Metal-free catalysts are preferred during these days in organic synthesis or in polymeriza- tions. Sulfonic acid is reported to be efficient in catalyzing reactions between isocyanates and alcohols. In this work, synt...Metal-free catalysts are preferred during these days in organic synthesis or in polymeriza- tions. Sulfonic acid is reported to be efficient in catalyzing reactions between isocyanates and alcohols. In this work, synthesis of sulfonic acid immobilized organic nanoparticles (nanoacid) and its application in catalyzing urethane formation, are elaborated. The nanoacid can be simply prepared by miniemulsion polymerization with a reactive surfacrant, namely sodium 4-((perfluoronon-8-en-l-yl)oxy)benzenesulfonate, followed by an acidification. From the images of scanning electron microscope, the nanoacid obtained is found to be narrowly dispersed and the average diameter is around 90 nm. The measured sulfur content is 0.5%, from which the content of sulfonic acid in the nanoparticles is calculated to be 0.16 mmol/g. When catalyzing urethane formation based on hexamethylene diisocyanate and n-butanol, the nanoacid catalyst exhibits considerable efficiency.展开更多
Stearic-acid-modified TiO2 (STA-TiO2) particles were prepared via the impregnation approach and used as a precursor for preparing TiO2 Janus particles. The morphology, structure, and properties of the TiO2 Janus parti...Stearic-acid-modified TiO2 (STA-TiO2) particles were prepared via the impregnation approach and used as a precursor for preparing TiO2 Janus particles. The morphology, structure, and properties of the TiO2 Janus particles were characterized using Fourier-transform infrared spectroscopy, ultraviolet- visible diffuse reflectance spectroscopy, thermogravimetric analysis, fluorescence microscopy, high-resolution transmission electron microscopy, contact angle analysis, dynamic light scattering, biological microscopy, X-ray photoelectron spectroscopy, and electrochemical impedance spectroscopy measurements. The results show that TiO2 Janus particles can be successfully prepared via toposelective surface modification. STA grafted on the surface of TiO2 enhances its hydrophobicity, promotes charge separation, and improves its adsorption capacity for organic compounds. The TiO2 Janus particles strongly adsorb on an oil-water interface to form a stable Pickering emulsion. The degradation rates of high-concentration kerosene and nitrobenzene wastewaters when the photocatalyst is pure TiO2, STA-TiO2, or TiO2 Janus particles are discussed and compared. The degradation rates were determined using an ultraviolet-visible spectrophotometer. It was found that the Pickering emulsion stabilized by the TiO2 Janus particles exhibited the best photocatalytic performance;these Janus particles show promising potential for catalytic application.展开更多
Pd-Ag bimetallic alloy nanoparticles were synthesized by the reverse microemulsion method, and then deposited on A1203 to form the supported catalyst. The nanoparticles of Pd-Ag and Pd-Ag/AI203 samples were characteri...Pd-Ag bimetallic alloy nanoparticles were synthesized by the reverse microemulsion method, and then deposited on A1203 to form the supported catalyst. The nanoparticles of Pd-Ag and Pd-Ag/AI203 samples were characterized by UV/ Vis, HRTEM, EDX, XRD, and XPS. The test results indicated that Pd-Ag bimetallic alloy nanoparticles with a size of about 2 nm and a face-centered cubic (fcc) structure were formed in the measured area of microemulsion. The growth of nanopar- ticles was effectively limited within the droplet of micoremulsion. TEM image exhibited that the Pd-Ag alloy nanoparticles were well-dispersed on the A1203 support. The catalytic performance of various catalysts for selective hydrogenation of acetylene showed that a higher acetylene conversion and selectivity to ethylene upon acetylene hydrogenation was achieved on a nano-sized Pd-Ag bimetallic catalyst with a Pd/Ag alloy supported molar ratio of 1:1.5.展开更多
Ce O2@Si O2 core-shell nanoparticles were prepared by microemulsion method, and metalloporphyrins were immobilized on the Ce O2@Si O2 core-shell nanoparticles surface via amide bond. The supported metalloporphyrin cat...Ce O2@Si O2 core-shell nanoparticles were prepared by microemulsion method, and metalloporphyrins were immobilized on the Ce O2@Si O2 core-shell nanoparticles surface via amide bond. The supported metalloporphyrin catalysts were characterized by N2 adsorption-desorption isotherm(BET), scanning electron microscopy(SEM), transmission electron microscopy(TEM), X-ray diffraction(XRD), ultraviolet and visible spectroscopy(UV-Vis), and Fourier transform infrared spectroscopy(FT-IR). The results show that the morphology of Ce O2@Si O2 nanoparticles is core-shell microspheres with about 30 nm in diameter, and metalloporphyrins are immobilized on the Ce O2@Si O2 core-shell nanoparticles via amide bond. Especially, the core-shell structure contains multi Ce O2 core and thin Si O2 shell, which may benefit the synergistic effect between the Ce O2 core and the porphyrin anchored on the very thin Si O2 shell. As a result, this supported metalloporphyrin catalysts present comparably high catalytic activity and stability for oxidation of ethylbenzene with molecular oxygen, namely, ethylbenzene conversion remains around 12% with identical selectivity of about 80% for acetophenone even after six-times reuse of the catalyst.展开更多
The systematic experimental studies were performed on the hydrate formation kinetics and gas-hydrate equilibrium for a simulated catalytic cracking gas in the water-in-oil emulsion. The effect of temperature, pressure...The systematic experimental studies were performed on the hydrate formation kinetics and gas-hydrate equilibrium for a simulated catalytic cracking gas in the water-in-oil emulsion. The effect of temperature, pressure and initial gas-liquid ratio on the hydrate formation was studied, respectively. The data were obtained at pressures ranging from 3.5 to 5 MPa and temperatur.es from 274.15 to 277.15 K. The results showed that hydrogen and methane can be separated Irom the (~2+ ti'action by tOrming hydrate at around 273.15 K which is much higher temperature than that of the cryogenic separation method, and the hydrate formation rate can be enhanced in the wa- ter-in-oil emulsion compared to pure water. The experiments provided the basic data for designing the industrial process, and setting the suitable operational conditions. The measured data ot gas-hydrate equilibria were compared with the predictions by using the Chen-Guo hydrate thermodynamic model.展开更多
A water-in-oil microemulsion made up of a cyclohexane/n-hexyl alcohol/Polyethylene glycol tertoctylphenyl/aqueous solution including Bi3+ and VO+3 ions yields the spherical BiVO4 precursors with the size from 5 to 300...A water-in-oil microemulsion made up of a cyclohexane/n-hexyl alcohol/Polyethylene glycol tertoctylphenyl/aqueous solution including Bi3+ and VO+3 ions yields the spherical BiVO4 precursors with the size from 5 to 300 nm. Well-crystallized monoclinic scheelite BiVO4 particles with nanometer or micrometer size are fabricated in control by heating microemulsion precursors under various temperatures. The corresponding nucleation and growth process of as-prepared samples has also been investigated via TEM,which demonstrates the detailed morphological evolution of nuclei inside the precursors. As-prepared BiVO4 photocatalysts exhibit enhanced photocatalytic activity under visible-light irradiation in comparison with the bulk BiVO4 prepared by solid-state reaction. The highest RB degrading efficiency of 98% in 180 min under visible-light irradiation is observed for the sample calcined at 600 °C.展开更多
We demonstrated a method to fabricate functional hybrid film patches that were used to form Pickering emulsions (PEs). The hybrid patches were made of carbon nanotubes, Fe3O4 nanoparticles, octadecyltrimethoxysilane...We demonstrated a method to fabricate functional hybrid film patches that were used to form Pickering emulsions (PEs). The hybrid patches were made of carbon nanotubes, Fe3O4 nanoparticles, octadecyltrimethoxysilane, and poly(diallyldimethylammonium chloride). The aqueous phase of the hybridpatch stabilized PEs can be easily separated by applying a magnetic field. The hybrid-film-patch stabilized PEs are extremely stable and lasted for eight months at room temperature. Furthermore, they are easily ruptured by adding ethanol, and regenerated by vortexing the patches in aqueous/oil mixtures, enabling the inner hydrophilic side of the patches to be easily modified with metal nanoparticles. As an example, palladium nanoparticles were embedded into the surface of the hybrid patches using an in situ reduction method. The Pd functionalized patch formed PEs showed an excellent catalytic performance for the hydrogenation of acetone with a yield of 99.5%. The same batch of Pd functionalized patches was recycled 13 times without loss of the catalytic activity. The hybrid-patch formed PEs have a great potential in the catalytic field.展开更多
文摘Metal-free catalysts are preferred during these days in organic synthesis or in polymeriza- tions. Sulfonic acid is reported to be efficient in catalyzing reactions between isocyanates and alcohols. In this work, synthesis of sulfonic acid immobilized organic nanoparticles (nanoacid) and its application in catalyzing urethane formation, are elaborated. The nanoacid can be simply prepared by miniemulsion polymerization with a reactive surfacrant, namely sodium 4-((perfluoronon-8-en-l-yl)oxy)benzenesulfonate, followed by an acidification. From the images of scanning electron microscope, the nanoacid obtained is found to be narrowly dispersed and the average diameter is around 90 nm. The measured sulfur content is 0.5%, from which the content of sulfonic acid in the nanoparticles is calculated to be 0.16 mmol/g. When catalyzing urethane formation based on hexamethylene diisocyanate and n-butanol, the nanoacid catalyst exhibits considerable efficiency.
基金supported by the National Natural Science Foundation of China(21808214)
文摘Stearic-acid-modified TiO2 (STA-TiO2) particles were prepared via the impregnation approach and used as a precursor for preparing TiO2 Janus particles. The morphology, structure, and properties of the TiO2 Janus particles were characterized using Fourier-transform infrared spectroscopy, ultraviolet- visible diffuse reflectance spectroscopy, thermogravimetric analysis, fluorescence microscopy, high-resolution transmission electron microscopy, contact angle analysis, dynamic light scattering, biological microscopy, X-ray photoelectron spectroscopy, and electrochemical impedance spectroscopy measurements. The results show that TiO2 Janus particles can be successfully prepared via toposelective surface modification. STA grafted on the surface of TiO2 enhances its hydrophobicity, promotes charge separation, and improves its adsorption capacity for organic compounds. The TiO2 Janus particles strongly adsorb on an oil-water interface to form a stable Pickering emulsion. The degradation rates of high-concentration kerosene and nitrobenzene wastewaters when the photocatalyst is pure TiO2, STA-TiO2, or TiO2 Janus particles are discussed and compared. The degradation rates were determined using an ultraviolet-visible spectrophotometer. It was found that the Pickering emulsion stabilized by the TiO2 Janus particles exhibited the best photocatalytic performance;these Janus particles show promising potential for catalytic application.
文摘Pd-Ag bimetallic alloy nanoparticles were synthesized by the reverse microemulsion method, and then deposited on A1203 to form the supported catalyst. The nanoparticles of Pd-Ag and Pd-Ag/AI203 samples were characterized by UV/ Vis, HRTEM, EDX, XRD, and XPS. The test results indicated that Pd-Ag bimetallic alloy nanoparticles with a size of about 2 nm and a face-centered cubic (fcc) structure were formed in the measured area of microemulsion. The growth of nanopar- ticles was effectively limited within the droplet of micoremulsion. TEM image exhibited that the Pd-Ag alloy nanoparticles were well-dispersed on the A1203 support. The catalytic performance of various catalysts for selective hydrogenation of acetylene showed that a higher acetylene conversion and selectivity to ethylene upon acetylene hydrogenation was achieved on a nano-sized Pd-Ag bimetallic catalyst with a Pd/Ag alloy supported molar ratio of 1:1.5.
基金Projects(J21103045,J1210040,J1103312) supported by the National Natural Science Foundation of ChinaProject supported by the Fundamental Research Funds for the Central Universities of China
文摘Ce O2@Si O2 core-shell nanoparticles were prepared by microemulsion method, and metalloporphyrins were immobilized on the Ce O2@Si O2 core-shell nanoparticles surface via amide bond. The supported metalloporphyrin catalysts were characterized by N2 adsorption-desorption isotherm(BET), scanning electron microscopy(SEM), transmission electron microscopy(TEM), X-ray diffraction(XRD), ultraviolet and visible spectroscopy(UV-Vis), and Fourier transform infrared spectroscopy(FT-IR). The results show that the morphology of Ce O2@Si O2 nanoparticles is core-shell microspheres with about 30 nm in diameter, and metalloporphyrins are immobilized on the Ce O2@Si O2 core-shell nanoparticles via amide bond. Especially, the core-shell structure contains multi Ce O2 core and thin Si O2 shell, which may benefit the synergistic effect between the Ce O2 core and the porphyrin anchored on the very thin Si O2 shell. As a result, this supported metalloporphyrin catalysts present comparably high catalytic activity and stability for oxidation of ethylbenzene with molecular oxygen, namely, ethylbenzene conversion remains around 12% with identical selectivity of about 80% for acetophenone even after six-times reuse of the catalyst.
基金Supported by the National iqatural Science Foundation of China (20925623, U1162205).
文摘The systematic experimental studies were performed on the hydrate formation kinetics and gas-hydrate equilibrium for a simulated catalytic cracking gas in the water-in-oil emulsion. The effect of temperature, pressure and initial gas-liquid ratio on the hydrate formation was studied, respectively. The data were obtained at pressures ranging from 3.5 to 5 MPa and temperatur.es from 274.15 to 277.15 K. The results showed that hydrogen and methane can be separated Irom the (~2+ ti'action by tOrming hydrate at around 273.15 K which is much higher temperature than that of the cryogenic separation method, and the hydrate formation rate can be enhanced in the wa- ter-in-oil emulsion compared to pure water. The experiments provided the basic data for designing the industrial process, and setting the suitable operational conditions. The measured data ot gas-hydrate equilibria were compared with the predictions by using the Chen-Guo hydrate thermodynamic model.
基金supported by the Foundation for Outstanding Young Scientist of Shandong Province (BS2010CL049)the Program for New Cen-tury Excellent Talents in University (NCET-08-0511)
文摘A water-in-oil microemulsion made up of a cyclohexane/n-hexyl alcohol/Polyethylene glycol tertoctylphenyl/aqueous solution including Bi3+ and VO+3 ions yields the spherical BiVO4 precursors with the size from 5 to 300 nm. Well-crystallized monoclinic scheelite BiVO4 particles with nanometer or micrometer size are fabricated in control by heating microemulsion precursors under various temperatures. The corresponding nucleation and growth process of as-prepared samples has also been investigated via TEM,which demonstrates the detailed morphological evolution of nuclei inside the precursors. As-prepared BiVO4 photocatalysts exhibit enhanced photocatalytic activity under visible-light irradiation in comparison with the bulk BiVO4 prepared by solid-state reaction. The highest RB degrading efficiency of 98% in 180 min under visible-light irradiation is observed for the sample calcined at 600 °C.
基金This work was supported by the National Natural Science Foundation of China (Nos. 21273059 and 21003032), State Key Laboratory of Urban Water Resource and Environment (Harbin Institute of Technology) (No. 2014DX09), the Fundamental Research Funds for the Central Universities (No. HIT. KISTP. 201407), and Harbin Science and Technology Research Council (No. 2014RFXXJ063).
文摘We demonstrated a method to fabricate functional hybrid film patches that were used to form Pickering emulsions (PEs). The hybrid patches were made of carbon nanotubes, Fe3O4 nanoparticles, octadecyltrimethoxysilane, and poly(diallyldimethylammonium chloride). The aqueous phase of the hybridpatch stabilized PEs can be easily separated by applying a magnetic field. The hybrid-film-patch stabilized PEs are extremely stable and lasted for eight months at room temperature. Furthermore, they are easily ruptured by adding ethanol, and regenerated by vortexing the patches in aqueous/oil mixtures, enabling the inner hydrophilic side of the patches to be easily modified with metal nanoparticles. As an example, palladium nanoparticles were embedded into the surface of the hybrid patches using an in situ reduction method. The Pd functionalized patch formed PEs showed an excellent catalytic performance for the hydrogenation of acetone with a yield of 99.5%. The same batch of Pd functionalized patches was recycled 13 times without loss of the catalytic activity. The hybrid-patch formed PEs have a great potential in the catalytic field.