3ε-A Versatile Operando Analytics Toolbox in Energy Storage
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Updated: Oct 9, 2025

Rapid in-silico Battery Electrolyte Electrochemical Reaction Generation using 3T-VASP Multi-Scale Energy Minimization
Published on: August 22, 2025
Sobana P Rangarajan1, Susmita Sarkar1, Yevgen Barsukov2
1School of Mechanical Engineering, Purdue University, West Lafayette, Indiana 47907, United States.
Abstract:
The performance and safety of lithium-ion batteries are plagued by several diverse, nonlinear aging mechanisms influenced by the electrochemical thermal interactions at the electrodes, usage history, and operating conditions. Understanding and deconvoluting the fundamental reaction mechanisms responsible for electrode degradation are key for developing technologies in Li-ion battery diagnostics and prognostics. Hence, there exists a need for high-precision operando techniques to investigate and characterize distinct electrode degradation modes over a gamut of operational variability. Cells embedded with a stable, nonpolarizable reference electrode offer an in situ and operando tool to decouple the complex electrochemical interplay between the electrode pair by measuring individual electrode responses simultaneously with the cell response in the time and frequency domains. This perspective comprehensively looks at 3-electrode (3ε) analytics as a versatile toolbox, highlighting recent techniques and parameters developed with an emphasis on degradation diagnostics and control strategies that is expected to drive the futuristic design of battery management systems.
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