A serial of ordered meso-macroporous phosphotungstic acid(HPW) supported on SiO2 nanocomposites were successfully prepared by a homogeneous precipitation method, using monodispersed polystyrene(PS) microspheres and ca...A serial of ordered meso-macroporous phosphotungstic acid(HPW) supported on SiO2 nanocomposites were successfully prepared by a homogeneous precipitation method, using monodispersed polystyrene(PS) microspheres and cationic surfactant as structure directing agent. These nanocomposites were used as catalysts for oxidative desulfurization(ODS) of model fuel. The materials were characterized by scanning electron microscopy(SEM), transmission electron microscopy(TEM), N2 adsorption-desorption isothrem, X-ray diffraction(XRD), and Fourier transform infrared spectra(FTIR). The characterization results suggested that the as-prepared material possessed ordered meso-macroporous architectures with Keggin type phosphotungstic acid dispersed homogeneously in SiO2 matrix. Under the selected reaction conditions, dibenzothiophene(DBT) in model fuel can be removed within 2 h at room temperature(30 ℃). In addition, only 1.2% of efficiency lose than the fresh catalyst even after 5 cycles.展开更多
The meso-macroporous Fe-doped Cu O was prepared by a simple hydrothermal method combined with post-annealing. The samples were characterized by X-ray powder diffraction(XRD), scanning electron microscopy(SEM), Brunaue...The meso-macroporous Fe-doped Cu O was prepared by a simple hydrothermal method combined with post-annealing. The samples were characterized by X-ray powder diffraction(XRD), scanning electron microscopy(SEM), Brunauer-Emmett-Teller N2 adsorption-desorption analyses and UV-vis diffuses reflectance spectroscopy. The Fe-doped Cu O sample shows higher adsorption capacity and photocatalytic activity for xanthate degradation than pure Cu O under visible light irradiation. In addition, the adsorption process is found to fit Langmuir isotherms and pseudo-second-order kinetics. The the first order kinetic Langmuir Hinshelwood model was used to study the reaction kinetics of photocatalytic degradation, and the apparent rate constant( k) was calculated. The value of k for Fe-doped Cu O is 1.5 times that of pure Cu O. The higher photocatalytic activity of Fe-doped Cu O is attributed to higher specific surface area together with stronger visible light absorption.展开更多
Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X...Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X represents Fe/Co molar ratio in bimetallic zeolite imidazole frameworks FeCo-ZIFs) catalysts derived from hierarchical M-FeCo-ZIFs-X was prepared. The micropores in M-FeCo-N-C-X have strong capability in O2 capture as well as dictate the nucleation and early-stage deposition of Li2O2,the mesopores provided a channel for the electrolyte wetting, and the macroporous structure promoted more available active sites when used as cathode for Li-O2 batteries. More importantly, M-Fe CoN-C-0.2 based cathode showed a high initial capacity(18,750 mAh g-1@0.1 A g-1), good rate capability(7900 m Ah g-1@0.5 A g-1), and cycle stability up to 192 cycles. Interestingly, the FeCo-N-C-0.2 without macropores suffered relatively poorer stability with only 75 cycles, although its discharge capacity was still as high as 17,200 mA h g-1(@0.1 A g-1). The excellent performance attributed to the synergistic contribution of homogeneous Fe, Co nanoparticles and N co-doping carbon frameworks with special micro–meso-macroporous structure. The results showed that hierarchical FeCo-N-C architectures are promising cathode catalysts for Li-O2 batteries.展开更多
The structures of electrode meso-macropore and the solvent polarity are the crucial factors dominating the performance of the electric double layer capacitors(EDLCs),but their impacts are usually tangled and difficult...The structures of electrode meso-macropore and the solvent polarity are the crucial factors dominating the performance of the electric double layer capacitors(EDLCs),but their impacts are usually tangled and difficult to decouple and quantitate.Here the effects of electrode meso-macropore structure and solvent polarity on the specific capacitance of an EDLC are quantitatively investigated using a steady-state continuum model.The simulation results indicate the specific capacitances are significantly affected by the meso-macropore surface structure.The specific capacitances significantly decrease for both convex surface structures but obviously increase for both concave surface structures,with the increase of curvature radius from 1 to 20 nm.As for solvents,the polar solvent with high saturated dielectric permittivity improves the capacitance performance.Moreover,the electrode meso-macropore structure is of more concern compared with solvent polarity when aiming at enhancing the specific capacitance.These results provide fundamentals for the rational design of porous electrodes and polar electrolytes for EDLCs.展开更多
基金Supported by the National Nature Science Foundation of China(No.21476177)
文摘A serial of ordered meso-macroporous phosphotungstic acid(HPW) supported on SiO2 nanocomposites were successfully prepared by a homogeneous precipitation method, using monodispersed polystyrene(PS) microspheres and cationic surfactant as structure directing agent. These nanocomposites were used as catalysts for oxidative desulfurization(ODS) of model fuel. The materials were characterized by scanning electron microscopy(SEM), transmission electron microscopy(TEM), N2 adsorption-desorption isothrem, X-ray diffraction(XRD), and Fourier transform infrared spectra(FTIR). The characterization results suggested that the as-prepared material possessed ordered meso-macroporous architectures with Keggin type phosphotungstic acid dispersed homogeneously in SiO2 matrix. Under the selected reaction conditions, dibenzothiophene(DBT) in model fuel can be removed within 2 h at room temperature(30 ℃). In addition, only 1.2% of efficiency lose than the fresh catalyst even after 5 cycles.
基金Project(51102285)supported by the National Natural Science Foundation of China
文摘The meso-macroporous Fe-doped Cu O was prepared by a simple hydrothermal method combined with post-annealing. The samples were characterized by X-ray powder diffraction(XRD), scanning electron microscopy(SEM), Brunauer-Emmett-Teller N2 adsorption-desorption analyses and UV-vis diffuses reflectance spectroscopy. The Fe-doped Cu O sample shows higher adsorption capacity and photocatalytic activity for xanthate degradation than pure Cu O under visible light irradiation. In addition, the adsorption process is found to fit Langmuir isotherms and pseudo-second-order kinetics. The the first order kinetic Langmuir Hinshelwood model was used to study the reaction kinetics of photocatalytic degradation, and the apparent rate constant( k) was calculated. The value of k for Fe-doped Cu O is 1.5 times that of pure Cu O. The higher photocatalytic activity of Fe-doped Cu O is attributed to higher specific surface area together with stronger visible light absorption.
基金sponsored by the National Natural Science Foundation of China(21475021 and 21427807)the Fundamental Research Funds for the Central Universities(2242017 K41023)
文摘Developing bifunctional catalysts that increase both the OER and ORR kinetics and transport reactants with high efficiency is desirable. Herein, micro–meso-macroporous FeCo-N-C-X(denoted as "MFeCo-N-C-X", X represents Fe/Co molar ratio in bimetallic zeolite imidazole frameworks FeCo-ZIFs) catalysts derived from hierarchical M-FeCo-ZIFs-X was prepared. The micropores in M-FeCo-N-C-X have strong capability in O2 capture as well as dictate the nucleation and early-stage deposition of Li2O2,the mesopores provided a channel for the electrolyte wetting, and the macroporous structure promoted more available active sites when used as cathode for Li-O2 batteries. More importantly, M-Fe CoN-C-0.2 based cathode showed a high initial capacity(18,750 mAh g-1@0.1 A g-1), good rate capability(7900 m Ah g-1@0.5 A g-1), and cycle stability up to 192 cycles. Interestingly, the FeCo-N-C-0.2 without macropores suffered relatively poorer stability with only 75 cycles, although its discharge capacity was still as high as 17,200 mA h g-1(@0.1 A g-1). The excellent performance attributed to the synergistic contribution of homogeneous Fe, Co nanoparticles and N co-doping carbon frameworks with special micro–meso-macroporous structure. The results showed that hierarchical FeCo-N-C architectures are promising cathode catalysts for Li-O2 batteries.
基金financially supported by the National Basic Research Program of China(2014CB239702)the National Natural Science Foundation of China(21676082,22008067)the China Postdoctoral Science Foundation(2020M681202,2021T140204)。
文摘The structures of electrode meso-macropore and the solvent polarity are the crucial factors dominating the performance of the electric double layer capacitors(EDLCs),but their impacts are usually tangled and difficult to decouple and quantitate.Here the effects of electrode meso-macropore structure and solvent polarity on the specific capacitance of an EDLC are quantitatively investigated using a steady-state continuum model.The simulation results indicate the specific capacitances are significantly affected by the meso-macropore surface structure.The specific capacitances significantly decrease for both convex surface structures but obviously increase for both concave surface structures,with the increase of curvature radius from 1 to 20 nm.As for solvents,the polar solvent with high saturated dielectric permittivity improves the capacitance performance.Moreover,the electrode meso-macropore structure is of more concern compared with solvent polarity when aiming at enhancing the specific capacitance.These results provide fundamentals for the rational design of porous electrodes and polar electrolytes for EDLCs.