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81.
Efficient solution-phase protocols for the high-throughput synthesis of 6-(1,2,3-triazol-1-yl)-dihydropyrimidones are reported. The multistep sequence involves the initial bromination of dihydropyrimidones precursors (DHPMs, Biginelli compounds) at the C6-methyl position, using a recyclable polymer-supported brominating agent under rapid flow-through conditions (residence time of 1 min). The 6-bromomethyldihydropyrimidone intermediates were subsequently subjected to a microwave-assisted azidation step (25 min), providing the key 6-azidomethyldihydropyrimidone precursors. In the final step of the sequence, the azides were treated with terminal acetylenes under Cu(I) catalysis (azide-acetylene ligation, "click chemistry") to provide the target 6-(1,2,3-triazol-1-yl)-dihydropyrimidones in a regiospecific fashion (1,4-triazoles) in moderate overall yield utilizing controlled microwave irradiation (20 min). In total, a library of 27 compounds was prepared with 4 points of diversity. 相似文献
82.
Gologan B Takáts Z Alvarez J Wiseman JM Talaty N Ouyang Z Cooks RG 《Journal of the American Society for Mass Spectrometry》2004,15(12):1874-1884
Protein ions, after mass spectrometric separation, can be soft-landed into liquid surfaces with preservation of their native structures. Retention of biological activity is strongly favored in glycerol-based surfaces but not in self-assembled monolayer solid surfaces. Soft-landing efficiency for multiply-charged hexokinase ions was found to be some four times higher for a glycerol/fructose liquid surface than for a fluorinated self-assembled monolayer surface. Soft-landing into liquid surfaces is also shown to allow (1) protein purification, (2) on-surface identification of the soft-landed material using MALDI, and (3) protein identification by in-surface tryptic digestion. Pure lysozyme was successfully isolated from different mixtures including an oxidized, partially decomposed batch of the protein and a partial tryptic digest. Liquid glycerol/carbohydrate mixtures could be used directly to record MALDI spectra on the soft-landed compounds provided they were fortified in advance with traditional MALDI matrices such as p-nitroaniline and alpha-cyano-4-hydroxycinnamic acid. Various proteins were soft-landed and detected on-target using these types of liquid surface. Soft-landing of multiply-charged lysozyme ions onto fluorinated self-assembled monolayer surfaces was found to occur with a limited amount of neutralization, and trapped multiply-charged ions could be desorbed from the surface by laser desorption. Initial data is shown for a new approach to protein identification that combines top-down and bottom-up approaches by utilizing protein ion soft-landing from a protein mixture, followed by tryptic digestion of the landed material and detection of characteristic tryptic fragments by MALDI. 相似文献
83.
Cichocki B Ekiel-Jezewska ML Nägele G Wajnryb E 《The Journal of chemical physics》2004,121(5):2305-2316
A system of many spherical particles, suspended in a quiescent fluid and touching a planar free fluid-gas interface, is considered. Stick fluid boundary conditions at the sphere surfaces are assumed. The free surface boundary conditions are taken into account with the use of the method of images. For such a quasi-two-dimensional system, the one-sphere resistance operator is calculated numerically. Moreover, the corresponding friction and mobility tensors are constructed from irreducible multipole expansion. Finally, the long-distance terms of the two-sphere mobility tensor are evaluated explicitly up to the order of 1/r3, where r is the interparticle distance. Experiments which have motivated this work are outlined. 相似文献
84.
Mihail?MeganEmail author Adina?Lumini?a?Sasu Bogdan?Sasu 《Integral Equations and Operator Theory》2004,50(4):489-504
The aim of this paper is to give necessary and sufficient conditions for pointwise and uniform exponential dichotomy of linear skew-product flows. We shall obtain that the pointwise exponential dichotomy of a linear skew-product flow is equivalent to the pointwise admissibility of the pair
As a consequence, we prove that a linear skew-product flow on
is uniformly exponentially dichotomic if and only if the pair
is uniformly admissible for . 相似文献
85.
Linear conductance across a large quantum dot via a single level epsilon(0) with large hybridization to the contacts is strongly sensitive to quasibound states localized in the dot and weakly coupled to epsilon(0). The conductance oscillates with the gate voltage due to interference of the Fano type. At low temperature and Coulomb blockade, Kondo correlations damp the oscillations on an extended range of gate voltage values, by freezing the occupancy of the epsilon(0) level itself. As a consequence, the antiresonances of Fano origin are washed out. The results are in good correspondence with experimental data for a large quantum dot in the semiopen regime. 相似文献
86.
Connections between uniform exponential expansiveness and complete admissibility of the pair
are studied. A discrete version for a theorem due to Van Minh, Räbiger and Schnaubelt is presented. Equivalent characterizations of Perron type for uniform exponential expansiveness of evolution families in terms of complete admissibility are given. 相似文献
87.
88.
Hodgson DM Stefane B Miles TJ Witherington J 《Chemical communications (Cambridge, England)》2004,(19):2234-2235
Organolithium-induced ring-opening of aziridines of 2,5-dihydrofuran (5 and 8) and 1,4-dimethoxybut-2-ene (16, 17 and 23) gives 3-substituted 2-aminobut-3-en-1-ols 9-15 and amino ethers 18-20 and 24-26. 相似文献
89.
90.