Regensburg 2022 – scientific programme

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O: Fachverband Oberflächenphysik

O 31: Solid-Liquid Interfaces 3: Reactions and Electrochemistry

O 31.3: Talk

Tuesday, September 6, 2022, 11:15–11:30, S054

First-principles molecular dynamics simulations of electrified Pt(111)/H2O interfaces — •Lang Li, Nicolas G. Hörmann, and Karsten Reuter — Fritz-Haber-Institut der Max-Planck- Gesellschaft, Berlin, Germany

Metal-water interfaces play a fundamental role in electrochemistry. An accurate understanding of their properties is required in any attempt to describe electrochemical phenomena such as electrocatalytic reactions or charge transfer processes.

In this work, we benchmark the description of electrified Pt(111)/water interfaces based on first-principles molecular dynamics simulations at applied potential conditions using density functional theory. We apply the potential by introducing excess electrons that are counterbalanced by partially charged hydrogen atoms. This method is tested with a variety of slab setups and cell sizes. Additionally, we investigate different methods to determine the reference potential.

We analyze in detail the structure of the interface as well as the obtained capacitance vs. potential curves and compare these with published theoretical and experimental results [1]. Our results highlight the response of interfacial water to an applied potential and its importance for understanding the hump in the capacitance, observed at high electrolyte concentrations [2].

[1] L. Li, J. -B. Le, J. Cheng, Cell Rep. Phys. Sci., 3, 100759 (2022). [2] J.B. Le, Q.Y. Fan, J.Q. Li, J. Cheng, Sci. Adv., 6, eabb1219 (2020).