Preparation of Li2S-GeSe2-P2S5 electrolytes by a single step ball milling for all-solid-state lithium secondary batteries

James E. Trevey, Yoon Seok Jung, Se Hee Lee

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30 Citations (Scopus)


Glass-ceramic and glass Li2S-GeSe2-P2S5 electrolytes were prepared by a single step ball milling (SSBM) process. Various compositions of Li4-xGe1-xPxS2(1+x)Se2(1-x) with/without heat treatment (HT) from x = 0.55 to x = 1.00 were systematically investigated. Structural analysis by X-ray diffraction (XRD) showed gradual increase of the lattice constant followed by significant phase change with increasing GeSe2. HT also affected the crystallinity. Incorporation of GeSe2 in Li2S-P2S5 kept high conductivity with a maximum value of 1.4 × 10-3 S cm-1 at room temperature for x = 0.95 in Li4-xGe1-xPxS2(1+x)Se2(1-x) without HT. All-solid-state LiCoO2/Li cells using Li2S-GeSe2-P2S5 as solid-state electrolytes (SE) were tested by constant-current constant-voltage (CCCV) charge-discharge cycling at a current density of 50 μA cm-2 between 2.5 and 4.3 V (vs. Li/Li+). In spite of the extremely high conductivity of the SE, LiCoO2/Li cells showed a large irreversible reaction especially during the first charging cycle. LiCoO2 with SEs heat-treated at elevated temperature exhibited a capacity over 100 mAh g-1 at the second cycle and consistently improved cycle retention, which is believed to be due to the better interfacial stability.

Original languageEnglish
Pages (from-to)4984-4989
Number of pages6
JournalJournal of Power Sources
Issue number15
Publication statusPublished - 2010 Aug 1

Bibliographical note

Funding Information:
This work has been supported by DARPA/DSO. Dr. Yoon Seok Jung acknowledges the Korea Research Foundation Grant funded by the Korean Government [ KRF-2008-357-D00066 ].

All Science Journal Classification (ASJC) codes

  • Renewable Energy, Sustainability and the Environment
  • Energy Engineering and Power Technology
  • Physical and Theoretical Chemistry
  • Electrical and Electronic Engineering


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