First-principles study of alkali-metal intercalation in disordered carbon anode materials

Abstract

The intercalation of alkali metals in disordered carbon anode materials is studied by a combination of first-principles and machine-learning methods. Graphite and non-graphitising (“hard”) carbons are important anode materials for battery technologies. The electrochemical intercalation of alkali metals in graphite has been widely studied by first-principles density-functional theory (DFT). However, similar investigations of disordered “hard” and nanoporous carbons have been challenging due to the structural complexity involved. Here, we combine DFT with machine-learning (ML) methods to study the intercalation of alkali metal (Li, Na, K) atoms in model carbon systems over a range of densities and degrees of disorder. We use a stochastic approach to compute voltage–filling profiles, studying the three metal species side-by-side, and we analyse the ionic charges of metal atoms as a function of filling. Our study provides atomic-scale insight into the intercalation of all three alkali metals that are relevant to batteries, and it thereby makes a key step towards the DFT/ML-driven modelling of energy materials.