4.7 Article

Structure of the electrical double layer at the ice-water interface

Journal

JOURNAL OF CHEMICAL PHYSICS
Volume 154, Issue 21, Pages -

Publisher

AIP Publishing
DOI: 10.1063/5.0048817

Keywords

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Funding

  1. University of Texas at Austin
  2. Laboratory Directed Research and Development program at Sandia National Laboratories
  3. U.S. Department of Energy's National Nuclear Security Administration [DE-NA-0003525]

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Research indicates that an electrical double layer exists at the ice-water interface, with over 99% of counterions contained in the Stern layer, and the electrical conduction and polarization in the diffuse layer can be negligible.
The surface of ice in contact with water contains sites that undergo deprotonation and protonation and can act as adsorption sites for aqueous ions. Therefore, an electrical double layer should form at this interface and existing models for describing the electrical double layer at metal oxide-water interfaces should be able to be modified to describe the surface charge, surface potential, and ionic occupancy at the ice-water interface. I used a surface complexation model along with literature measurements of the zeta potential of ice in brines of various strength and pH to constrain equilibrium constants. I then made predictions of ion site occupancy, surface charge density, and partitioning of counterions between the Stern and diffuse layers. The equilibrium constant for cation adsorption is more than 5 orders of magnitude larger than the other constants, indicating that this reaction dominates even at low salinity. Deprotonated OH sites are predicted to be slightly more abundant than dangling O sites, consistent with previous work. Surface charge densities are on the order of +/- 0.001 C/m(2) and are always negative at the moderate pH values of interest to atmospheric and geophysical applications (6-9). In this pH range, over 99% of the counterions are contained in the Stern layer. This suggests that diffuse layer polarization will not occur because the ionic concentrations in the diffuse layer are nearly identical to those in the bulk electrolyte and that electrical conduction and polarization in the Stern layer will be negligible due to reduced ion mobility.

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