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31.
Matano Y Miyajima T Ochi N Nakabuchi T Shiro M Nakao Y Sakaki S Imahori H 《Journal of the American Chemical Society》2008,130(3):990-1002
The syntheses, structures, and coordination chemistry of phosphole-containing hybrid calixphyrins (P,N2,X-hybrid calixphyrins) and the catalytic activities of their transition-metal complexes are reported. The 5,10-porphodimethene type 14pi-P,(NH)2,X- and 16pi-P,N2,X-hybrid calixphyrins (X = O, S, NH) are prepared via acid-promoted dehydrative condensation between a sigma4-phosphatripyrrane and the corresponding 2,5-bis[hydroxy(phenyl)methyl]heteroles followed by DDQ oxidation. Both spectroscopic and crystallographic data of the hybrid calixphyrins have revealed that the conformation and size of the macrocyclic platforms as well as the oxidation state of the -conjugated pyrrole-heterole-pyrrole (N-X-N) units vary considerably depending on the combination of heteroles. The sigma3-P,(NH)2,S- and sigma3-P,N2,S-hybrids react with Pd(OAc)2 and Pd(dba)2, respectively, to afford the same Pd(II)-P,N2,S-hybrid complex, in which the calixphyrin platform is regarded as a dianionic ligand. In the complexation with [RhCl(CO)2]2 in dichloromethane, the sigma3-P,N2,S-hybrid behaves as a neutral ligand to afford an ionic Rh(I)-P,N2,S-hybrid complex, whereas the sigma3-P,N2,NH-hybrid behaves as an anionic ligand to produce Rh(III)-P,N3-hybrid complexes. In the latter reaction, it is likely that a neutral Rh(I)-P,N3-hybrid complex, generated as a highly nucleophilic intermediate, undergoes C-Cl bond activation of the solvent. The complexation of AuCl(SMe2) with the sigma3-P,N2,X-hybrids (X = S, NH) leads to the formation of the corresponding Au(I)-monophosphine complexes. The spectral data and crystal structures of these metal complexes exhibit the hemilabile nature of the phosphole-containing hybrid calixphyrin platforms derived from the flexible phosphole unit and the redox active N-X-N units. The hybrid calixphyrin-palladium and -rhodium complexes catalyze the Heck reaction and hydrosilylations, respectively, implying that the metal center in the core is capable of activating the substrates under appropriate reaction conditions. The present results demonstrate the potential utility of the phosphole-containing hybrid calixphyrins as a new class of macrocyclic P,N2,X-mixed donor ligands for designing highly reactive transition-metal complexes. 相似文献
32.
H. Okuno N. Fukunishi H. Hasebe H. Imao O. Kamigaito M. Kase H. Kuboki 《Journal of Radioanalytical and Nuclear Chemistry》2014,299(2):945-949
The accelerator complex at the RIKEN Radioisotope Beam Factory accelerates heavy ions ranging from oxygen to uranium using triple stripping system to provide the beams at required charge. In many cases, the charge strippers cause problems during high-intensity beams accelerator operation. The charge stripper problem has been most significant during uranium beam acceleration because the lifetimes of the conventional carbon foils are extremely short. We conducted extensive R&D on the first stripper and found a solution using a low-Z gas stripper. We also plan to modify a second stripper operating recently with short-lifetime carbon foils. The stripper with better parameters will be needed when the beam intensity is increased by a new injector system for acceleration of uranium beam with higher charge. 相似文献
33.
Mutsumi Tashiro Pradeep K. Pujari Shu Seki Yoshihide Honda Shigehiro Nishijima Seiichi Tagawa 《Radiation Physics and Chemistry》2000,58(5-6):587-592
Temperature dependence of positron annihilation lifetime spectra of polysilanes such as, poly(methyl-n-propylsilane) (PMPrS) and poly(di-n-hexylsilane) (PDHS) has been investigated. The τ3 in PMPrS is seen to increase monotonically around the solid–liquid transition temperature. The transition temperature and free volume are observed to depend on the molecular weight and/or packing of the backbones. For PDHS, a sharp change in τ3 and I3 is seen at the solid–solid transition temperature. Free volume radius probability density functions, above and below the transition temperature, are presented in PMPrS and PDHS. Positron studies are complimented by conventional thermal analysis studies. 相似文献
34.
Vossen A Seidl R Adachi I Aihara H Aushev T Balagura V Bartel W Bischofberger M Bondar A Bračko M Browder TE Chang MC Chen A Chen P Cheon BG Cho K Choi Y Eidelman S Feindt M Gaur V Gabyshev N Garmash A Golob B Perdekamp MG Haba J Hayasaka K Horii Y Hoshi Y Hou WS Hyun HJ Inami K Ishikawa A Iwabuchi M Iwasaki Y Iwashita T Joshi NJ Kichimi H Kim HO Kim MJ Ko BR Kumita T Lange JS Lee MJ Lee SH Leitgab M Li Y Liu C Liventsev D Louvot R McOnie S Miyata H Miyazaki Y Mizuk R Mohanty GB Nakano E 《Physical review letters》2011,107(7):072004
The interference fragmentation function translates the fragmentation of a quark with a transverse projection of the spin into an azimuthal asymmetry of two final-state hadrons. In e(+)e(-) annihilation the product of two interference fragmentation functions is measured. We report nonzero asymmetries for pairs of charge-ordered π(+)π(-) pairs, which indicate a significant interference fragmentation function in this channel. The results are obtained from a 672 fb(-1) data sample that contains 711 × 10(6) π(+)π(-) pairs and was collected at and near the Υ(4S) resonance, with the Belle detector at the KEKB asymmetric-energy e(+)e(-) collider. 相似文献
35.
Numerical Algorithms - The LP-Newton method solves linear programming (LP) problems by repeatedly projecting a current point onto a certain relevant polytope. In this paper, we extend the... 相似文献
36.
Yasumitsu Matsuo Yoshihide Tokoyoda Junko Hatori Masaru Komukae Seiichiro Ikehata 《Acta Crystallographica. Section C, Structural Chemistry》2005,61(4):i39-i40
The structure of thallium selenate, Tl2SeO4, in a paraelastic phase (above 661 K) has been analysed by Rietveld analysis of the X‐ray powder diffraction pattern. Atomic parameters based on the isomorphic K2SO4 crystal in the paraelastic phase were used as the starting model. The structure was determined in the hexagonal space group P63/mmc, with a = 6.2916 (2) Å and c = 8.1964 (2) Å. From the Rietveld refinement it was found that two orientations are possible for the SeO4 tetrahedra, in which one of their apices points randomly up and down with respect to [001]. One Tl atom lies at the origin with symmetry, the other Tl and one of the O atoms occupy sites with 3m symmetry, the Se atom is at a site with symmetry and the remaining O atom is at a site with m symmetry. Furthermore, it was also found that the Tl atoms display anomalously large positional disorder along [001] in the paraelastic phase. 相似文献
37.
We performed the first investigations of coherent acoustic phonons in Au-Ag core-shell nanorods, which were compared with the results of parental Au nanorods. Both breathing and extensional modes were observed in Au-Ag core-shell nanorods with ~11 nm Ag shell while only extensional modes were detected in other core-shell nanorods with 4-7 nm Ag shell. Young's modulus estimated from the oscillation period of extensional modes was found to be larger for Au-Ag core-shell nanorods with ~4 nm Ag shell, as compared with that of Au nanorods. The value of Young's modulus decreases with the increase of the Ag shell thickness and finally becomes smaller than that of Au nanorods. This phenomenon is interpreted in terms of the surface effects and the existence of grain boundaries in the lattice structure of Ag shell. 相似文献
38.
Jun-ichi Matsuo Ryosuke Okuno Kosuke Takeuchi Mizuki Kawano Hiroyuki Ishibashi 《Tetrahedron letters》2010,51(29):3736-3737
Optimized reaction conditions for the preparation of various 2-monosubstituted 3-ethoxycyclobutanones are described. 2-Monoalkyl 3-ethoxycyclobutanones were efficiently prepared by the reaction of the corresponding carboxylic acid chlorides and an excess amount of ethyl vinyl ether in the presence of diisopropylethylamine at 90 °C in a sealed tube. 2-Monoaryl 3-ethoxycyclobutanones were prepared by using 2,6-lutidine as a base in the above-mentioned procedure. 相似文献
39.
A sealed tube dry combustion method that is simple, accurate, and precise for ultramicro determination of halogens in organic compounds has been developed. Samples below 1 mg are heated at 580 °C for 1 h in an electric furnace. After the combustion and absorption of the gaseous halogen, the interior of the tube is rinsed. Subsequent titration is carried out potentiometrically with silver nitrate and yielded standard deviations of 0.21% for chlorine, 0.17% for bromine, and 0.25% for iodine. 相似文献
40.
Okuno Y. Ohtsu Y. Fujita H. 《IEEE transactions on plasma science. IEEE Nuclear and Plasma Sciences Society》1994,22(3):253-259
Effects of a magnetic held collimation on ion behavior in the downstream region of an electron cyclotron resonance (ECR) plasma device are clarified experimentally using a directional ion energy analyzer. The drift energy and its spread of the ion beam observed in the downstream region decrease and the beam temperature increases with the collimating magnetic flux density. Then, the ion temperature measured perpendicular to the axis of the plasma stream slightly decreases. The ion beam is found to be almost parallel to the magnetic field lines, that is, the beam tends to be collimated 相似文献