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排序方式: 共有93条查询结果,搜索用时 15 毫秒
1.
Qingde Zhang Yisheng Tan Caihong Yang Yizhuo Han Jun Shamoto Noritatsu Tsubaki 《天然气化学杂志》2007,16(3):322-325
The attractive utilization route for one-step catalytic oxidation of dimethyl ether to dimethoxymethane was successfully carried out over the H3PW12O40(40%)/SiO2 catalyst, modified by Cs, K, Ni, and V. The Cs modification of H3PW12O40(40%)/SiO2 gave the most promising result of 20% dimethyl ether conversion and 34.8% dimethoxymethane selectivity. Dimethoxymethane could be synthe- sized via methoxy groups decomposed from dimethyl ether through the synergistic effect between the acid sites and the redox sites of Cs modified H3PW12O40(40%)/SiO2. 相似文献
2.
Yang Wang Weizhe Gao Kangzhou Wang Xinhua Gao Baizhang Zhang Heng Zhao Qingxiang Ma Peipei Zhang Guohui Yang Mingbo Wu Noritatsu Tsubaki 《Chemical science》2021,12(22):7786
Even though the transformation of syngas into aromatics has been realized via a methanol-mediated tandem process, the low product yield is still the bottleneck, limiting the industrial application of this technology. Herein, a tailor-made zeolite capsule catalyst with Ga doping and SiO2 coating was combined with the methanol synthesis catalyst Cr2O3 to boost the synthesis of value-added aromatics, especially para-xylene, from syngas. Multiple characterization studies, control experiments, and density functional theory (DFT) calculation results clarified that Ga doped zeolites with strong CO adsorption capability facilitated the transformation of the reaction intermediate methanol by optimizing the first C–C coupling step under a high-pressure CO atmosphere, thereby driving the reaction forward for aromatics synthesis. This work not only reveals the synergistic catalytic network in the tandem process but also sheds new light on principles for the rational design of a catalyst in terms of oriented conversion of syngas.The single-pass conversion of syngas into para-xylene was realized using a bifunctional catalyst Cr2O3/Ga-ZSM-5@SiO2. The Ga species facilitates the methanol consumption process by C–C coupling optimization, enhancing the yield of the target aromatics. 相似文献
3.
Tsubaki H Tohyama S Koike K Saitoh H Ishitani O 《Dalton transactions (Cambridge, England : 2003)》2005,(2):385-395
Intramolecular pi-pi and CH-pi interactions between the bpy and PR3 ligands of fac-[Re(bpy)(CO)3(PR3)]+ affect their structure, and electrochemical and spectroscopic properties. Intramolecular CH-pi interaction was observed between the alkyl groups on the phosphine ligand (R =nBu, Et) and the bpy ligand, and intramolecular pi-pi and CH-pi interactions were both observed between the aryl group(s) on the phosphorus ligand (R =p-MeOPh, p-MePh, Ph, p-FPh, OPh) and the bpy ligand, while no such interactions were found in the trialkylphosphite complexes (R = OiPr, OEt, OMe). The intramolecular interactions distort the pyridine rings of the bpy ligand as long as 3.7 x 10(-2)A in crystals. Molecular orbital calculations of the bpy ligand suggest that this distortion decreases the energy gap between its pi and pi* orbitals. An absorption band attributed to the pi-pi*(bpy) transition of the distorted rhenium complexes, measured in a KBr pellet, was red-shifted by 1-5 nm compared to the complexes without the distorted bpy ligand. Even in solution, similar red shifts of the pi-pi*(bpy) absorption were observed. The redox potential E1/2(bpy/bpy*-) of the complexes with the trialkylphosphine and triarylphosphine ligand are shifted positively by 110-120 mV and 60-80 mV respectively, compared with those derived from the electron-attracting property of the phosphorus ligand. In contrast with these properties, three nu(CO) IR bands, which are sensitive to the electron density on the central rhenium because of pi-back bonding, were shifted to higher energy, and a Re(I/II)-based oxidation wave was observed at a more positive potential according to the electron-attracting property of the phosphorus ligand. 相似文献
4.
H Harada K Iizuka T Kamijo K Akahane R Yamamoto Y Nakano A Tsubaki T Kubota I Shimaoka H Umeyama 《Chemical & pharmaceutical bulletin》1990,38(11):3042-3047
The experimental details for the synthesis of human renin inhibitors are described. In order to avoid metabolic degradation of the Phe-His (P3-P2) amide bond in transition-state analogs, structurally modified acyl residues (P4-P3) were incorporated into the inhibitors. Compound 1a, which contained 2-(1-naphthylmethyl)-3-(N-phenethylcarbamoyl)propionyl residue (P4-P3) with a retro-inverso amide bond, L-histidine, and norstatine isoamylamide residue (P1-P1) as a transition-state mimic, had potent human renin inhibitory activity, and it lowered blood pressure when administered orally to common marmosets. 相似文献
5.
Dr. Yohei Hattori Shunsuke Tsubaki Dr. Ryota Matsuoka Dr. Tetsuro Kusamoto Prof. Hiroshi Nishihara Prof. Kingo Uchida 《化学:亚洲杂志》2021,16(17):2538-2544
Polychlorinated pyridyldiphenylmethyl radicals having substituents meta to the position bearing the carbon-centered radical (α-carbon) are synthesized. All of them are stable in ambient conditions in solutions and fluorescent in cyclohexane. The fluorescence of the radicals with bromo, phenyl, 4-chlorophenyl, or 2-pyridyl substituents are enhanced in chloroform, while the emission of the radicals with 2-thienyl or 2-furyl substituents are quenched in chloroform. DFT and TD-DFT calculations indicate that the first doublet excited states of the former are locally excited, while the first doublet excited states of the latter are charge transfer states from the π-electron-donating substituent to the accepting radical. The latter also show much higher photostability under 370-nm light irradiation compared with the first reported photostable fluorescent radical, (3,5-dichloro-4-pyridyl)bis(2,4,6-trichlorophenyl)methyl radical (PyBTM), with pronounced bathochromic shifts of the fluorescence. 相似文献
6.
The design secret of Kyokusui-no-En’s meandering channel 总被引:1,自引:0,他引:1
The purpose of this study is to investigate the characteristics of the flow through the Jonangu channel which is used for
ceremonial game called as ‘Kyokusui-no-En’ in Japanese. The geometry of the channel is measured, a visualization technique
is used to measure the actual flow characteristics, and then a numerical flow model is used to represent the flow including
unsteady flow characteristics. Numerical model of drifting cup is introduced to investigate an interaction between flow and
motion of the cup. Finally, the intention of the channel design is interpreted from the viewpoint of fluid mechanics using
observed and calculated results. 相似文献
7.
Morimoto T Henmi M Naito R Tsubaki K Aoki N Bird JP Ochiai Y 《Physical review letters》2006,97(9):096801
We report on a remarkable resonance in the differential conductance of long quantum point contacts (QPCs) that is observed as a precursor to regular quantized transport. This effect is increasingly pronounced in longer QPCs, in which the differential conductance may resonantly exceed 2e2/h. From a study of the experimental characteristics of this feature, we suggest that it may be associated with the formation of a well-resolved energy gap that opens dynamically as a result of enhanced many-body interactions in long QPCs. 相似文献
8.
Host 1 based on the phenolphthalein skeleton and two crown ether moieties demonstrated opposite behaviors toward sodium and potassium cations caused by bidirectional complexation. [reaction: see text] 相似文献
9.
10.
Dr. Masashi Hasegawa Chika Hasegawa Yuki Nagaya Prof. Dr. Kazunori Tsubaki Prof. Dr. Yasuhiro Mazaki 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(59):e202202218
Chiral macrocyclic dimers, trimers, and tetramers composed of paraphenylene and tethered binaphthyl were synthesized, and their molecular structures and chiroptical properties were investigated. X-ray analysis and theoretical calculations revealed that multiple twisted molecular structures – dimers, trimers, and tetramers – adopt figure-of-eight, Möbius triangle, and concave rectangle structures, respectively. These homologues have large ϵ values in their UV-vis absorption spectra because of the π-conjugation of the naphthalene-phenylene-naphthalene frameworks. Owing to the shape-persistent ring structure and tethering with −OCH2CH2O−, high fluorescence quantum yields and a relatively high dissymmetry factor gCPL in circularly polarized luminescence (CPL) spectra were achieved. This results in CPL brightness (BCPL) of over 100, which is greater than that of the conventional organic CPL dye. 相似文献