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Hydride-based antiperovskites with soft anionic sublattices as fast alkali ionic conductors
Shenghan Gao1, Thibault Broux1, Susumu Fujii2
1Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto, 615-8510, Japan.
Nature Communications
|January 9, 2021
Summary
Researchers developed new hydride-chalcogenide antiperovskites (M3HCh) with soft anionic sublattices. These materials exhibit promising ionic conductivity for lithium-ion and sodium-ion transport, enhanced by aliovalent substitution.
Area of Science:
- Solid-state chemistry
- Materials science
- Inorganic chemistry
Background:
- Solid-state materials typically use p-block anions.
- Recent advances include hydride anions (H-) in oxides, revealing novel properties.
- Hydride anions offer unique electronic and structural characteristics.
Purpose of the Study:
- To construct and investigate a new family of antiperovskites (M3HCh) incorporating hydride and chalcogenide anions.
- To explore the structural stability and ionic conductivity of these novel materials.
- To understand the role of hydride anions in determining material properties.
Main Methods:
- Synthesis and structural characterization of M3HCh antiperovskites (M=Li, Na).
- Theoretical calculations and experimental studies to probe ion transport mechanisms.
- Aliovalent substitution to introduce vacancies and enhance ionic conductivity.
Main Results:
- M3HCh antiperovskites generally adopt a robust cubic structure due to the size-flexibility of H-.
- Low migration barriers for Li+/Na+ transport were identified.
- A soft phonon mode associated with HM6 octahedra rotation promotes ionic conductivity.
- Aliovalent substitution significantly enhanced ionic conductivity, reaching ~1x10^-4 S/cm in Na2.9H(Se0.9I0.1) at 100°C.
Conclusions:
- Hydride-chalcogenide antiperovskites represent a promising class of solid electrolytes.
- The unique properties stem from the soft anionic sublattice and the hydride anion's characteristics.
- These materials hold potential for advanced energy storage applications.
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