Constrainment Effects of Interleaved Organic Molecules into Layered Double Hydroxides
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Constrainment Effects of Interleaved Organic Molecules into Layered Double Hydroxides Marc Dubois, El Mostafa Moujahid, Jean-Pierre Besse, and Fabrice Leroux* Laboratoire des Matériaux Inorganiques, CNRS-UMR n°6002, Université Blaise Pascal, 63177 Aubière cédex, France; E-mail: [email protected] ABSTRACT Incorporation and subsequent stabilization of organic molecules into layered double hydroxide are investigated. Through two types of hybrid materials, organic dyes and anilinebased monomers interleaved between LDH materials of cation composition Zn2Al and Cu2Cr respectively, it is shown that the effect of the constrainment is revealed by the interactions different according to the molecule size and stacking as exemplified by dye molecules, orange 6 and green 25 acids and two aniline-based monomers, m-amino-4-benzenesulfonic and 3-aniline-1-propanesulfonic acids. INTRODUCTION Inorganic organic hybrid materials have received a lot of attention for the past few years. The possibility to combine the properties of the two components has been the driving force in a numerous fields of application. Indeed such assemblies may provide mixed properties arising from the two parts unreachable by only one of the components, the lamellar host structure supplies a constrained environment in which the polymer is forced to locate and both parts may also act synergistically. The present work is dealing with the incorporation of negatively charged organic molecules into the gap of layered double hydroxides. Previous reviews were devoted to LDH hybrid material [1]. The LDH structure is referred to the natural hydrotalcite, and described with the ideal formula, [MIIxM1-xIII(OH)2]intra[Am-x/m. nH2O]inter, where MII and MIII are metal cations, A the anions and intra and inter denote the intralayer and interlayer domain, respectively. The structure consists of brucite-like layers constituted of edge-sharing M(OH)6 octahedra. Partial MII to MIII substitution induces a positive charge for the layers, balanced with the presence of the interlayered anions. Two LDH frameworks of cation composition Zn2Al and Cu2Cr were considered. Fonctionalized organic molecules have been incorporated between the sheets of layered double hydroxides. Two commercialized dye molecules, tropaeolin (acid Orange 6) (I) and acid Green 25 (II), which are mono- and di-functional macromolecules and two aniline-based monomers, m-amino-4-benzenesulfonic (III) and 3-aniline-1-propanesulfonic (IV) acids were chosen according to the following criteria: possibility of in-situ polymerization for the anilinebased monomers and of different stackings for the dye molecules. A combination of techniques (XRD, 13C CP-MAS NMR, UV-visible and ESR spectroscopies) was used to characterize the hybrid materials. EXPERIMENTAL SECTION Chemicals. Dye molecules, tropaeolin (C12H9N2O5SNa, acid Orange 6, Aldrich 65%) (I) and acid Green 25 (C28H20N2O8S2Na2, Acros 70%) (II), and monomer molecule, metanilic acid (III) (m-aminobenzenesulfonic acid, 97%, Aldrich), CuCl2. 2H2O
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