The main goal of this project is to employ computational studies to rationalize the development of calcium based rechargeable batteries. The Ca battery technology is especially attractive due to its potential high energy density and the abundance of Ca in the Earth’s crust. This project has received financial support from the European Union through the European Union’s Horizon 2020 research and innovation programme H2020-FETOPEN-1-2016-2017. The specific goals are:
1. To apply several modeling approaches based on DFT and COSMO-RS to rationalize the development of electrolytes for Ca batteries. This must be performed through a high-throughput screening procedure to evaluate and extract the best candidates.
2. To proceed with a detailed investigation of the proposed electrolytes by also understanding the underlying mechanisms of the reactions on the Ca metal surface.
The initial stage of this project will investigate the solubility of Ca based salts in organic solvents. This task will be performed by employing the framework of DFT to predict the salts Gibbs free energy of fusion together with the COSMO-RS approach to evaluate the solvation energy of the ions in a number of different organic solvents. This procedure will indicate, together with the computation of properties such as viscosity and flash point, attractive electrolyte compositions. The following stage considers the interactions of the electrolyte with the metal Ca anode interface. Ab initio molecular dynamics (AIMD) simulations will be performed to gain deep understanding of the formation of decomposition products and the stability of the anion and solvent molecules on the Ca metal surface. Moreover, important information regarding the kinetics of the electrolyte decomposition on the Ca metal surface can be revealed from analysis of the AIMD trajectories.