Re-investigating the structure-property relationship of the solid electrolytes Li In Zr Cl and the impact of In-Zr(iv) substitution.

Chloride-based solid electrolytes are considered interesting candidates for catholytes in all-solid-state batteries due to their high electrochemical stability, which allows the use of high-voltage cathodes without protective coatings. Aliovalent Zr(iv) substitution is a widely applicable strategy to increase the ionic conductivity of LiM(iii)Cl solid electrolytes. In this study, we investigate how Zr(iv) substitution affects the structure and ion conduction in Li In Zr Cl (0 ≤ ≤ 0.

Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor LiYBr Cl.

LiYX (X = Cl, Br) materials are Li-ion conductors that can be used as solid electrolytes in all solid-state batteries. Solid electrolytes ideally have high ionic conductivity and (electro)chemical compatibility with the electrodes. It was proven that introducing Br to LiYCl increases ionic conductivity but, according to thermodynamic calculations, should also reduce oxidative stability.

Quantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurements.

A key challenge for solid-state-batteries development is to design electrode-electrolyte interfaces that combine (electro)chemical and mechanical stability with facile Li-ion transport. However, while the solid-electrolyte/electrode interfacial area should be maximized to facilitate the transport of high electrical currents on the one hand, on the other hand, this area should be minimized to reduce the parasitic interfacial reactions and promote the overall cell stability. To improve these aspects simultaneously, we report the use of an interfacial inorganic coating and the study of its impact on the local Li-ion transport over the grain boundaries.

Clarifying the relationship between redox activity and electrochemical stability in solid electrolytes.

All-solid-state Li-ion batteries promise safer electrochemical energy storage with larger volumetric and gravimetric energy densities. A major concern is the limited electrochemical stability of solid electrolytes and related detrimental electrochemical reactions, especially because of our restricted understanding. Here we demonstrate for the argyrodite-, garnet- and NASICON-type solid electrolytes that the favourable decomposition pathway is indirect rather than direct, via (de)lithiated states of the solid electrolyte, into the thermodynamically stable decomposition products.

Analysis of Diffusion in Solid-State Electrolytes through MD Simulations, Improvement of the Li-Ion Conductivity in β-LiPS as an Example.

Molecular dynamics simulations are a powerful tool to study diffusion processes in battery electrolyte and electrode materials. From molecular dynamics simulations, many properties relevant to diffusion can be obtained, including the diffusion path, amplitude of vibrations, jump rates, radial distribution functions, and collective diffusion processes. Here it is shown how the activation energies of different jumps and the attempt frequency can be obtained from a single molecular dynamics simulation.