Dynamic constitutional hybrid materials-toward adaptive self-organized devices
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Dynamic constitutional hybrid materials-toward adaptive self-organized devices Mihail Barboiu,* Adinela Cazacu, Simona Mihai, Yves-Marie Legrand, Arie van der Lee Adaptative Supramolecular Nanosystems Group, Institut Européen des Membranes, UMRCNRS5635, IEM/UMII, Place Eugène Bataillon CC047, 34095 Montpellier cedex 5, France. E-mail: [email protected] ABSTRACT Dynamic constitutional hybrid materials in which the functional self-organized macrocycles are reversibly connected with the inorganic silica mesopores through hydrophobic non-covalent interactions. Supramolecular columnar self-organized architectures confined within scaffolding hydrophobic silica mesopores can be structurally determined by using X-ray diffraction techniques. INTRODUCTION Hybrid organic–inorganic materials produced by sol-gel process are the subject of various investigations, offering the opportunity to achieve nanostructured functional materials.[1] These materials reveal great potentialities as well on the level of their chemical composition or organization as to that of the concerned applications.[1-6] Organogels resulting by multiple selfassembly processes and acting as robust organic templates for the TEOS sol-gel process have been used for the synthesis of different inorganic structures.[4] Many groups including our own[5,8] have found new methods for the elaboration of hybrid self-organized materials based on silsesquioxanes in which the functional organic (supramolecular) and inorganic siloxane networks are covalently connected. Rigid aromatic molecules,[6] urea ribbons,[7,8] are nonexhaustively used to transcribe a oriented supramolecular self-organization in a siloxane matrix by a sol-gel process. Of special interest is structure-directed function of hybrid materials and to control their build-up by self-organization. Toward this objective, our interest in this field is to develop new functional hybrid membrane materials using simple molecules bearing hydrophilic moieties that form patterns by collective self-assembly so as to enable efficient translocation events. Herein we describe several findings related to this aim and we report new hybrid organic-inorganic dense materials in which protons, ions and molecules are envisioned to diffuse along the hydrophilic pathways. We previously proved the possibility to create hybrid complexant membranes, selforganized in directional superstructures. They have been employed successfully to design an ionpowered ATP2- pump,[8] hybrid devices mimicking directional ion-channels systems[9] or mimetic materials for specific biomolecular recognition of amino acids.[10] Moreover, we have recently reported macrocyclic supramolecular systems, leading to columnar arrangements of crown-ethers, so as to enable efficient ion-translocation events in lipid bilayers or liquid and solid hybrid membranes.[8] In homogenous solution at least two types of hydrogenbonded parallel and anti-parallel aggregates form. They can self-organize as a dimer followed by a discrete higher oligomer
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