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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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When an electric field passes from one homogeneous medium to another, crossing the boundary between the two mediums imparts a discontinuity in the electric field. This results in electrostatic boundary conditions that depend on the type of mediums the field propagates through.
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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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A type of Lewis acid-base chemistry involves the formation of a complex ion (or a coordination complex) comprising a central atom, typically a transition metal cation, surrounded by ions or molecules called ligands. These ligands can be neutral molecules like H2O or NH3, or ions such as CN− or OH−. Often, the ligands act as Lewis bases, donating a pair of electrons to the central atom. These types of Lewis acid-base reactions are examples of a broad subdiscipline called coordination...
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Direct correlation between void formation and lithium dendrite growth in solid-state electrolytes with interlayers.

Vikalp Raj1, Victor Venturi2, Varun R Kankanallu1

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Metallic interlayers prevent void growth, a precursor to lithium dendrites in solid-state batteries. This enhances dendrite tolerance and battery safety by stabilizing the lithium metal anode interface.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Solid-state Li-ion batteries promise higher energy density and safety compared to liquid electrolyte counterparts.
  • Lithium dendrite growth across solid-state electrolytes causes premature cell failure, hindering practical application.
  • Understanding interfacial phenomena is crucial for overcoming dendrite issues in solid-state batteries.

Purpose of the Study:

  • To investigate the role of interfacial void growth in lithium dendrite formation in solid-state batteries.
  • To evaluate the effectiveness of metallic interlayers in mitigating void and dendrite growth.
  • To explore the relationship between interlayer properties and lithium vacancy accumulation.

Main Methods:

  • Fabrication of solid-state Li half-cells utilizing garnet-based solid electrolytes and lithium metal anodes.
  • Incorporation of metallic interlayers between the solid electrolyte and lithium anode.
  • In-situ observation of interfacial phenomena and dendrite growth under electrochemical cycling.
  • Computational modeling to assess thermodynamic and kinetic barriers for lithium vacancy accumulation.

Main Results:

  • Interfacial void growth was observed to precede lithium dendrite nucleation and propagation.
  • Void growth initiated at approximately two-thirds of the critical current density for dendrite formation.
  • Metallic interlayers with higher critical current densities exhibited greater thermodynamic and kinetic barriers against lithium vacancy accumulation.
  • Interfacial modification with metallic interlayers significantly reduced void formation and improved dendrite tolerance.

Conclusions:

  • Void growth at the lithium anode/solid electrolyte interface is a critical precursor to dendrite formation.
  • Metallic interlayers effectively suppress void growth by increasing barriers to lithium vacancy accumulation.
  • Interfacial engineering with suitable metallic interlayers enhances the dendrite growth tolerance of solid-state electrolytes, improving battery safety and longevity.