The intricacies of computational electrochemistry

Govindarajan, N.; Kastlunger, G.; Gauthier, J.A.; Cheng, J.; Filot, I.; Hagopian, A.M.V.; ... ; Doblhoff-Dier, K. (2025)

Article / Letter to editor

Computational electrochemistry is hard-anybody 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.

• All authors: Govindarajan, N.; Kastlunger, G.; Gauthier, J.A.; Cheng, J.; Filot, I.; Hagopian, A.M.V.; Hansen, H.A.; Huang, J.; Kowalski, P.M.; Liu J.; Lombardi, J.M.; Maraschin, M.; Peterson, A.; Pillai, H.S.; Prats, H.; Price, C.J.; Roij, R. van; Rossmeisl, J.; Seemakurthi, R.R.; Shin, S.J.; Smith, A.; Zhu, J.X.; Doblhoff-Dier, K.
• Date: 2025-08-08
• Journal: ACS Energy Letters
• Volume: 10
• Issue: 9
• Pages: 4277 - 4288
• DOI: doi:10.1021/acsenergylett.5c00748
• Link: https://pubs.acs.org/doi/10.1021/acsenergylett.5c00748