Journal
SOFT MATTER
Volume 10, Issue 47, Pages 9496-9505Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4sm01461h
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Funding
- CNRS [2010/52411-6]
- FAPESP [2010/52411-6]
- Brazilian Agency Capes
- CNPq (Conselho Nacional de Desenvolvimento Cientifco e Tecnologico) in Brazil
- ANR (Agence Nationale de la Recherche)
- CGI (Commissariat a l'Investissement d'Avenir) [ANR 11 LABX 086, ANR 11 IDEX 05 02]
- Agence Nationale de la Recherche (PANORAMA) [ANR-13-BS08-0015]
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Recent studies have pointed out the importance of polyelectrolyte assembly in the elaboration of innovative nanomaterials. Beyond their structures, many important questions on the thermodynamics of association remain unanswered. Here, we investigate the complexation between poly(diallyldimethylammonium chloride) (PDADMAC) and poly(sodium acrylate) (PANa) chains using a combination of three techniques: isothermal titration calorimetry (ITC), static and dynamic light scattering and electrophoresis. Upon addition of PDADMAC to PANa or vice-versa, the results obtained by the different techniques agree well with each other, and reveal a two-step process. The primary process is the formation of highly charged polyelectrolyte complexes of size 100 nm. The secondary process is the transition towards a coacervate phase made of rich and poor polymer droplets. The binding isotherms measured are accounted for using a phenomenological model that provides the thermodynamic parameters for each reaction. Small positive enthalpies and large positive entropies consistent with a counterion release scenario are found throughout this study. Furthermore, this work stresses the importance of the underestimated formulation pathway or mixing order in polyelectrolyte complexation.
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