Defect Chemistry of Disordered Solid-State Electrolyte Li10GeP2S12

Prashun Gorai, Hai Long, Eric Jones, Shriram Santhanagopalan, Vladan Stevanović

Research output: Contribution to journalArticlepeer-review

31 Scopus Citations

Abstract

Several classes of materials, including thiophosphates, garnets, argyrodites, and anti-perovskites, have been considered as electrolytes for all-solid-state batteries. Native point defects and dopants play a critical role in impeding or facilitating fast ion conduction in these solid electrolytes. Despite its significance, comprehensive studies of the native defect chemistry of well-known solid electrolytes is currently lacking, in part due their compositional and structural complexity. Most of these solid-state electrolytes exhibit significant structural disorder, which requires careful consideration when modeling the point defect energetics. In this work, we model the native defect chemistry of a disordered solid electrolyte, Li10GeP2S12 (LGPS), by uniquely combining ensemble statistics, accurate electronic structure, and modern first-principles defect calculations. We find that VLi, Lii, and PGe are the dominant defects. From these calculations, we determine the statistics of defect energetics; formation energies of the dominant defects vary over ∼140 meV. Combined with previously reported ab initio molecular dynamics simulations, we find that anti-sites PGe promote Li ion conductivity, suggesting LGPS growth under P-rich/Ge-poor conditions will enhance ion conductivity. To this end, we offer practical experimental guides to enhance ion conductivity.

Original languageAmerican English
Pages (from-to)3851-3858
Number of pages8
JournalJournal of Materials Chemistry A
Volume8
Issue number7
DOIs
StatePublished - 21 Feb 2020

Bibliographical note

Publisher Copyright:
This journal is © The Royal Society of Chemistry.

NREL Publication Number

  • NREL/JA-5K00-75130

Keywords

  • computations
  • defects
  • electrolyte
  • first-principles
  • solid-state battery

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