TY - JOUR
T1 - Frequency-dependent conductivity of concentrated electrolytes
T2 - A stochastic density functional theory
AU - Bonneau, Haggai
AU - Avni, Yael
AU - Andelman, David
AU - Orland, Henri
N1 - Publisher Copyright:
© 2024 Author(s).
PY - 2024/12/28
Y1 - 2024/12/28
N2 - The response of ionic solutions to time-varying electric fields, quantified by a frequency-dependent conductivity, is essential in many electrochemical applications. Yet, it constitutes a challenging problem due to the combined effect of Coulombic interactions, hydrodynamics, and thermal fluctuations. Here, we study the frequency-dependent conductivity of ionic solutions using a stochastic density functional theory. In the limit of small concentrations, we recover the classical Debye and Falkenhagen (DF) result, predicting an increase in conductivity with field frequency. At higher concentrations, we use a modified Coulomb interaction potential that accounts for the hard-core repulsion between the ions, which was recently employed in the zero-frequency case. Consequently, we extend the DF result to concentrated electrolytes. We discuss experimental and numerical studies and the complexity of observing the DF effect in such setups.
AB - The response of ionic solutions to time-varying electric fields, quantified by a frequency-dependent conductivity, is essential in many electrochemical applications. Yet, it constitutes a challenging problem due to the combined effect of Coulombic interactions, hydrodynamics, and thermal fluctuations. Here, we study the frequency-dependent conductivity of ionic solutions using a stochastic density functional theory. In the limit of small concentrations, we recover the classical Debye and Falkenhagen (DF) result, predicting an increase in conductivity with field frequency. At higher concentrations, we use a modified Coulomb interaction potential that accounts for the hard-core repulsion between the ions, which was recently employed in the zero-frequency case. Consequently, we extend the DF result to concentrated electrolytes. We discuss experimental and numerical studies and the complexity of observing the DF effect in such setups.
UR - http://www.scopus.com/inward/record.url?scp=85212961306&partnerID=8YFLogxK
U2 - 10.1063/5.0236073
DO - 10.1063/5.0236073
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C2 - 39713999
AN - SCOPUS:85212961306
SN - 0021-9606
VL - 161
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 24
M1 - 244501
ER -