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101.
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
102.
Naofumi Nishida Yuki Hori Akane Yamauchi Hazuki Fujiwara Makoto Sakurai Yuya Fujiwara Shin-ichi Honda Shunjiro Fujii Hiroyuki A. Sakaue Daiji Kato Tomohiro Yamaguchi Koji Ishibashi Toshifumi Terui Kuei-Yi Lee 《X射线光谱测定》2020,49(1):99-103
Interaction of highly charged ions (HCIs) with surfaces produce various specific phenomena as a consequence of the potential energy that HCI possesses. In the present study, we have observed photon emission, structural, magnetic, and electronic modification on various carbon-based materials such as carbon nanotube by the impact of HCIs using an electron beam ion source named Kobe EBIS installed at the Kobe University. In order to study the potential effect, HCIs of Arq+ (q = 6–16) with the intensity of 0.1–1 nA are projected on the surface with a constant kinetic energy (16 keV). For photon emission measurements, we observed spatial and spectral distribution of visible light emission from the surface during irradiation with HCIs. On the other hand, the structural modification of multi-walled carbon nanotubes (MWCNTs) irradiated with HCIs has been analyzed using a transmission electron microscopy and Raman spectroscopy. Irradiation effects on the resistivity of single MWCNT supported on micrometer scale bridge pattern were also measured. We have also measured magnetic structure of highly oriented pyrolytic graphite irradiated with HCIs using electron spin resonance at low temperature. At the present paper, we will review our recent experimental results on the interaction of HCI with various carbon-based materials. 相似文献
103.
Nobuyuki Otozawa Rio Hamajima Masataka Yoshioka Raito Kato Arisa Tanaka Hiroto Fukuma Toshiki Terao Kei Manabe Syuji Fujii Yoshinobu Nakamura Atsushi Takahara Tomoyasu Hirai 《Journal of polymer science. Part A, Polymer chemistry》2020,58(14):1960-1964
This study investigates the effect of ionic liquids (ILs) on the anionic polymerization of methyl methacrylate (MMA). Polymethyl methacrylate (PMMA), an isotactic polymer, is prepared by anionic polymerization at a high reaction temperature with an IL that acts as both solvent and additive. The most plausible reaction mechanism is determined using 1H NMR and Fourier-transform infrared spectroscopy. The electrostatic interaction between MMA and the IL increases the apparent steric hindrance in MMA, resulting in the isotactic PMMA. 相似文献
104.
Dr. Yohei Hattori Tatsuya Maejima Yumi Sawae Jun-ichiro Kitai Prof. Masakazu Morimoto Dr. Ryojun Toyoda Prof. Hiroshi Nishihara Prof. Satoshi Yokojima Dr. Shinichiro Nakamura Prof. Kingo Uchida 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(50):11441-11450
The cyclization reaction of diarylethenes having an azulene ring occurs only via higher excited states. Novel diarylethenes having an azulene ring with a strong donor or acceptor were synthesized and examined in these reactions. A derivative having an electron-donating 1,3-benzodithiol-2-ylidenemethyl group at the 1-position of the azulene ring showed photochromism, whereas neither a derivative having a π-conjugated electron-donating group at the 3-position of the azulene ring nor derivatives having a π-conjugated electron-withdrawing group at the 1- or 3-position of the azulene ring showed any photochromism. The photoreactivities of these compounds were explained by calculating forces and bond orders on the excited states using density functional theory (DFT) and time-dependent (TD)-DFT. 相似文献
105.
Prof. Isao Fujii Dr. Makoto Hashimoto Kaori Konishi Akiko Unezawa Haruka Sakuraba Kenta Suzuki Harue Tsushima Miho Iwasaki Satsuki Yoshida Akane Kudo Rina Fujita Aika Hichiwa Koharu Saito Dr. Takashi Asano Dr. Jun Ishikawa Dr. Daigo Wakana Dr. Yukihiro Goda Ayumi Watanabe Mamoru Watanabe Yui Masumoto Dr. Junichiro Kanazawa Dr. Hajime Sato Prof. Masanobu Uchiyama 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(22):8542-8548
Shimalactones A and B are neuritogenic polyketides possessing characteristic oxabicyclo[2.2.1]heptane and bicyclo[4.2.0]octadiene ring systems that are produced by the marine fungus Emericella variecolor GF10. We identified a candidate biosynthetic gene cluster and conducted heterologous expression analysis. Expression of ShmA polyketide synthase in Aspergillus oryzae resulted in the production of preshimalactone. Aspergillus oryzae and Saccharomyces cerevisiae transformants expressing ShmA and ShmB produced shimalactones A and B, thus suggesting that the double bicyclo-ring formation reactions proceed non-enzymatically from preshimalactone epoxide. DFT calculations strongly support the idea that oxabicyclo-ring formation and 8π-6π electrocyclization proceed spontaneously after opening of the preshimalactone epoxide ring through protonation. We confirmed the formation of preshimalactone epoxide in vitro, followed by its non-enzymatic conversion to shimalactones in the dark. 相似文献
106.
Ryota Tsutsumi Tokio Sasaki Chisato Hashiguchi Ryota Yamazaki Syuji Fujii 《Composite Interfaces》2018,25(8):743-760
In order to reinforce the composite consisting of isoprene rubber (IR) and calcium carbonate (CaCO3) particles, the surface treatment of CaCO3 particles with a mixture of amino- and mercapto-functional silane coupling agents was investigated. The quantity of chemisorbed silanes in treated CaCO3 measured using thermogravimetry was greater for amino- than for mercapto-silane and for the tri- than for the dialkoxy structure. Second, the molecular mobility of polycondensate of the mixtures with the trialkoxy structure measured using 1H pulse nuclear magnetic resonance had the least molecular mobility, i.e., formed the highest density network. The greater values of stress at 500% strain, fracture stress, and elongation at break were determined for the treatment with amino- and mercapto-functional silanes having a trialkoxy structure from the stress-strain curves of composite. The mixture treatment with dialkoxy structure and with amino- or mercapto-functional silane only did not improve the mechanical properties sufficiently. Interactions between the amino group and the CaCO3 surface, covalent bonding between the mercapto group and the IR, and high density network formation of trialkoxy silane were important for improving the mechanical properties of the composite. 相似文献
107.
K. Ikematsu K. Fujii Z. Hioki Y. Sumino T. Takahashi 《The European Physical Journal C - Particles and Fields》2003,29(1):1-10
We developed a new method for the full kinematical reconstruction of the system near its threshold at future linear e
+
e
-
colliders. In the core of the method lies likelihood fitting which is designed to improve measurement accuracies of the kinematical
variables that specify the final states resulting from decays. The improvement is demonstrated by applying this method to a Monte Carlo sample generated with various experimental effects including beamstrahlung, finite acceptance and resolution of the detector
system, etc. In most cases the fit takes a broad non-Gaussian distribution of a given kinematical variable to a nearly Gaussian
shape, thereby justifying phenomenological analyses based on simple Gaussian smearing of the parton-level momenta. The standard
deviations of the resultant distributions of various kinematical variables are given in order to facilitate such phenomenological
analyses. A possible application of the kinematical fitting method and its expected impact are also discussed.
Received: 4 March 2003 / Published online: 23 May 2003
RID="a"
ID="a" e-mail: ikematsu@post.kek.jp
RID="b"
ID="b" e-mail: fujiik@jlcuxf.kek.jp
RID="c"
ID="c" e-mail: hioki@ias.tokushima-u.ac.jp
RID="d"
ID="d" e-mail: sumino@tuhep.phys.tohoku.ac.jp
RID="e"
ID="e" e-mail: tohrut@hiroshima-u.ac.jp 相似文献
108.
109.
Mikiyasu Shirai Matthew Beard James T. Pearson Takashi Sonobe Hirotsugu Tsuchimochi Yutaka Fujii Emily Gray Keiji Umetani Daryl O. Schwenke 《Journal of synchrotron radiation》2013,20(3):441-448
Synchrotron radiation microangiography is a powerful tool for assessing adverse changes in pulmonary vessel density associated with primary pulmonary hypertension (PH). Congestive heart failure (CHF) leads to a `secondary' onset of PH, yet it is unknown whether secondary PH is also associated with reduced vessel density. This study utilized synchrotron radiation to assess both pulmonary vessel density and endothelial function in a Dahl rat model of CHF with secondary PH. High salt‐fed Dahl salt‐sensitive (Dahl‐S) and salt‐resistant (Dahl‐R) rats were anesthetized and microangiography was performed to assess the pulmonary vessel density and vascular responses to (i) sodium nitroprusside (5.0 µg kg?1 min?1), (ii) acetylcholine (3.0 µg kg?1 min?1) and (iii) ET‐1A receptor blockade, BQ‐123 (1 mg kg?1). Dahl‐S rats developed CHF and secondary PH as evident by endothelial dysfunction, impaired vasodilatory responses to acetylcholine, enhanced vasodilatory responses to BQ‐123 and extensive pulmonary vascular remodeling. Consequently, the pulmonary vessel density was adversely reduced. Interestingly, the etiology of secondary PH manifests with structural and functional changes that are comparable with that previously reported for primary PH. One important discrepancy, however, is that ET‐1 modulation of pulmonary vessels is most striking in vessels with a diameter range of 100–200 µm in secondary PH, in contrast to a range of 200–300 µm in primary PH. Such discrepancies should be considered in future studies investigating primary and secondary forms of PH. 相似文献
110.
Akiko Takeda Katsuki Fujisawa Yusuke Fukaya Masakazu Kojima 《Journal of Global Optimization》2002,24(2):237-260
As computing resources continue to improve, global solutions for larger size quadrically constrained optimization problems become more achievable. In this paper, we focus on larger size problems and get accurate bounds for optimal values of such problems with the successive use of SDP relaxations on a parallel computing system called Ninf (Network-based Information Library for high performance computing). 相似文献