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A biosupramolecular approach to graphene: Complementary nucleotide-nucleobase combinations as enhanced stabilizers towards aqueous-phase exfoliation and functional graphene-nucleotide hydrogels

AuthorsCaridad Cañizo, Bárbara; Paredes Nachón, Juan Ignacio ; Pérez Vidal, Óscar; Villar Rodil, Silvia ; Pagán, A.; Cenis, J. L.; Martínez Alonso, Amelia ; Díez Tascón, Juan Manuel
Issue Date5-Dec-2017
CitationCarbon 129: 321-334 (2018)
AbstractThe ability to use RNA/DNA nucleotides as colloidal stabilizers for graphene would be an important asset, as a close graphene-nucleotide association would facilitate access to hybrid systems where the rich covalent and supramolecular chemistry of these biomolecules could be exploited alongside graphene in a number of applications. Unfortunately, single RNA/DNA nucleotides are inefficient graphene dispersants. Here we propose and demonstrate a supramolecular strategy which overcomes this limitation, affording aqueous dispersions of high quality graphene flakes with much improved colloidal stability. A nucleotide is combined with its complementary nucleobase yielding stable hydrogen-bonded supramolecular entities that adsorb more strongly on the graphene surface than their individual components. Based on this approach, graphene-nucleotide hybrid hydrogels could be readily obtained, where the graphene flakes were intimately and uniformly intermixed with the nucleotide-based gel phase. Such hydrogels exhibited higher uptakes and/or slower release profiles of dyes and drugs (rhodamine B, methylene blue and tetracycline) than their graphene-free counterparts. Cell proliferation tests suggested the graphene materials obtained with nucleotide-nucleobase stabilizers to be biocompatible. The present results constitute a novel strategy in the processing and molecular integration of graphene that could be extended to other (bio)molecules of interest towards the realization of functional materials for different applications.
Publisher version (URL)https://doi.org/10.1016/j.carbon.2017.12.007
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