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排序方式: 共有735条查询结果,搜索用时 140 毫秒
1.
Bo Huang Hirokazu Kobayashi Tomokazu Yamamoto Takaaki Toriyama Syo Matsumura Yoshihide Nishida Katsutoshi Sato Katsutoshi Nagaoka Masaaki Haneda Wei Xie Yusuke Nanba Michihisa Koyama Fenglong Wang Shogo Kawaguchi Yoshiki Kubota Hiroshi Kitagawa 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(8):2252-2257
Ru is an important catalyst in many types of reactions. Specifically, Ru is well known as the best monometallic catalyst for oxidation of carbon monoxide (CO) and has been practically used in residential fuel cell systems. However, Ru is a minor metal, and the supply risk often causes violent fluctuations in the price of Ru. Performance‐improved and cost‐reduced solid‐solution alloy nanoparticles of the Cu‐Ru system for CO oxidation are now presented. Over the whole composition range, all of the CuxRu1?x nanoparticles exhibit significantly enhanced CO oxidation activities, even at 70 at % of inexpensive Cu, compared to Ru nanoparticles. Only 5 at % replacement of Ru with Cu provided much better CO oxidation activity, and the maximum activity was achieved by 20 at % replacement of Ru by Cu. The origin of the high catalytic performance was found as CO site change by Cu substitution, which was investigated using in situ Fourier transform infrared spectra and theoretical calculations. 相似文献
2.
3.
Dr. Hirokazu Tsukamoto Saki Nakamura Akito Tomida Prof. Dr. Takayuki Doi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(55):12528-12532
Haouamines A, B, and their derivatives were synthesized via Suzuki–Miyaura coupling and three key cyclization reactions as follows: the newly developed palladium(0)-catalyzed arylative cyclization of phenylalanine-derived alkyne–aldehydes with 2-bromoarylboronic acid (an “anti-Wacker”-type cyclization); BF3 ⋅ OEt2-promoted Friedel–Crafts-type cyclization of symmetrical electron-rich aromatic rings adjacent to a tertiary allylic alcohol leading to the indeno-tetrahydropyridine skeleton; and (cyanomethyl)trimethylphosphonium iodide-mediated macrocyclization of amino alcohols to afford aza-paracyclophane precursors. The palladium-catalyzed reduction of mono- and di-triflate intermediates in the later stages enabled the alteration of both the position and number of hydroxyl groups on the C-ring. The instability of haouamine B was dramatically improved by salt formation with formic acid. An unambiguous evaluation of the cytotoxicity of the prepared haouamine derivative formates with and without hydroxyl groups at different positions on the C-ring indicated that the catechol structure in haouamine B produced weak cytotoxicity. 相似文献
4.
Mitsunori Fukaya Shota Nagamine Dr. Taro Ozaki Yaping Liu Miina Ozeki Taro Matsuyama Dr. Kazunori Miyamoto Prof. Dr. Hirokazu Kawagishi Prof. Dr. Masanobu Uchiyama Prof. Dr. Hideaki Oikawa Dr. Atsushi Minami 《Angewandte Chemie (International ed. in English)》2023,62(44):e202308881
Mushroom terpenoids are biologically and chemically diverse fungal metabolites. Among them, melleolides are representative sesquiterpenoids with a characteristic protoilludane skeleton. In this study, we applied a recently established hot spot knock-in method to elucidate the biosynthetic pathway leading to 1α-hydroxymelleolide. The biosynthesis of the sesquiterpene core involves the cytochrome P450 catalyzing stepwise hydroxylation of the Δ6-protoilludene framework and a stereochemical inversion process at the C5 position catalyzed by short-chain dehydrogenase/reductase family proteins. The highlight of the biosynthesis is that the flavoprotein Mld7 catalyzes an oxidation-triggered double-bond shift accompanying dehydration and acyl-group-assisted substitution with two different nucleophiles at the C6 position to afford the Δ7-protoilludene derivatives, such as melleolide and armillarivin. The complex reaction mechanism was proposed by DFT calculations. Of particular importance is that product distribution is regulated by interaction with the cell membrane. 相似文献
5.
Hirokazu Okuda Kohei Taniguchi Shinsuke Inagi Toshio Fuchigami 《Electroanalysis》2021,33(11):2296-2301
Electrochemical oxidation of O-(4-chlorobenzyl) S-methyl dithiocarbonate using tris(2,4-dibromophenyl)amine as a redox mediator was studied by cyclic voltammetric measurements. The triarylamine mediated anodic fluorodesulfurization of O-(4-chlorobenzyl) and O-(4-bromobenzyl) S-methyl dithiocarbonates provided 4-chloro- and 4-bromobenzyl fluorides, respectively in moderate yields. On the other hand, similar anodic fluorination of O-(2-phenethyl) S-octyl dithiocarbonate and O-(4-bromophenyl) S-methyl dithiocarbonate afforded 2-phenethyl trifluoromethyl ether and difluoro(methylthio)methyl 4-bromophenyl ether, respectively. Mechanistic aspects are also discussed. 相似文献
6.
7.
Ruthenium‐Immobilized Periodic Mesoporous Organosilica: Synthesis,Characterization, and Catalytic Application for Selective Oxidation of Alkanes 下载免费PDF全文
Nobuhiro Ishito Dr. Hirokazu Kobayashi Dr. Kiyotaka Nakajima Yoshifumi Maegawa Dr. Shinji Inagaki Dr. Kenji Hara Prof. Dr. Atsushi Fukuoka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(44):15564-15569
Periodic mesoporous organosilica (PMO) is a unique material that has a crystal‐like wall structure with coordination sites for metal complexes. A Ru complex, [RuCl2(CO)3]2, is successfully immobilized onto 2,2’‐bipyridine (BPy) units of PMO to form a single‐site catalyst, which has been confirmed by various physicochemical analyses. Using NaClO as an oxidant, the Ru‐immobilized PMO oxidizes the tertiary C?H bonds of adamantane to the corresponding alcohols at 57 times faster than the secondary C?H bonds, thereby exhibiting remarkably high regioselectivity. Moreover, the catalyst converts cis‐decalin to cis‐9‐decalol in a 63 % yield with complete retention of the substrate stereochemistry. The Ru catalyst can be separated by simple filtration and reused without loss of the original activity and selectivity for the oxidation reactions. 相似文献
8.
Yoshihisa Morita Hirokazu Ninomiya 《Journal of Dynamics and Differential Equations》2006,18(4):841-861
We deal with a reaction–diffusion equation u
t
= u
xx
+ f(u) which has two stable constant equilibria, u = 0, 1 and a monotone increasing traveling front solution u = φ(x + ct) (c > 0) connecting those equilibria. Suppose that u = a (0 < a < 1) is an unstable equilibrium and that the equation allows monotone increasing traveling front solutions u = ψ1(x + c
1
t) (c
1 < 0) and ψ2(x + c
2
t) (c
2 > 0) connecting u = 0 with u = a and u = a with u = 1, respectively. We call by an entire solution a classical solution which is defined for all
. We prove that there exists an entire solution such that for t≈ − ∞ it behaves as two fronts ψ1(x + c
1
t) and ψ2(x + c
2
t) on the left and right x-axes, respectively, while it converges to φ(x + ct) as t→∞. In addition, if c > − c
1, we show the existence of an entire solution which behaves as ψ1( − x + c
1
t) in
and φ(x + ct) in
for t≈ − ∞. 相似文献
9.
Masataka Sugimoto Hirokazu Hida Takashi Taniguchi Kiyohito Koyama Yuji Aoki 《Rheologica Acta》2007,46(7):957-964
Poly(vinyl chloride) (PVC)/di-isononyl phthalate systems with PVC content of 45.5 (PVC8) and 70.4 wt% (PVC6) were prepared
by a hot roller at 150 °C and press molded at 180 °C. The dynamic viscoelasticity and elongational viscosity of PVC8 and PVC6
were measured in the temperature range from 150 to 220 °C. We have found that the storage and loss shear moduli, G′ and G″, of PVC8 and PVC6 exhibited the power-law dependence on the angular frequency ω at 190 and 210 °C, respectively. Correspondingly, the tan δ values did not depend on ω. These temperatures indicate the critical gel temperature T
gel of each system. The critical relaxation exponent n obtained from these data was 0.75 irrespective of PVC content, which was in agreement with the n values reported previously for the low PVC concentration samples. These results suggest that the PVC gels of different plasticizer
content have a similar fractal structure. Below T
gel, the gradual melting of the PVC crystallites takes place with elevating temperature, and above T
gel, a densely connected network throughout the whole system disappears. Correspondingly, the elongational viscosity behavior
of PVC8 and PVC6 exhibited strong strain hardening below T
gel, although it did not show any strain hardening above T
gel. These changes in rheological behavior are attributed to the gradual melting of the PVC crystallites worked as the cross-linking
domains in this physical gel, thereby inapplicability of the of time–temperature superposition for PVC/plasticizer systems. 相似文献
10.
On the ‐boundedness of solution operator families of the generalized Stokes resolvent problem in an infinite layer 下载免费PDF全文
Hirokazu Saito 《Mathematical Methods in the Applied Sciences》2015,38(9):1888-1925
In this paper, we prove the ‐boundedness of solution operator families of the generalized Stokes resolvent problem in an infinite layer with resolvent parameter , where , and our boundary conditions are nonhomogeneous Neumann on upper boundary and Dirichlet on lower boundary. We want to emphasize that we can choose 0 < ? < π ∕ 2 and γ0 > 0 arbitrarily, although usual parabolic theorem tells us that we must choose a large γ0 > 0 for given 0 < ? < π ∕ 2. We also prove the maximal Lp ? Lq regularity theorem of the nonstationary Stokes problem as an application of the ‐boundedness. The key of our approach is to apply several technical lemmas to the exact solution formulas of a resolvent problem. The formulas are obtained through the solutions of the ODEs, in the Fourier space, driven by the partial Fourier transform with respect to tangential space variable . Copyright © 2014 John Wiley & Sons, Ltd. 相似文献