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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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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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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Amorphous Oxyhalide Matters for Achieving Lithium Superionic Conduction.

Shumin Zhang1, Feipeng Zhao1, Lo-Yueh Chang2

  • 1Department of Mechanical and Materials Engineering, Western University, London, ON N6A 5B9, Canada.

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|January 29, 2024
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Summary
This summary is machine-generated.

Amorphous components in halide solid electrolytes (SEs) are crucial for fast ion conduction in all-solid-state batteries (ASSBs). Incorporating oxygen into zirconium-based halide SEs creates amorphous structures that enhance ionic conductivity and battery performance.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Halide-based solid electrolytes (SEs) are promising for all-solid-state batteries (ASSBs) due to their ionic conductivity and electrochemical stability.
  • The role of amorphous components in halide SEs, particularly in Li-ion conduction, remains underexplored.

Purpose of the Study:

  • To investigate the common presence and impact of amorphous components in mechanochemically prepared halide SEs.
  • To elucidate the relationship between local chemistry in amorphous phases and fast Li-ion migration.
  • To explore the effect of oxygen incorporation on the amorphization and properties of Zr-based halide SEs.

Main Methods:

  • Mechanochemical preparation of halide SEs.
  • X-ray absorption spectroscopy (XAS) for structural analysis.
  • Pair distribution function (PDF) analyses.
  • Reverse Monte Carlo (RMC) modeling.
  • Ionic conductivity measurements.

Main Results:

  • Amorphous components are prevalent in mechanochemically synthesized halide SEs and are linked to fast Li-ion transport.
  • Incorporating oxygen into Zr-based halide SEs (e.g., Li3ZrCl4O1.5) induces amorphization, forming corner-sharing Zr-O/Cl polyhedrons.
  • This unique amorphous structure significantly lowers Li-ion transport energy barriers, achieving an ionic conductivity of (1.35 ± 0.07) × 10^-3 S cm^-1 at 25 °C.
  • Amorphization via oxygen incorporation also improves mechanical deformability and electrochemical performance.

Conclusions:

  • The presence and specific local chemistry of amorphous phases are critical for optimizing Li-ion conduction in halide SEs.
  • Oxygen incorporation offers a viable strategy to engineer amorphous halide SEs with enhanced ionic conductivity, mechanical properties, and electrochemical performance for ASSBs.
  • This study provides fundamental insights for the rational design of advanced halide SEs for high-performance ASSBs.