X-ray Nanoimaging of Crystal Defects in Single Grains of Solid-State Electrolyte Li7–3xAlxLa3Zr2O12

Sun, Yifei; Gorobstov, Oleg; Mu, Linqin; Weinstock, Daniel; Bouck, Ryan; Cha, Wonsuk; Bouklas, Nikolaos; Lin, Feng; Singer, Andrej

doi:10.1021/acs.nanolett.1c00315

X-ray Nanoimaging of Crystal Defects in Single Grains of Solid-State Electrolyte Li_7–3xAl_xLa₃Zr₂O₁₂

Journal Article · Thu Apr 29 00:00:00 EDT 2021 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.1c00315· OSTI ID:1834541

^[1]; ^[1]; ^[2]; Weinstock, Daniel ^[1]; Bouck, Ryan ^[1]; Cha, Wonsuk ^[3]; Bouklas, Nikolaos ^[1]; ^[2]; ^[1]

Cornell Univ., Ithaca, NY (United States)
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

All-solid-state lithium batteries promise significant improvements in energy density and safety over traditional liquid electrolyte batteries. The Al-doped Li₇La₃Zr₂O₁₂ (LLZO) solid-state electrolyte shows excellent potential given its high ionic conductivity and good thermal, chemical, and electrochemical stability. Nevertheless, further improvements on electrochemical and mechanical properties of LLZO call for an in-depth understanding of its local microstructure. Here, we employ Bragg coherent diffractive imaging to investigate the atomic displacements inside single grains of LLZO with various Al-doping concentrations, resulting in cubic, tetragonal, and cubic-tetragonal mixed structures. We observe coexisting domains of different crystallographic orientations in the tetragonal structure. We further show that Al doping leads to crystal defects such as dislocations and phase boundaries in the mixed- and cubic-phase grain. This study addresses the effect of Al doping on the nanoscale structure within individual grains of LLZO, which is informative for the future development of solid-state batteries.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1834541

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 11 Vol. 21; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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X-ray Nanoimaging of Crystal Defects in Single Grains of Solid-State Electrolyte Li_7–3xAl_xLa₃Zr₂O₁₂