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Dr. Alice C. Harnden Dr. Andrei S. Batsanov Prof. Dr. David Parker 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(24):6212-6225
A zinc-selective probe based on a set of rare earth complexes of a modified DO3A macrocyclic ligand incorporating a tris-pyridylamine (TPA) moiety has been structurally characterised in solution and in the solid-state. One pyridine group possesses a tert-butyl substituent to serve as an NMR reporter group. The mono-capped square-antiprismatic Dy complex has a long bond (2.83 Å) to an apical N atom (pKa 5.70 Eu) and binds to one water molecule on zinc binding. Zinc binding is reversible and involves all of the exocyclic ligand N donors; it is signalled by large (ratiometric) changes in Eu emission intensity, and by dramatic changes in the size (>50 ppm) and sign of the chemical shift of the paramagnetically shifted tBu resonances in Tb, Dy and Tm complexes. Slow trans-metallation was observed, leading to formation of an unusual di-zinc species in which one zinc ion is seven-coordinate and the other is six-coordinate. 相似文献
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Ziyi Yu Jing Zhang Roger J. Coulston Richard M. Parker Frank Biedermann Xin Liu Oren A. Scherman Chris Abell 《Chemical science》2015,6(8):4929-4933
Host–guest assembly in droplet-based microfluidics opens a new avenue for fabricating supramolecular hydrogel microcapsules with high monodispersity and controlled functionality. In this paper, we demonstrate a single emulsion microdroplet platform to prepare microcapsules with supramolecular hydrogel skins from host molecule cucurbit[8]uril and guest polymer anthracene-functionalized hydroxyethyl cellulose. In contrast to construction of microcapsules from a droplet-in-droplet double emulsion, here the electrostatic attraction between charged polymer and surfactant facilitates formation of defined supramolecular hydrogel skins in a single emulsion. Furthermore, by taking advantage of dynamic interactions and the tunable cross-linked supramolecular hydrogel network, it is possible to prepare microcapsules with triggered and UV-controlled molecular permeability. These could be potentially used in a delivery system for e.g. agrochemicals, nutraceuticals or cosmetics. 相似文献
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Kassandra Cendejas Hope E. Parker Dennis Molina Rajib Choudhury 《Journal of inclusion phenomena and macrocyclic chemistry》2017,89(1-2):199-205
In this study, we have examined supramolecular self-assembly process of a hydrophobic guest with a water-soluble host known by the trivial name octa acid (OA). Two octa acids form a capsular assembly only in presence of a nonpolar guest(s). Size and shape of the guest control the stoichiometry of the capsular complex. Here, all atom molecular dynamics simulation has been utilized to investigate complex formation mechanisms of a nonpolar guest (nonylbenzene) with two OA cavitands. Nonylbenzene was encapsulated into the nonpolar cavity of OA capsule owing to solvophobic interactions. Upon encapsulation it was twisted and bent due to lack of free space within the capsule. These unusual forms obtained from the simulation study were in accord with experimental findings. The post-complexation attributes of the guest were regulated by the available free space within the OA and favorable non-covalent interactions between the guest and the walls of the OA capsule. In the identical simulation condition two OA cavitands did not form a capsule without a guest, thus indicating requirement of a guest during the self-assembly of OA cavitands. 相似文献
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The effect of sound on the flow around plates with semicircular or square leading edges and square trailing edges located in a low turbulence open jet has been studied. In all circumstances the length of the leading edge separation bubbles associated with square leading edge plates was found to oscillate. When sound was applied to the flow around these plates, the leading edge shear layers reattached closer to the leading edge and the oscillations in bubble length occurred at the applied sound frequency, generating patches of concentrated vorticity in the boundary layers. These vorticity patches moved downstream near the plate surface and then beyond the trailing edge to form vortex cores in a street with a Strouhal number equal to the applied sound value. Sometimes these vortex streets are unstable and break down into streets with Strouhal numbers approaching those observed without sound. These effects of sound were not observed in the flow around plates with semicircular leading edges. Without sound, square leading edge plates of intermediate length did not shed regular vortex streets. 相似文献
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Linear elastic surface waves are nondispersive. All wavelengths travel at the Rayleigh wave speed c
R. This absence of frequency dispersion means that nonlinear waves of permanent form cannot be determined as a small perturbation from a sinusoidal wavetrain. By representing the general Rayleigh wave of the linear theory in terms of a pair of conjugate harmonic functions, waves which propagate without distortion are characterized as those having surface elevation profiles which satisfy a certain nonlinear functional equation. In the small-strain limit, this reduces to a quadratic functional equation. Methods for the analysis of this equation are presented for both periodic and nonperiodic waveforms. For periodic waveforms, the infinite system of quadratic equations for the Fourier coefficients of the profile is solved numerically in the case of a certain harmonic elastic material. Two distinct families of profiles having phase speed differing from the linearized Rayleigh wave speed are found. Additionally, two families of exceptional waveforms are found, describing profiles which travel at the Rayleigh wave speed. 相似文献
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Experimental and theoretical studies of edge effects in rectangular composite strips under tension are discussed. The objective of the study was to investigate the effect of various parameters, including reinforcement material, fiber orientation and the structure of the reinforcement, on the various quantities which are observed in the vicinity of free edges in multidirectionally reinforced laminates. Of particular interest was the confirmation of theoretical results related to differences in response of graphite- and boron-reinforced laminates. Experiments consisted of moiré measurements of surface-displacement patterns which were compared with theoretical predictions, and examination of failure levels. The experiments were carried out on AVCO 5505 boron and Whitaker 5206 MODMOR II graphite-reinforced angle-ply laminates in which both stacking sequence and fiber orientation were varied parametrically. Moiré techniques were developed which allowed observation of displacements on both the wide surface and along the narrow edge of 1 in.-wide × 16-ply-thick (.085 in.-.105 in.) laminates. 相似文献