Spatial resolution of the electrical conductance of ionic fluids using a Green-Kubo method

Jones, R. E.; Ward, D. K.; Templeton, J. A.

doi:10.1063/1.4901035

Title: Spatial resolution of the electrical conductance of ionic fluids using a Green-Kubo method

Journal Article · Fri Nov 14 00:00:00 EST 2014 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4901035· OSTI ID:1502449

Jones, R. E. ^[1]; Ward, D. K. ^[2]; Templeton, J. A. ^[3]

Sandia National Lab. (SNL-CA), Livermore, CA (United States). Mechanics of Materials Dept.
Sandia National Lab. (SNL-CA), Livermore, CA (United States). Materials Chemistry Dept.
Sandia National Lab. (SNL-CA), Livermore, CA (United States). Thermal/Fluid Science and Engineering Dept.

We present a Green-Kubo method to spatially resolve transport coefficients in compositionally heterogeneous mixtures. We develop the underlying theory based on well-known results from mixture theory, Irving-Kirkwood field estimation, and linear response theory. Then, using standard molecular dynamics techniques, we apply the methodology to representative systems. With a homogeneous salt water system, where the expectation of the distribution of conductivity is clear, we demonstrate the sensitivities of the method to system size, and other physical and algorithmic parameters. Then we present a simple model of an electrochemical double layer where we explore the resolution limit of the method. In this system, we observe significant anisotropy in the wall-normal vs. transverse ionic conductances, as well as near wall effects. Lastly, we discuss extensions and applications to more realistic systems such as batteries where detailed understanding of the transport properties in the vicinity of the electrodes is of technological importance.

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Research Organization:: Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1502449

Report Number(s):: SAND-2014-15846J; 672036

Journal Information:: Journal of Chemical Physics, Vol. 141, Issue 18; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 4 works

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