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Hybri'lytes PEO
Sol-gel derived bi-functionalized nano-porous hybrid silica-PEO single-ion conducting solid electrolyte
Abstract
We report the development of a novel composite solid-state electrolyte (SSE) that consists of a nanoporous silica backbone, bifunctionalized with 2-[(Trifluoromethanesulfonylimido)-N-4-sulfonylphenyl] ethyl (TFSISPE) anion and 2-[Methoxy(polyethyleneoxy)6-9propyl] trimethoxysilane (oligo-PEG). The backbone is synthesized through a sol-gel route based on tetraethyl-orthosilicate (TEOS), which produces a low-density nanoporous structure. The functionalization process occurs in an optimally timed and phased manner, facilitating the condensation reaction between pre-hydrolyzed TFSISPE anion, oligo-PEG, and partially gelled silica backbone. This improves anion loading without disrupting backbone gelation. Finally, the solvent in the nanopores is replaced with low-molecular-weight Polyethylene oxide (PEO, Mw = 600 g mol^(–1)). Grafting the oligo-PEG onto the backbone greatly enhances ionic conductivity. For a one molar Li+ concentration, the material with oligo-PEG exhibits an unprecedented ionic conductivity of 5.2×10^(–4) S cm^(–1) at 20°C. We attribute the conductivity improvement to the reduction of osmotic drag resulting from the entanglement between oligo-PEG and PEO. Additionally, a high lithium-ion transference number (t+ ∼ 0.91) is achieved by anchoring the TFSISPE anion to the backbone. Compared to common polymer matrix composite SSE, this single-ion conducting hybrid SSE exhibits about an order of magnitude higher ionic conductivity, near unity transference number, and a higher thermal stability window of up to 110°C.
Hybri'lytes PEO Collaborators
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