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51.
Fluctuating Carbonaceous Networks with a Persistent Molecular Shape: A Saddle‐Shaped Geodesic Framework of 1,3,5‐Trisubstituted Benzene (Phenine) 下载免费PDF全文
Dr. Koki Ikemoto Jennie Lin Ryo Kobayashi Dr. Sota Sato Prof. Dr. Hiroyuki Isobe 《Angewandte Chemie (International ed. in English)》2018,57(28):8555-8559
A saddle‐shaped macromolecule has been synthesized. The molecule was designed as a geodesic saddle with 1,3,5‐trisubstituted benzene (named phenine) as the fundamental unit. The phenines were woven into a polygonal framework that was composed of 168 sp2‐hybridized carbon atoms. The saddle‐shaped structure with unique symmetry showed atypical conformational changes. The biaryl linkages in this molecule had a small energy barrier for rotation, and these structural fluctuations resulted in seven 1H NMR resonances representing 84 aromatic hydrogen atoms. Nevertheless, the overall saddle shape of the molecule was persistent, and the “up” and “down” orientations of phenine moieties circulated to give average 1H resonances. The structural characteristics of this molecule, including the anomalous entropy‐driven dimerization, may deepen our understanding of defect‐rich graphitic sheets. 相似文献
52.
Fujimoto H Pinak M Nemoto T O'Neill P Kume E Saito K Maekawa H 《Journal of computational chemistry》2005,26(8):788-798
Clustered DNA damage sites induced by ionizing radiation have been suggested to have serious consequences to organisms, such as cancer, due to their reduced probability to be repaired by the enzymatic repair machinery of the cell. Although experimental results have revealed that clustered DNA damage sites effectively retard the efficient function of repair enzymes, it remains unclear as to what particular factors influence this retardation. In this study, approaches based on molecular dynamics (MD) simulation have been applied to examine conformational changes and energetic properties of DNA molecules containing clustered damage sites consisting of two lesioned sites, namely 7,8-dihydro-8-oxoguanine (8-oxoG) and apurinic/apyrimidinic (AP) site, located within a few base pairs of each other. After 1 ns of MD simulation, one of the six DNA molecules containing a clustered damage site develops specific characteristic features: sharp bending at the lesioned site and weakening or complete loss of electrostatic interaction energy between 8-oxoG and bases located on the complementary strand. From these results it is suggested that these changes would make it difficult for the repair enzyme to bind to the lesions within the clustered damage site and thereby result in a reduction of its repair capacity. 相似文献
53.
M Mitsukuchi T Ikemoto M Taguchi S Higuchi S Abe H Yasui K Hatayama 《Chemical & pharmaceutical bulletin》1990,38(3):692-697
As part of our search for new topical antiinflammatory agents, a series of corticosteroid 17-(alkylthio)- and methoxyalkanoate derivatives was prepared and tested for vasoconstrictive activities. Several compounds were proved to have activity superior or comparable to that of 9 alpha-fluoro-11 beta,21-dihydroxy-16 beta-methyl-17 alpha-valeryloxy-1,4-pregnadiene-3,20-dione (betamethasone 17-valerate, BV). Among these compounds, 21-chloro-11 beta-hydroxy-17 alpha-(methylthio)acetoxy-4-pregnene-3,20-dione (5Aa) was found to have the most potent activity, being more active than BV. The structure-activity relationships of the series revealed that introduction of a (methylthio)acetate function into the 17-position as well as the 21-position of corticosteroids was effective for enhancing the topical antiinflammatory activity. 相似文献
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55.
Katsuhide Terada Hiroyuki Kurobe Masataka Ito Yasuo Yoshihashi Etsuo Yonemochi Kotarou Fujii Hidehiro Uekusa 《Journal of Thermal Analysis and Calorimetry》2013,113(3):1261-1267
Acyclovir (ACV) has two polymorphs, anhydrate 1 and anhydrate 2, and two hydrates, 2/3 hydrate and dihydrate. The effect of polymorphic transformation of ACV on the temperature and humidity was evaluated by simultaneous XRD-DSC and vapor sorption analysis. Each crystal structure of ACV was analyzed by single crystal analysis and powder X-ray diffraction analysis. On the polymorphic and pseudomorphic transformation, anhydrate 1 did not directly transform to anhydrate 2, but transform through 2/3 hydrate and dihydrate due to relative humidity and temperature. According to the molecular packing for four crystals, there are two packing manners for purine moiety. Anhydrate 1, anhydrate 2, 2/3 hydrate and dihydrate were packed in parallel, anti parallel, mixture of parallel–anti parallel and parallel manners, respectively. Base on the packing manner of ACV, it can be seen why the phase transformation occurs with readily or with difficulty. The thermodynamic relation of anhydrate form 1 and form 2 was evaluated by DSC and microcalorimetry. It was found that these two forms are monotropic forms, with anhydrate form I is stable form and it transform to a new form 3 at 443.2 K. 相似文献
56.
Eric A. Voight Matthew S. Bodenstein Norihiro Ikemoto Michael H. Kress 《Tetrahedron letters》2006,47(11):1717-1720
Conditions have been developed for the selective reduction of N-Boc-protected amino acid-derived secondary amides, avoiding the formation of overreduction and cyclic urea byproducts. The method is showcased by the efficient formal synthesis of NK-1 antagonist LY303870. 相似文献
57.
58.
Tetsu Tsubogo Yuichiro Kano Koki Ikemoto Yasuhiro Yamashita Shū Kobayashi 《Tetrahedron: Asymmetry》2010,21(9-10):1221-1225
The first catalytic asymmetric 1,4-addition reactions of azlactones with acrylic esters have been developed. A chiral coordinative calcium catalyst was found to be effective for these reactions, and the desired 1,4-adducts were obtained in good yields and enantioselectivities. The product was converted to the corresponding α-alkylated glutamic acid by acid hydrolysis. 相似文献
59.
Takehisa Hanawa Etsuo Yonemochi Toshio Oguchi Yoshinobu Nakai Keiji Yamamoto 《Journal of inclusion phenomena and macrocyclic chemistry》1993,15(1):91-101
Characterization of an inclusion complex prepared from amorphous ground mixtures of heptakis (2,6-di-O-methyl)--cyclodextrin (DMCD) and benzoic acid was carried out by a sealed heating method. The formation of the crystalline inclusion complex and the variation in physicochemical properties of the ground mixture were investigated as a function of heating temperature. On the basis of X-ray diffractometry and Fourier transform infrared spectroscopy, the crystallization of the ground mixture was confirmed to take place at about 135°C. The crystallization temperature was shifted to lower temperatures and the bound molar ratio of benzoic acid to DMCD increased as the mixing molar ratio of benzoic acid to DMCD was raised.Tsumura & Co., 3586 Yoshiwara, Amimachi, Inashikigun, Ibaraki 300-11, Japan. 相似文献
60.
Tozuka Y Tashiro E Yonemochi E Oguchi T Yamamoto K 《Journal of colloid and interface science》2002,248(2):239-243
Naphthalene adsorption profile on porous materials was studied using solid-state fluorescence spectroscopy. When naphthalene crystals were simply mixed with porous crystalline cellulose (PCC), excimer emission of naphthalene was observed after 1 min of mixing, suggesting a drastic change in the naphthalene molecular environment during the mixing procedure. For the naphthalene-octadesyl silane (ODS)-80A or naphthalene-ODS-2 systems, the changes in adsorption profiles and fluorescence spectral pattern of naphthalene were similar to those of the naphthalene-PCC system. The final amounts of naphthalene adsorbed to ODS-80A and ODS-2 were 0.05 and 0.024 g/g adsorbent, respectively, even though the two materials had comparable values of specific surface area. The relative emission intensity (I(excimer)/I(monomer)) in the ODS-80A system was higher than that in the ODS-2 system when compared at the same amount of naphthalene adsorbed. It was concluded that the pore size of porous materials affected the naphthalene excimer formation on the surface. 相似文献