Kinetically Corrected Monte Carlo–Molecular Dynamics Simulations of Solid Electrolyte Interphase Growth

We
present a kinetic approach to the Monte Carlo–molecular
dynamics (MC-MD) method for simulating reactive liquids using nonreactive
force fields. A graphical reaction representation allows definition
of reactions of arbitrary complexity, including their local solvation
environment. Reaction probabilities and molecular dynamics (MD) simulation
times are derived from ab initio calculations. Detailed validation
is followed by studying the development of the solid electrolyte interphase
(SEI) in lithium-ion batteries. We reproduce the experimentally observed
two-layered structure on graphite, with an inorganic layer close to
the anode and an outer organic layer. This structure develops via
a near-shore aggregation mechanism.