Electrolyte Design Chart Reframed by Intermolecular Interactions for High-Performance Li-Ion Batteries.

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• Advanced electrolytes are crucial for improving battery performance.
• Current electrolyte design criteria lack clarity, hindering progress.

Purpose of the Study:

• To develop a novel electrolyte design chart based on intermolecular interactions.
• To establish correlations between electrolyte components and electrochemical reversibility.
• To enable prediction and rapid screening of electrolytes.

Main Methods:

• Systematic nuclear magnetic resonance (NMR) and Fourier transform infrared (FTIR) spectroscopy.
• Molecular dynamics (MD) simulations.
• Machine learning (ML)-assisted classifications.

Main Results:

• Established semiquantitative correlations between electrolyte components and electrochemical reversibility.
• Proposed the concept of equivalent increment of lithium salt based on intermolecular interactions.
• Demonstrated highly reversible and nonflammable phosphate-based electrolytes for graphite||NCM811 full cells.

Conclusions:

• The proposed electrolyte design chart, guided by intermolecular interactions, offers a foundation for future electrolyte development.
• This approach enables rapid screening and prediction of electrolytes using machine learning.
• Developed advanced, safer electrolytes for high-performance batteries.