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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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Acid halides are reduced to alcohols in the presence of a strong reducing agent like lithium aluminum hydride.
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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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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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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Anion Engineering for Stabilizing Li Interstitial Sites in Halide Solid Electrolytes for All-Solid-State Li

Kern-Ho Park1, Se Young Kim2,3, Mina Jung1

  • 1Advanced Batteries Research Center, Korea Electronics Technology Institute, Seongnam 13509, South Korea.

ACS Applied Materials & Interfaces
|December 11, 2023
PubMed
Summary

Hard-base substitution, like oxygen in Li2ZrCl6, significantly boosts halide solid electrolyte ionic conductivity. This method stabilizes lithium ion migration pathways, enhancing battery performance.

Keywords:
Li pathwayall-solid-state batteryhalide solid electrolyteinterstitial siteionic conductor

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Halide solid electrolytes (SEs) are recognized for their high-voltage stability, crucial for advanced battery technologies.
  • Previous improvements in halide SE ionic conductivity involved aliovalent metal substitutions or adopting specific crystal structures (e.g., monoclinic C2/m with ccp anion arrangement).

Purpose of the Study:

  • To introduce and investigate a novel 'hard-base substitution' approach to enhance ionic conductivity in halide SEs.
  • To elucidate the underlying mechanism responsible for conductivity improvements.
  • To assess the potential of oxyhalide SEs for practical all-solid-state battery applications.

Main Methods:

  • Synthesized and characterized Li2ZrCl6 substituted with oxygen, sulfur, and fluorine.
  • Measured ionic conductivity of the synthesized materials.
  • Conducted systematic comparative studies to understand the role of anion sublattice structure and interstitial site stabilization.

Main Results:

  • Oxygen substitution in Li2ZrCl6 (trigonal, hcp) to form Li3.1ZrCl4.9O1.1 (monoclinic, ccp) increased ionic conductivity from 0.33 to 1.3 mS cm⁻¹.
  • Sulfur and fluorine substitutions did not yield significant improvements in ionic conductivity.
  • Energetic stabilization of interstitial sites for lithium ion migration was identified as the key factor for enhanced conductivity, not solely the ccp-like anion sublattice.

Conclusions:

  • Hard-base substitution, specifically oxygen incorporation, is an effective strategy for increasing ionic conductivity in halide SEs.
  • The stabilization of Li migration pathways is more critical than the anion arrangement alone for achieving high ionic conductivity.
  • Oxyhalide SEs show promise for future all-solid-state battery development.