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Ionic Crystal Structures02:42

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Ionic crystals consist of two or more different kinds of ions that usually have different sizes. The packing of these ions into a crystal structure is more complex than the packing of metal atoms that are the same size.
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Metallic solids such as crystals of copper, aluminum, and iron are formed by metal atoms. The structure of metallic crystals is often described as a uniform distribution of atomic nuclei within a “sea” of delocalized electrons. The atoms within such a metallic solid are held together by a unique force known as metallic bonding that gives rise to many useful and varied bulk properties.
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Li6SiO4Cl2: A Hexagonal Argyrodite Based on Antiperovskite Layer Stacking.

Alexandra Morscher1, Matthew S Dyer1, Benjamin B Duff1,2

  • 1Department of Chemistry, University of Liverpool, Crown Street, L69 7ZD Liverpool, U.K.

Chemistry of Materials : a Publication of the American Chemical Society
|April 12, 2021
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Researchers discovered a new hexagonal solid electrolyte, Li6SiO4Cl2, by combining computation and experiments. This material exhibits enhanced lithium-ion conductivity above a specific temperature, opening new avenues for solid electrolyte research.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Computational Materials Science

Background:

  • Solid electrolytes are crucial for advanced battery technologies.
  • Lithium argyrodites are a promising class of solid electrolytes.
  • Understanding structure-property relationships is key to designing new materials.

Purpose of the Study:

  • To computationally and experimentally discover a hexagonal analogue of lithium argyrodite solid electrolytes.
  • To investigate the structural and ionic conductivity properties of the newly synthesized material.
  • To establish a structural connection between hexagonal and cubic argyrodite and perovskite structures.

Main Methods:

  • Computational modeling and energy minimization to predict stable compositions.
  • Synthesis and X-ray diffraction for structure determination.
  • Nuclear Magnetic Resonance (NMR) and AC impedance spectroscopy to study ionic conductivity and lithium dynamics.

Main Results:

  • Identification and synthesis of hexagonal Li6SiO4Cl2 with a predicted ordered structure.
  • Observation of a low room-temperature lithium conductivity (∼10-10 S cm-1).
  • Discovery of an order-disorder transition at 469.3(1) K, leading to dynamic lithium site disorder and increased Li-ion mobility.

Conclusions:

  • Hexagonal Li6SiO4Cl2 exhibits properties analogous to cubic argyrodites, with enhanced conductivity above the transition temperature.
  • The established structural link between hexagonal/cubic argyrodites and perovskites reveals significant unexplored chemical space for solid electrolyte development.
  • This work provides a pathway for designing novel solid electrolytes with tunable properties by exploring stacking motifs.