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Defect structure in δ-Bi5PbY2O11.5.

Anna Borowska-Centkowska1, Xi Liu2, Marcin Krynski1

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This study reveals how oxide-ion vacancies in δ-Bi5PbY2O11.5 prefer to associate with lead (Pb2+) cations, influencing conductivity. Vacancy ordering and cation clustering were observed, with a preference for 〈100〉 alignment.

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Area of Science:

  • Solid-state chemistry
  • Materials science
  • Crystallography

Background:

  • The δ-Bi2O3 type phases are known for their high oxide-ion conductivity.
  • Understanding defect structures is crucial for optimizing ionic conductivity in solid electrolytes.
  • δ-Bi5PbY2O11.5 serves as a model system with a higher vacancy concentration than unsubstituted δ-Bi2O3.

Purpose of the Study:

  • To characterize the average and local defect structure of δ-Bi5PbY2O11.5.
  • To investigate oxide-ion vacancy ordering and cation-cation interactions.
  • To elucidate the relationship between defect structure and ionic transport.

Main Methods:

  • Conventional Rietveld analysis of neutron diffraction data.
  • Reverse Monte Carlo (RMC) analysis of total neutron scattering data.
  • Ab initio molecular dynamics (MD) simulations.

Main Results:

  • Oxide-ion vacancies exhibit a preference for association with Pb2+ cations.
  • Evidence of Pb2+ cation clustering was observed.
  • A non-random distribution of vacancy pair alignments with a preference for 〈100〉 ordering was identified.
  • Thermal variation in vacancy ordering and a predominance of oxide-ion jumps in the 〈100〉 direction were indicated by MD simulations.

Conclusions:

  • The defect structure of δ-Bi5PbY2O11.5 is characterized by preferential association of oxide-ion vacancies with Pb2+ cations and 〈100〉 ordering.
  • These findings provide insights into the mechanisms governing ionic conductivity in substituted δ-Bi2O3 phases.
  • The developed methodology allows for the study of vacancy ordering and cation interactions in complex oxide systems.