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A Chemical-Potential-Driven Self-Mitigation Mechanism during Calendar Aging.

Jiawang Meng1, Junwei Liang1, Weijie Liu1

  • 1Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR), Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, P. R. China.

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Summary

Sulfide-based all-solid-state batteries (ASSBs) degrade during storage due to thermodynamic instability. Lowering the state-of-charge (SOC) to 25% preserves battery structure and capacity, mitigating calendar aging effects.

Keywords:
all-solid-state batteriescalendar agingnickel-rich cathodeself-mitigationspontaneous lithiation

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Sulfide-based all-solid-state batteries (ASSBs) face significant performance decay during storage, termed calendar aging, due to inherent thermodynamic instability.
  • Understanding the mechanisms of capacity fade during open-circuit storage is crucial for improving ASSB longevity.

Purpose of the Study:

  • To systematically investigate the impact of varying states-of-charge (SOC) on the calendar aging behavior of ASSBs.
  • To elucidate the underlying mechanisms of capacity decay and identify strategies for mitigating performance loss during storage.

Main Methods:

  • Investigated calendar aging effects across different SOC levels in Li6PS5Cl-based ASSBs.
  • Analyzed the electrochemical behavior and structural integrity of cathode active materials (CAMs) after storage at various SOCs.

Main Results:

  • A lower equilibrium voltage of the Li6PS5Cl electrolyte (2.06 V) compared to the cathode active material (LiNi0.94Co0.04Al0.02O2 >2.96 V) drives Li+ migration from electrolyte to CAMs, acting as a self-mitigation mechanism.
  • High SOC aging (>50%) leads to lattice oxygen release and particle cracking in CAMs.
  • Storage at 25% SOC maintains the well-ordered structure of CAMs, resulting in a significantly higher capacity (179.5 mAh/g) compared to 100% SOC (77 mAh/g).

Conclusions:

  • Optimizing storage SOC is critical for mitigating calendar aging in ASSBs.
  • Storing ASSBs at lower SOCs (e.g., 25%) effectively preserves structural integrity and electrochemical performance, offering a viable strategy for practical storage management.