The Intricacies of Computational Electrochemistry
Nitish Govindarajan, Georg Kastlunger, Joseph A. Gauthier, Jun Cheng, Ivo A. W. Filot, Arthur Hagopian, Heine Anton Hansen, Jun Huang, Piotr M. Kowalski, Jinwen Liu, Juan M. Lombardi, Mikael Maraschin, Andrew A. Peterson, Hemanth Somarajan Pillai, Hèctor Prats, Conor Jason Price, René van Roij, Jan Rossmeisl, Ranga Rohit Seemakurthi, Seung‐Jae Shin, Audrey D. Smith, Jiaxin Zhu, Katharina Doblhoff-Dier
Abstract
Computational electrochemistry is hardanybody who has ever tried will know. We argue that the reasons for its complexity lie not only in the multiscale nature of electrochemical processes but also in the rapid, ongoing method development in the field. This has resulted in a lack of clear guidelines and many open discussions in the community. These issues were also the topic of a recent Lorentz Center workshop, the key take-away messages of which are highlighted in this Perspective. In particular, we discuss why the choice between constant potential and constant charge simulations is less trivial than it may seem, why interpreting electrochemical reaction free energy diagrams can be challenging, why the Poisson-Nernst-Planck equation is not all there is, and why we desperately need more benchmarking in the field.