POS10-1470
Mechanistic Insights into Boron-Regulated Solvation Structure and Li+ Transport in Lithium Metal Batteries via Molecular Simulations
Topic
S10. AI-assisted Design and Simulation of Polymers
When and Where
Sep 30, 2026
08:30 - 09:30
Room 301 (Grand Ballroom)
Session Chairs
Heesuk KIM
Jinhye BAE
Presenter(s)
Yubhin Cho (Hanyang University)
Co-Author(s)
Abstract
Lithium metal batteries (LMBs) offer high energy density, but their practical use requires electrolytes that balance solvation chemistry, interfacial stability, ionic conductivity, and mechanical robustness. However, conventional gel polymer electrolytes (GPEs) are often limited by mobile anions and strong Li+ solvation, leading to low Li+ transference numbers, sluggish interfacial kinetics, concentration polarization, and Li dendrite growth. To address this, we incorporate a sp2-hybridized boron crosslinker (TMAB) into an EMC/FEC binary solvent system to construct GPE_TMAB, enabling an anion-trapping solvation environment with enhanced Li+ transport and interfacial stability. Molecular simulations were performed to elucidate Li+ solvation structures and transport in GPE_TMAB. The Li+ solvation free energy indicates weakened Li+ coordination and facilitated desolvation. This originates from the boron sites of the TMAB crosslinker trapping TFSI- anions within the polymer network, which suppresses their participation in the Li+ solvation shell, while Li+ coordination is concurrently reorganized with reduced EMC coordination and enhanced FEC coordination. This combined TFSI- immobilization and FEC-enriched coordination forms a less tightly bound solvation environment, promoting Li+ transport. Overall, this study highlights boron-mediated TFSI- trapping as an effective strategy to regulate Li+ solvation and transport, offering molecular-level design principles for anion-immobilized and dendrite-resistant LMB electrolytes.
