guest ::
| Home > Publications database > Interface Properties of the Partially Oxidized Pt(111) Surface Using Hybrid DFT–Solvation Models |
| Home > Publications database > Interface Properties of the Partially Oxidized Pt(111) Surface Using Hybrid DFT–Solvation Models |
| Journal Article | FZJ-2020-00386 |
;
2019
Soc.
Washington, DC
This record in other databases: 
Please use a persistent id in citations: doi:10.1021/acsami.9b16326
Abstract: This article reports a theoretical–computational effort to model the interface between an oxidized platinum surface and aqueous electrolyte. It strives to account for the impact of the electrode potential, formation of surface-bound oxygen species, orientational ordering of near-surface solvent molecules, and metal surface charging on the potential profile along the normal direction. The computational scheme is based on the DFT/ESM-RISM method to simulate the charged Pt(111) surface with varying number of oxygen adatoms in acidic solution. This hybrid solvation method is known to qualitatively reproduce bulk metal properties like the work function. However, the presented calculations reveal that vital interface properties such as the electrostatic potential at the outer Helmholtz plane are highly sensitive to the position of the metal surface slab relative to the DFT-RISM boundary region. Shifting the relative position of the slab also affects the free energy of the system. It follows that there is an optimal distance for the first solvent layer within the ESM-RISM framework, which could be found by optimizing the position of the frozen Pt(111) slab. As it stands, manual sampling of the position of the slab is impractical and betrays the self-consistency of the method. Based on this understanding, we propose the implementation of a free energy optimization scheme of the relative position of the slab in the DFT-RISM boundary region. This optimization scheme could considerably increase the applicability of the hybrid method.
; Clarivate Analytics Master Journal List ; Current Contents - Engineering, Computing and Technology ; Current Contents - Physical, Chemical and Earth Sciences ; IF >= 5 ; JCR ; NCBI Molecular Biology Database ; SCOPUS ; Science Citation Index ; Science Citation Index Expanded ; Web of Science Core Collection
|
The record appears in these collections: |
PDF
PDF (PDFA)