Argyrodite-type advanced lithium conductors and transport mechanisms beyond paddle-wheel effect

Hong Fang () and Puru Jena ()
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Hong Fang: Virginia Commonwealth University
Puru Jena: Virginia Commonwealth University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Development of next-generation solid-state Li-ion batteries requires not only electrolytes with high room-temperature (RT) ionic conductivities but also a fundamental understanding of the ionic transport in solids. In spite of considerable work, only a few lithium conductors are known with the highest RT ionic conductivities ~ 0.01 S/cm and the lowest activation energies ~0.2 eV. New design strategy and novel ionic conduction mechanism are needed to expand the pool of high-performance lithium conductors as well as achieve even higher RT ionic conductivities. Here, we theoretically show that lithium conductors with RT ionic conductivity over 0.1 S/cm and low activation energies ~ 0.1 eV can be achieved by incorporating cluster-dynamics into an argyrodite structure. The extraordinary superionic metrics are supported by conduction mechanism characterized as a relay between local and long-range ionic diffusions, as well as correlational dynamics beyond the paddle-wheel effect.

Date: 2022
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DOI: 10.1038/s41467-022-29769-5

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