New Family of Argyrodite Thioantimonate Lithium Superionic Conductors

Zhou, Laidong; Assoud, Abdeljalil; Zhang, Qiang; Wu, Xiaohan; Nazar, Linda F.

doi:10.1021/jacs.9b08357

Title: New Family of Argyrodite Thioantimonate Lithium Superionic Conductors

Journal Article · Wed Oct 23 00:00:00 EDT 2019 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b08357· OSTI ID:1606830

^[1]; Assoud, Abdeljalil ^[1]; Zhang, Qiang ^[2]; Wu, Xiaohan ^[3];

^[1]

Univ. of Waterloo, ON (Canada)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
BASF SE, Ludwigshafen (Germany)

We report on a new family of argyrodite lithium superionic conductors, as solid solutions Li_6+xMxSb_1–xS₅I (M = Si, Ge, Sn), that exhibit superionic conductivity. These represent the first antimony argyrodites to date. Exploration of the series using a combination of single crystal X-ray and synchrotron/neutron powder diffraction, combined with impedance spectroscopy, reveals that an optimal degree of substitution (x), and substituent induces slight S^2–/I^– anion site disorder—but more importantly drives Li⁺ cation site disorder. The additional, delocalized Li-ion density is located in new high energy lattice sites that provide intermediate interstitial positions (local minima) for Li⁺ diffusion and activate concerted ion migration, leading to a low activation energy of 0.25 eV. Excellent room temperature ionic conductivity of 14.8 mS·cm^–1 is exhibited for cold-pressed pellets—up to 24 mS·cm^–1 for sintered pellets—among the highest values reported to date. This enables all-solid-state battery prototypes that exhibit promising properties. Furthermore, even at -78 °C, suitable bulk ionic conductivity of the electrolyte is retained (0.25 mS·cm^–1). Selected thioantimonate iodides demonstrate good compatibility with Li metal, sustaining over 1000 h of Li stripping/plating at current densities up to 0.6 mA·cm^–2. The significantly enhanced Li ion conduction and lowered activation energy barrier with increasing site disorder reveals an important strategy toward the development of superionic conductors.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1606830

Journal Information:: Journal of the American Chemical Society, Vol. 141, Issue 48; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 131 works

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