Inducing High Ionic Conductivity in the Lithium Superionic Argyrodites Li6+xP1-xGexS5I for All-Solid-State Batteries

Marvin Kraft, Saneyuki Ohni, Tatiana Zinkevich, Raimund Koerver, Sean Culver, Till Fuchs, Anatoliy Senyshyn, Sylvio Indris, Benjamin Morgan, Wolfgang Zeier

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Solid-state batteries with inorganic solid electrolytes are currently being discussed as a more reliable and safer future alternative to the current lithium-ion battery technology. To compete with state-of-the-art lithium-ion batteries, solid electrolytes with higher ionic conductivities are needed, especially if thick electrode configurations are to be used. In the search for optimized ionic conductors, the lithium argyrodites have attracted a lot of interest. Here, we systematically explore the influence of aliovalent substitution in Li6+xP1-xGexS5I using a combination of X-ray and neutron diffraction, as well as impedance spectroscopy and nuclear magnetic resonance. With increasing Ge content, an anion site disorder is induced and the activation barrier for ionic motion drops significantly, leading to the fastest lithium argyrodite so far with 5.4 ± 0.8 mS cm-1 in a cold-pressed state and 18.4 ± 2.7 mS cm-1 upon sintering. These high ionic conductivities allow for successful implementation within a thick-electrode solid-state battery that shows negligible capacity fade over 150 cycles. The observed changes in the activation barrier and changing site disorder provide an additional approach toward designing better performing solid electrolytes.
Original languageEnglish
Pages (from-to)16330-16339
Number of pages10
JournalJournal of the American Chemical Society
Issue number47
Early online date1 Nov 2018
Publication statusPublished - 28 Nov 2018

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry


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