Multiscale Modeling of Solid Electrolyte Interphase Formation on Oxygen-Functionalized Graphite Anodes for...

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• The solid electrolyte interphase (SEI) is critical for lithium-ion battery (LIB) performance but its formation is complex.
• Limited understanding of SEI mechanisms hinders rational design of high-performance LIBs.

Purpose of the Study:

• To elucidate the atomistic mechanisms of SEI formation on graphite anodes.
• To investigate the impact of surface functionalization on SEI growth kinetics and properties.

Main Methods:

• Integrated multiscale simulation framework: Density Functional Theory (DFT) and Molecular Dynamics (MD).
• REACTer protocol with topology-mapped reaction templates and physics-informed constraints.
• Simulations on pristine and functionalized (O-, OH-, O/OH-terminated) graphite anodes.

Main Results:

• Identified three-stage SEI growth kinetics (initial, transition, steady-state) on functionalized surfaces.
• OH-terminated surfaces promote thin, dense inorganic/organic composite SEI layers, suppressing component dissolution.
• Optimized SEI exhibits enhanced ionic conductivity and favorable viscosity.

Conclusions:

• Electrode surface functionalization is a viable strategy for controlling SEI formation.
• Fundamental principles for designing advanced battery interfaces are provided.