Improving Continuum Models to Define Practical Limits for Molecular Models of Electrified Interfaces
Year: 2017
Type: article
Abstract: We develop a continuum theory of electrolyte solutions in contact with a metal electrode, based on a generalized free energy functional, and use it to explore the structure of the electric double layer at different electrochemical conditions.The model captures the effects of specific adsorption of ions and solvent polarization, and can be applied on the same footing to cases with non-zero faradaic current, beyond the classical double-layer regime.These advances permit the prediction of peculiar character in the ion profiles at electrode potentials near the redox level, exploration of the electrochemical stability of the interface, and differentiation between the mechanisms of electron and ion transport and associated time scales.The developed methodology enables us to selfconsistently determine the fundamental limits for a microscopic description of biased interfaces, in terms characteristic sizes and time scales of relevant processes, within atomistic and ab initio molecular dynamics simulations.
DOI: 10.1149/2.0461711jes
Authors: Artem Baskin, David Prendergast
Institutions: Lawrence Berkeley National Laboratory, Molecular Foundry
Language: English
Subfield: Physical and Theoretical Chemistry
Field: Chemistry
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $1,950
OpenAlex ID: W2632541580