Dilute solutions of sodium poly(styrene sulfonate) (NaPSS) in the presence of Al, Ca, and Ba were analysed by means of isothermal titration calorimetry (ITC) in order to investigate the heat effect of bond formation between those cations and the anionic SO residues of NaPSS. The selection of the cations was guided by the solution behavior of the corresponding PSS salts from a preceding study [M. Hansch et al., J. Chem. Phys. 148(1), 014901 (2018)], where bonds between Ba and anionic PSS showed an increasing solubility with decreasing temperature and Al exhibited the inverse trend. Unlike to Al and Ba, Ca is expected to behave as a purely electrostatically interacting bivalent cation and was thus included in the present study. Results from ITC satisfactorily succeeded to explain the temperature-dependent solution behavior of the salts with Al and Ba and confirmed the non-specific behavior of Ca. Additional ITC experiments with salts of Ca and Ba and sodium poly(acrylate) complemented the results on PSS by data from a chemically different polyanion. Availability of these joint sets of polyanion-cation combinations not only offers the chance to identify common features and subtle differences in the solution behavior of polyelectrolytes in the presence of multi-valent cations but also points to a new class of responsive materials.
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