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Masatake Haruta

Publications and source records attributed to Masatake Haruta.

9 recordsLinked to original sources

In situ UV-vis and EPR study on the formation of hydroperoxide species during direct gas phase propylene epoxidation over Au/Ti-SiO(2) catalyst.

In recent years, there have been great experimental and theoretical advances in the understanding of the epoxidation of propylene by O(2) and H(2) over Au supported on titanium-containing oxidic supports; however, thus far spectroscopic evidence of reacting species for proposed mechanisms has been lacking. Hydroperoxide species have been postulated as an intermediate responsible for the epoxidation of propylene with O(2) and H(2). In order to obtain direct evidence for the different type of active oxygen species, in situ UV-vis and EPR measurements were carried out during the epoxidation of propylene with O(2) and H(2) over a Au/Ti-SiO(2) (Ti/Si = 3:100) catalyst. It was determined that the adsorbed species of oxygen (O(2)(-)) resided on Au, more likely at a perimeter site, and it led to the formation of titanium hydroperoxo species. These results support the possible mechanism of formation of these hydroperoxo species via H(2)O(2) produced from O(2) and H(2) adsorbed on the Au surfaces.

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TEM observations of Au and Ir particles supported on CeO2.

Au/CeO2 and Ir/CeO2 catalysts were observed by a transmission electron microscope in order to investigate the nano-structures of Au and Ir particles and CeO2 grains and the interface structure between metallic particles and CeO2. An annular dark field scanning transmission electron microscope (ADF-STEM) and an energy dispersive X-ray spectroscopy (EDS) revealed that the metallic particles smaller than 2 nm in diameter are highly dispersed on CeO2 supports in both catalysts. For model samples of larger CeO2 particles with flat facets of low-index surfaces, high resolution transmission electron microscopy observations of Au/CeO2 and Ir/CeO2 interfaces were made and the epitaxial relationship between Au and CeO2, (111)[110]Au//(111)[110]CeO2 has been found for the first time.

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When gold is not noble: catalysis by nanoparticles.

Bulk gold is chemically inert and is generally regarded as a poor catalyst. However, when gold is in very small particles with diameters below 10 nm and is deposited on metal oxides or activated carbon, it becomes surprisingly active, especially at low temperatures, for many reactions such as CO oxidation and propylene epoxidation. The catalytic performance of Au is defined by three major factors: contact structure, support selection, and particle size. The role of the perimeter interfaces of Au particles as the sites for reactions is discussed as well as the change in chemical reactivity of Au clusters composed of fewer than 300 atoms.

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Electron holographic 3-D nano-analysis of Au/TiO2 catalyst at interface.

Three-dimensional (3-D) nanostructures of gold catalysts supported on TiO2 were analysed by electron holography and high-resolution electron microscopy. The contact angle of the gold particle on TiO2 tended to be >90 degrees in the case of gold particles with a size (height) of >4 nm and it tended to be <90 degrees for gold particles with a height of <2 nm. The change in morphology increases the perimeter at the Au/TiO2 interface as the particle size decreases. This change in 3-D structure should be attributed to a change in electronic structure at the interface. It was found that electron holography enabled 3-D analysis at the atomic level and was effective for analysing nanostructured particles.

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Analytical TEM observation of Au and Ir deposited on rutile TiO2.

As a model catalyst, gold and iridium were co-deposited on a single crystal of rutile TiO2 using the deposition precipitation method in order to clarify the synergetic effect of the combination of Au with Ir on the catalytic performance of the oxidative decomposition of odour and dioxins. Analyses by means of high-resolution transmission electron microscopy, energy-dispersive X-ray spectroscopy and electron energy-loss spectroscopy revealed that pillars of IrO2 grew on the TiO2 substrate to each of which one Au nanoparticle was attached. This mushroom-like structure appeared to be formed by self-organization of Au, Ir and oxygen. Epitaxial contact was observed between the Au nanoparticle/IrO2 pillar and IrO2 pillar/TiO2 substrate interfaces. The growth process of the structure was investigated by transmission electron microscope observations of the Au-Ir complex before and after heating in air.

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