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排序方式: 共有1363条查询结果,搜索用时 250 毫秒
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Dr. Hiromi Oshita Takashi Suzuki Kyohei Kawashima Prof. Dr. Hitoshi Abe Prof. Dr. Fumito Tani Prof. Dr. Seiji Mori Prof. Dr. Tatsuo Yajima Prof. Dr. Yuichi Shimazaki 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(32):7649-7658
In order to gain new insights into the effect of the π–π stacking interaction of the indole ring with the CuII–phenoxyl radical as seen in the active form of galactose oxidase, we have prepared a CuII complex of a methoxy-substituted salen-type ligand, containing a pendent indole ring on the dinitrogen chelate backbone, and characterized its one-electron-oxidized forms. The X-ray crystal structures of the oxidized CuII complex exhibited the π–π stacking interaction of the indole ring mainly with one of the two phenolate moieties. The phenolate moiety in close contact with the indole moiety showed the characteristic phenoxyl radical structural features, indicating that the indole ring favors the π–π stacking interaction with the phenoxyl radical. The UV/Vis/NIR spectra of the oxidized CuII complex with the pendent indole ring was significantly different from those of the complex without the side-chain indole ring, and the absorption and CD spectra exhibited a solvent dependence, which is in line with the phenoxyl radical–indole stacking interaction in solution. The other physicochemical results and theoretical calculations strongly support that the indole ring, as an electron donor, stabilizes the phenoxyl radical by the π–π stacking interaction. 相似文献
3.
Yoshino Katsurayama Prof. Yasuhiro Ikabata Prof. Hajime Maeda Prof. Masahito Segi Prof. Hiromi Nakai Prof. Taniyuki Furuyama 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(2):e202103223
The high penetration of near-infrared (NIR) light makes it effective for use in selective reactions under light-shielded conditions, such as in sealed reactors and deep tissues. Herein, we report the development of phthalocyanine catalysts directly activated by NIR light to transform small organic molecules. The desired photocatalytic properties were achieved in the phthalocyanines by introducing the appropriate peripheral substituents and central metal. These phthalocyanine photocatalysts promote cross-dehydrogenative-coupling (CDC) under irradiation with 810 nm NIR light. The choice of solvent is important, and a mixture of a reaction-accelerating (pyridine) and -decelerating (methanol) solvents was particularly effective. Moreover, we demonstrate photoreactions under visible-light-shielded conditions through the transmission of NIR light. A combined experimental and computational mechanistic analysis revealed that this NIR reaction does not involve a photoredox-type mechanism with electron transfer, but instead a singlet-oxygen-mediated mechanism with energy transfer. 相似文献
4.
Yu Dong Tariq Mosaval Hazim J. Haroosh Rehan Umer Hitoshi Takagi Kin‐Tak Lau 《Journal of Polymer Science.Polymer Physics》2014,52(9):618-623
This pilot study elaborates the development of novel epoxy/electrospun polylactic acid (PLA) nanofiber composites at the fiber contents of 3, 5, and 10 wt % to evaluate their mechanical and thermal properties using flexural tests and differential scanning calorimetry (DSC). The flexural moduli of composites increase remarkably by 50.8 and 24.0% for 5 and 10 wt % fiber contents, respectively, relative to that of neat epoxy. Furthermore, a similar trend is also shown for corresponding flexural strengths being enhanced by 31.6 and 4.8%. Fractured surface morphology with scanning electron microscopy (SEM) confirms a full permeation of cured epoxy matrix into nanofiber structures and existence of nondestructive fibrous networks inside large void cavities. The glass transition temperature (Tg) of composites increases up to 54–60 °C due to embedded electrospun nanofibers compared to 50 °C for that of epoxy, indicating that fibrous networks may further restrict the intermolecular mobility of matrix in thermal effects. © 2014 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2014 , 52, 618–623 相似文献
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The extrapolation scheme of correlation energy is revisited to evaluate the complete basis set limit from double‐zeta (DZ) and triple‐zeta levels of calculations. The DZ level results are adjusted to the standard asymptotic behavior with respect to the cardinal number, observed at the higher levels of basis sets. Two types of adjusting schemes with effective scaling factors, which recover errors in extrapolations with the DZ level basis set, are examined. The first scheme scales the cardinal number for the DZ level energy, while the second scheme scales the prefactor of the extrapolation function. Systematic assessments on the Gaussian‐3X and Gaussian‐2 test sets reveal that these calibration schemes successfully and drastically reduce errors without additional computational efforts. © 2015 Wiley Periodicals, Inc. 相似文献
7.
Synergic Catalysis of PdCu Alloy Nanoparticles within a Macroreticular Basic Resin for Hydrogen Production from Formic Acid 下载免费PDF全文
Prof. Dr. Kohsuke Mori Dr. Hiromasa Tanaka Masahiro Dojo Prof. Dr. Kazunari Yoshizawa Prof. Dr. Hiromi Yamashita 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(34):12085-12092
Highly dispersed PdCu alloy nanoparticles have been successfully prepared within a macroreticular basic resin bearing ?N(CH3)2 functional groups. This previously unappreciated combination of alloy is first proven to be responsible for the efficient production of high‐purity H2 from formic acid (HCOOH) dehydrogenation for chemical hydrogen storage. By the addition of Cu, the electronically promoted Pd sites show significantly higher catalytic activity as well as a better tolerance towards CO poisoning as compared to their monometallic Pd counterparts. Experimental and DFT calculation studies revealed not only the synergic alloying effect but also cooperative action by the ?N(CH3)2 groups within the resin play crucial roles in achieving exceptional catalytic performances. In addition to the advantages such as, facile preparation method, free of additives, recyclable without leaching of active component, and suppression of unfavorable CO formation less than 3 ppm, the present catalytic system is cost‐effective because of the superior catalytic activity compared with that of well‐established precious PdAg or PdAu catalysts. The present catalytic system is particularly desirable for an ideal hydrogen vector in terms of potential industrial application for fuel cells. 相似文献
8.
Hiromi NAKANISHI Atsushi MORI Kouki TAKEDA Houdo TANAKA Natsuko KOBAYASHI Keitaro TANOI Takashi YAMAKAWA Satoshi MORI 《Proceedings of the Japan Academy. Series B, Physical and biological sciences》2015,91(4):160-174
Six months after the explosion of TEPCO’s Fukushima Dai-ichi nuclear power plant, radioactive
silver (110mAg), was detected in concentrations of 3754 Bq/kg in Nephila
clavata (the orb-web spider; Joro-gumo in Japanese) collected at
Nimaibashi, Iitate village in Fukushima Prefecture, whereas 110mAg in the soil was
43.1 Bq/kg. A survey of 35 faunal species in the terrestrial environment during the 3.5 years
after the accident showed that most of Anthropoda had two orders higher 110mAg in
their tissues than soils, although silver is not an essential element for their life. However,
tracing of the activity of 110mAg detected in spider Atypus karschi
collected regularly at a fixed location showed that it declined much faster than the physical
half-life. These results suggest that 110mAg was at once biologically concentrated
by faunal species, especially Arthropoda, through food chain. The factors affecting the
subsequent rapid decline of 110mAg concentration in faunal species are
discussed. 相似文献
9.
Takashi Yoshimoto Prof. Dr. Hisako Hashimoto Dr. Nozomi Takagi Prof. Dr. Shigeyoshi Sakaki Naoki Hayakawa Dr. Tsukasa Matsuo Prof. Dr. Hiromi Tobita 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(15):3795-3798
A tungsten silylyne complex having a W≡Si triple bond reacted with two molecules of aldehydes at room temperature to give W−Si−O−C four-membered metallacycles by [2+2] cycloaddition and subsequent formyl hydrogen transfer from one aldehyde molecule to another. Upon heating to 70 °C, the four-membered metallacycles underwent metathesis-like fragmentation cleanly to afford carbyne complexes and “silanoic esters,” in a manner similar to that of metallacyclobutadiene, an intermediate of alkyne metathesis reactions, and dimerization of the latter products gave 1,3-cyclodisiloxanes. The “silanoic ester” was also trapped by pivalaldehyde to give a [2+2] cycloaddition product in high yield. 相似文献
10.
Total Synthesis and Structure Elucidation of JBIR‐39: A Linear Hexapeptide Possessing Piperazic Acid and γ‐Hydroxypiperazic Acid Residues 下载免费PDF全文
Dr. Masahito Yoshida Naoki Sekioka Dr. Miho Izumikawa Dr. Ikuko Kozone Dr. Motoki Takagi Dr. Kazuo Shin‐ya Prof. Dr. Takayuki Doi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(7):3031-3041
The total synthesis and stereochemical structural elucidation of JBIR‐39, containing four nonproteinogenic piperazic acid (Piz) residues, is reported. The synthesis includes Sc(OTf)3‐catalyzed acylation of a Piz(γ‐OTBS) derivative with piperazic acid chloride, providing the desired Piz‐Piz(γ‐OTBS) dipeptide in high yield without epimerization. After assembling two additional Piz moieties and (S)‐isoleucic acid at the N‐terminus, amidation with the (R)‐α‐methylserine ester at the C‐terminus, and deprotection afforded the desired (2R,8S)‐hexapeptide, which is the assumed structure of JBIR‐39. Although the spectral data of the (2R,8S)‐hexapeptide was not identical to JBIR‐39, further synthesis of three stereoisomers confirmed the stereochemical structure of JBIR‐39 to be (2S,6S,8S,11R,16S,21R,26S,27S). 相似文献