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Saeed S I Almishal1, Matthew Furst2, Yueze Tan2

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Controlling oxygen chemical potential in high-entropy oxides (HEOs) forces multivalent cations into divalent states. This discovery enables predicting HEO stability and synthesis, expanding material design possibilities.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Thermodynamics

Background:

  • High-entropy oxides (HEOs) exhibit complex thermodynamics influenced by factors beyond temperature.
  • Oxygen chemical potential is a critical, yet often overlooked, variable in HEO systems.
  • Understanding cation valence states is crucial for predicting HEO properties and stability.

Purpose of the Study:

  • To experimentally demonstrate the influence of oxygen chemical potential on cation valence in rock salt HEOs.
  • To develop a predictive framework for HEO stability and synthesizability.
  • To explore new HEO compositions with tunable properties.

Main Methods:

  • Experimental control of oxygen chemical potential to influence cation valence.
  • Construction of preferred valence phase diagrams and enthalpic stability maps.
  • Synthesis and characterization of equimolar rock salt HEOs using XRD, XRF, EDS, and XAFS.
  • Atomistic calculations with machine learning interatomic potentials.

Main Results:

  • Demonstrated coercion of multivalent cations (Mn, Fe) into predominantly divalent states in rock salt HEOs by controlling oxygen chemical potential.
  • Successfully synthesized seven new equimolar, single-phase rock salt HEOs.
  • Validated homogeneous cation distribution and confirmed divalent cation states.
  • Developed a preferred valence phase diagram and an enthalpic stability map.

Conclusions:

  • Oxygen chemical potential is a key thermodynamic parameter for HEO design and synthesis.
  • Oxygen chemical potential overlap serves as a crucial descriptor for predicting HEO stability.
  • The developed framework is broadly applicable to various HEO compositions and structures.