Gel
polymer electrolytes (GPEs) based on polyacrylonitrile elastomer
(HNBR) are investigated for lithium-ion batteries application. This
study examines the acrylonitrile content, as well as the solvent used
to make the GPE, to understand their impact on lithium solvation.
To do so, we propose a three-component system comprising HNBR:solvent:LiTFSI
to pinpoint the correct ratio to provide the GPE with competitive
conductivity. Infrared spectroscopy is used to shed light on the interactions
between nitriles and lithium ions. Spin–lattice relaxation
times (T
1) and diffusion coefficients
of 7Li and 19F for various HNBR-based GPEs are
obtained through PFG-NMR, enabling determination of the transport
number of lithium cations (t
+) and activation
energy (E
a). Among the GPEs tested, those
composed of propylene carbonate with 2 M LiTFSI and HNBR with an acrylonitrile
content of 50% are the most promising, with an ionic conductivity
of 2.1 × 10–3 S/cm, D
7Li of 12.0 × 10–8 cm/s,
and a t
+ of 0.42 at room temperature.
When this GPE was tested in Li5Ti4O12/LiFePO4 coin cells, a capacity of 135 mAh/g was obtained
at a discharge rate of D/5, showing promising results
for its use in Li-ion batteries. This study highlights the benefits
of high acrylonitrile content in the polymer and a solvent with a
moderate donor number to promote interactions between nitriles and
Li+.