Polymer gel electrolytes (PGE) have seen a renewed interest in their development because they have high ionic conductivities but low electrochemical degradation and flammability. PGEs are formed by mixing a liquid lithium-ion electrolyte with a polymer at a sufficiently large concentration to form a gel. PGEs have been extensively studied, but the direct connection between their microscopic structure and macroscopic properties remains controversial. For example, it is still unknown whether the polymer in the PGE acts as an inert, stabilizing scaffold for the electrolyte or it interacts with the ionic components. Here, a PGE composed of a prototypical lithium-carbonate electrolyte and polyacrylonitrile (PAN) is pursued at both microscopic and macroscopic levels. Specifically, this study focused on describing the microscopic and macroscopic changes in the PGE at different polymer concentrations. The results indicated that the polymer-ion and polymer–polymer interactions are strongly dependent on the concentration of the polymer and the lithium salt. In particular, the polymer interacts with itself at very high PAN concentrations (10% weight) resulting in a viscous gel. However, the conductivity and dynamics of the electrolyte liquid components are significantly less affected by the addition of the polymer. The observations are explained in terms of the PGE structure, which transitions from a polymer solution to a gel, containing a polymer matrix and disperse electrolyte, at low and high PAN concentrations, respectively. The results highlight the critical role that the polymer concentration plays in determining both the macroscopic properties of the system and the molecular structure of the PGE.
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14 April 2023
Research Article|
April 13 2023
Relation between microscopic structure and macroscopic properties in polyacrylonitrile-based lithium-ion polymer gel electrolytes
Special Collection:
Celebrating 25 Years of Two-dimensional Infrared (2D IR) Spectroscopy
Jeramie C. Rushing
;
Jeramie C. Rushing
(Data curation, Formal analysis, Investigation, Methodology, Validation, Writing – original draft)
Department of Chemistry, Louisiana State University
, Baton Rouge, Louisiana 70803, USA
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Anit Gurung
;
Anit Gurung
(Investigation, Methodology, Validation, Writing – review & editing)
Department of Chemistry, Louisiana State University
, Baton Rouge, Louisiana 70803, USA
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Daniel G. Kuroda
Daniel G. Kuroda
a)
(Conceptualization, Investigation, Methodology, Project administration, Supervision, Validation, Writing – original draft)
Department of Chemistry, Louisiana State University
, Baton Rouge, Louisiana 70803, USA
a)Author to whom correspondence should be addressed: dkuroda@lsu.edu
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a)Author to whom correspondence should be addressed: dkuroda@lsu.edu
Note: This paper is part of the JCP Special Topic on Celebrating 25 Years of Two-dimensional Infrared (2D IR) Spectroscopy.
J. Chem. Phys. 158, 144705 (2023)
Article history
Received:
November 21 2022
Accepted:
March 23 2023
Citation
Jeramie C. Rushing, Anit Gurung, Daniel G. Kuroda; Relation between microscopic structure and macroscopic properties in polyacrylonitrile-based lithium-ion polymer gel electrolytes. J. Chem. Phys. 14 April 2023; 158 (14): 144705. https://doi.org/10.1063/5.0135631
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