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In Situ Neutron Powder Diffraction Using Custom-made Lithium-ion Batteries
Published on: November 10, 2014
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Dynamic Lithium Transport Pathway via Crack Formation in Phase-Separating Battery Particles
Chihyun Nam1, Bonho Koo1, Juwon Kim1
1Department of Chemistry, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea.
ACS Nano
|March 5, 2025
Summary
Nanoscale cracks in battery particles form from lithium insertion stress, propagating as new pathways emerge. This study reveals a recursive loop between lithium movement, stress, and crack growth, impacting battery life.
Area of Science:
- Materials Science
- Electrochemistry
- Battery Technology
Background:
- Nanoscale cracks are common in battery particles during cycling, affecting battery performance.
- Understanding crack formation and propagation is vital for improving battery cycle life and kinetics.
- The influence of nanocracks on lithium (de)insertion pathways and local strain fields is not well understood.
Purpose of the Study:
- To visualize the relationship between lithium (de)insertion pathways and crack formation/propagation in individual LiFePO4 particles.
- To elucidate the generation mechanism of nanocracks and their propagation dynamics.
- To understand how nanocracks influence internal stress fields and lithium distribution.
Main Methods:
- Utilized *operando* scanning transmission X-ray microscopy on individual LiFePO4 particles.
- Observed lithium (de)insertion pathways and crack formation in real-time.
- Employed 3D phase-field simulations to support experimental observations.
Main Results:
- Demonstrated nanocrack generation due to tensile stress from edge lithium insertion.
- Observed nanocrack propagation activated by new fast lithium (de)insertion pathways.
- Showed delithiation induces crack-opening tensile stress, while lithiation causes crack-closing compressive stress.
- Confirmed dynamic lithium distribution shapes internal stress fields.
Conclusions:
- Revealed a recursive chemo-mechanical loop involving lithium (de)insertion, stress fields, and crack development in battery particles.
- Provided critical insights into the mechanisms governing nanocrack formation and propagation.
- Established a link between nanostructure evolution and electrochemical performance in LiFePO4 batteries.
Keywords:
3D phase field simulationlithium transport pathwaynanoscale crack formationoperando soft X-ray imagingphase separating materialMore Related Videos
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