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Perforated Bicontinuous Cubic Phases with pH‐Responsive Topological Channel Interconnectivity
Author(s) -
Zabara Alexandru,
Negrini Renata,
OnacaFischer Ozana,
Mezzenga Raffaele
Publication year - 2013
Publication title -
small
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.785
H-Index - 236
eISSN - 1613-6829
pISSN - 1613-6810
DOI - 10.1002/smll.201300348
Subject(s) - mesophase , interconnectivity , materials science , membrane , lyotropic , molecule , lyotropic liquid crystal , phase (matter) , confined space , lipid bilayer , crystallography , topology (electrical circuits) , liquid crystal , chemical physics , nanotechnology , chemical engineering , chemistry , liquid crystalline , optoelectronics , organic chemistry , biochemistry , mathematics , combinatorics , artificial intelligence , computer science , engineering
Lipidic lyotropic liquid crystals are at the frontline of current research for release of target therapeutic molecules due to their unique structural complexity and the possibility of engineering stimuli‐triggered release of both hydrophilic and hydrophobic molecules. One of the most suitable lipidic mesophases for the encapsulation and delivery of drugs is the reversed double diamond bicontinuous cubic phase, in which two distinct and parallel networks of ∼4 nm water channels percolate independently through the lipid bilayers, following a Pn3m space group symmetry. In the unperturbed Pn3m structure, the two sets of channels act as autonomous and non‐communicating 3D transport pathways. Here, a novel type of bicontinuous cubic phase is introduced, where the presence of OmpF membrane proteins at the bilayers provides unique topological interconnectivities among the two distinct sets of water channels, enabling molecular active gating among them. By a combination of small‐angle X‐ray scattering, release and ion conductivity experiments, it is shown that, without altering the Pn3m space group symmetry or the water channel diameter, the newly designed perforated bicontinuous cubic phase attains transport properties well beyond those of the standard mesophase, allowing faster, sustained release of bioactive target molecules. By further exploiting the pH‐mediated pore‐closing response mechanism of the double amino acid half‐ring architecture in the membrane protein, the pores of the perforated mesophase can be opened and closed with a pH trigger, enabling a fine modulation of the transport properties by only moderate changes in pH, which could open unexplored opportunities in the targeted delivery of bioactive compounds.