Paddle-wheel mechanism in doped succinonitrile–glutaronitrile plastic electrolyte: a joint magnetic resonance, dielectric, and viscosimetry study of Li ion translational and molecular reorientational dynamics

Glutaronitrile (GN) doped with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) at concentrations below and above the room-temperature conductivity optimum near 1M of Li salt is investigated using dielectric spectroscopy and shear rheology. The experiments are carried out from ambient down to the glass transition temperature Tg, which increases considerably as LiTFSI is admixed to GN. As the temperature is lowered, the conductivity optimum shifts to lower salt concentrations, while the power-law exponents connecting resistivity and molecular reorientation time remain smallest for the 1M composition. By contrast, the rheologically detected time constants, as well as those obtained using dielectric spectroscopy, increase monotonically with increasing Li salt concentration for all temperatures. It is demonstrated that the shear mechanical measurements are, nevertheless, sensitive to the 1M conductivity optimum, thus elucidating the interplay of the dinitrile matrix with the mobile species. The data for the Li doped GN and other nitrile solvents all follow about the same Walden line, in harmony with their highly conductive character. The composition dependent relation between the ionic and the reorientational dynamics is also elucidated.

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Paddle-wheel mechanism in doped succinonitrile–glutaronitrile plastic electrolyte: a joint magnetic resonance, dielectric, and viscosimetry study of Li ion translational and molecular reorientational dynamics

Abstract: Dielectric and NMR spectroscopy combined with viscosimetry reveal that a paddle-wheel mechanism couples Li-ion motion and reorienting nitrile molecules.

Cited by 3 publications

References 75 publications

Conformation inversion of succinonitrile towards long-life solid-state lithium metal batteries

Conformation inversion of succinonitrile towards long-life solid-state lithium metal batteries

Research progress on interfacial problems and solid-state electrolytes in lithium batteries

Shear rheology senses the electrical room-temperature conductivity optimum in highly Li doped dinitrile electrolytes

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