Effect of Gallium Substitution on Lithium-Ion Conductivity and Phase Evolution in Sputtered Li7-3 xGa xLa3Zr2O12 Thin Films

M Rawlence; A N Filippin; A Wäckerlin; T-Y Lin; E Cuervo-Reyes; A Remhof; C Battaglia; J L M Rupp; S Buecheler

doi:10.1021/acsami.8b03163

Effect of Gallium Substitution on Lithium-Ion Conductivity and Phase Evolution in Sputtered Li_{7-3 x}Ga _xLa₃Zr₂O₁₂ Thin Films

ACS Appl Mater Interfaces. 2018 Apr 25;10(16):13720-13728. doi: 10.1021/acsami.8b03163. Epub 2018 Apr 12.

Authors

M Rawlence¹, A N Filippin, A Wäckerlin, T-Y Lin, E Cuervo-Reyes, A Remhof, C Battaglia, J L M Rupp^{1

2}, S Buecheler

Affiliations

¹ Electrochemical Materials , ETH Zurich , CH-8093 Zurich , Switzerland.
² Electrochemical Materials , Massachusetts Institute of Technology (MIT) , Cambridge , Massachusetts 02139 , United States.

PMID: 29608054
DOI: 10.1021/acsami.8b03163

Abstract

Replacing the liquid electrolyte in conventional lithium-ion batteries with thin-film solid-state lithium-ion conductors is a promising approach for increasing energy density, lifetime, and safety. In particular, Li₇La₃Zr₂O₁₂ is appealing due to its high lithium-ion conductivity and wide electrochemical stability window. Further insights into thin-film processing of this material are required for its successful integration into solid-state batteries. In this work, we investigate the phase evolution of Li_{7-3 x}Ga _xLa₃Zr₂O₁₂ in thin films with various amounts of Li and Ga for stabilizing the cubic phase. Through this work, we gain valuable insights into the crystallization processes unique to thin films and are able to form dense Li_{7-3 x}Ga _xLa₃Zr₂O₁₂ layers stabilized in the cubic phase with high in-plane lithium-ion conductivities of up to 1.6 × 10^-5 S cm^-1 at 30 °C. We also note the formation of cubic Li₇La₃Zr₂O₁₂ at the relatively low temperature of 500 °C.

Keywords: LLZO; solid-state electrolyte; sputtering; thin-film LLZO.