Dissecting the Solid Polymer Electrolyte-Electrode Interface in the Vicinity of Electrochemical Stability Limits.
ACS Appl Mater Interfaces
; 14(25): 28716-28728, 2022 Jun 29.
Article
em En
| MEDLINE
| ID: mdl-35708265
ABSTRACT
Proper understanding of solid polymer electrolyte-electrode interfacial layer formation and its implications on cell performance is a vital step toward realizing practical solid-state lithium-ion batteries. At the same time, probing these solid-solid interfaces is extremely challenging as they are buried within the electrochemical system, thereby efficiently evading exposure to surface-sensitive spectroscopic methods. Still, the probing of interfacial degradation layers is essential to render an accurate picture of the behavior of these materials in the vicinity of their electrochemical stability limits and to complement the incomplete picture gained from electrochemical assessments. In this work, we address this issue in conjunction with presenting a thorough evaluation of the electrochemical stability window of the solid polymer electrolyte poly(ε-caprolactone)lithium bis(trifluoromethanesulfonyl)imide (PCLLiTFSI). According to staircase voltammetry, the electrochemical stability window of the polyester-based electrolyte was found to span from 1.5 to 4 V vs Li+/Li. Subsequent decomposition of PCLLiTFSI outside of the stability window led to a buildup of carbonaceous, lithium oxide and salt-derived species at the electrode-electrolyte interface, identified using postmortem spectroscopic analysis. These species formed highly resistive interphase layers, acting as major bottlenecks in the SPE system. Resistance and thickness values of these layers at different potentials were then estimated based on the impedance response between a lithium iron phosphate reference electrode and carbon-coated working electrodes. Importantly, it is only through the combination of electrochemistry and photoelectron spectroscopy that the full extent of the electrochemical performance at the limits of electrochemical stability can be reliably and accurately determined.
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Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
ACS Appl Mater Interfaces
Assunto da revista:
BIOTECNOLOGIA
/
ENGENHARIA BIOMEDICA
Ano de publicação:
2022
Tipo de documento:
Article
País de afiliação:
Suécia