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A battery is a galvanic cell that is used as a source of electrical power for specific applications. Modern batteries exist in a multitude of forms to accommodate various applications, from tiny button batteries such as those that power wristwatches to the very large batteries used to supply backup energy to municipal power grids. Some batteries are designed for single-use applications and cannot be recharged (primary cells), while others are based on conveniently reversible cell reactions that...
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Crystalline solids are divided into four types: molecular, ionic, metallic, and covalent network based on the type of constituent units and their interparticle interactions.
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Ions are atoms or molecules bearing an electrical charge. A cation (a positive ion) forms when a neutral atom loses one or more electrons from its valence shell, and an anion (a negative ion) forms when a neutral atom gains one or more electrons in its valence shell. Compounds composed of ions are called ionic compounds (or salts), and their constituent ions are held together by ionic bonds: electrostatic forces of attraction between oppositely charged cations and anions. 
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An ionic compound is stable because of the electrostatic attraction between its positive and negative ions. The lattice energy of a compound is a measure of the strength of this attraction. The lattice energy (ΔHlattice) of an ionic compound is defined as the energy required to separate one mole of the solid into its component gaseous ions. For the ionic solid sodium chloride, the lattice energy is the enthalpy change of the process:
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High-Entropy Lithium Argyrodite Solid Electrolytes Enabling Stable All-Solid-State Batteries.

Shenghao Li1, Jing Lin2, Mareen Schaller3

  • 1Center of Smart Materials and Devices, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing &, School of Material Science and Engineering, Wuhan University of Technology, Wuhan, 430070, China.

Angewandte Chemie (International Ed. in English)
|October 30, 2023
PubMed
Summary
This summary is machine-generated.

Configurational entropy in solid electrolytes positively impacts ion mobility. This study demonstrates that tailoring compositional complexity in lithium argyrodites enhances ionic conductivity for advanced solid-state batteries.

Keywords:
ArgyroditeHigh-Entropy MaterialsSolid ElectrolyteSolid-State Batteries

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Superionic solid electrolytes (SEs) are critical for solid-state battery (SSB) development.
  • Understanding the role of configurational entropy (ΔSconf) in ionic conductivity of multicomponent SEs is crucial but lacking.
  • Lithium argyrodites are promising SE materials.

Purpose of the Study:

  • To investigate the correlation between configurational entropy and ionic conductivity in halogen-rich lithium argyrodites.
  • To synthesize and characterize a series of Li5.5 PS4.5 Clx Br1.5-x compounds.
  • To demonstrate the potential of these materials in high-performance SSBs.

Main Methods:

  • Synthesis of halogen-rich lithium argyrodites (Li5.5 PS4.5 Clx Br1.5-x).
  • Neutron powder diffraction and 31 P magic-angle spinning nuclear magnetic resonance spectroscopy for structural and compositional analysis.
  • Ionic conductivity measurements at room temperature.

Main Results:

  • Quantitative analysis of S2-/Cl-/Br- occupancy on the anion sublattice.
  • Positive correlation observed between anion sublattice disorder (ΔSconf) and Li-ion dynamics.
  • Achieved a room-temperature ionic conductivity of 22.7 mS cm-1 for Li5.5 PS4.5 Cl0.8 Br0.7 (ΔSconf =1.98R).
  • Demonstrated stable cycling of single-crystal LiNi0.9 Co0.06 Mn0.04 O2 (s-NCM90) composite cathodes in SSB cells using the optimized SE.

Conclusions:

  • First experimental evidence linking configurational entropy of the anion sublattice to ion mobility in SEs.
  • Tailoring compositional complexity is a viable strategy to enhance ionic conductivity in ceramic ion conductors.
  • Dual-substituted lithium argyrodites show significant promise for high-performance electrochemical energy storage applications.