A tale of two sites: On defining the carrier concentration in garnet-based ionic conductors for advanced Li batteries

Thompson, Travis; Sharafi, Asma; Johannes, Michelle D.; Huq, Ashfia; Allen, Jan L.; Wolfenstine, Jeff; Sakamoto, Jeff

doi:10.1002/aenm.201500096

A tale of two sites: On defining the carrier concentration in garnet-based ionic conductors for advanced Li batteries

Journal Article · Sat Mar 21 04:00:00 EDT 2015 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201500096· OSTI ID:1356887

Thompson, Travis ^[1]; Sharafi, Asma ^[1]; Johannes, Michelle D. ^[2]; Huq, Ashfia ^[3]; Allen, Jan L. ^[4]; Wolfenstine, Jeff ^[4]; Sakamoto, Jeff ^[1]

Univ. of Michigan, Ann Arbor, MI (United States)
Naval Research Lab., Anacostia, VA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Army Research Lab., Adelphi, MD (United States)

Solid electrolytes based on the garnet crystal structure have recently been identified as a promising material to enable advance Li battery cell chemistries because of the unprecedented combination of high ionic conductivity and electrochemical stability against metallic Li. To better understand the mechanisms that give rise to high conductivity, the goal of this work is to correlate Li site occupancy with Li-ion transport. Toward this goal, the Li site occupancy is studied in cubic garnet as a function of Li concentration over the compositions range: Li_7-xLa₃Zr_2-xTa_xO₁₂ (x = 0.5, 0.75, and 1.5). The distribution of Li between the two interstitial sites (24d and 96h) is determined using neutron and synchrotron diffraction. The bulk conductivity is measured on >97% relative density polycrystalline specimens to correlate Li-ion transport as a function of Li site occupancy. It is determined that the conductivity changes nonlinearly with the occupancy of the octahedral (96h) Li site. It is shown that the effective carrier concentration is dependent on the Li site occupancy and suggests that this is a consequence of significant carrier-carrier coulombic interactions. Moreover, the observation of maximum conductivity near Li = 6.5 mol is explained.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Revolutionary Materials for Solid State Energy Conversion (RMSSEC); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1356887

Alternate ID(s):: OSTI ID: 1184231

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 11 Vol. 5; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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