Physical gels made
of poly(ethylene oxide) (PEO) and deep eutectic
solvents urea-Li bis(trifluoromethanesulfonyl)imide (TFSI) and ethylene
glycol/LiTFSI, or pyrrolidinium ionic liquid solutions PYR13TFSI-LiTFSI
and PYR14TFSI-LiTFSI, are prepared by a fast, single-step process,
which involves no auxiliary solvents or intermediates and is reproducible
and scalable. The properties of these gels are studied as a function
of the PEO content and its molecular weight and the nature of the
liquid electrolyte. The gels prepared with a low concentration (1–5
wt %) of ultrahigh molecular weight (UHMW) PEO are tough, stretchable
materials which resemble soft elastomers and are also self-healing
and transparent. Their rheology shows the conventional behavior of
physical polymer gels, so that the higher the molecular weight of
PEO, the lower the polymer concentration needed to produce the gel.
However, the ion conductivities and diffusivities of the gels are
striking, in many cases being equal to or significantly higher than
those of pure liquid electrolytes. This ion conductivity enhancement
is the highest for the lowest PEO concentration with the highest molecular
weight. This unprecedented molecular weight dependence of conductivity
and diffusivity is the result of two combined effects: the liquid
electrolyte chemical structure modification as a consequence of the
addition of PEO and the development of elastic networks, where ion
mobility and rheology are uncoupled when the PEO added is of UHMW.