Effect of Electronic Exchange-Correlation Interaction in the Physics of Ion Insertion in Organic Salts

Abstract: The intense increase in energy consumption around the world has prompted a great deal of research on alternative and sustainable energy storage systems such as organic batteries. The fundamental understanding of the physics of organic salts and the ion insertion mechanism plays a key role in the development of electrode materials used in such sustainable batteries. The system studied in this project is of Lithium (2,5-dilithium-oxy)-terephthalate where a previous project studied this system from a different angle.  The electronic structure generation of the system is based on Density Functional Theory (DFT) along with an evolutionary algorithm to find the structures with minimum energy. The effects of varying the description of the exchange-correlation interaction were studied while introducing lithium ions to the system. This was done while also monitoring the repercussions of crystal structure optimization on the voltages, charge redistribution, and bonds of the system. The geometrical optimization of the hybrid functional resulted in the potential of the 2-electron step between Li2-p-DHT/ Li4-p-DHT of 2.6 V being closer to the experimental value recorded at 2.7 V.