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31.
Dr. Yusaku Nomura Dr. Frédéric Thuaud Dr. Daisuke Sekine Prof. Dr. Akihiro Ito Satoko Maeda Dr. Hiroyuki Koshino Dr. Daisuke Hashizume Dr. Atsuya Muranaka Dr. Thomas Cruchter Prof. Dr. Masanobu Uchiyama Prof. Dr. Satoshi Ichikawa Prof. Dr. Akira Matsuda Prof. Dr. Minoru Yoshida Prof. Dr. Go Hirai Prof. Dr. Mikiko Sodeoka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(35):8387-8392
A synthetic methodology to access all possible stereoisomers of spectomycin A1 (SMA1) and A2 (SMA2) has been established through late-stage diversification. The key reaction for the construction of all four diastereomers is an intramolecular cyclization based on the umpolung of π-allyl palladium species with bis(pinacolato)diborane (B2(pin)2). Silyl group assisted direct benzylic oxidation of each isomer enabled construction of the fragile β-hydroxytetralone skeleton to provide the SMAs. The relative and absolute stereochemistry of SMA2 was also determined, and the absolute stereochemistry of SMA1 was extrapolated based on the optical rotation of SMA2. The axial chirality of SMAs is discussed based on circular dichroism spectra and DFT calculations, and it is concluded that the M isomer is predominant in solution. Biochemical assessment of all isomers in vitro revealed that the C9 hydroxyl group and dimeric structure were both important for protein SUMOylation-inhibitory activity. 相似文献
32.
Tatsuya Kikuchi Masumi Yoshida Shiki Matsuura Shungo Natsui Etsuji Tsuji Hiroki Habazaki Ryosuke O. Suzuki 《Journal of Physics and Chemistry of Solids》2014
Micro-, submicron-, and nano-scale titanium dioxide particles were reduced by reduction with a metallic calcium reductant in calcium chloride molten salt at 1173 K, and the reduction mechanism of the oxides by the calcium reductant was explored. These oxide particles, metallic calcium as a reducing agent, and calcium chloride as a molten salt were placed in a titanium crucible and heated under an argon atmosphere. Titanium dioxide was reduced to metallic titanium through a calcium titanate and lower titanium oxide, and the materials were sintered together to form a micro-porous titanium structure in molten salt at high temperature. The reduction rate of titanium dioxide was observed to increase with decreasing particle size; accordingly, the residual oxygen content in the reduced titanium decreases. The obtained micro-porous titanium appeared dark gray in color because of its low surface reflection. Micro-porous metallic titanium with a low oxygen content (0.42 wt%) and a large surface area (1.794 m2 g−1) can be successfully obtained by reduction under optimal conditions. 相似文献
33.
Masataka Hakamada Motohiro Yuasa Takashi Yoshida Fumi Hirashima Mamoru Mabuchi 《Applied Physics A: Materials Science & Processing》2014,114(4):1061-1066
ZnO deposited on nanoporous Au showed photocatalytic decomposition toward methyl orange under visible light, unlike ZnO sputtered on flat Au without a nanoporous structure. First-principles calculations suggested that the surface lattice disorder in nanoporous Au induced a band gap narrowing and a large built-in electric field in the adjacent ZnO, resulting in the visible-light photocatalytic response. 相似文献
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Yoshiaki Yoshida Takeshi Endo 《Journal of polymer science. Part A, Polymer chemistry》2018,56(19):2255-2262
Polyaddition of various diisothiocyanates and dithiols was achieved with triethylamine in dimethylformamide at 25 °C for 12 h under nitrogen, and then the corresponding polydithiourethanes (PDTUs) were obtained with high yield and molecular weight without depending on the monomer structures, although the dithiol monomer of the low nucleophilicity was unsuitable for polyaddition in this system. The chemical and physical properties of the obtained PDTUs such as solvent solubility, glass transition temperature, thermal stability, transparency, refractive index, and tensile strength, were analyzed in detail by gel permeation chromatography, nuclear magnetic resonance, Fourier transform infrared–attenuated total reflection, ultraviolet–visible, differential scanning calorimetry, thermogravimetric analysis, and tensile testing measurements. These results proved that PDTUs and their cast films having the aliphatic diisothiocyanate and dithiol moieties exhibited excellent chemical and physical properties compared to that of the aromatic PDTUs. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2018 , 56, 2255–2262 相似文献
36.
We introduce a quantum key distribution protocol using mean multi-kings’ problem. Using this protocol, a sender can share a bit sequence as a secret key with receivers. We consider a relation between information gain by an eavesdropper and disturbance contained in legitimate users’ information. In BB84 protocol, such relation is known as the so-called information disturbance theorem. We focus on a setting that the sender and two receivers try to share bit sequences and the eavesdropper tries to extract information by interacting legitimate users’ systems and an ancilla system. We derive trade-off inequalities between distinguishability of quantum states corresponding to the bit sequence for the eavesdropper and error probability of the bit sequence shared with the legitimate users. Our inequalities show that eavesdropper’s extracting information regarding the secret keys inevitably induces disturbing the states and increasing the error probability. 相似文献
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Shuichi Hirata Kouichi Tanaka Katsuya Matsui Fernando Arteaga Arteaga Yasushi Yoshida Shinobu Takizawa Hiroaki Sasai 《Tetrahedron: Asymmetry》2013,24(19):1189-1192
The introduction of a 1,3-propanediamine unit at the 3-position of (S)-BINOL using a methylene spacer led to the formation of a chiral bifunctional organocatalyst for the aza-Morita–Baylis–Hillman (aza-MBH) reaction. The organocatalyst 1k mediated aza-MBH transformations with high chemical yields and with up to 82% ee. 相似文献
40.
The reactions of carbon dioxide, primary or secondary aliphatic amines and oxetanes at a CO2 pressure of 40 atm at 100–120°C without any catalysts afforded new monocarbamates of 1,3-propanediols, with concomitant formation of amino alcohols from oxetanes and amines. 相似文献