Linking Macroscopic and Nanoscopic Ionic Conductivity: A Semiempirical Framework for Characterizing Grain Boundary Conductivity in Polycrystalline Ceramics

William J. Bowman, Amith Darbal, Peter A. Crozier

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

Abstract

Understanding the chemical and charge transport properties of grain boundaries (GBs) with high point defect concentrations (beyond the dilute solution limit) in polycrystalline materials is critical for developing ion-conducting solids for electrochemical energy conversion and storage. Elucidation and optimization of GBs are hindered by large variations in atomic structure, composition, and chemistry within nanometers or Ångstroms of the GB interface, which limits a fundamental understanding of electrical transport across and along GBs. Here we employ a novel correlated approach that is generally applicable to polycrystalline materials whose properties are affected by GB composition or chemistry. We demonstrate the connection between the nanoscopic chemical and transport properties of individual boundaries and the macroscopic ionic conductivity in oxygen-conducting Pr0.04Gd0.11Ce0.85O2-δ. The key finding is that GBs with higher solute concentration have lower activation energy for cross-GB ion conduction through a polycrystalline conductor. The resultant semiempirical framework presented here provides a tool for understanding, designing and optimizing polycrystalline ionic conductors.

Original languageEnglish (US)
Pages (from-to)507-517
Number of pages11
JournalACS Applied Materials and Interfaces
Volume12
Issue number1
DOIs
StatePublished - Jan 8 2020

Keywords

  • aberration-corrected scanning transmission electron microscopy
  • correlated electron microscopy
  • electroceramics
  • electron energy-loss spectroscopy
  • grain boundaries
  • ionic conductivity
  • precession electron diffraction

ASJC Scopus subject areas

  • Materials Science(all)

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