Journal
ACS ENERGY LETTERS
Volume 5, Issue 6, Pages 2098-2105Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.0c00942
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Funding
- NMF software tool on GitHub [JP 17H02792]
- Japan Society for the Promotion of Science
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The rate capability of bulk-type solid-state Li-ion batteries is limited by the solid-state diffusion of Li ions in the cathodes that typically form micrometer-sized polycrystalline particles composed of aggregated nanocrystals. This necessitates nanoscale and dynamic observations of Li ions to establish a detailed understanding of Li conduction in the complicated particle structure. This study demonstrates Li-ion dynamics in particle cathodes under low- and high-rate charge-discharge reaction conditions using operando scanning transmission electron microscopy coupled with electron energy-loss spectroscopy. Direct observation results reveal the slow diffusion through nanocrystal grain boundaries as the primary factor limiting Li conduction in particle cathodes. Therefore, rate-capability enhancement of Li-ion batteries requires either optimization of the interfacial structure along with nanocrystal orientation or the use of large single crystals without boundaries.
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