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91.
Jagesar DC Hartl F Buma WJ Brouwer AM 《Chemistry (Weinheim an der Bergstrasse, Germany)》2008,14(6):1935-1946
The macrocycle in rotaxane 1 is preferentially hydrogen bonded to the succinamide station in the neutral form, but can be moved to the naphthalimide station by one-electron reduction of the latter. The hydrogen bonding between the amide NH groups of the macrocycle and the C double bond O groups in the binding stations in the thread was studied with IR spectroscopy in different solvents in both states. In addition, the solvent effect on the vibrational frequencies was analyzed; a correlation with the solvent acceptor number (AN) was observed. The conformational switching upon reduction could be detected by monitoring the hydrogen-bond-induced shifts of the nu(CO) frequencies of the C double bond O groups of the succinamide and the reduced naphthalimide stations. The macrocycle was found to shield the encapsulated station from the solvent: wavenumbers of nu(CO) bands of the C double bond O groups residing inside the macrocycle cavity remain unaffected by the solvent polarity. 相似文献
92.
(1)H magic-angle spinning (MAS) NMR spectra of p-tert-butylcalix[4]arene inclusion compounds with toluene and pyridine show large complexation-induced shifts of the guest proton resonances arising from additional magnetic shielding caused by the aromatic rings of the cavities of the host calixarene lattice. In combination with ab initio calculations, these observations can be employed for NMR crystallography of host-guest complexes, providing important spatial information about the location of the guest molecules in the host cavities. 相似文献
93.
Catherine Paradis-Bleau Adrian Lloyd François Sanschagrin Tom Clarke Ann Blewett Timothy DH Bugg Roger C Levesque 《BMC biochemistry》2008,9(1):33
Background
To develop antibacterial agents having novel modes of action against bacterial cell wall biosynthesis, we targeted the essential MurF enzyme of the antibiotic resistant pathogen Pseudomonas aeruginosa. MurF catalyzes the formation of a peptide bond between D-Alanyl-D-Alanine (D-Ala-D-Ala) and the cell wall precursor uridine 5'-diphosphoryl N-acetylmuramoyl-L-alanyl-D-glutamyl-meso-diaminopimelic acid (UDP-MurNAc-Ala-Glu-meso-A2pm) with the concomitant hydrolysis of ATP to ADP and inorganic phosphate, yielding UDP-N-acetylmuramyl-pentapeptide. As MurF acts on a dipeptide, we exploited a phage display approach to identify peptide ligands having high binding affinities for the enzyme. 相似文献94.
Andries E. Brouwer Sebastian M. Cioabă Willem H. Haemers Jason R. Vermette 《Journal of Algebraic Combinatorics》2016,43(4):783-799
The simplicial rook graph \(\mathrm{SR}(m,n)\) is the graph of which the vertices are the sequences of nonnegative integers of length m summing to n, where two such sequences are adjacent when they differ in precisely two places. We show that \(\mathrm{SR}(m,n)\) has integral eigenvalues, and smallest eigenvalue \(s = \max \left( -n, -{m \atopwithdelims ()2}\right) \), and that this graph has a large part of its spectrum in common with the Johnson graph \(J(m+n-1,n)\). We determine the automorphism group and several other properties. 相似文献
95.
Baggerman J Jagesar DC Vallée RA Hofkens J De Schryver FC Schelhase F Vögtle F Brouwer AM 《Chemistry (Weinheim an der Bergstrasse, Germany)》2007,13(4):1291-1299
[2]- and [3]-rotaxanes with a tetraphenoxy perylene diimide core were synthesized. Hydrogen bonding between the wheel and the imide changes the optical properties of the perylene chromophore: the absorption and fluorescence spectra are red-shifted. The decay times of the rotaxanes are shorter in comparison with that of the axle. Single molecule fluorescence measurements reveal relatively narrow distributions of emission maxima and decay times. The averages are in agreement with ensemble measurements. The observed red shifts make the perylene diimide a suitable chromophore for sensing the position of the wheel on the axle. 相似文献
96.
Ratera I Sporer C Ruiz-Molina D Ventosa N Baggerman J Brouwer AM Rovira C Veciana J 《Journal of the American Chemical Society》2007,129(19):6117-6129
The solvent dependence of spectroscopic data of two neutral paramagnetic donor-acceptor dyads, based on a polychlorinated triphenylmethyl radical acceptor unit linked through a vinylene pi-bridge to a ferrocene (compound 1) or a nonamethylferrocene donor (compound 2) unit, is described. Both compounds exhibit broad absorptions in the near-IR region, with band maxima appearing around 1000 and 1500 nm for 1 and 2, respectively. These bands correspond to the excitation of a neutral DA ground state to the charge-separated D+A- state, indicative of an intramolecular electron-transfer process. Compounds 1 and 2 show two reversible one-electron redox processes associated with the oxidation of the ferrocene and the reduction of the polychlorotriphenylmethyl radical subunits. The solvent dependence of the redox potentials was also investigated, allowing the determination of the redox asymmetries DeltaG degrees of both dyads. The latter values, along with the experimental Eopt spectroscopic data, allow us to estimate, using the total energy balance Eopt = lambda + DeltaG degrees , the reorganization energy values, lambda, and their solvent polarity dependence. Since DeltaG degrees and lambda are of the same order of magnitude but exhibit opposite trends in their solvent polarity dependence, a unique shift from the normal to the inverted Marcus region with the change in solvent polarity is found. The kinetics of the charge recombination step of the excited charge-separated D+A- state was studied by picosecond transient absorption spectroscopy, which allows us to observe and monitor for the first time the charge-separated D+A- state, thereby confirming unambiguously the photoinduced electron-transfer phenomena. 相似文献
97.
Direct demonstration of enhanced diffusion in mesoporous ZSM-5 zeolite obtained via controlled desilication 总被引:2,自引:0,他引:2
Groen JC Zhu W Brouwer S Huynink SJ Kapteijn F Moulijn JA Pérez-Ramírez J 《Journal of the American Chemical Society》2007,129(2):355-360
A 2 orders of magnitude gas transport improvement in a medium pore ZSM-5 zeolite has been achieved upon introduction of intracrystalline mesoporosity in gradient-free crystals by desilication post-treatment in alkaline medium. 相似文献
98.
This work reports the high-yield formation of pyrazoline derivatives mediated by gold(I) catalysts. The reaction utilizes a diaziridine, which has seen only limited usage in organic methodology. Mechanistic studies suggest a gold-mediated opening of the diazridine ring, alkyne insertion, and finally an intramolecular hydroamination to furnish the product. 相似文献
99.
S. Abramovich P. Brouwer 《International Journal of Mathematical Education in Science & Technology》2013,44(6):779-795
This paper suggests that mathematics teacher educators should listen carefully to what their students are saying. More specifically, it demonstrates how from one pre-teacher's non-traditional geometric representation of a unit fraction, a variety of learning environments that lead to the enrichment of mathematics for teaching can be developed. The paper shows how new knowledge may be generated through an attempt to validate an intuitive idea; in other words, how the quest for rigour may serve as a catalyst for the growth of mathematical concepts in the context of K-16 mathematics. 相似文献
100.
Arwin J. Brouwer 《Tetrahedron letters》2009,50(26):3391-2522
Substituted taurine sulfonyl fluorides derived from taurine or protected amino acids are conveniently synthesized from β-aminoethanesulfonyl chlorides using KF/18-crown-6 or from β-aminoethanesulfonates using DAST. 相似文献