First principles-based methods for chemical mechanisms in advanced batteries and energy storage materials

Abstract

Advances in theor. chem. and supercomputers are making it practical to consider first principles (de novo) predictions of new materials for batteries and energy storage. Our approach is to start with accurate quantum mechanics on which we build a hierarchy of models each based on the results of more fundamental methods but coarsened to make practical the consideration of much larger length and time scales. The connection this multi-paradigm multi-scale hierarchy back to quantum mechanics enables the application of first principles to the coarse levels essential for practical simulations of complex systems. We will highlight some recent advances in methodol. such as: PBE-lg and XYGJ-OS quantum mechanics methods for accurate intermol. interactions. The 2PT method for fast accurate calcns. of entropy from mol. dynamics of large (50,000 atom) systems. The ReaxFF reactive force field for predicting of reactive processes in large (millions of atoms) complex systems. The eFF method for electron dynamics of (millions of electrons) highly excited complex systems which we will illustrate with recent applications selected from: Electrochem. H2O oxidn. to form H2 and O2. Photosynthetic H2O oxidn. to form H2 and O2 CO2 redn. to form orgs. Li air batteries Org. cathodes for Li batteries. [Figure] Mechanism of catalysis at fuel cell anodes and cathodes.