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1.
Dr. Nozomi Mihara Dr. Yasuyuki Yamada Dr. Hikaru Takaya Prof. Yasutaka Kitagawa Dr. Kazunobu Igawa Prof. Katsuhiko Tomooka Prof. Hiroshi Fujii Prof. Kentaro Tanaka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(13):3369-3375
Development of supramolecular methods to further activate a highly reactive intermediate is a fascinating strategy to create novel potent catalysts for activation of inert chemicals. Herein, a supramolecular approach to enhance the oxidizing ability of a high-valent oxo species of a nitrido-bridged iron porphyrinoid dimer that is a known potent molecular catalyst for light alkane oxidation is reported. For this purpose, a nitrido-bridged dinuclear iron complex of porphyrin-phthalocyanine heterodimer 3 5+, which is connected through a fourfold rotaxane, was prepared. Heterodimer 3 5+ catalyzed ethane oxidation in the presence of H2O2 at a relatively low temperature. The site-selective complexation of 3 5+ with an additional anionic porphyrin (TPPS4−) through π–π stacking and electrostatic interactions afforded a stable 1:1 complex. It was demonstrated that the supramolecular post-synthetic modification of 3 5+ enhances its catalytic activity efficiently. Moreover, supramolecular conjugates achieved higher catalytic ethane oxidation activity than nitrido-bridged iron phthalocyanine dimer, which is the most potent iron-oxo-based molecular catalyst for light-alkane oxidation reported so far. Electrochemical measurements proved that the electronic perturbation from TPPS4− to 3 5+ enhanced the catalytic activity. 相似文献
2.
3.
Takayuki Yaegashi Shinya Yodoya Masahiko Nakamura Hiroki Takeshita Katsuhiko Takenaka Tomoo Shiomi 《Journal of polymer science. Part A, Polymer chemistry》2004,42(4):999-1007
Free‐radical homo‐ and copolymerization behavior of N,N‐diethyl‐2‐methylene‐3‐butenamide (DEA) was investigated. When the monomer was heated in bulk at 60 °C for 25 h without initiator, rubbery, solid gel was formed by the thermal polymerization. No such reaction was observed when the polymerization was carried out in 2 mol/L of benzene solution with with 1 mol % of azobisisobutyronitrile (AIBN) as an initiator. The polymerization rate (Rp) equation was Rp ∝ [DEA]1.1[AIBN]0.51, and the overall activation energy of polymerization was calculated 84.1 kJ/mol. The microstructure of the resulting polymer was exclusively a 1,4‐structure where both 1,4‐E and 1,4‐Z structures were included. From the product analysis of the telomerization with tert‐butylmercaptan as a telogen, the modes of monomer addition were estimated to be both 1,4‐ and 4,1‐addition. The copolymerizations of this monomer with styrene and/or chloroprene as comonomers were also carried out in benzene solution at 60 °C. In the copolymerization with styrene, the monomer reactivity ratios obtained were r1 = 5.83 and r2 = 0.05, and the Q and e values were Q = 8.4 and e = 0.33, respectively. © 2004 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 42: 999–1007, 2004 相似文献
4.
T. Kinoshita K. Fukuda Y. Takahashi T. Yabuzaki 《Zeitschrift für Physik B Condensed Matter》1995,98(3):387-390
We report on the optical properties of alkali atoms (Cs and Rb) in the pressurized superfluid helium. We observed excitation and emission spectra at various pressures from the saturated vapor pressure to about 25 atm. The theoretical calculations on the basis of the atomic bubble model have also been worked out. The qualitative agreement between the theoretical and experimental results with respect to the peak shift, the linewidth, and their pressure dependence is achieved in the framework of the spherical atomic bubble model. TheD
2 excitation spectra with the double peaks are interpreted qualitatively in terms of the Jahn-Teller effect, indicating the existence of the nontotally symmetrical density distribution of the surrounding helium atoms. 相似文献
5.
Yukio Iida Masahiro Shibutani Katsuhiko Kobayashi Kazuhiko Ohnuma Yoichi Miyake Toru Noda 《Optical Review》2006,13(2):87-92
The double-pass method is thought to obtain the point spread function (PSF) in human eyes based on two techniques: the symmetric
double-pass method using the same pupil size and the asymmetric double-pass method using a different pupil size. The symmetric
double-pass method provides autocorrelation of the retinal PSF and, thus, the modulation transfer function. The asymmetric
double-pass method provides low-frequency partial-phase information and the partial phase-retrieval algorithm is applied to
obtain the complete-phase information, and to estimate the PSF. The partial phase-retrieval algorithm is based on the iteration
method proposed by Fineup and Kowalczyk and requires a lengthy computation. In this study, we propose a new high-speed phase-retrieval
algorithm based on the property that the real and imaginary parts of optical transfer functions (OTFs) continuously change
in value. 相似文献
6.
Precise measurement of magnetic moment of short-lived β-emitting nuclei12B ( I π=1+, T 1/2=20.18 ms)
Zhou Dongmei Zheng Yongnan Du Enpeng Xu Yongjun Zhu Jiazheng Yuan Daqing Wang Zhiqiang Luo Hailong Zuo Yi Ma Ruigang Duan Xiao M. Mihara M. Fukuda K. Matsuta T. Minamisono Zhu Shengyun 《中国科学G辑(英文版)》2004,47(5):531-539
The spin polarized β-emitting nuclei12B (I
π=1+,T
1/2=20.18 ms) were produced by the nuclear reaction11B(d, p)12B and by the selection technique of the incident deuteron energy and the12B recoil angle following the nuclear reaction. The nuclear magnetic moment of the short-lived nuclei12B was measured by β-NMR with the β-NMR and β-NQR setup established for the first time in China. The nuclear magnetic moment
of12B was determined to be μ=0.99993±0.00048 nm org=0.99993±0.00048 after the precise correction of the Knight shift. 相似文献
7.
Teruhisa Horita Katsuhiko Yamaji Natsuko Sakai Yueping Xiong Harumi Yokokawa Tatsuya Kawada 《Ionics》2002,8(1-2):108-117
The oxygen reduction active sites were visualized around the O2/SOFC cathode/electrolyte triple phase boundaries (TPB) by the16O/18O exchange techniques and secondary ion mass spectrometry (SIMS) analysis. The higher18O concentration is observed on the cathode top surfaces (La0.9Sr0.1MnO3-mesh, Au-mesh, and Ag-porous), which suggested the promotion of oxygen adsorption and oxygen surface exchange at the cathode.
The oxygen diffusion through the bulk of cathode occurred at the La0.9Sr0.1MnO3-mesh and the Ag-porous cathodes, not at the Au-mesh cathode. On the YSZ surfaces after removing the cathode, the active sites
for oxygen incorporation were analyzed by SIMS. The active sites for oxygen incorporation were at the La0.9Sr0.1MnO3/YSZ interface as well as the TPB. On the other hand, the active sites for oxygen incorporation are limited to the TPB in
the case of the Au-mesh removed YSZ surface. From the SIMS analysis, the expansion of the active sites for oxygen incorporation
is less than a few μm from the TPB lines.
Paper presented at the 8th EuroConference on Ionics, Carvoeiro, Algarve, Portugal, Sept. 16–22, 2001. 相似文献
8.
Yozo Miura Hiroyuki Dote Hiroyuki Kubonishi Kenichi Fukuda Tomoko Saka 《Journal of polymer science. Part A, Polymer chemistry》2007,45(6):1159-1169
A dendritic macroinitiator having 16 TEMPO‐based alkoxyamines, Star‐16 , was prepared by the reaction of a dendritic macroinitiator having eight TEMPO‐based alkoxyamines, [G‐3]‐OH , with 4,4′‐bis(chlorocarbonyl)biphenyl. The nitroxide‐mediated radical polymerization (NMRP) of styrene (St) from Star‐16 gave 16‐arm star polymers with PDI of 1.19–1.47, and NMPR of 4‐vinylpyridine from the 16‐arm star polymer gave 16‐arm star diblock copolymers with PDI of 1.30–1.43. The ring‐opening polymerization of ε‐caprolactone from [G‐3]‐OH and the subsequent NMRP of St gave AB8 9‐miktoarm star copolymers with PDI of 1.30–1.38. The benzyl ether linkages of the 16‐arm star polymers and the AB8 9‐miktoarm star copolymers were cleaved by treating with Me3SiI, and the resultant poly(St) arms were investigated by size exclusion chromatography (SEC). The SEC results showed PDIs of 1.23–1.28 and 1.18–1.22 for the star polymers and miktoarm stars copolymers, respectively, showing that they have well‐controlled poly(St) arms. © 2006 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 45: 1159–1169, 2007. 相似文献
9.
Y. Fukuda T. Kobayashi H. Yoshida T. Sekizawa N. Sanada 《Applied Surface Science》2002,190(1-4):279-283
Adsorption and decomposition of triethylindium (TEI: (C2H5)3In) on a GaP(0 0 1)-(2×1) surface have been studied by low-energy electron diffraction (LEED), Auger electron spectroscopy (AES), temperature-programmed desorption (TPD) and high-resolution electron energy loss spectroscopy (HREELS). It is found from the TPD result that ethyl radical and ethylene are evolved at about 300–400 and 450–550 K, respectively, as decomposition products of TEI on the surface. This result is quite different from that on the GaP(0 0 1)-(2×4) surface. The activation energy of desorption of ethyl radical is estimated to be about 93 kJ/mol. It is suggested that TEI is adsorbed molecularly on the surface at 100 K and that some of TEI molecules are dissociated into C2H5 to form P–C2H5 bonds at 300 K. The vibration modes related to ethyl group are decreased in intensity at about 300–400 and 450–550 K, which is consistent with the TPD result. The TEI molecules (including mono- and di-ethylindium) are not evolved from the surface. Based on the TPD and HREELS results, the decomposition mechanism of TEI on the GaP(0 0 1)-(2×1) surface is discussed and compared with that on the (2×4) surface. 相似文献
10.