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31.
Campbell CD Duguet N Gallagher KA Thomson JE Lindsay AG O'Donoghue AC Smith AD 《Chemical communications (Cambridge, England)》2008,(30):3528-3530
Cascade reaction sequences incorporating N-heterocyclic carbene-based organocatalysis have been developed that allow the direct preparation of a range of (+/-)-4-phenoxycarbonylazlactones in good isolated yields (66-84%) from the corresponding N-p-anisoyl amino acids. 相似文献
32.
Pordea A Creus M Panek J Duboc C Mathis D Novic M Ward TR 《Journal of the American Chemical Society》2008,130(25):8085-8088
Nature's catalysts are specifically evolved to carry out efficient and selective reactions. Recent developments in biotechnology have allowed the rapid optimization of existing enzymes for enantioselective processes. However, the ex nihilo creation of catalytic activity from a noncatalytic protein scaffold remains very challenging. Herein, we describe the creation of an artificial enzyme upon incorporation of a vanadyl ion into the biotin-binding pocket of streptavidin, a protein devoid of catalytic activity. The resulting artificial metalloenzyme catalyzes the enantioselective oxidation of prochiral sulfides with good enantioselectivities both for dialkyl and alkyl-aryl substrates (up to 93% enantiomeric excess). Electron paragmagnetic resonance spectroscopy, chemical modification, and mutagenesis studies suggest that the vanadyl ion is located within the biotin-binding pocket and interacts only via second coordination sphere contacts with streptavidin. 相似文献
33.
Doherty WJ Friedlein R Renouard T Mathis C Salaneck WR 《The Journal of chemical physics》2007,126(9):094708
The role of nitrogen in the charge transfer and storage capacity of lithium-intercalated heterocyclic oligophenylenes was investigated using photoelectron spectroscopy. The development of new occupied states at low binding energies in the valence band region, as well as core level chemical shifts at both carbon and nitrogen sites, demonstrates partial charge transfer from lithium atoms to the organic component during formation of the intercalated compound. In small compounds, i.e., biphenyl and bipyridine derivatives, the position of the nitrogen heteroatom significantly affects the spacing between gap states in the Li-intercalated film; yet it has minimal effects on the charge storage capacity. In larger, branched systems, the presence of nitrogen in the aromatic system significantly enhances the charge storage capacity while the Li-N bond strength at high intercalation levels is significantly weakened relative to the nitrogen-free derivative. These observations have strong implications towards improved deintercalation processes in organic electrodes in lithium-ion batteries. 相似文献
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We report a fabrication route of silica nanoparticles with two, three or six patches with an easily tunable patch-to-particle size ratio. The synthetic pathway includes two main stages: the synthesis of silica/polystyrene multipod-like templates and the selective growth of their silica core through an iterative approach. Electron microscopy of the dimpled nanoparticles obtained after dissolution of the polystyrene nodules of the multipod-like nanoparticles provides evidence of the conformational growth of the silica core. Thanks to the presence of some polymer chains, which remained grafted at the bottom of the dimples after the dissolution of the PS nodules, the solvent-induced assembly of the patchy nanoparticles is performed. Chains, hexagonal suprastructures and cubic lattices are obtained from the assembly of two-, three- and six-patch silica nanoparticles, respectively. Our study can guide future work in both patchy nanoparticle synthesis and self-assembly. It also opens new routes towards the fabrication of specific classes of one-, two- and three-dimensional colloidal lattices, including complex tilings. 相似文献
36.
König AM Düwel M Du B Kunze M Johannsmann D 《Langmuir : the ACS journal of surfaces and colloids》2006,22(1):229-233
We discuss the influence of a limited contact size on measurements of high-frequency interfacial viscoelasticity performed with a combination of a quartz crystal microbalance (QCM) and the Johnson-Kendall-Roberts (JKR) apparatus. In this instrument, a sphere-plate contact is established between an elastomeric lens and a quartz resonator. The analysis is carried out in the frame of the sheet-contact model, which states that both the shift of resonance frequency and the bandwidth are proportional to the contact area as long as the contact area is much smaller than the crystal itself. In particular, the ratio of the shift in bandwidth and the shift in frequency (termed the D-f ratio) is predicted to be constant and independent of geometry. However, the experiment does show a slight increase in the D-f ratio with the contact radius when the contact radius is comparable to the wavelength of sound inside the crystal. This effect can be explained by acoustic scattering. 相似文献
37.
Assaad Alsahlani Frank B. Mathis Ranjan Mukherjee 《Journal of sound and vibration》2012,331(20):4395-4405
A new method for the control of string vibration is presented. The method relies on application and removal of a constraint at one point on the string close to one of its boundaries. Application of the constraint temporarily results in two vibrating strings, one of which is significantly shorter in length than the other. The vibration of the shorter length string decays rapidly due to high damping and results in reduction in the overall energy of the system. Removal of the constraint does not change the energy of the system but allows the constraint to be applied repeatedly for vibration suppression. A mathematical model of the cycle of constraint application and removal is presented and multiple cycles of constraint application and removal are simulated. Experiments were performed with a coiled extension spring which behaves like a lightly damped string. Simulation and experimental results match well with each other and demonstrate the efficacy of the simple control strategy. 相似文献
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W. Mathis Rink Dr. Franziska Thomas 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(7):1665-1677
Coiled coils (CCs) are well-understood protein-folding motifs. They appear in a variety of oligomer states and as homo- and heteromeric assemblies. This versatility and the general accessibility by de novo design makes them ideal building blocks for synthetic biology. This Minireview highlights the efforts being made in designing small peptide catalysts or reaction templates based on the CC scaffold. The first reports described autocatalysis or mediation of peptide ligation based on CC recognition. Over the years, the designs became more advanced, catalyzing ester hydrolysis, acyl transfer and redox reactions with partial enzyme-like reactivity. Due to the ability to control CC assembly, and, in heterodimeric systems, the association and dissociation, the CC motif has become a common peptide tag in chemical biology. 相似文献