Biomedical subjects
Gareth W V Cave
Publications and source records attributed to Gareth W V Cave.
Hydrogen-bonded hexamers self-assemble as spherical and tubular superstructures on the sub-micron scale.
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Toward the isolation of functional organic nanotubes.
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Hydrogen-bonded supramolecular assemblies as robust templates in the synthesis of large metal-coordinated capsules.
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Nano-dimensions for the pyrogallol[4]arene cavity.
The cup-like cavity of pyrogallol[4]arenes has been deepened by the addition of four hydrogen bonded bipyridine molecules to the upper-rim of the calixarene, enabling the extended cup-like molecules to stack inside one another and consequently trap and completely enshroud a single guest molecule within the 250 angstroms3 cavitand formed between two of these stacked "nano-cups".
Supramolecular blueprint approach to metal-coordinated capsules.
An important problem in designing any large network is the assembly of systems that are resilient to change. From a chemical point of view, an analogy can be used where one requires supramolecular assemblies to maintain their dimensionality combined with limited structural perturbation in response to variation in its intermolecular framework. The identification of hydrogen-bonded framework patterns within experimentally known supramolecular assemblies that are structurally robust to disruption and selective hydrogen substitution are envisioned to act as a supramolecular blueprint or template for metal-ion retroinsertion. Here, we report the formation of a large neutral discrete pseudo-spherical coordination capsule assembled from 6 pyrogallol[4]arene ligands and 24 Cu(II) metal ions. Amazingly, this coordination capsule is structurally analogous to its hydrogen-bonded counterpart. This result shows a robust ability of pyrogallol[4]arene molecules to self-assemble into large hexameric cage structures from either the hydrogen-bonding or metal-ligand coordination process. The identification of robust supramolecular assemblies that conserve their structure in response to interchangeability between hydrogen-bonded networks for metal coordination, or inversely, represents an important advancement in supramolecular design.
Solvent-free, direct synthesis of supramolecular nano-capsules.
The single step direct synthesis of pyrogallol[4]arene via a solvent free protocol yields the pure product as a self-assembled nano-capsule, comprised of six macrocyclic building blocks.
Inner core structure responds to communication between nanocapsule walls.
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Molecular borromean rings.
The realization of the Borromean link in a wholly synthetic molecular form is reported. The self-assembly of this link, which is topologically achiral, from 18 components by the template-directed formation of 12 imine and 30 dative bonds, associated with the coordination of three interlocked macrocycles, each tetranucleating and decadentate overall, to a total of six zinc(II) ions, is near quantitative. Three macrocycles present diagonally in pairs, six exo-bidentate bipyridyl and six endo-diiminopyridyl ligands to the six zinc(II) ions. The use, in concert, of coordination, supramolecular, and dynamic covalent chemistry allowed the highly efficient construction, by multiple cooperative self-assembly processes, of a nanoscale dodecacation with an approximate diameter of 2.5 nanometers and an inner chamber of volume 250 A(3), lined with 12 oxygen atoms.
Nanocage encapsulation of two ortho-carborane molecules.
Bowl-shaped C-methylcalix[4]resorcinarene forms a 1:1 ball-and-socket nanostructure with o-carborane through two endo-cavity BC-H...pi hydrogen bonds. In the presence of 4',2:6,4"-terpyridine, two of these nanostructures are held together by four terpyridines through sixteen OH...N hydrogen bonds, completely shrouding two carboranes.