Tackling electrified interfaces using density functional theory and machine learning

Recently, a number of studies have found that electrochemical processes in batteries and electrolyzers are highly sensitive to the electrified solid-liquid interface. In order to accurately predict reaction kinetics or the stability of electrochemical system compounds, it is essential to develop methods that can model such interfaces on a quantum accuracy level. In addition, for most state-of-the-art energy systems such as carbon materials, single atom catalysts, 2D materials (MoS₂, etc.) or semiconductors the effect of electrification remains largely unknown and could potentially lead to the development of new technologies. In this project, we develop and apply several computational techniques from continuum over classical approaches up to full first-principles machine learning to upscale quantum chemical calculations with Density Functional Theory towards a full representation of the solid-liquid interface and its realistic reaction environment.

• S. Ringe* et al., Cation effects on electrocatalytic reduction processes at the example of the hydrogen evolution reaction, Current Opinion in Electrochemistry 2023, 39, 101268.
• S. M. R. Islam et al., An implicit electrolyte model for plane wave density functional theory exhibiting nonlinear response and a nonlocal cavity definition, J. Chem. Phys. 2023, 159, 234117.
• S. Shin† et al., On the importance of the electric double layer structure in aqueous electrocatalysis, Nat. Commun. 2022, 13, 174.
• S. Ringe†* et al., Implicit Solvation Methods for Catalysis at Electrified Interfaces, Chem. Rev. 2022, 122, 10777 - 10820.
• S. Ringe†* et al., Understanding cation effects in electrochemical CO₂ reduction, Energy Environ. Sci. 2019, 12, 3001 - 3014.
• Y. Wu† et al., A Two-Dimensional MoS₂ Catalysis Transistor by Solid-State Ion Gating Manipulation and Adjustment (SIGMA), Nano Lett. 2019, 19, 7293 - 7300.
• C. Hille† et al., Generalized molecular solvation in non-aqueous solutions by a single parameter implicit solvation scheme, J. Chem. Phys. 2019, 150, 041710.
• S. Ringe†* et al., Transferable ionic parameters for first-principles Poisson-Boltzmann solvation calculations: Neutral solutes in aqueous monovalent salt solutions, J. Chem. Phys. 2017, 146, 134103.
• S. Ringe† et al., Function-Space-Based Solution Scheme for the Size-Modified Poisson-Boltzmann Equation in Full-Potential DFT, J. Chem. Theory Comput. 2016, 12, 4052 - 4066.