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Mahesh Vishe Radim Hrdina Amalia I. Poblador-Bahamonde Céline Besnard Laure Guénée Thomas Bürgi Jér?me Lacour 《Chemical science》2015,6(8):4923-4928
The thermodynamically disfavored isomerization of α,β-unsaturated esters to deconjugated β,γ-unsaturated analogues occurs readily when coupled to an amidation. Within the framework of macrocyclic derivatives, it is shown that 15, 16, and 18 membered macrocycles react with tBuOK and anilines to generate, in one-pot, β,γ-unsaturated amides (yields up to 88%). Importantly, single (chiral) diastereomers are isolated (d.r. > 49 : 1, 1H NMR) irrespective of the size and nature of the rings, showing an effective transmission of remote stereochemistry during the isomerization process. CSP-chromatographic resolution and absolute configuration determination by VCD are achieved. 相似文献
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Igor Krivtsov Dariusz Mitoraj Christiane Adler Marina Ilkaeva Mariana Sardo Luís Mafra Christof Neumann Andrey Turchanin Chunyu Li Benjamin Dietzek Robert Leiter Johannes Biskupek Ute Kaiser Changbin Im Bjrn Kirchhoff Timo Jacob Radim Beranek 《Angewandte Chemie (International ed. in English)》2020,59(1):487-495
Heptazine‐based polymeric carbon nitrides (PCN) are promising photocatalysts for light‐driven redox transformations. However, their activity is hampered by low surface area resulting in low concentration of accessible active sites. Herein, we report a bottom‐up preparation of PCN nanoparticles with a narrow size distribution (ca. 10±3 nm), which are fully soluble in water showing no gelation or precipitation over several months. They allow photocatalysis to be carried out under quasi‐homogeneous conditions. The superior performance of water‐soluble PCN, compared to conventional solid PCN, is shown in photocatalytic H2O2 production via reduction of oxygen accompanied by highly selective photooxidation of 4‐methoxybenzyl alcohol and benzyl alcohol or lignocellulose‐derived feedstock (ethanol, glycerol, glucose). The dissolved photocatalyst can be easily recovered and re‐dissolved by simple modulation of the ionic strength of the medium, without any loss of activity and selectivity. 相似文献
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The attenuation and dispersion of elastic waves in fluid-saturated rocks due to the viscosity of the pore fluid is investigated using an idealized exactly solvable example of a system of alternating solid and viscous fluid layers. Waves in periodic layered systems at low frequencies are studied using an asymptotic analysis of Rytov’s exact dispersion equations. Since the wavelength of shear waves in fluids (viscous skin depth) is much smaller than the wavelength of shear or compressional waves in solids, the presence of viscous fluid layers necessitates the inclusion of higher terms in the long-wavelength asymptotic expansion. This expansion allows for the derivation of explicit analytical expressions for the attenuation and dispersion of shear waves, with the directions of propagation and of particle motion being in the bedding plane. The attenuation (dispersion) is controlled by the parameter which represents the ratio of Biot’s characteristic frequency to the viscoelastic characteristic frequency. If Biot’s characteristic frequency is small compared with the viscoelastic characteristic frequency, the solution is identical to that derived from an anisotropic version of the Frenkel–Biot theory of poroelasticity. In the opposite case when Biot’s characteristic frequency is greater than the viscoelastic characteristic frequency, the attenuation/dispersion is dominated by the classical viscoelastic absorption due to the shear stiffening effect of the viscous fluid layers. The product of these two characteristic frequencies is equal to the squared resonant frequency of the layered system, times a dimensionless proportionality constant of the order 1. This explains why the visco-elastic and poroelastic mechanisms are usually treated separately in the context of macroscopic (effective medium) theories, as these theories imply that frequency is small compared to the resonant (scattering) frequency of individual pores. 相似文献
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Radim Bělohlávek 《Archive for Mathematical Logic》2002,41(1):83-90
Presented is a completeness theorem for fuzzy equational logic with truth values in a complete residuated lattice: Given
a fuzzy set Σ of identities and an identity p≈q, the degree to which p≈q syntactically follows (is provable) from Σ equals the degree to which p≈q semantically follows from Σ. Pavelka style generalization of well-known Birkhoff's theorem is therefore established.
Received: 15 March 2000 / Revised version: 20 September 2000 Published online: 12 December 2001 相似文献
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The electrophoretic properties of boron cluster compounds were determined in water, methanol and ACN as solvents of the BGE and discussed based on the principles of ion migration. Two types of boron cluster compounds were investigated. One type consisted of derivatives of the nido-7,8-dicarbaundecaborate cluster, the other types are derivatized cobalt bis(dicarbollide) ions (COSANs) whose central cobalt atom is sandwiched by two 7,8-dicarbaundecaborate clusters. The BGE in all solvents was acetate/acetic acid buffer with pH 4.75 in water, 9.7 in methanol and 22.3 in ACN, respectively, at different ionic strength between 5 and 30 mM. The dependence of the mobility on ionic strength could not be explained by the theory of Debye, Hückel and Onsager, but good agreement was found upon considering an ion size parameter. Limiting mobilities were derived by curve fitting, and by the aid of the solvent viscosities the hydrodynamic radii of the analyte anions were calculated. They are between 0.25 and 0.48 nm, and were nearly independent of the solvent. Electrophoresis of the analytes in a BGE consisting of 6 mM perchloric acid in ACN allows the conclusion that the present boron cluster compounds behave as stronger acids than perchloric acid. 相似文献
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Alkyl glycosides as potential anti-<Emphasis Type="Italic">Candida albicans</Emphasis> growth agents
Tomáš Klunda Eva Machová Alžzbeta Čížzová Radim Horák Monika Poláková Slavomír Bystrický 《Chemical Papers》2016,70(9):1166-1170
Candida infections are becoming increasingly prevalent and many clinical isolates are resistant to common azole derivatives treatment. Accordingly, the capacity of a series of 19 alkyl glycosides, mainly mannosides and glucosides but also a cellobioside with aglycone chain-length from C-6 to C-20, to inhibit the growth of laboratory and clinically isolated strains of Candida albicans, was investigated. The study showed that only glycosides with the C-10 and C-12 aglycones were effective growth inhibitors of both types of Candida, strains, whose metabolic activity was also significantly reduced as revealed by an XTT assay. 相似文献
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Belokon YN Bespalova NB Churkina TD Císarová I Ezernitskaya MG Harutyunyan SR Hrdina R Kagan HB Kocovský P Kochetkov KA Larionov OV Lyssenko KA North M Polásek M Peregudov AS Prisyazhnyuk VV Vyskocil S 《Journal of the American Chemical Society》2003,125(42):12860-12871
Achiral, diamagnetic Ni(II) complexes 1 and 3 have been synthesized from Ni(II) salts and the Schiff bases, generated from glycine and PBP (7) and PBA (11), respectively, in MeONa/MeOH solutions. The requisite carbonyl-derivatizing agents pyridine-2-carboxylic acid(2-benzoyl-phenyl)-amide 7 (PBP) and pyridine-2-carboxylic acid(2-formyl-phenyl)-amide 11 (PBA) were readily prepared from picolinic acid and o-aminobenzophenone or picolinic acid and methyl o-anthranilate, respectively. The structure of 1 was established by X-ray crystallography. Complexes 1 and 3 were found to undergo C-alkylation with alkyl halides under PTC conditions in the presence of beta-naphthol or benzyltriethylammonium bromide as catalysts to give mono- and bis-alkylated products, respectively. Decomposition of the complexes with aqueous HCl under mild conditions gave the required amino acids, and PBP and PBA were recovered. Alkylation of 1 with highly reactive alkyl halides, carried out under the PTC conditions in the presence of 10% mol of (S)- or (R)-2-hydroxy-2'-amino-1,1'-binaphthyl 31a (NOBIN) and/or its N-acyl derivatives and by (S)- or (R)-2-hydroxy-8'-amino-1,1'-binaphthyl 32a (iso-NOBIN) and its N-acyl derivatives, respectively, gave rise to alpha-amino acids with high enantioselectivities (90-98.5% ee) in good-to-excellent chemical yields at room temperature within several minutes. An unusually large positive nonlinear effect was observed in these reactions. The Michael addition of acrylic derivatives 37 to 1 was conducted under similar conditions with up to 96% ee. The (1)H NMR and IR spectra of a mixture of the sodium salt of NOBIN and 1 indicated formation of a complex between the two components. Implications of the association and self-association of NOBIN for the observed sense of asymmetric induction and nonlinear effects are discussed. 相似文献
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