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In the region where two bulk phases meet, an intricate electric charge distribution arises due to charge transfer, ion adsorption, molecular orientation, and charge distortion. This complex distribution is commonly referred to as the electrical double layer.When a solid electrode interfaces with ions in an electrolyte solution, the speed of electron transfer dictates the rates of oxidation and reduction. The electrode acquires a charge through the escape of atoms into the solution as cations or...
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Cation Mixing Properties toward Co Diffusion at the LiCoO2 Cathode/Sulfide Electrolyte Interface in a Solid-State

Jun Haruyama, Keitaro Sodeyama1,2, Yoshitaka Tateyama1

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All-solid-state Li-ion batteries (ASS-LIBs) face high interfacial resistance. This study reveals that Co-P mixing at the LiCoO2/Li3PS4 interface drives this resistance, a process mitigated by a LiNbO3 buffer layer.

Keywords:
first-principles calculationsinterfacial resistancelithium ionic conductormutual diffusionsolid electrolyte

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Computational Chemistry

Background:

  • All-solid-state Li-ion batteries (ASS-LIBs) promise enhanced safety and energy density.
  • High interfacial resistance between solid cathode and electrolyte components is a major bottleneck for ASS-LIB performance.
  • Understanding interfacial phenomena is crucial for developing next-generation batteries.

Purpose of the Study:

  • To investigate the cation diffusion mechanisms at the LiCoO2 (LCO) cathode and β-Li3PS4 (LPS) solid electrolyte interface.
  • To evaluate the impact of a LiNbO3 buffer layer on interfacial stability and ion transport.
  • To elucidate the atomistic origins of interfacial resistance in ASS-LIBs.

Main Methods:

  • First-principles calculations were employed to simulate interfacial interactions and diffusion pathways.
  • Calculations included evaluating ion exchange energies and defect states at the interface.
  • Analysis focused on the LiCoO2/β-Li3PS4 interface with and without a LiNbO3 buffer layer.

Main Results:

  • Energetically favorable mixing of Cobalt (Co) and Phosphorus (P) was identified at the LCO/LPS interface.
  • The LiNbO3 buffer layer effectively suppresses Co-P mixing due to unfavorable Co-Nb exchange.
  • Interfacial defect states and anion bonding preferences contribute to the stabilization of Co-P exchange, leading to Li depletion.

Conclusions:

  • The Co-P intermixing at the cathode-electrolyte interface is a primary cause of high interfacial resistance in ASS-LIBs.
  • A LiNbO3 buffer layer can significantly mitigate this resistance by preventing detrimental cation mixing.
  • These findings provide atomistic insights for designing ASS-LIBs with improved interfacial properties and reduced resistance.