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Effective transport network driven by tortuosity gradient enables high-electrochem-active solid-state batteries.

Qing-Song Liu1,2, Han-Wen An1, Xu-Feng Wang1

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|March 6, 2023
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Summary

Designing solid-state batteries with thick electrodes is challenging due to slow ion transport. This study reveals tortuous pathways limit ion movement, but a new electrode design improves ion percolation and battery performance.

Keywords:
all-solid-state batterieslithiation/delithiation heterogeneitysynchrotron techniquesthick electrodestortuosity gradient

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Solid-state batteries offer safety advantages over liquid electrolyte systems.
  • Achieving high energy density requires thick electrodes, which are limited by slow ion transport.
  • Understanding ion transport mechanisms in solid electrodes is crucial for improving battery performance.

Purpose of the Study:

  • To investigate the fundamental reasons for slow ion transport in thick solid-state electrodes.
  • To develop a novel electrode architecture that enhances ion transport and electrochemical activity.
  • To demonstrate improved performance in thick solid-state battery electrodes.

Main Methods:

  • Synchronized electrochemical analysis combined with X-ray tomography and ptychography.
  • Spatially probing thickness-dependent delithiation kinetics.
  • Fabricating and characterizing tortuosity-gradient electrodes.

Main Results:

  • Identified tortuous and slow longitudinal pathways as the origin of low delithiation kinetics.
  • Demonstrated that tortuosity-gradient electrodes create effective ion-percolation networks.
  • Observed enhanced electrochemical activity and extended cycle life in thick electrodes with the new architecture.

Conclusions:

  • Effective ion transport pathways are critical for high-loading solid-state cathodes.
  • Tortuosity-gradient electrodes represent a promising design for overcoming ion transport limitations.
  • This work provides key design principles for advancing solid-state battery technology.