Molecular Dynamics Study of Dendrite Formation in Lithium-Metal Anodes

In recent years, the relentless growth in global electricity demand, reaching 29,471 TWh in 2023, has underscored the urgent need for advanced energy storage technologies. This thesis addresses key challenges in developing next-generation high-energy rechargeable batteries with a focus on lithium-based anodes. Chapter I provides a concise review of state-of-the-art battery chemistry, highlighting the superior specific energy and efficiency of Li-ion systems and the imperative to push beyond current limits for electric vehicles and portable electronics. Chapters II and III employ classical molecular dynamics simulations to elucidate the fundamental mechanisms of lithium dendrite nucleation and growth on both silicon-based and pure lithium metal anodes. In Chapter II, we demonstrate how cracks in the solid electrolyte interphase (SEI) catalyze dendritic deposition under varying temperatures and C-rates, emphasizing the critical role of SEI integrity. Chapter III extends this analysis to ionic-liquid electrolytes, showing that a pristine LiF SEI coating in a Pyr14-TFSI/LiTFSI medium significantly mitigates dendrite formation, especially at moderate charging currents. Building on these atomistic insights, Chapter IV investigates SEI formation in lithium-metal anodes using an EMIM-TFSI electrolyte with partial TFSI>BF4 substitution and EC additives, revealing how electrolyte composition and open-circuit conditions govern interphase stability. Finally, Chapter V introduces a reactive machine-learning force field for Li-F and Li-F-B systems, trained with the FitSNAP framework, which achieves near-ab initio accuracy at classical-MD cost and paves the way for large-scale simulations of emerging boron-based anodes. Together, these studies advance our understanding of interfacial phenomena in lithium batteries and propose molecular-level strategies for designing safer, higher-capacity anodes, thereby charting a path toward the Battery 500 goal of 500 Wh/kg energy density.

Name thesis:degree_name

Master of Science

Level thesis:degree_level

Masters

Discipline thesis:degree_discipline

Electrical Engineering

Grantor

Texas A&M University

Year dc:date.issued

2025

Author dc:creator

• Selis Vasquez, Luis Antonio 1995-

Advisor dc:contributor.advisor

• Seminario, Jorge

Committee members dc:contributor.committeemember

• Zou, Jun
• Silva-Martinez, Jose
• Balbuena, Perla

• Engineering, Electronics and Electrical

Language dc:language.iso

English

Handle dc:identifier.uri

https://hdl.handle.net/1969.1/1599917

OAI record oai:identifier

https://oaktrust.library.tamu.edu/server/oai/request?verb=GetRecord&metadataPrefix=dim&identifier=oai%3Aoaktrust.library.tamu.edu%3A1969.1%2F1599917