Thermodynamics-Inspired High-Entropy Oxide Synthesis
Fuente:
arXiv
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| Autori principali: | , , , , , , , , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2025
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| _version_ | 1866914017770995712 |
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| author | Almishal, Saeed S. I. Furst, Matthew Tan, Yueze Sivak, Jacob T. Bejger, Gerald Srikanth, Dhiya Petruska, Joseph Rost, Christina M. Sinnott, Susan B. Chen, Long-Qing Maria, Jon-Paul |
| author_facet | Almishal, Saeed S. I. Furst, Matthew Tan, Yueze Sivak, Jacob T. Bejger, Gerald Srikanth, Dhiya Petruska, Joseph Rost, Christina M. Sinnott, Susan B. Chen, Long-Qing Maria, Jon-Paul |
| contents | 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 that accommodate multivalent Mn, Fe, or both, as confirmed by X-ray diffraction and fluorescence. X-ray absorption fine structure spectra reveal predominantly divalent cations. Ultimately, we introduce oxygen chemical potential overlap as a key complementary descriptor 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2503_07865 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Thermodynamics-Inspired High-Entropy Oxide Synthesis Almishal, Saeed S. I. Furst, Matthew Tan, Yueze Sivak, Jacob T. Bejger, Gerald Srikanth, Dhiya Petruska, Joseph Rost, Christina M. Sinnott, Susan B. Chen, Long-Qing Maria, Jon-Paul Materials Science 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 that accommodate multivalent Mn, Fe, or both, as confirmed by X-ray diffraction and fluorescence. X-ray absorption fine structure spectra reveal predominantly divalent cations. Ultimately, we introduce oxygen chemical potential overlap as a key complementary descriptor 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. |
| title | Thermodynamics-Inspired High-Entropy Oxide Synthesis |
| topic | Materials Science |
| url | https://arxiv.org/abs/2503.07865 |