Journal
ACS ENERGY LETTERS
Volume 2, Issue 2, Pages 462-468Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.6b00593
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Funding
- U.S. Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy (EERE) Vehicle Technologies Office (VTO)
- Advanced Battery Material Research (BMR) program [DE-EE-0006821]
- National Science Foundation [DMR-1561008]
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- U.S. Army Research Laboratory (ARL)
- Kwanjeong Educational Foundation
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1561008] Funding Source: National Science Foundation
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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 (similar to 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.
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