Dual aperture control on pH- and anion-driven supramolecular nanoscopic hybrid gate-like ensembles

Journal of the American Chemical Society
Rosa CasasúsEliseo Ruiz

Abstract

The development of gate-like systems able to perform certain programmed functions is an interesting way of taking chemistry to the frontiers of nanoscience. In relation to this field, we report a complete study of the behavior of a pH-driven and anion-controlled nano-supramolecular gate-like ensemble obtained by anchoring suitable polyamines on the pore outlets of mesoporous materials of the type MCM-41 (solid N3-S). The release of an entrapped dye (Ru(bipy)3(2+)) from the pore voids into the bulk solution allows us to study the gating effect. A pH-driven open/close mechanism was observed that arises from the hydrogen-bonding interaction between amines at neutral pH (open gate) and Coulombic repulsions at acidic pH between closely located polyammoniums at the pore openings (closed gate). Molecular dynamics simulations using force field methods have been carried out to explain the pH-driven open/close mechanism. For this purpose, a mesoporous silica structure was constructed, taking as base the (111) plane of the beta-crystoballite structure on which large hexagonal nanopores and anchored polyamines were included. From these calculations, it was observed how completely unprotonated amines display poor coverage of the pore (fully...Continue Reading

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Citations

Mar 19, 2014·Colloids and Surfaces. B, Biointerfaces·Hongyan HeYubin Huang
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Jul 4, 2009·Angewandte Chemie·Andrea BernardosPedro Amorós

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