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New epoxy-amine networks issue from epoxydized imidazolium ionic liquid monomers (ILMs) and isophorone diamine (IPD) were modified for the first time by incorporating unmodified trisilanol phenyl POSS® (POSS®Ph-triol) and two ionic liquid-modified POSS®Ph (IL-g-POSS®Ph) having chloride (Cl−) and bis-trifluoromethanesulfonimidate (NTf2−) counter anions. Then, 5 wt.% of unmodified and IL-modified POSS®Ph were introduced in order to develop new solid electrolytes. First, a homogeneous dispersion of the POSS®Ph aggregates (diameters from 80 to 400 nm) into epoxy networks was observed. As a consequence, ILM/IPD networks with glass transition temperatures between 45 and 71 °C combined with an enhancement of the thermal stability (&gt;380 °C) were prepared. Moreover, a significant increase of the hydrophobic character and high oil repellency of the network surfaces were obtained by using IL-g-POSS®Ph (19–20 mJ.m−2), opening up promising prospects for surface coating applications. Finally, these new epoxy networks exhibited outstanding high ionic conductivities (from 3.4 × 10−8 to 6.8 × 10−2 S.m−1) combined with an increase in permitivity.

New Epoxy Thermosets Organic-Inorganic Hybrid Nanomaterials Derived from Imidazolium Ionic Liquid Monomers and POSS®Ph