Thesis defense of Simon Ahlmann

The current global interest in energy storage has triggered the development of new composite materials and, consequently, new methodologies for manufacturing and testing these products.  In the energy storage research field their mechanical behavior is less investigated, despite of their high both fundamental and technological relevance. To assess the interplay between charge and mass transport, this thesis focusses on a large variety of electrolytes using shear rheology and dielectric spectroscopy as examination methods. Tailoring the mechanical behavior of these materials, this work investigates the impact of their local and macroscopic viscoelasticity on their conductivity, with the ultimate goal of finding new recipes for improving the latter. Our investigations from a series of mixtures with an ionic liquidand a dipolar one shows an unusual shifting in the coupling between the mechanical and conductvity processes. A survey of ionogels demonstrate that the interaction of charge carriers with their gel-like matrix can affect conductivity even in the presence of a strong dynamical disparity between its macroscopic mechanical and electrical parameters. Finally, comparing ionic and proton conductors, it is shown that this decoupling significantly enhances the conductivity in acid hydrates. Our results and their analysis show that enhancing the degree of decoupling between the mechanical and electrical degrees of freedom, combined with a reduction of charge correlations in highly concentrated electrolytes are essential for the development of the next generation of energy storage materials.

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