Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 10, Pages 4131-4137Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201914478
Keywords
all-solid-state battery; composite electrolyte; Li-ion conductivity; Li-ion transfer mechanism; solid-state NMR
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Funding
- Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) [DE-EE0007762]
- National Science Foundation [DMR-1808517, NSF/DMR-1644779]
- State of Florida
- TAFEL [UTA18-000175]
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Li+-conducting oxides are considered better ceramic fillers than Li+-insulating oxides for improving Li+ conductivity in composite polymer electrolytes owing to their ability to conduct Li+ through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li+-insulating oxides (fluorite Gd0.1Ce0.9O1.95 and perovskite La0.8Sr0.2Ga0.8Mg0.2O2.55) with a high concentration of oxygen vacancies to demonstrate two oxide/poly(ethylene oxide) (PEO)-based polymer composite electrolytes, each with a Li+ conductivity above 10(-4) S cm(-1) at 30 degrees C. Li solid-state NMR results show an increase in Li+ ions (>10 %) occupying the more mobile A2 environment in the composite electrolytes. This increase in A2-site occupancy originates from the strong interaction between the O2- of Li-salt anion and the surface oxygen vacancies of each oxide and contributes to the more facile Li+ transport. All-solid-state Li-metal cells with these composite electrolytes demonstrate a small interfacial resistance with good cycling performance at 35 degrees C.
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