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Mechanistic study of a Pd/C-catalyzed reduction of aryl sulfonates using the Mg-MeOH-NH(4)OAc system
Mori A Mizusaki T Ikawa T Maegawa T Monguchi Y Sajiki H 《Chemistry (Weinheim an der Bergstrasse, Germany)》2007,13(5):1432-1441
A method for the deoxygenation of phenolic hydroxy groups via aryl triflates or mesylates has been established by using a combination of Pd/C-Mg-MeOH. The addition of NH(4)OAc to the system markedly accelerated the reaction rate and expanded the scope of the reaction. Mechanistic studies suggested that a single-electron transfer process from the Pd(0) center to the benzene ring is involved in the reduction of aryl sulfonates and that NH(4)OAc works as a solubilization reagent of the Mg salt and as an accelerator of the electron transfer, thus enhancing the reaction process. Our method was also applicable to the regioselective deuteration of benzene derivatives with CH(3)OD as the solvent and deuterium source: the original hydroxy group could be efficiently replaced with a deuterium atom. 相似文献
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Hirakawa Y Suzuto M Ohnishi H Shingaki T Eyring EM Tokunaga M Masujima T 《The Analyst》2003,128(6):676-680
The nano-kinetic movement of a single DNA molecule was observed and analyzed by a newly developed video-microscope system with an optical fiber, called a pin-fiber video scope. A single lambda-DNA molecule was put in focus using fiber-illumination, and the stretching and shrinking motion was measured. The molecule's kinetics were analyzed by numerical calculations and are discussed. A photocleavage phenomenon of DNA molecules was also visualized by the pin-fiber video scope. The new video-microscope system has the potential to observe and analyze the nano-kinetics of a single molecule. 相似文献
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Jens R. Stellhorn Shinya Hosokawa Naohisa Happo Hiroo Tajiri Tomohiro Matsushita Kenichi Kaminaga Tomoteru Fukumura Tetsuya Hasegawa Koji Kimura Kouichi Hayashi 《Surface and interface analysis : SIA》2019,51(1):70-73
We report on the characterization of a thin film of yttrium oxide by X-ray fluorescence holography. The sample has a layered structure with an YO base layer and an oxidized Y2O3 surface. Both layers are clearly observed in the atomic image reconstructions, and their local structure is analyzed. We show that by using incident energies close to the absorption edge of the fluorescing atom, it becomes possible to observe the thin surface layer clearly, even next to a base layer containing the same fluorescing element. 相似文献
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Abstract PbSe/SnSe superlattice, phase transition, high pressure, SR x-ray diffraction) Synchrotron x-ray diffraction experiments have revealed successive phase transitions in epitaxially-grown PbSe/SnSe superlattices. The transition pressures from the low-pressre cubic B1- to the high-pressure orthorhombic B16-type structures are observed to vary systematically depending upon thickness of the PbSe layer. For example, a [PbSe(36A)/SnSe(12A)]19, with the B1 structure in both layers stabilized in its asgrown state, undergoes the [B1/B1]-to-[B1/B16] and [B1/B16]-to-[B16/B16] structural transitions at 1.9 and 3.8GPa, respectively. This result is in contrast to their bulk data that the B1-to-B16 transition takes place at 5.3GPa in PbSe while the B16 phase is stable in SnSe at atmospheric pressure. 相似文献
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Selective N-alkylation of amines using nitriles under hydrogenation conditions: facile synthesis of secondary and tertiary amines 总被引:1,自引:0,他引:1
Ikawa T Fujita Y Mizusaki T Betsuin S Takamatsu H Maegawa T Monguchi Y Sajiki H 《Organic & biomolecular chemistry》2012,10(2):293-304
Nitriles were found to be highly effective alkylating reagents for the selective N-alkylation of amines under catalytic hydrogenation conditions. For the aromatic primary amines, the corresponding secondary amines were selectively obtained under Pd/C-catalyzed hydrogenation conditions. Although the use of electron poor aromatic amines or bulky nitriles showed a lower reactivity toward the reductive alkylation, the addition of NH(4)OAc enhanced the reactivity to give secondary aromatic amines in good to excellent yields. Under the same reaction conditions, aromatic nitro compounds instead of the aromatic primary amines could be directly transformed into secondary amines via a domino reaction involving the one-pot hydrogenation of the nitro group and the reductive alkylation of the amines. While aliphatic amines were effectively converted to the corresponding tertiary amines under Pd/C-catalyzed conditions, Rh/C was a highly effective catalyst for the N-monoalkylation of aliphatic primary amines without over-alkylation to the tertiary amines. Furthermore, the combination of the Rh/C-catalyzed N-monoalkylation of the aliphatic primary amines and additional Pd/C-catalyzed alkylation of the resulting secondary aliphatic amines could selectively prepare aliphatic tertiary amines possessing three different alkyl groups. According to the mechanistic studies, it seems reasonable to conclude that nitriles were reduced to aldimines before the nucleophilic attack of the amine during the first step of the reaction. 相似文献
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Masashi Suzuto Yasuyuki Hirakawa Hitoshi Ohnishi Shinji Tachino Tomoteru Shingaki Edward M Eyring Tsutomu Masujima 《Analytical sciences》2003,19(1):43-47
The nano-kinetics of colloidal particles and living cells with the colloidal particles were visualized by a newly developed video scope. The system of the new video scope has a feature of fine controlling the illumination conditions by using a single optical fiber. This characteristic enables one to obtain clear images of living cells and the motions of colloidal particles by light-scattering effects. In the experiments, RBL-2H3 cells and gold colloidal particles were observed. Scattering images with high contrast and a dark background like in dark-field observations could be attained. In the experiments, a pulsed laser was also applied. The results obtained in this study could validate the effectiveness and possibility of a new video scope for applications to biological and biomedical fields. 相似文献
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Pd/C-catalyzed deoxygenation of phenol derivatives using Mg metal and MeOH in the presence of NH(4)OAc 总被引:2,自引:0,他引:2
[STRUCTURE: SEE TEXT] A Pd/C-catalyzed deoxygenation method of phenolic hydroxyl groups via aryl triflates or mesylates using Mg metal in MeOH at room temperature was developed. The addition of NH4OAc dramatically affects the reactivity and reaction rate. This method is particularly attractive to provide an environmentally benign and widely applicable removal method of phenolic alcohols under quite mild reaction conditions. 相似文献
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We discuss the effects of vertical gravity force on wave propagation when a material is intermediate between solid and fluid, especially we focus on what kinds of phase are generated and how it propagates on the surface. We introduce gravity terms into the 2D linear finite element method in order to account for the contribution from the gravity. Numerical simulations are conducted for a half-space model and a two-layered, single horizontal layer overlain on a half-space, model. Both models are compared between the results including and excluding the viscosity. The fastest phase propagating from a surface point source, a leaking Rayleigh wave for usual elastic material, is transformed into an interesting phase including some common features to the gravity wave when the gravity effect becomes significant. The viscosity does not affect the fastest phases, whereas it affects other latter phases appearing only for the two-layered model. 相似文献
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