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. 2020 Feb 3;5(6):2931-2938.
doi: 10.1021/acsomega.9b03773. eCollection 2020 Feb 18.

Macrophase-Separated Organic Ionic Plastic Crystals/PAMPS-Based Ionomer Electrolyte: A New Design Perspective for Flexible and Highly Conductive Solid-State Electrolytes

Nicolas Goujon  1   2 , Robert Kerr  1 , Charlotte Gervillié  1 , Yogita V Oza  1 , Luke A O'Dell  1 , Patrick C Howlett  1 , Maria Forsyth  1   2
Affiliations

Macrophase-Separated Organic Ionic Plastic Crystals/PAMPS-Based Ionomer Electrolyte: A New Design Perspective for Flexible and Highly Conductive Solid-State Electrolytes

Nicolas Goujon et al. ACS Omega. .

Abstract

A material design approach was taken for the preparation of an organic ionic plastic crystal (OIPC)-polymer electrolyte material that exhibited both good mechanical and transport properties. Previous attempts to form this type of electrolyte material resulted in the solvation of the OIPC by the ionomer and loss of the plastic crystal component. Here, we prepared, in situ, a macrophase-separated OIPC-polymer electrolyte system by adding lithium bis(fluorosulfonyl)imide (LiFSI) to a (PAMPS-N1222) ionomer. It was found that an optimal compositional window of 40-50 mol % LiFSI exists whereby the electrolyte conductivity suddenly increased 4 orders of magnitude while exhibiting elastic and flexible mechanical properties. The phase behavior and transport properties were studied using differential scanning calorimetry and 7Li and 19F solid-state nuclear magnetic resonance spectroscopy. This is the first example of a fabrication principle that lends itself to a wide range of promising OIPC and ionomeric materials. Subsequent studies are required to characterize and understand the morphology and conductive nature of these systems and their application as electrolyte materials.

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Figure 1
Figure 1
Chemical structure of the N1222-PAMPS ionomer (a) and the LIFSI salt (b).
Figure 2
Figure 2
(a) DSC traces (vertical bars are a scale for the Y-axis) and (b) room temperature XRD patterns of N1222-PAMPS:LiFSI mixtures as a function of LiFSI molar fraction.
Figure 3
Figure 3
Temperature-dependent ionic conductivity of N1222-PAMPS:LiFSI mixtures as a function of LiFSI molar fraction. Solid lines are fitted functions based on Arrhenius equation.
Figure 4
Figure 4
(a) 7Li and (b) 19F static solid-state NMR line widths at 7.05 T as a function of temperature for the N1222-PAMPS:LiFSI mixtures. The dashed lines are fitted functions based on BPP theory (see the Experimental Section for details).
Figure 5
Figure 5
(a) 7Li and (b)19F correlation time as a function of temperature for the N1222-PAMPS:LiFSI mixtures.
See this image and copyright information in PMC

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