Stripping away ion hydration shells in electrical double-layer formation: Water networks matter
-
- Serena R. Alfarano
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
-
- Simone Pezzotti
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
-
- Christopher J. Stein
- Department of Chemistry, University of California, Berkeley, CA 94720;
-
- Zhou Lin
- Department of Chemistry, University of California, Berkeley, CA 94720;
-
- Federico Sebastiani
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
-
- Sarah Funke
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
-
- Claudius Hoberg
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
-
- Inga Kolling
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
-
- Chun Yu Ma
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
-
- Katja Mauelshagen
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
-
- Thorsten Ockelmann
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
-
- Gerhard Schwaab
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
-
- Li Fu
- Université de Lyon, Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière F-69622 Villeurbanne, France;
-
- Jean-Blaise Brubach
- Synchrotron Soleil, AILES beamline, L’Orme des Merisiers 91192 Gif sur Yvette Cedex, France;
-
- Pascale Roy
- Synchrotron Soleil, AILES beamline, L’Orme des Merisiers 91192 Gif sur Yvette Cedex, France;
-
- Martin Head-Gordon
- Department of Chemistry, University of California, Berkeley, CA 94720;
-
- Kristina Tschulik
- Faculty of Chemistry and Biochemistry, Chair of Analytical Chemistry II, Ruhr University Bochum 44780 Bochum, Germany
-
- Marie-Pierre Gaigeot
- Université Paris-Saclay, Univ Evry, CNRS, LAMBE UMR8586, Evry-Courcouronnes 91025, France;
-
- Martina Havenith
- Lehrstuhl für Physikalische Chemie II, Ruhr–Universität Bochum 44780 Bochum, Germany;
抄録
<jats:title>Significance</jats:title> <jats:p> For centuries the double layer at the solid/electrolyte interface has been a central concept in electrochemistry. Today, it is still crucial for virtually all renewable energy storage and conversion technologies. Here, the double-layer formation is probed by THz spectroscopy with ultrabright synchrotron light as a source. Our results capture the molecular details of double-layer formation at positively/negatively charged Au electrodes for an NaCl electrolyte. We reveal a contrasting response applying positive versus negative bias, which is dictated by the interfacial water network and rationalized by accompanying molecular dynamics simulations and electronic-structure calculations. While Na <jats:sup>+</jats:sup> is directly attracted toward the negatively charged electrode, stripping of the Cl <jats:sup>−</jats:sup> hydration shell is observed only at larger potential values. </jats:p>
収録刊行物
-
- Proceedings of the National Academy of Sciences
-
Proceedings of the National Academy of Sciences 118 (47), 2021-11-15
Proceedings of the National Academy of Sciences