Electrochemical Window of the Li-Ion Solid Electrolyte Li₇La₃Zr ₂O₁₂

Journal Article · Fri Jan 27 00:00:00 EST 2017 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.6b00593· OSTI ID:1485483

Thompson, Travis  ^[1]; Yu, Seungho  ^[1]; Williams, Logan ^[2]; Schmidt, Robert D. ^[1]; Garcia-Mendez, Regina ^[2]; Wolfenstine, Jeff ^[3]; Allen, Jan L. ^[3]; Kioupakis, Emmanouil ^[2]; Siegel, Donald J. ^[4]; Sakamoto, Jeff ^[4]

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1. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Mechanical Engineering
2. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Materials Science & Engineering
3. Army Research Laboratory, RDRL-SED-C, 2800 Powder Mill Road, Adelphi, Maryland 20783, United States
4. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Mechanical Engineering and Dept. of Materials Science & Engineering

The recent discovery of fast ion-conducting solid electrolytes could enable solid-state and other advanced battery chemistries with higher energy densities and enhanced safety. In addition to high ionic conductivity, a viable electrolyte should also exhibit an electrochemical window that is wide enough to suppress undesirable electronic transport (i.e., self-discharge and/or short circuiting) arising from charge injection or extraction from the electrodes. Here, direct current chronoamperometry, alternating current electrochemical impedance spectroscopy, and optical absorption band gap measurements are combined with first-principles calculations to systematically characterize the electrochemical window of the promising superionic conductor Li₇La₃Zr₂O₁₂ (LLZO). Negligible electronic current was measured within LLZO for a wide range of voltages relevant for high-voltage cathodes. This auspicious behavior is consistent with both the large band gap (~6 eV) predicted for LLZO and the absolute positions of its band edges. These features imply that a wide electrochemical window is an intrinsic property of LLZO, facilitating its use in next-generation batteries.

• Research Organization: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
• Sponsoring Organization: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC)
• DOE Contract Number: EE0006821; AC02-05CH11231
• OSTI ID: 1485483
• Journal Information: ACS Energy Letters, Vol. 2, Issue 2; ISSN 2380-8195
• Publisher: American Chemical Society (ACS)
• Country of Publication: United States
• Language: English