Stripping away ion hydration shells in electrical double-layer formation: Water networks matter.

double layer electrochemistry electrolyte hydrogen bonding operando

Journal

Proceedings of the National Academy of Sciences of the United States of America
ISSN: 1091-6490
Titre abrégé: Proc Natl Acad Sci U S A
Pays: United States
ID NLM: 7505876

Informations de publication

Date de publication:
23 11 2021
Historique:
accepted: 06 10 2021
entrez: 16 11 2021
pubmed: 17 11 2021
medline: 17 11 2021
Statut: ppublish

Résumé

The double layer at the solid/electrolyte interface is a key concept in electrochemistry. Here, we present an experimental study combined with simulations, which provides a molecular picture of the double-layer formation under applied voltage. By THz spectroscopy we are able to follow the stripping away of the cation/anion hydration shells for an NaCl electrolyte at the Au surface when decreasing/increasing the bias potential. While Na

Identifiants

pubmed: 34782461
pii: 2108568118
doi: 10.1073/pnas.2108568118
pmc: PMC8617503
pii:
doi:

Types de publication

Journal Article Research Support, U.S. Gov't, Non-P.H.S. Research Support, Non-U.S. Gov't

Langues

eng

Sous-ensembles de citation

IM

Déclaration de conflit d'intérêts

Competing interest statement: M.H.-G. is a part-owner of Q-Chem Inc., whose software was used for some of the calculations reported here.

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Auteurs

Serena R Alfarano (SR)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany.

Simone Pezzotti (S)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany.
Université Paris-Saclay, Univ Evry, CNRS, LAMBE UMR8586, Evry-Courcouronnes 91025, France.

Christopher J Stein (CJ)

Department of Chemistry, University of California, Berkeley, CA 94720.
Theoretische Physik, Center for Nanointegration Duisburg-Essen, Universität Duisburg-Essen 47048 Duisburg, Germany.

Zhou Lin (Z)

Department of Chemistry, University of California, Berkeley, CA 94720.
Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720.

Federico Sebastiani (F)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany.

Sarah Funke (S)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany.

Claudius Hoberg (C)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany.

Inga Kolling (I)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany.

Chun Yu Ma (CY)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany.

Katja Mauelshagen (K)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany.

Thorsten Ockelmann (T)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany.

Gerhard Schwaab (G)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany.

Li Fu (L)

Université de Lyon, Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière F-69622 Villeurbanne, France.

Jean-Blaise Brubach (JB)

Synchrotron Soleil, AILES beamline, L'Orme des Merisiers 91192 Gif sur Yvette Cedex, France.

Pascale Roy (P)

Synchrotron Soleil, AILES beamline, L'Orme des Merisiers 91192 Gif sur Yvette Cedex, France.

Martin Head-Gordon (M)

Department of Chemistry, University of California, Berkeley, CA 94720; mhg@cchem.berkeley.edu kristina.tschulik@rub.de mgaigeot@univ-evry.fr martina.havenith@rub.de.
Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, CA 94720.

Kristina Tschulik (K)

Faculty of Chemistry and Biochemistry, Chair of Analytical Chemistry II, Ruhr University Bochum 44780 Bochum, Germany mhg@cchem.berkeley.edu kristina.tschulik@rub.de mgaigeot@univ-evry.fr martina.havenith@rub.de.

Marie-Pierre Gaigeot (MP)

Université Paris-Saclay, Univ Evry, CNRS, LAMBE UMR8586, Evry-Courcouronnes 91025, France; mhg@cchem.berkeley.edu kristina.tschulik@rub.de mgaigeot@univ-evry.fr martina.havenith@rub.de.

Martina Havenith (M)

Lehrstuhl für Physikalische Chemie II, Ruhr-Universität Bochum 44780 Bochum, Germany; mhg@cchem.berkeley.edu kristina.tschulik@rub.de mgaigeot@univ-evry.fr martina.havenith@rub.de.

Classifications MeSH