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81.
Hiromi Yamashita Kohsuke Mori Sayoko Shironita Yu Horiuchi 《Catalysis Surveys from Asia》2008,12(2):88-100
The isolated and tetrahedrally coordinated metal oxide (Ti, V, Cr, Mo and W-oxides) moieties can be included in the silica
matrixes of silica-based microporous zeolite and mesoporous silica materials and named as “single-site photocatalysts”. Under
UV-light irradiation these single-site photocatalysts form the charge transfer excited state, i.e., the excited electron–hole
pair state which is located quite near to each other in different from the manner observed on semiconducting materials such
as TiO2, and play a significant role in various photocatalytic reactions. These single-site photocatalysts not only can promote photocatalytic
reactions but also can be utilized to synthesis of functional materials. The nano-sized metal catalyst and visible-light sensitive
binary oxide photocatalyst can be synthesized on the excited single-site photocatalyst under UV-light irradiation. The transparent
mesoporous silica thin film with single-site photocatalyst generates the super-hydrophilic surface. In this review, our recent
applications of single-site photocatalysts to synthesis of the surface functional materials have been introduced. 相似文献
82.
83.
Phase transition behavior of monomolecular water in solid polystyrene was examined by temperature variable Fourier transform infrared spectroscopy. Spectral changes showed for the first time that monomolecular water in a polymer matrix (in a closed system) could be condensed and then frozen and also that the ice formed could be grown and diminished by vapor deposition in cooling process and sublimation in heating process, respectively. 相似文献
84.
Interaction of wheat germ agglutinin with an N-acetylglucosamine-carrying telomer brush accumulated on a colloidal gold monolayer 总被引:1,自引:0,他引:1
A disulfide-carrying telomer with many pendent N-acetylglucosamine (GlcNAc) residues (Cys-PMHGlcNAc) was obtained by photo-polymerization of 1-(6'-methacryloylaminohexyl)-2-N-acetoamido-2-deoxy d-glucopyranoside) (MHGlcNAc) using a benzyl N,N-diethyldithiocarbamoyl (BDC) derivative that shows abilities of initiation, transfer, and termination (iniferter). The disulfide-carrying telomer was accumulated on a monolayer of colloidal Au on a glass substrate, and the interaction of wheat germ agglutinin (WGA) with GlcNAc residue at the polymer brush-solution interface was examined by using the localized surface plasmon resonance (LSPR) technique. For comparison, an amphiphile carrying many pendent GlcNAc residues was also prepared with MHGlcNAc and a lipophilic radical initiator and was incorporated in a phospholipid liposome to examine interaction of the GlcNAc residue with WGA on the liposome surface using turbidity measurements. Both the colloidal gold optical device and the liposome showed a concentration-dependent specific binding of WGA, and the GlcNAc-carrying liposome had a detection limit of 100 nM for WGA, whereas that of the colloidal gold device was 10nM. The sugar-carrying telomer-coated device examined here is not only useful as a simple biosensor chip but is also expected to expand our knowledge of bio-related phenomena at the liquid-telomer brush interfaces on a colloidal Au. 相似文献
85.
Kohsuke Mori Makoto Shimada Yuu Horiuchi Tetsutaro Ohmichi Norikazu Nishiyama Hidetoshi Fujii Hiromi Yamashita 《Research on Chemical Intermediates》2008,34(5-7):495-505
We have investigated a novel technique for the preparation of nano-sized Pt metals on Ti-containing mesoporous silica (TMS) thin film by photo-assisted deposition (PAD). The transparent TMS thin film was prepared on a quartz plate through sol—gel/spin coating. XRD, UV-Vis and Ti K-edge XAFS measurements revealed the formation of isolated Ti oxide species with a tetrahedral-coordination geometry in the silica framework. Deposition of Pt metal precursor on TMS thin film under UV-light irradiation, followed by reduction with molecular hydrogen, afforded a transparent thin film (Pt/TMS). The formation of highly dispersed nano-sized Pt metals having narrow size distributions was determined by Pd LIII-edge XANES and TEM analysis. The TMS and Pt/TMS thin films have been demonstrated to exhibit a strong hydrophilic property, even before UV irradiation, compared to the common mesoporous silica and TiO2 thin films. After UV-light irradiation, the contact angle of water droplet on the TMS and Pt/TMS thin films became extremely lower, indicating the appearance of the photo-induced super-hydrophilic property. 相似文献
86.
Skeletal Ni Catalysts Prepared from Amorphous Ni–Zr Alloys: Enhanced Catalytic Performance for Hydrogen Generation from Ammonia Borane 下载免费PDF全文
Ai Nozaki Yasutomo Tanihara Dr. Yasutaka Kuwahara Tetsutaro Ohmichi Dr. Kohsuke Mori Dr. Takeshi Nagase Prof. Dr. Hiroyuki Y. Yasuda Prof. Dr. Hiromi Yamashita 《Chemphyschem》2016,17(3):412-417
Skeletal Ni catalysts were prepared from Ni–Zr alloys, which possess different chemical composition and atomic arrangements, by a combination of thermal treatment and treatment with aqueous HF. Hydrogen generation from ammonia borane over the skeletal Ni catalysts proceeded efficiently, whereas the amorphous Ni–Zr alloy was inactive. Skeletal Ni prepared from amorphous Ni30Zr70 alloy had a higher catalytic activity than that prepared from amorphous Ni40Zr60 and Ni50Zr50 alloys. The atomic arrangement of the Ni–Zr alloy also strongly affected the surface structure and catalytic activities. Thermal treatment of the amorphous Ni–Zr alloys at a temperature slightly lower than the crystallization temperature led to an increase of the number of surface‐exposed Ni atoms and an enhancement of the catalytic activities for hydrogen generation from ammonia borane. The skeletal Ni catalysts also showed excellent durability and recyclability. 相似文献
87.
We propose a novel analysis method of ab initio molecular dynamics (AIMD) simulation using a continuous wavelet transform (c-WT) technique. The c-WT technique, one of the time-frequency signal analysis methods, provides a clear view of the dynamical information in time developments. Combined with the auto-correlation function of velocity by AIMD simulation, c-WT analysis enables us to well understand dynamical distribution, such as the vibrational properties following a change of electronic structure in a molecular system. As a practical application, AIMD simulation of core-excited BF(3) (B1s --> 2a(2) (')) is illustrated. AIMD simulation leads to the change of vibrational motion as well as structural deformation by core-excitation. The c-WT analysis clarifies the relationship between structural deformation and the related significant vibrational modes in core-excitation within 50 fs. 相似文献
88.
Grid-based energy density analysis (grid-EDA) that decomposes the total energy into atomic energies by a space-partitioning function is proposed. The kinetic energy, nuclear attraction, and exchange-correlation functional are evaluated on grid points and are split into atomic contributions. To reduce numerical errors in the conventional scheme of numerical integration, the electronic Coulomb and HF exchange interactions are evaluated by the pseudospectral method, which was first applied to an ab initio method by Friesner [Chem. Phys. Lett. 116, 39 (1985)], and are decomposed into atomic contributions. Grid-EDA using the pseudospectral method succeeds in ensuring less than 1 kcalmol error in total energies for small molecules and providing reliable atomic energy contributions for the problematic lithium cluster, which exhibits a strong basis-set dependence for Mulliken-type EDA. Also, site-dependent atomization energies are estimated by grid-EDA for cluster models such as Li(48), C(41)H(60), and Mg(32)O(32). Grid-EDA reveals that these models imitate crystal environments reasonably because atomization energies estimated from the inner atoms of the models are close to the experimental cohesive energies. 相似文献
89.
Tanaka T Ogino H Iwamoto M 《Langmuir : the ACS journal of surfaces and colloids》2007,23(23):11417-11420
Azobenzene (Az) groups were planted on the pore wall of mesoporous silica MCM-41 (M41) by silylation of triethoxy[4-phenylazo(phenyl)]silane. The optimal surface density of Az groups was 0.9 group nm-2, and too much loading of Az induced the lowering of the efficiency of the trans-cis isomerization due to the congestion of the groups. The reversible change in the pore diameters upon UV-vis irradiation could not be confirmed by N2 adsorption at 77 K but was revealed to be ca. 1.0 nm by the shift of the UV-vis absorption band of p-N,N-dimethylaminobenzylidenemalononitrile introduced into the Az-modified pores. 相似文献
90.
Sung Ick Park Hiromi Sakai Shinji Takeoka Hiroyuki Nishide Eishun Tsuchida 《先进技术聚合物》1997,8(6):366-370
A polymer composite film of hemoglobin (Hb–polymer film) was prepared by the casting of an Hb–polymer mixed solution (weight ratio of Hb to polymer is 1 to 1). The percentages of O2 and CO saturation of the Hb–dextran film were 46% and 70%, respectively. In the Hb solution, 100% saturation was observed for both ligands, and a humidified Hb–dextran film also showed 100% saturation. Water molecules would provide flexibility to the matrix polymer and promote a structural change in the Hb from a tense state (T) to a relaxed state (R). Thus the ligand binding to the Hb in the polymer films was strongly affected by the degree of interaction of Hb with the matrix polymers and the physical properties of the polymers. Inositol hexaphosphate (IHP) worked as an allosteric effector even in the solid polymer film and lowered the oxygen affinity of Hb. The O2 transport through an Hb–polyethyleneimine (PEI) film with IHP showed the facilitated O2 transport in comparison with the film without IHP because of the high dissociation rate of O2 from Hb with IHP. © 1997 John Wiley & Sons, Ltd. 相似文献