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Lattice Compatibility and Energy Barriers in Intercalation Compounds

Delin Zhang

Ananya Renuka Balakrishna*

  • *Contact author: ananyarb@ucsb.edu
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PRX Energy 4, 043002 – Published 15 October, 2025

DOI: https://doi.org/10.1103/w6lw-cwbp

Abstract

We present a continuum model for symmetry-breaking phase transformations in intercalation compounds, based on Ericksen’s multiwell energy formulation. The model predicts the nucleation and growth of crystallographic microstructures in Li2Mn2O4—a representative intercalation compound—with twin boundary orientations and volume fractions that closely match experimental observations. Our chemomechanically coupled model not only generates geometrically accurate microstructures through energy minimization, but also reveals a subtle interplay between twinned domains and electrochemomechanical behavior. A key finding is that intercalation compounds satisfying specific compatibility conditions (e.g., λ2=1 or |detU−1|=0) show lower elastic energy barriers, require smaller driving forces, and display narrower voltage hysteresis loops. Furthermore, we show that twinned domains act as conduits for fast Li diffusion. These results establish quantitative design guidelines for intercalation compounds, which focuses on tailoring lattice deformations (rather than suppressing them) and reducing energy barriers to mitigate structural degradation and enhance the electrochemical performance of battery electrodes.

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Popular Summary

Intercalation compounds, commonly used as electrodes in rechargeable batteries and as electrochemical actuators, undergo abrupt lattice distortions when a chemical species (e.g., atom or ion) is inserted into or removed from the host structure. These distortions accelerate structural degradation and impair the electrochemical performance of intercalation compounds. Today, most design strategies aim to eliminate such distortions entirely--a criterion referred to as the zero-strain condition. In contrast, the authors propose a less restrictive approach that focuses on tailoring lattice compatibility and minimizing elastic energy barriers to reduce structural decay and improve the electrochemical performance of intercalation compounds. To this end, the authors develop a new continuum model for intercalation compounds, reveal nsights into the interplay between twinned microstructures and electrochemomechanical performance, and establish material design rules to extend the lifespans of battery materials.

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PRX Energy 4, 043002– Published 15 October, 2025
  • Received 23 June 2025
  • Accepted 22 September 2025
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