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Probing Electrochemical Potential Differences over the Solid/Liquid Interface in Li-Ion Battery Model Systems

Källquist, Ida; Lindgren, Fredrik; Lee, Ming-Tao; Shavorskiy, Andrey; Edström, Kristina; Rensmo, Håkan; Nyholm, Leif; Maibach, Julia 1; Hahlin, Maria
1 Karlsruher Institut für Technologie (KIT)


The electrochemical potential difference (Δμ̅) is the driving force for the transfer of a charged species from one phase to another in a redox reaction. In Li-ion batteries (LIBs), Δμ̅ values for both electrons and Li-ions play an important role in the charge-transfer kinetics at the electrode/electrolyte interfaces. Because of the lack of suitable measurement techniques, little is known about how Δμ̅ affects the redox reactions occurring at the solid/liquid interfaces during LIB operation. Herein, we outline the relations between different potentials and show how ambient pressure photoelectron spectroscopy (APPES) can be used to follow changes in Δμ̅e over the solid/liquid interfaces operando by measuring the kinetic energy (KE) shifts of the electrolyte core levels. The KE shift versus applied voltage shows a linear dependence of ∼1 eV/V during charging of the electrical double layer and during solid electrolyte interphase formation. This agrees with the expected results for an ideally polarizable interface. During lithiation, the slope changes drastically. We propose a model to explain this based on charge transfer over the solid/liquid interface.

Verlagsausgabe §
DOI: 10.5445/IR/1000137342
Veröffentlicht am 16.12.2021
DOI: 10.1021/acsami.1c07424
Zitationen: 4
Web of Science
Zitationen: 4
Zitationen: 4
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Angewandte Materialien – Energiespeichersysteme (IAM-ESS)
Publikationstyp Zeitschriftenaufsatz
Publikationsmonat/-jahr 07.2021
Sprache Englisch
Identifikator ISSN: 1944-8244, 1944-8252
KITopen-ID: 1000137342
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in ACS applied materials & interfaces
Verlag American Chemical Society (ACS)
Band 13
Heft 28
Seiten 32989–32996
Vorab online veröffentlicht am 12.07.2021
Schlagwörter electrical double layer ambient pressure photoelectron spectroscopy operando spectroscopy electrochemical potentials lithium-ion batteries
Nachgewiesen in Dimensions
Web of Science
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