Papers by Author: Shingo Tanaka

Abstract: The structures of Au particles on CeO2 surfaces were observed by an analytical transmission electron microscopy (TEM) equipped with annular dark field scanning transmission electron microscopy (HAADF-STEM) systems. The Au/CeO2 model catalysts were prepared by using the poly-crystalline CeO2 substrates. The Au particles of 2-5 nm in diameter were deposited on the substrates. The preferential orientation relationship of (111)[1-10]Au//(111)[1-10]CeO2 was frequently observed in profile-view HRTEM images on CeO2 (111) surface. High resolution HAADF-STEM images were also obtained for Au-CeO2 interfaces. The position of atomic columns of Au and Ce at Au-CeO2 interface is directly investigated from HAADF-STEM images. The structure of the interfaces between Au particles and CeO2 (111), (100), (110) surfaces were discussed.

Abstract: We performed first-principles calculations of stable atomic structure and partial density of states (PDOS) analysis of Ethylene (C2H4) adsorption on Pd(100) surface stacked on fcc-Au using the projector augmented-wave (PAW) method. In case of Pd overlayers on the Au(100) substrate, from the analysis of PDOS around surface, highest occupied states become sharpen compared with the case of C2H4 adsorption on Pd monometallic slab surface in both di- and  adsorption model.

Abstract: First-principles calculations based on density-functional theory are powerful tools to investigate the structure and properties of ceramic interfaces. The Schottky-barrier heights of SiC/metal and Al2O3/metal interfaces have been examined, and significant effects of the interface stoichiometry (termination species) and metallic species have been found. Ab initio tensile tests have been applied to Al2O3/Cu and Al2O3/Ni interfaces, where the strength and features of failure also greatly depend on the interface stoichiometry and metallic species.

Abstract: Atomic and electronic structures of H-adsorbed Pd overlayers on Au(100) substrates have been studied by first-principles calculations. The geometric strain effects change the electronic structure and local reactivity of the surface. The lattice strained Pd overlayers on Au surfaces have larger adsorption energies for atomic hydrogen than the unstrained Pd slabs. Adsorption energies for several adsorption sites on the models with different numbers of Pd overlayers have been analyzed from the viewpoints of strains and H-Pd and H-substrate interactions.

Abstract: Pt nano-particles are supported on carbon materials at the electrode catalysts of protonexchange menbrane fuel cells. Pt nano-particles are desirable to be strongly adsorbed on carbon materials for high dispersion, although strong Pt-C interactions may affect the catalytic activity of small clusters. Thus we have examined H-atom absorption on Pt clusters supported or unsupported on graphene sheets, using first-principles calculations. For Pt-atom/graphene systems, a H atom is more weakly adsorbed than for a free Pt atom, and the H-Pt interaction becomes weaker if the interaction between a Pt atom and graphene becomes stronger. For the Ptn-cluster/graphene systems (n=2-4), the H-Pt interactions are also substantially changed from those for free Pt clusters. In the Pt clusters on graphene, the Pt-Pt distances are substantially changed associated with the electronicstructure changes by the Pt-C interactions. These structural and electronic changes in the Pt clusters as well as the presence of graphene itself seem to cause the changes in the absorption energies and preferential sites of H-atom absorption.

Abstract: We performed first-principles calculations using the projector augmented-wave (PAW) method for Au/Pd slab interface models. The calculations of relaxed configurations and energies for the thin Pd layers (3 layers) stacking on Au (111) and Au (100) slabs with an epitaxial relationship represent that Pd overlayers have a lateral expansion in both cases. This trend is in good agreement with experimental results for Pd/Au slabs and Au-Pd core-shell nanoparticles, obtained by electron microscopy, X-ray diffraction, and positron annihilation. In addition, an intermixing configuration near the Au-Pd interface was shown to be more stable than the binary separated one.