Harnessing Li-Ion Binding Energy for Solvation-Guided Electrolyte Additive Design and Robust Solid Electrolyte...

Area of Science:

• Materials Science
• Electrochemistry
• Battery Technology

Background:

• Stabilizing the electrode-electrolyte interface is crucial for improving lithium-ion battery (LIB) performance.
• Understanding the link between additive molecular structure and interface enrichment is limited.

Purpose of the Study:

• To propose and validate a solvation-guided strategy for designing electrolyte additives.
• To establish Li-ion binding energy as a key factor for solid electrolyte interphase (SEI) reinforcement.

Main Methods:

• Utilized a σ-bonding-insulation-based model system with allyl methyl sulfone (AMS), allyl methyl carbonate (AMC), and allyl methyl ether (AME) additives.
• Employed computational simulations and spectroscopic analyses to study additive behavior.

Main Results:

• AMS, with the highest Li-ion binding energy, preferentially solvated Li-ions.
• This affinity promoted spontaneous additive migration to the negative electrode, forming a robust SEI layer.
• Demonstrated a correlation between Li-ion binding affinity and SEI reinforcement.

Conclusions:

• Additive-electrolyte interactions are critical for effective interface engineering in LIBs.
• Solvation-guided design offers a systematic approach for developing high-performance electrolyte additives.
• The study provides a framework for optimizing SEI formation through tailored additive selection.