Thermodynamics-inspired high-entropy oxide synthesis

Saeed S. I. Almishal (), Matthew Furst, Yueze Tan, Jacob T. Sivak, Gerald Bejger, Joseph Petruska, Sai Venkata Gayathri Ayyagari, Dhiya Srikanth, Nasim Alem, Christina M. Rost, Susan B. Sinnott, Long-Qing Chen and Jon-Paul Maria
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Saeed S. I. Almishal: The Pennsylvania State University
Matthew Furst: The Pennsylvania State University
Yueze Tan: The Pennsylvania State University
Jacob T. Sivak: The Pennsylvania State University
Gerald Bejger: Virginia Polytechnic Institute and State University
Joseph Petruska: The Pennsylvania State University
Sai Venkata Gayathri Ayyagari: The Pennsylvania State University
Dhiya Srikanth: The Pennsylvania State University
Nasim Alem: The Pennsylvania State University
Christina M. Rost: Virginia Polytechnic Institute and State University
Susan B. Sinnott: The Pennsylvania State University
Long-Qing Chen: The Pennsylvania State University
Jon-Paul Maria: The Pennsylvania State University

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract High-entropy oxide (HEO) thermodynamics transcend temperature-centric approaches, spanning a multidimensional landscape where oxygen chemical potential plays a decisive role. Here, we experimentally demonstrate how controlling the oxygen chemical potential coerces multivalent cations into divalent states in rock salt HEOs. We construct a preferred valence phase diagram based on thermodynamic stability and equilibrium analysis, alongside a high throughput enthalpic stability map derived from atomistic calculations leveraging machine learning interatomic potentials. We identify and synthesize seven equimolar, single-phase rock salt compositions incorporating Mn, Fe, or both, as confirmed by X-ray diffraction and fluorescence. Energy-dispersive X-ray spectroscopy confirms homogeneous cation distribution, whereas X-ray absorption fine structure analysis reveals predominantly divalent Mn and Fe states, despite their inherent multivalent tendencies. Ultimately, we introduce oxygen chemical potential overlap as a key complementary descriptor for predicting HEO stability and synthesizability. Although we focus on rock salt HEOs, our methods are chemically and structurally agnostic, providing a broadly adaptable framework for navigating HEOs thermodynamics and enabling a broader compositional range with contemporary property interest.

Date: 2025
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DOI: 10.1038/s41467-025-63567-z

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