Revisiting the domain model for lithium intercalated graphite

TL;DR

This study evaluates the stability of the domain model for lithium intercalated graphite using computational methods, confirming its thermodynamic and kinetic stability and linking domain structures to observed diffusivity variations.

Contribution

It provides a comprehensive analysis of the domain model's stability in stages III and II, supported by DFT and Monte Carlo simulations, and correlates domain structures with experimental diffusivity data.

Findings

Domain model is thermodynamically stable in stages III and II.

Domain structures are supported by high-resolution microscopy observations.

Diffusivity varies widely due to domain staging sequences.

Abstract

In this letter, we study the stability of the domain model for lithium intercalated graphite in stages III and II by means of Density Functional Theory and Kinetic Lattice Monte Carlo simulations. We find that the domain model is either thermodynamically or kinetically stable when compared to the standard model in stages III and II. The existence of domains in the intercalation sequence is well supported by recent high resolution transmission electron microscope observations in lithiated graphite. Moreover, we predict that such domain staging sequences leads to a wide range of diffusivity as reported in experiments.