The Intricacies of Computational Electrochemistry

Area of Science:

• Computational electrochemistry
• Theoretical chemistry
• Materials science

Background:

• Computational electrochemistry is challenging due to multiscale processes and rapid method development.
• Lack of clear guidelines and ongoing community discussions indicate field-wide complexities.
• A Lorentz Center workshop identified key challenges in computational electrochemistry.

Purpose of the Study:

• To highlight key take-away messages from a Lorentz Center workshop on computational electrochemistry.
• To discuss the complexities and challenges in the field of computational electrochemistry.
• To emphasize the need for improved methods and benchmarking in computational electrochemistry.

Main Methods:

• Perspective piece synthesizing discussions from a Lorentz Center workshop.
• Analysis of common challenges in computational electrochemistry simulations.
• Review of theoretical underpinnings and simulation methodologies.

Main Results:

• The choice between constant potential and constant charge simulations is non-trivial.
• Interpreting electrochemical reaction free energy diagrams presents significant challenges.
• The Poisson-Nernst-Planck equation alone is insufficient for all electrochemical modeling.

Conclusions:

• Addressing the complexities of computational electrochemistry requires careful consideration of simulation choices.
• Further development and rigorous benchmarking are crucial for advancing the field.
• Standardized guidelines and clear interpretations are needed for reliable computational electrochemistry.