Accurate Prediction of Oxygen Vacancy Concentration with Disordered A-Site Cations in High-Entropy Perovskite Oxides: Article No. 29

Jiyun Park, Boyuan Xu, Jie Pan, Dawei Zhang, Stephan Lany, Xingbo Liu, Jian Luo, Yue Qi

Research output: Contribution to journalArticlepeer-review

9 Scopus Citations

Abstract

Entropic stabilized ABO3 perovskite oxides promise many applications, including the two-step solar thermochemical hydrogen (STCH) production. Using binary and quaternary A-site mixed {A}FeO3 as a model system, we reveal that as more cation types, especially above four, are mixed on the A-site, the cell lattice becomes more cubic-like but the local Fe–O octahedrons are more distorted. By comparing four different Density Functional Theory-informed statistical models with experiments, we show that the oxygen vacancy formation energies (EVf) distribution and the vacancy interactions must be considered to predict the oxygen non-stoichiometry (δ) accurately. For STCH applications, the EVf distribution, including both the average and the spread, can be optimized jointly to improve Δδ (difference of δ between the two-step conditions) in some hydrogen production levels. This model can be used to predict the range of water splitting that can be thermodynamically improved by mixing cations in {A}FeO3 perovskites.

Original languageAmerican English
Article number29
Number of pages13
Journalnpj Computational Materials
Volume9
Issue number1
DOIs
StatePublished - 2023

Bibliographical note

Publisher Copyright:
© 2023, The Author(s).

NREL Publication Number

  • NREL/JA-5K00-84166

Keywords

  • cations
  • oxygen vacancy formation energies
  • perovskite
  • perovskite oxides
  • solar thermochemical hydrogen

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