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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 LU ; Edström, Kristina ; Rensmo, Håkan ; Nyholm, Leif ; Maibach, Julia and Hahlin, Maria (2021) In ACS Applied Materials and Interfaces 13(28). p.32989-32996
Abstract

The electrochemical potential difference (Δμ¯) 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), Δμ¯ 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 Δμ¯ 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 Δμ¯ e over the solid/liquid interfaces operando by measuring the kinetic energy (KE)... (More)

The electrochemical potential difference (Δμ¯) 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), Δμ¯ 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 Δμ¯ 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 Δμ¯ e 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.

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author
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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
ambient pressure photoelectron spectroscopy, electrical double layer, electrochemical potentials, electrochemical reactions, electrode/electrolyte interface, lithium-ion batteries, operando spectroscopy
in
ACS Applied Materials and Interfaces
volume
13
issue
28
pages
8 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • pmid:34251812
  • scopus:85111222696
ISSN
1944-8244
DOI
10.1021/acsami.1c07424
language
English
LU publication?
yes
id
74b534c0-e2e2-47e1-9d54-c7f4511d69e3
date added to LUP
2021-12-27 13:20:33
date last changed
2024-04-20 18:21:04
@article{74b534c0-e2e2-47e1-9d54-c7f4511d69e3,
  abstract     = {{<p>The electrochemical potential difference (Δμ¯) 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), Δμ¯ 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 Δμ¯ 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 Δμ¯ e 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. </p>}},
  author       = {{Källquist, Ida and Lindgren, Fredrik and Lee, Ming Tao and Shavorskiy, Andrey and Edström, Kristina and Rensmo, Håkan and Nyholm, Leif and Maibach, Julia and Hahlin, Maria}},
  issn         = {{1944-8244}},
  keywords     = {{ambient pressure photoelectron spectroscopy; electrical double layer; electrochemical potentials; electrochemical reactions; electrode/electrolyte interface; lithium-ion batteries; operando spectroscopy}},
  language     = {{eng}},
  number       = {{28}},
  pages        = {{32989--32996}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Applied Materials and Interfaces}},
  title        = {{Probing Electrochemical Potential Differences over the Solid/Liquid Interface in Li-Ion Battery Model Systems}},
  url          = {{http://dx.doi.org/10.1021/acsami.1c07424}},
  doi          = {{10.1021/acsami.1c07424}},
  volume       = {{13}},
  year         = {{2021}},
}