Abstract
While the traditional consensus dictates that high ion concentrations lead to negligible long-range electrostatic interactions, we demonstrate that electrostatic correlations prevail in deep eutectic solvents where intrinsic ion concentrations often surpass 2.5 M. Here we present an investigation of intermicellar interactions in 1:2 choline chloride:glycerol and 1:2 choline bromide:glycerol using small-angle neutron scattering. Our results show that long-range electrostatic repulsions between charged colloidal particles occur in these solvents. Interestingly, micelle morphology and electrostatic interactions are modulated by specific counterion condensation at the micelle interface despite the exceedingly high concentration of the native halide from the solvent. This modulation follows the trends described by the Hofmeister series for specific ion effects. The results are rationalized in terms of predominant ion–ion correlations, which explain the reduction in the effective ionic strength of the continuum and the observed specific ion effects.
Highlights
Electrostatic interactions play an essential role in biological and technological processes
The scattering of h-C12TAC in 1:2 deuterated 1:2 choline chloride:glycerol (d-ChCl):d-Glyc was initially measured at different surfactant concentrations, and these concentrations were decided based on previous investigations
Small-angle neutron scattering was used to probe particle structure and particle−particle correlation in micellar systems dispersed in 1:2 choline chloride:glycerol and 1:2 choline bromide:glycerol
Summary
Electrostatic interactions play an essential role in biological and technological processes. Recent investigations have shown that ion−ion correlations at high ion concentrations, such as in concentrated electrolytes and ionic liquids, reduce the apparent ionic strength of the continuum.[8,9] This prompts complex ionic systems to show a reversion in the Debye−Hückel theoretical predictions, and larger Debye lengths are observed with increasing ion concentrations at high ionic strength
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