Applied Potentials in Variable-Charge Reactive Force Fields for Electrochemical Systems

Tao Liang, Andrew C. Antony, Sneha A. Akhade, Michael J. Janik, Susan B. Sinnott

Research output: Contribution to journalArticle

3 Scopus citations

Abstract

An atomic description of water dynamics and electrochemical properties at electrode-electrolyte interfaces is presented using molecular dynamics with the third generation of the charge-optimized many-body (COMB3) potential framework. Externally applied potentials in electrochemical applications were simulated by offsetting electronegativity on electrode atoms. This approach is incorporated into the variable charge scheme within COMB3 and is used to investigate electrochemical systems consisting of two Cu electrodes and a water electrolyte with varying concentrations of hydroxyls (OH-) and protons (H+). The interactions between the electronegativity offset method and the charge equilibration method in a variable charge scheme are analyzed. In addition, a charge equilibration method for electrochemical applications is proposed, where the externally applied potentials are treated by the electronegativity offset on the electrodes thus enforcing charge neutrality on the electrolyte. This method is able to qualitatively capture the relevant electrochemistry and predict consistently correct voltages with precalibration.

Original languageEnglish (US)
Pages (from-to)631-638
Number of pages8
JournalJournal of Physical Chemistry A
Volume122
Issue number2
DOIs
StatePublished - Jan 18 2018

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry

Fingerprint Dive into the research topics of 'Applied Potentials in Variable-Charge Reactive Force Fields for Electrochemical Systems'. Together they form a unique fingerprint.

  • Cite this