The effect of a wide variety of metal oxide （MOx） supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co‐precipitation and deposition–precipitation methods and under id...The effect of a wide variety of metal oxide （MOx） supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co‐precipitation and deposition–precipitation methods and under identical calcination conditions, supported gold catalysts were prepared on a wide variety of MOx supports, and the temperature for 50%conversion was measured to qualita‐tively evaluate the catalytic activities of these simple MOx and supported Au catalysts. Furthermore, the difference in these temperatures for the simple MOx compared to the supported Au catalysts is plotted against the metal–oxygen binding energies of the support MOx. A clear volcano‐like correla‐tion between the temperature difference and the metal–oxygen binding energies is observed. This correlation suggests that the use of MOx with appropriate metal–oxygen binding energies （300–500 kJ/atom O） greatly improves the catalytic activity of MOx by the deposition of Au NPs.展开更多
Since Haruta et al. discovered that small gold nanoparticles finely dispersed on certain metal oxide supports can exhibit surprisingly high activity in CO oxidation below room temperature, heterogeneous catalysis by s...Since Haruta et al. discovered that small gold nanoparticles finely dispersed on certain metal oxide supports can exhibit surprisingly high activity in CO oxidation below room temperature, heterogeneous catalysis by supported gold nanoparticles has attracted tremendous attention. The majority of publications deal with the preparation and characterization of conventional gold catalysts （e.g., Au/TiO2）, the use of gold catalysts in various catalytic reactions, as well as elucidation of the nature of the active sites and reaction mechanisms. In this overview, we highlight the development of novel supported gold catalysts from a materials perspective. Examples, mostly from those reported by our group, are given concerning the development of simple gold catalysts with single metal-support interfaces and heterostructured gold catalysts with complicated interfacial structures. Catalysts in the first category include active Au/SiO2 and Au/metal phosphate catalysts, and those in the second category include catalysts prepared by pre-modification of supports before loading gold, by post-modification of supported gold catalysts, or by simultaneous dispersion of gold and an inorganic component onto a support. CO oxidation has generally been employed as a probe reaction to screen the activities of these catalysts. These novel gold catalysts not only provide possibilities for applied catalysis, but also furnish grounds for fundamental research.展开更多
In this work, the intensification of luminol electrochemiluminescence (ECL) by metallic oxide nanoparticles (MONPs), as ZnO, MnO2,In2O3 and TiO2 , under alkaline condition is reported and the related mechanism is stud...In this work, the intensification of luminol electrochemiluminescence (ECL) by metallic oxide nanoparticles (MONPs), as ZnO, MnO2,In2O3 and TiO2 , under alkaline condition is reported and the related mechanism is studied. It is found that all four types of those MONPs exhibit the effect toward the ECL intensification of luminol. Furthermore, the silica sol-gel film is taken to immobilize the MONPs onto the platinum electrodes. The so-obtained modified electrodes also show the enhanced ECL and better signal/noise ratio, as well improved signal stability. Finally, the ECL reagent, luminol, is immobilized together with the MONPs onto the electrode surface to perform as the ECL sensor. On resulting sensors, good linear responses are obtained toward hydrogen peroxide. The mechanism of intensification of luminol ECL by MONPs is discussed in this paper. It is proposed that the ECL intensification can be attributed to the production of reactive oxygen species, as well as the adsorption of luminol on surface of MONPs.展开更多
Au has been loaded （1% wt.） on different commercial oxide supports （CuO, La2O3, Y2O3, NiO） by three different methods： double impregnation （DIM）, liquid-phase reductive deposition （LPRD）, and ultrasonication ...Au has been loaded （1% wt.） on different commercial oxide supports （CuO, La2O3, Y2O3, NiO） by three different methods： double impregnation （DIM）, liquid-phase reductive deposition （LPRD）, and ultrasonication （US）. Samples were characterised by N2 adsorption at -196℃, high-resolution transmission electron microscopy, selected area electron diffraction, energy dispersive X-ray spectrometry, high-angle annular dark-field imaging （Z-contrast）, X-ray diffraction, and temperature programmed reduction. CO oxidation was used as a test reaction to compare the catalytic activities. The best results were obtained with Au loaded by DIM on the NiO support, with an activity of 7.2 × 10^（-4） molco·gAu^（-1）·s^（-1） at room temperature. This is most likely related to the Au nanoparticle size being the smallest in this catalyst （average 4.8 nm）, since it is well known that gold particle size determines the catalytic activity. Other samples, having larger Au particle sizes （in the 2-12 nm range, with average sizes ranging from 4.8 to 6.8 nm）, showed lower activities. Nevertheless, all samples prepared by DIM had activities （from 1.1 × 10^（-4） to 7.2 × 10^（-4） molco·gAu^（-1）·S^（-1）, at room temperature） above those reported in the literature for gold on similar oxide supports. Therefore, this method gives better results than the most usual methods of deposition-precipitation or co-precipitation.展开更多
文摘The effect of a wide variety of metal oxide （MOx） supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co‐precipitation and deposition–precipitation methods and under identical calcination conditions, supported gold catalysts were prepared on a wide variety of MOx supports, and the temperature for 50%conversion was measured to qualita‐tively evaluate the catalytic activities of these simple MOx and supported Au catalysts. Furthermore, the difference in these temperatures for the simple MOx compared to the supported Au catalysts is plotted against the metal–oxygen binding energies of the support MOx. A clear volcano‐like correla‐tion between the temperature difference and the metal–oxygen binding energies is observed. This correlation suggests that the use of MOx with appropriate metal–oxygen binding energies （300–500 kJ/atom O） greatly improves the catalytic activity of MOx by the deposition of Au NPs.
文摘Since Haruta et al. discovered that small gold nanoparticles finely dispersed on certain metal oxide supports can exhibit surprisingly high activity in CO oxidation below room temperature, heterogeneous catalysis by supported gold nanoparticles has attracted tremendous attention. The majority of publications deal with the preparation and characterization of conventional gold catalysts （e.g., Au/TiO2）, the use of gold catalysts in various catalytic reactions, as well as elucidation of the nature of the active sites and reaction mechanisms. In this overview, we highlight the development of novel supported gold catalysts from a materials perspective. Examples, mostly from those reported by our group, are given concerning the development of simple gold catalysts with single metal-support interfaces and heterostructured gold catalysts with complicated interfacial structures. Catalysts in the first category include active Au/SiO2 and Au/metal phosphate catalysts, and those in the second category include catalysts prepared by pre-modification of supports before loading gold, by post-modification of supported gold catalysts, or by simultaneous dispersion of gold and an inorganic component onto a support. CO oxidation has generally been employed as a probe reaction to screen the activities of these catalysts. These novel gold catalysts not only provide possibilities for applied catalysis, but also furnish grounds for fundamental research.
基金supported by the National Natural Science Foundation of China (20275025 & 20675055)the Natural Science Foundation of Jiangsu Province (BK2009111)Technology Plan of Suzhou (SYJG0901)
文摘In this work, the intensification of luminol electrochemiluminescence (ECL) by metallic oxide nanoparticles (MONPs), as ZnO, MnO2,In2O3 and TiO2 , under alkaline condition is reported and the related mechanism is studied. It is found that all four types of those MONPs exhibit the effect toward the ECL intensification of luminol. Furthermore, the silica sol-gel film is taken to immobilize the MONPs onto the platinum electrodes. The so-obtained modified electrodes also show the enhanced ECL and better signal/noise ratio, as well improved signal stability. Finally, the ECL reagent, luminol, is immobilized together with the MONPs onto the electrode surface to perform as the ECL sensor. On resulting sensors, good linear responses are obtained toward hydrogen peroxide. The mechanism of intensification of luminol ECL by MONPs is discussed in this paper. It is proposed that the ECL intensification can be attributed to the production of reactive oxygen species, as well as the adsorption of luminol on surface of MONPs.
文摘Au has been loaded （1% wt.） on different commercial oxide supports （CuO, La2O3, Y2O3, NiO） by three different methods： double impregnation （DIM）, liquid-phase reductive deposition （LPRD）, and ultrasonication （US）. Samples were characterised by N2 adsorption at -196℃, high-resolution transmission electron microscopy, selected area electron diffraction, energy dispersive X-ray spectrometry, high-angle annular dark-field imaging （Z-contrast）, X-ray diffraction, and temperature programmed reduction. CO oxidation was used as a test reaction to compare the catalytic activities. The best results were obtained with Au loaded by DIM on the NiO support, with an activity of 7.2 × 10^（-4） molco·gAu^（-1）·s^（-1） at room temperature. This is most likely related to the Au nanoparticle size being the smallest in this catalyst （average 4.8 nm）, since it is well known that gold particle size determines the catalytic activity. Other samples, having larger Au particle sizes （in the 2-12 nm range, with average sizes ranging from 4.8 to 6.8 nm）, showed lower activities. Nevertheless, all samples prepared by DIM had activities （from 1.1 × 10^（-4） to 7.2 × 10^（-4） molco·gAu^（-1）·S^（-1）, at room temperature） above those reported in the literature for gold on similar oxide supports. Therefore, this method gives better results than the most usual methods of deposition-precipitation or co-precipitation.
