Rapid in-silico Battery Electrolyte Electrochemical Reaction Generation using 3T-VASP Multi-Scale Energy...

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• Electrolyte degradation in lithium-ion batteries limits operational lifetime due to irreversible electrochemical reactions.
• Identifying electrolyte reaction pathways is challenging due to complex chemical species and byproduct formation (e.g., solid electrolyte interphase).

Purpose of the Study:

• To provide a detailed description of the 3T-VASP code and its workflow for simulating electrolyte electrochemical reaction byproducts.
• To enable researchers to apply the 3T-VASP method to new electrolyte systems for improved battery reliability.

Main Methods:

• Utilized the tiered tensor transform technique combined with Vienna Ab-initio Simulation Package (VASP) software, termed 3T-VASP.
• Developed a workflow for ab-initio simulation of electrolyte degradation byproducts within 100-150 DFT steps.
• Detailed the simulation preparation steps for setting up the 3T-VASP workflow.

Main Results:

• The 3T-VASP method enables practical ab-initio generation of physically meaningful electrolyte electrochemical reaction byproducts.
• The code is publicly available on Github, facilitating broader research application.
• The workflow setup is described for new electrolyte systems.

Conclusions:

• The 3T-VASP method offers an efficient approach to study electrolyte degradation pathways in lithium-ion batteries.
• This computational tool can aid in designing more reliable and longer-lasting batteries.
• Further research can leverage 3T-VASP for diverse electrolyte systems.