Non-solvating, side-chain polymer electrolytes with more dissociable pendent anion chemistries exhibit a dielectric relaxation dominated lithium ion transport mechanism.
The development of
advanced electrolytes compatible with lithium
metal and lithium-ion batteries is crucial for meeting ever growing
energy storage demands. One such class of materials, single-ion conducting
polymer electrolytes (SIPEs), prevents the formation of ion concentration
gradients and buildup of anions at the electrode surface, improving
performance. One of the ongoing challenges for SIPEs is the development
of materials that are conductive enough to compete with liquid electrolytes.
Presented herein is a class of gel SIPEs based on crosslinked poly(tetrahydrofuran)
diacrylate that present enhanced room temperature conductivities of
3.5 × 10–5 S/cm when gelled with lithium metal
relevant 1,3-dioxolane/dimethoxyethane, 2.5 × 10–4 S/cm with carbonate solutions, and approaching 10–3 S/cm with dimethyl sulfoxide. Remarkably, these materials also demonstrate
high ionic conductivity at low temperatures, 1.8 × 10–5 S/cm at −20 °C in certain solvents. Most importantly,
however, when contrasted with identical SIPEs formulated with poly(ethylene
glycol) diacrylate, the mechanisms responsible for the enhanced conductivity
are elucidated: decreasing Li+–polymer interactions
and gel solvent–polymer interactions leads to an increase in
Li+ mobility. These findings are generalizable to various
SIPE chemistries and can therefore be seen as an additional set of
design parameters for developing future high conductivity SIPEs.
Batteries based on alternatives to lithium are now of global research interest. Magnesium metal batteries are particularly attractive for their potential high energy density. Polymer electrolytes for high density rechargeable batteries have been sought for decades, due to their improved thermal stability compared with liquids and their lower density and cost compared with inorganic solids. Yet, little success has so far been realized in polymer electrolytes for magnesium metal batteries. In this review, the magnesium polymer electrolyte literature is comprehensively explored. Differences between requirements for lithium polymer and magnesium polymer batteries are discussed as well as the consequences on necessary considerations for impactful magnesium polymer electrolyte research.
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