Aromatic ionene topology and counterion-tuned gelation of acidic aqueous solutions
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Data publicació2017-04-28
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Abstract
Unusual gelation of acidic solutions was achieved using polycations bearing quaternary ammonium moieties. These ionene polymers are based on a disubstituted phenylene dibenzamide core, which allows the construction of different topomers (i.e. ortho-1, meta-2 and para-3). The topology of the polymers was found to play a key role on their aggregation behaviour both in pure water and in a variety of aqueous acidic solutions leading to the formation of stable acidic gels. Specifically, ortho-1 showed superior gelation ability than the analogues meta-2 and para-3 in numerous solutions of different pH and ionic strengths. Lower critical gelation concentrations, higher gel-to-sol transition temperatures and faster gelation were usually observed for ortho-1 regardless the solvent system. Detailed computational molecular dynamic simulations revealed a major role of the counterion (Cl-) and specific polymer¿polymer interactions. In particular, hydrogen bonds, N–H¿p interactions and intramolecular p–p stacking networks are distinctive in ortho-1. In addition, counterions located at internal hydration regions also affect to such polymer¿polymer interactions, acting as binders and, therefore, providing additional stability.
CitacióBachl, J., Bertran, O., Mayr, J., Aleman, C., Díaz-Díaz, D. Aromatic ionene topology and counterion-tuned gelation of acidic aqueous solutions. "Soft matter", 28 Abril 2017, vol. 13, núm. 16, p. 3031-3041.
ISSN1744-683X
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Soft Matter_2017_Ionene HCl gelation.pdf | Postprint | 1,230Mb | Visualitza/Obre |