We present a set of precise single-ion conducting ionomers that demonstrate decoupled transport of metal cations within self-assembled percolated aggregates in glassy polymer matrices. These precise ionomers consist of a polyethylene backbone with a sulfonated phenyl group pendant on every 5th carbon, that is fully neutralized by a counterion X (Li+, Na+, or Cs+), p5PhSA-X. The morphologies of these ionomers are characterized with X-ray scattering, and the ion transport properties are characterized with electrical impedance spectroscopy. Both experiments are performed under vacuum, from room temperature up to 180°C. Atomistic molecular dynamics simulations elucidate that the structure of the aggregates in the ionomers is a percolated network. The characteristic length scales of these percolated aggregates as measured by X-ray scattering are ~2nm and independent of ion type. There is good agreement between simulations and experimental X-ray scattering data. The ionomers exhibit conductivity of 10-7 to 10-6 S/cm at 180°C and demonstrate Arrhenius behavior up to 180°C. This indicates that the ion transport is decoupled from the polymer backbone, which is consistent with a percolated aggregate within which ions travel.

Percolated ionic aggregates in precise sulfophenylated polyethylene ionomers: Morphology and ion transport

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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