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When atoms gain or lose electrons to achieve a more stable electron configuration they form ions. Ionic bonds are electrostatic attractions between ions with opposite charges. Ionic compounds are rigid and brittle when solid and may dissociate into their constituent ions in water. Covalent compounds, by contrast, remain intact unless a chemical reaction breaks them.
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Substances that undergo either a physical or a chemical change in solution to yield ions that can conduct electricity are called electrolytes. If a substance yields ions in solution, that is, if the compound undergoes 100% dissociation, then the substance is a strong electrolyte. Complete dissociation is indicated by a single forward arrow. For example, water-soluble ionic compounds like sodium chloride dissociate into sodium cations and chloride anions in aqueous solution.
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Ionic Conduction through Reaction Products at the Electrolyte-Electrode Interface in All-Solid-State Li+ Batteries.

Chuhong Wang1, Koutarou Aoyagi1,2, Muratahan Aykol3

  • 1Department of Materials Science and Engineering, Johns Hopkins University, Baltimore, Maryland 21218, United States.

ACS Applied Materials & Interfaces
|December 1, 2020
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Summary

Solid-state lithium-ion batteries face challenges in maintaining high performance due to electrode-electrolyte interface issues. This study reveals that ion conduction through interface product phases often limits battery rate capability.

Keywords:
active learning interatomic potentialsfirst-principles calculationsinterface stabilitylithium ionic conductionmolecular dynamicssolid electrolyte−electrode interphases

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • All-solid-state lithium-ion batteries offer enhanced safety and energy density.
  • Maintaining high rate capability in these batteries is hindered by electrode-electrolyte interface resistance.
  • Reactivity at interfaces leads to degradation and limits long-term performance.

Purpose of the Study:

  • To investigate the interfacial phenomena limiting rate capability in all-solid-state lithium-ion batteries.
  • To identify the critical pathways for lithium-ion diffusion at electrode-electrolyte interfaces.
  • To understand the role of product phases formed at interfaces in battery performance.

Main Methods:

  • Examined interfaces between eight solid electrolytes (e.g., garnet, LiPON, LGPS) and seven electrode materials (e.g., NCM cathode, Li metal anode).
  • Utilized density functional theory (DFT) with statistical sampling of phase diagrams to account for errors, metastability, and temperature.
  • Employed machine-learned interatomic potentials for on-the-fly evaluation of lithium-ion conductivities in interfacial product phases.

Main Results:

  • Identified rapid lithium-ion diffusion pathways through metastable product phases at interfaces.
  • Nearly all evaluated electrode-electrolyte interfaces showed limited lithium-ion conduction within the interphase product layers.
  • The formation of specific product phases significantly impacts interfacial resistance.

Conclusions:

  • Lithium-ion conduction through interfacial product phases is predicted to be the rate-limiting step for most all-solid-state battery configurations.
  • Understanding and mitigating interfacial resistance is crucial for advancing high-rate solid-state battery technology.
  • This research provides fundamental insights into interfacial chemistry governing solid-state battery performance.