New Family of Argyrodite Thioantimonate Lithium Superionic Conductors

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

doi:10.1021/jacs.9b08357

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.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1606830

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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New Family of Argyrodite Thioantimonate Lithium Superionic Conductors

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