Water binding and mobility in polyelectrolyte complexes*

Water is central in the assembly and the dynamics of charged macromolecular systems including polyelectrolyte assemblies. Nevertheless, it remains a challenge to resolve how water influences assembly characteristics and materials properties of these systems. We have examined via molecular modelling and interconnected experiments the role of water at molecular level on polyelectrolyte complexes and multilayers. We compare different polyelectrolyte systems under varying hydration and salt content and report that the hydration and water binding at especially intrinsic ion pairs connects with the thermal and mechanical response of hydrated polyelectrolyte assemblies. The findings rise attention to water and water partitioning as a control parameter of polyelectrolyte materials properties.

[1] P. Batys, S. Kivistö, S. M. Lalwani, J. L. Lutkenhaus, and M. Sammalkorpi, Soft Matter 15, 7823 (2019).
[2] P. Batys, Y. Zhang, J. L. Lutkenhaus, and M. Sammalkorpi, Macromolecules 51, 8268 (2018).
[3] Y. Zhang, P. Batys, J. T. O’Neal, F. Li, M. Sammalkorpi, J. L. Lutkenhaus ACS Central Science 4, 638 (2018).