquinoline to afford 2-methyl-1,2,3,4-tetrahydroquinoline with 90%ee.Studies have shown that polymer/C and polymer/CNTs composites are more active than pure polymers.The polymer/CNTs composite exhibited the highest activity among all the solid chiral catalysts under identical conditions,owing to the unique morphology of CNTs.The recycling stabilities of the solid chiral catalysts were greatly improved when ionic liquids(ILs)were employed as solvents;this is mainly attributed to the decreased leaching amount of anions owing to the confinement effect of ILs on ionic compounds.
基金supported by the National Natural Science Foundation of China (20905038, 20903057, 20974046, 50803027, 20874048 & 20804020)the National Basic Research Program of China (2009CB930600)+1 种基金the Natural Science Foundation of Jiangsu Province (08KJB150011 & 09KJB150007)the Fok Ying-Tong Education Foundation under Grant 111051
文摘Nitrogen-doped carbon nanotubes (N-CNTs)/polyaniline (PANI) composites are developed as an electrode material for biosensors. The morphology, composition, and optical properties of the resulting products were characterized by transmission electron microscopy (TEM), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FT-IR), and ultraviolet-visible absorption spectra (UV-vis). Furthermore, N-CNTs/PANI composite was immobilized on the surface of a glassy carbon electrode (GCE) and applied to construct a sensor. The obtained N-CNTs/PANI-modified GCE showed one pair of redox peaks and high catalytic activity for the oxidation of dopamine (DA) in a neutral environment. Differential pulse voltam-mograms results illustrate that the fabricated DA biosensor has high anti-interference ability towards ascorbic acid (AA). In addition, the fabricated biosensor showed superior performances with two wide linear ranges from 1 to 80 μM and from 1.5 to 3.5 mM and a low detection limit of 0.01 μM.
基金supported by the National Natural Science Foundation of China(21174126,51333005,21374095)the National Basic Research Program of China(2011CB606203)+2 种基金Research Fund for the Doctoral Program of Higher Education of China(20110101110037,20120101130013)the Qianjiang Excellence Project of Zhejiang Province(2013R10035)International Science&Technology Cooperation Program of China(2014DFG52320)
文摘Based on the noncovalent functionalization of ferrocene-grafted polyethylenimine （PEI-Fc） and carbon nanotubes （CNTs）, CNT bundles are exfoliated by PEI-Fc solution and thus form stable compounds PEI-Fc@CNTs, which is used to construct the PEI-Fc@CNTs/DNA multilayers through layer-by-layer assembly. The multilayers show a highly uniform and homogeneous characteristic, which significantly improve the electrical property of the multilayers. Upon the oxidation electrical potential, the ferrocene groups are switched from reduction state （[Fe（C5H5）2]） to oxidation state （[Fe（C5H5）2]^＋）, leading to change of microenvironments＇ charge density, resulting in swelling of the multilayers and a final degree of swelling of 37 % and the decrease of multilayer stiffness. We maintain that electrochemical control over the swelling behavior of multilayers could have important implications for responsive coatings of nanoscale devices, including mechanically tunable surfaces which are used to modulate cellular activities and control drug delivery.
