Implicit Solvation Methods for Catalysis at Electrified Interfaces
-
- Stefan Ringe
- Department of Chemistry, Korea University, Seoul 02841, Republic of Korea
-
- Nicolas G. Hörmann
- Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin, Germany
-
- Harald Oberhofer
- Chair for Theoretical Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstraße 4, D-85747 Garching, Germany
-
- Karsten Reuter
- Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin, Germany
書誌事項
- 公開日
- 2021-12-20
- 権利情報
-
- https://creativecommons.org/licenses/by/4.0/
- DOI
-
- 10.1021/acs.chemrev.1c00675
- 10.48550/arxiv.2108.02461
- 公開者
- American Chemical Society (ACS)
この論文をさがす
説明
Implicit solvation is an effective, highly coarse-grained approach in atomic-scale simulations to account for a surrounding liquid electrolyte on the level of a continuous polarizable medium. Originating in molecular chemistry with finite solutes, implicit solvation techniques are now increasingly used in the context of first-principles modeling of electrochemistry and electrocatalysis at extended (often metallic) electrodes. The prevalent ansatz to model the latter electrodes and the reactive surface chemistry at them through slabs in periodic boundary condition supercells brings its specific challenges. Foremost this concerns the diffculty to describe the entire double layer forming at the electrified solid-liquid interface (SLI) within supercell sizes tractable by commonly employed density-functional theory (DFT). We review liquid solvation methodology from this specific application angle, highlighting in particular its use in the widespread {\em ab initio} thermodynamics approach to surface catalysis. Notably, implicit solvation can be employed to mimic a polarization of the electrode's electronic density under the applied potential and the concomitant capacitive charging of the entire double layer beyond the limitations of the employed DFT supercell. Most critical for continuing advances of this effective methodology for the SLI context is the lack of pertinent (experimental or high-level theoretical) reference data needed for parametrization.
収録刊行物
-
- Chemical Reviews
-
Chemical Reviews 122 (12), 10777-10820, 2021-12-20
American Chemical Society (ACS)