Ion Transport and Mechanical Properties of Non-Crystallizable Molecular Ionic Composite Electrolytes

Bostwick, Joshua E.; Zanelotti, Curt J.; Iacob, Ciprian; Korovich, Andrew G.; Madsen, Louis A.; Colby, Ralph H.

doi:10.1021/acs.macromol.9b02125

Ion Transport and Mechanical Properties of Non-Crystallizable Molecular Ionic Composite Electrolytes

Journal Article · Thu Feb 13 00:00:00 EST 2020 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.9b02125· OSTI ID:2006856

^[1]; Zanelotti, Curt J. ^[2]; ^[3]; Korovich, Andrew G. ^[2]; ^[2]; ^[4]

Pennsylvania State University, University Park, PA (United States); Virginia Tech
Virginia Polytechnic Institute and State University (Virginia Tech), Blacksburg, VA (United States)
National Research and Development Institute for Cryogenic and Isotopic Technologies, Valcea (Romania); Karlsruhe Institute of Technology (KIT) (Germany)
Pennsylvania State University, University Park, PA (United States)

Polymer electrolytes show promise as alternatives to conventional electrolytes in energy storage and conversion devices but have been limited due to their inverse correlation between ionic conductivity and modulus. In this study, we examine surface morphology, linear viscoelastic, dielectric and diffusive properties of molecular ionic composites (MICs), materials produced through the combination of a rigid and charged double helical polymer, known as poly(2,2’)-disulfonyl-4,4’benzidine terepthalamide (PBDT), with ionic liquids (ILs). To probe temperature extremes, we incorporate a non-crystallizable IL to allow measurements from to -90 to 200°C. As we increase PBDT weight percentage (wt%), shear moduli increase and do not decay up to 200°C while maintaining room temperature ionic conductivity within a factor of two of the neat IL. We connect diffusion coefficients of IL ions with ionic conductivity through the Haven ratio across a wide temperature range and analyze trends in ion transport based on a relatively high and composition-dependent static dielectric constant. This behavior may result from collective rearrangement of IL ions in these networks. We propose that these properties are driven by a two-phase system in MICs corresponding to IL-rich “puddles” and PBDT-IL associated “bundles” where IL ions form alternating sheaths of cations and anions around each PBDT rod. Furthermore, these polymer-based MIC electrolytes show great promise for use in electrochemical devices that require fast ion transport, high modulus, and a broad thermal window.

View Accepted Manuscript (DOE)

Research Organization:: Virginia Polytechnic Institute and State University (Virginia Tech), Blacksburg, VA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO). Batteries for Advanced Transportation Technologies (BATT) Program

Grant/Contract Number:: EE0008860

OSTI ID:: 2006856

Journal Information:: Macromolecules, Journal Name: Macromolecules Journal Issue: 4 Vol. 53; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Diffusion
Ionic conductivity
Ions
Salts
Solvents

Ion Transport and Mechanical Properties of Non-Crystallizable Molecular Ionic Composite Electrolytes

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