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Exploiting Nanoscale Complexion in LATP Solid-State Electrolyte via Interfacial Mg2+ Doping.

Sina Stegmaier1, Karsten Reuter2, Christoph Scheurer2,3

  • 1Department of Chemistry, Technical University of Munich, 85747 Garching, Germany.

Nanomaterials (Basel, Switzerland)
|September 9, 2022
PubMed
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Doping magnesium into solid-state electrolyte grain boundaries enhances battery performance by preventing lithium dendrites and decomposition. This nanoscale interfacial engineering improves ion conductivity and battery stability for advanced energy storage.

Area of Science:

  • Materials Science
  • Electrochemistry
  • Computational Chemistry

Background:

  • All-solid-state batteries (ASSBs) face challenges at solid-solid interfaces, including lithium dendrite penetration and electrolyte decomposition.
  • Nanoscale protective layers on ceramic Li1+xAlxTi2-x(PO4)3 (LATP) solid-state electrolyte (SSE) grains can mitigate these issues.

Purpose of the Study:

  • Investigate the effects of doping divalent Mg2+ into LATP grain boundaries.
  • Explore nanoscale interfacial engineering for improved ASSB performance.

Main Methods:

  • Utilized Molecular Dynamics simulations with a realistic atomistic model of LATP grain boundaries.
  • Analyzed the behavior and impact of Mg2+ dopants at the nanoscale interface.

Main Results:

Keywords:
cationic dopingcomplexioninterface engineeringmolecular dynamicsprotective coatingsolid state electrolyte

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  • Mg2+ was identified as a suitable dopant, rarely penetrating the protective complexion and preserving bulk electrolyte integrity.
  • Tuning interphase stoichiometry with Mg2+ suppressed reductive degradation by lowering Ti4+ content.
  • Local Li+ conductivity at the interface was enhanced.

Conclusions:

  • Interfacial doping with Mg2+ offers a promising strategy for nanoscale engineering of LATP SSEs.
  • This approach can improve the performance and stability of all-solid-state batteries.