Continuum Modelling As Tool for Optimizing the Cell Design of Magnesium Batteries

Magnesium-based next-generation batteries are of great interest since magnesium is not only very abundant, which allows economic and sustainable applications, but also less prone to dendrite formation than many other metals. Together with the bivalency cations resulting possibility safely use a metal anode enables high specific capacities. However, for successful commercialization there still some challenges overcome. The charge density bivalent cation causes strong coulomb interactions anions solvent molecules. Therefore, salts form ion pairs bigger clusters – especially at concentrations, may adversely affect transport in electrolyte electrochemical reaction electrode. [1] Moreover, energetic barriers desolvation solid-state diffusion double-charged usually high, can have crucial impact on battery performance. Former significantly hinder electron-transfer reaction, [2] whereas latter makes choice suitable cathode materials challenging. Consequently, good understanding limiting processes rechargeable key develop novel high-capacity / high-voltage materials. For instance, it well-known that morphology an intercalation material strongly influence performance smaller particles as well thinner electrodes common strategies avoiding adverse effects limitations. mass loadings separators essential bottlenecks magnesium-ion batteries. Up date Chevrel phase (CP) Mo 6 S 8 considered benchmark Mg[B(hfip) 4 ] 2 DME seen most promising chloride-free electrolyte. [3,4] In our contribution we carefully study this model system get better how overcome undesired present newly-developed continuum model, able describe complex process into CP cathode. considers different thermodynamics kinetics two sites their interplay reactions possible agglomeration. parameterization validation based DFT calculations experimental data. Different kind (transport) limitations studied detail. All all, combination modelling techniques measurements provides important insights operation optimization cell design. Acknowledgements This project has received funding from European Union's Horizon 2020 research innovation programme under grant agreement No 824066 (E-MAGIC). Furthermore, work contributes performed CELEST (Center Electrochemical Energy Storage Ulm-Karlsruhe) was funded by German Research Foundation (DFG) Project ID 390874152 (POLiS Cluster Excellence). simulations were carried out JUSTUS cluster supported state Baden-Württemberg through bwHPC INST 40/575-1 FUGG. References Drews, T. Danner, P. Jankowski et al., ChemSusChem , 3 (2020), 3599-3604. Jankowski, J. Häcker 14 (2021), 4820-4835. Aurbach, Z. Lu, A. Schlechter Nature 407 (2000), 724-727. Zhao-Karger, R. Liu, W. Dai ACS Lett. (2018), 2005-2013.