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Pre-Lithiated Silicon-Based Composite Anode for High-Performance All-Solid-State Batteries.

Cheng Li1, Yuqi Wu1, Fucheng Ren1

  • 1College of Energy, Xiamen University, Xiamen, Fujian, 361102, China.

Small (Weinheim an Der Bergstrasse, Germany)
|January 17, 2025
PubMed
Summary

This study introduces a pre-lithiated silicon-based composite anode (c-Li1Si) for all-solid-state batteries (ASSBs). The novel composite effectively mitigates silicon

Keywords:
ASSBsComposite anodeSi‐based anodeSulfide solid electrolytes

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Silicon anodes offer high capacity for all-solid-state batteries (ASSBs) but suffer from volume expansion and degradation.
  • Existing silicon anodes face challenges with structural integrity and electrochemical stability during cycling.
  • Addressing these limitations is crucial for realizing high-energy-density ASSBs.

Purpose of the Study:

  • To develop a pre-lithiated silicon-based composite anode (c-Li1Si) to overcome volume expansion and stability issues.
  • To enhance the electrochemical performance and structural integrity of silicon anodes in ASSBs.
  • To investigate the role of a sulfide solid electrolyte in mitigating silicon anode degradation.

Main Methods:

  • Preparation of c-Li1Si composite anodes by incorporating Li1Si powders with Li6PS5Cl (LPSCl) solid electrolyte.
  • Electrochemical testing of ASSBs using the c-Li1Si-60 anode, including cycling stability, rate capability, and impedance spectroscopy (EIS).
  • Structural analysis using X-ray micro-CT and scanning electron microscopy (SEM), alongside pressure measurements.

Main Results:

  • The c-Li1Si-60 anode demonstrated excellent rate capability and retained 84.4% capacity after 1000 cycles at 1 C.
  • High performance was achieved even at a low anode-to-cathode capacity ratio (N/P ratio) of 1.68.
  • EIS and pressure measurements indicated improved kinetics and reduced volume expansion, with structural analysis confirming mitigated volume changes.

Conclusions:

  • The developed c-Li1Si composite anode effectively addresses the intrinsic limitations of silicon anodes in ASSBs.
  • Incorporation of LPSCl enhances conductivity and structural integrity, leading to superior electrochemical performance.
  • This work presents a promising strategy for advancing high-energy-density ASSBs utilizing silicon anodes.