Highly disordered amorphous Li-battery electrolytes

Yuntong Zhu, Zachary D. Hood, Haemin Paik, Pedro B. Groszewicz, Steffen P. Emge, Farheen N. Sayed, Chengjun Sun, Moran Balaish, David Ehre, Lincoln J. Miara, Anatoly I. Frenkel, Igor Lubomirsky, Clare P. Grey, Jennifer L.M. Rupp

Research output: Contribution to journalArticlepeer-review

Abstract

“Medium-entropy” highly disordered amorphous Li garnets, with ≥4 unique local bonding units (LBUs), hold promise for use as solid-state electrolytes in hybrid or all-solid-state batteries owing to their grain-boundary-free nature and low-temperature synthesis requirement. Through this work, we resolved the local structure of amorphous Li garnet and understood their implication for Li dynamics. These medium-entropy amorphous structures possess unique characteristics with edge- and face-sharing LBUs, not conforming to the classic Zachariasen glass formation rules, and can be synthesized in a wide but processing-friendly temperature range (<680°C). Within these amorphous structures, Li and Zr are identified as the network formers and La as network modifier, with maxima in Li dynamics observed for smaller Li–O and Zr–O coordination; this structure understanding serves as a baseline for identifying additional network formers to further modulate Li transport. Our insight provides fundamental guidelines for the structure and phase design for amorphous Li garnets and paves the way for their integration in next-generation batteries.

Original languageEnglish
Pages (from-to)500-522
Number of pages23
JournalMatter
Volume7
Issue number2
DOIs
StatePublished - 7 Feb 2024

Keywords

  • LLZO
  • Li-ion conductors
  • LiLaZrO
  • MAP 3: Understanding
  • amorphous Li garnets
  • amorphous oxides
  • medium-entropy oxides
  • solid electrolytes
  • solid-state batteries

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