Deutsch
 
Hilfe Datenschutzhinweis Impressum
  DetailsucheBrowse

Datensatz

DATENSATZ AKTIONENEXPORT
  Thermodynamic Cyclic Voltammograms Based on Ab Initio Calculations: Ag(111) in Halide-Containing Solutions

Hörmann, N., & Reuter, K. (2021). Thermodynamic Cyclic Voltammograms Based on Ab Initio Calculations: Ag(111) in Halide-Containing Solutions. Journal of Chemical Theory and Computation, 17(3), 1782-1794. doi:10.1021/acs.jctc.0c01166.

Item is

Basisdaten

einblenden: ausblenden:
Genre: Zeitschriftenartikel

Dateien

einblenden: Dateien
ausblenden: Dateien
:
acs.jctc.0c01166.pdf (Verlagsversion), 4MB
Name:
acs.jctc.0c01166.pdf
Beschreibung:
-
OA-Status:
Sichtbarkeit:
Öffentlich
MIME-Typ / Prüfsumme:
application/pdf / [MD5]
Technische Metadaten:
Copyright Datum:
2021
Copyright Info:
The Author(s)

Externe Referenzen

einblenden:

Urheber

einblenden:
ausblenden:
 Urheber:
Hörmann, Nicolas1, 2, Autor           
Reuter, Karsten2, Autor           
Affiliations:
1Chair of Theoretical Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstr. 4, 85748 Garching, Germany, ou_persistent22              
2Theory, Fritz Haber Institute, Max Planck Society, ou_634547              

Inhalt

einblenden:
ausblenden:
Schlagwörter: -
 Zusammenfassung: Cyclic voltammograms (CVs) are a central experimental tool for assessing the structure and activity of electrochemical interfaces. Based on a mean-field ansatz for the interface energetics under applied potential conditions, we here derive an ab initio thermodynamics approach to efficiently simulate thermodynamic CVs. All unknown parameters are determined from density functional theory (DFT) calculations coupled to an implicit solvent model. For the showcased CVs of Ag(111) electrodes in halide-anion-containing solutions, these simulations demonstrate the relevance of double-layer contributions to explain experimentally observed differences in peak shapes over the halide series. Only the appropriate account of interfacial charging allows us to capture the differences in equilibrium coverage and total electronic surface charge that cause the varying peak shapes. As a case in point, this analysis demonstrates that prominent features in CVs do not only derive from changes in adsorbate structure or coverage but can also be related to variations of the electrosorption valency. Such double-layer effects are proportional to adsorbate-induced changes in the work function and/or interfacial capacitance. They are thus especially pronounced for electronegative halides and other adsorbates that affect these interface properties. In addition, the analysis allows us to draw conclusions on how the possible inaccuracy of implicit solvation models can indirectly affect the accuracy of other predicted quantities such as CVs.

Details

einblenden:
ausblenden:
Sprache(n): eng - English
 Datum: 2020-11-062021-02-192021-03-09
 Publikationsstatus: Erschienen
 Seiten: 13
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/acs.jctc.0c01166
 Art des Abschluß: -

Veranstaltung

einblenden:

Entscheidung

einblenden:

Projektinformation

einblenden: ausblenden:
Projektname : EuroTechPostdoc - International Network of Excellence in Science Technology
Grant ID : 754462
Förderprogramm : Horizon 2020 (H2020)
Förderorganisation : European Commission (EC)

Quelle 1

einblenden:
ausblenden:
Titel: Journal of Chemical Theory and Computation
  Andere : J. Chem. Theory Comput.
Genre der Quelle: Zeitschrift
 Urheber:
Affiliations:
Ort, Verlag, Ausgabe: Washington, D.C. : American Chemical Society
Seiten: 13 Band / Heft: 17 (3) Artikelnummer: - Start- / Endseite: 1782 - 1794 Identifikator: ISSN: 1549-9618
CoNE: https://pure.mpg.de/cone/journals/resource/111088195283832