Fast Sodium-Ion Conductivity in Supertetrahedral Phosphidosilicates

Haffner, A.; Hatz, A.; Moudrakovski, I.; Lotsch, B. V.; Johrendt, D.

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Fast Sodium-Ion Conductivity in Supertetrahedral Phosphidosilicates

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Lotsch, B. V.
Department Nanochemistry (Bettina V. Lotsch), Max Planck Institute for Solid State Research, Max Planck Society;

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Citation

Haffner, A., Hatz, A., Moudrakovski, I., Lotsch, B. V., & Johrendt, D. (2018). Fast Sodium-Ion Conductivity in Supertetrahedral Phosphidosilicates. Angewandte Chemie International Edition, 57(21), 6155-6160.

Cite as: https://hdl.handle.net/21.11116/0000-000E-DA82-9

Abstract

Fast sodium-ion conductors are key components of Na-based all-solid-state batteries which hold promise for large-scale storage of electrical power. We report the synthesis, crystal-structure determination, and Na+-ion conductivities of six new Na-ion conductors, the phosphidosilicates Na19Si13P25, Na23Si19P33, Na23Si28P45, Na23Si37P57, LT-NaSi2P3 and HT-NaSi2P3, based entirely on earth-abundant elements. They have SiP4 tetrahedra assembled interpenetrating networks of T3 to T5 supertetrahedral clusters and can be hierarchically assigned to sphalerite- or diamond-type structures. Na-23 solid-state NMR spectra and geometrical pathway analysis show Na+-ion mobility between the supertetrahedral cluster networks. Electrochemical impedance spectroscopy shows Na+-ion conductivities up to sigma(Na+) = 4 x 10(-4) Scm(-1). The conductivities increase with the size of the supertetrahedral clusters through dilution of Na+-ions as the charge density of the anionic networks decreases.