High entropy oxide nanoparticles (HEO NPs) with multiple component elements possess improved stability and multiple uses for functional applications, including catalysis, data memory, and energy storage. However, the synthesis of homogenous HEO NPs containing five or more immiscible elements with a single-phase structure is still a great challenge due to the strict synthetic conditions. In particular, several synthesis methods of HEO NPs require extremely high temperatures. In this study, we demonstrate a low cost, facile, and effective method to synthesize three- to eight-element HEO nanoparticles by a combination of electrospinning and low-temperature ambient annealing. HEO NPs were generated by annealing nanofibers at 330 °C for 30 minutes under air conditions. The average size of the HEO nanoparticles was ∼30 nm and homogenous element distribution was obtained from post-electrospinning thermal decomposition. The synthesized HEO NPs exhibited magnetic properties with the highest saturation magnetization at 9.588 emu g −1 and the highest coercivity at 147.175 Oe for HEO NPs with four magnetic elements while integrating more nonmagnetic elements will suppress the magnetic response. This electrospun and low-temperature annealing method provides an easy and flexible design for nanoparticle composition and economic processing pathway, which offers a cost- and energy-effective, and high throughput entropy nanoparticle synthesis on a large scale.
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This content will become publicly available on July 3, 2025
From fabrication to mechanical properties: exploring high-entropy oxide thin films and coatings for high-temperature applications
High-entropy oxides (HEOs) containing five or more cations have garnered significant attention recently due to their vastly tunable compositional space, along with their remarkable physical and mechanical properties, exceptional thermal stability, and phase reversibility at elevated temperatures. These characteristics position HEOs as promising candidates for structural components and coatings in high-temperature applications. While much of the ongoing research on HEOs centers around understanding processing-structure relationships, there remains a dearth of knowledge concerning their mechanical properties, crucial for their prospective high-temperature applications. Whether in bulk form or as coatings, the efficacy of HEOs hinges on robust mechanical properties across a spectrum of temperatures, to ensure structural integrity, fracture resistance, and resilience to thermal stress. This review offers a succinct synthesis of recent advancements in HEO research, spanning from processing techniques to mechanical behaviors under extreme conditions. Emphasis is placed on three key aspects: (1) Investigating the influence of processing parameters on HEO crystal structures. (2) Analyzing the interplay between crystal structure and mechanical properties, elucidating deformation mechanisms. (3) Examining the mechanical behavior of HEOs under extreme temperatures and pressures. Through this review, we aim to illuminate the effective control of HEOs’ unique structures and mechanical properties, paving the way for their future applications in extreme environments.
more » « less- Award ID(s):
- 2104655
- PAR ID:
- 10528154
- Publisher / Repository:
- Frontiers
- Date Published:
- Journal Name:
- Frontiers in Coatings, Dyes and Interface Engineering
- Volume:
- 2
- ISSN:
- 2813-6861
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract As a new class of multi-principal component oxides with high chemical disorder, high-entropy oxides (HEOs) have attracted much attention. The stability and tunability of their structure and properties are of great interest and importance, but remain unclear. By using in situ synchrotron radiation X-ray diffraction, Raman spectroscopy, ultraviolet–visible absorption spectroscopy, and ex situ high-resolution transmission electron microscopy, here we show the existence of lattice distortion in the crystalline (Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2−δHEO according to the deviation of bond angles from the ideal values, and discover a pressure-induced continuous tuning of lattice distortion (bond angles) and band gap. As continuous bending of bond angles, pressure eventually induces breakdown of the long-range connectivity of lattice and causes amorphization. The amorphous state can be partially recovered upon decompression, forming glass–nanoceramic composite HEO. These results reveal the unexpected flexibility of the structure and properties of HEOs, which could promote the fundamental understanding and applications of HEOs.
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Abstract High entropy oxides (HEOs), based on the incorporation of multiple‐principal cations into the crystal lattice, offer the possibility to explore previously inaccessible oxide compositions and unconventional properties. Here it is demonstrated that despite the chemical complexity of HEOs external stimuli, such as epitaxial strain, can selectively stabilize certain magneto‐electronic states. Epitaxial (Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)3O4‐HEO thin films are grown in three different strain states: tensile, compressive, and relaxed. A unique coexistence of rocksalt and spinel‐HEO phases, which are fully coherent with no detectable chemical segregation, is revealed by transmission electron microscopy. This dual‐phase coexistence appears as a universal phenomenon in (Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)3O4epitaxial films. Prominent changes in the magnetic anisotropy and domain structure highlight the strain‐induced bidirectional control of magnetic properties in HEOs. When the films are relaxed, their magnetization behavior is isotropic, similar to that of bulk materials. However, under tensile strain, the hardness of the out‐of‐plane (OOP) axis increases significantly. On the other hand, compressive straining results in an easy OOP magnetization and a maze‐like magnetic domain structure, indicating the perpendicular magnetic anisotropy. Generally, this study emphasizes the adaptability of the high entropy design strategy, which, when combined with coherent strain engineering, opens additional prospects for fine‐tuning properties in oxides.
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null (Ed.)Ceramics derived from organic polymer precursors, which have exceptional mechanical and chemical properties that are stable up to temperatures slightly below 2000 °C, are referred to as polymer-derived ceramics (PDCs). These molecularly designed amorphous ceramics have the same high mechanical and chemical properties as conventional powder-based ceramics, but they also demonstrate improved oxidation resistance and creep resistance and low pyrolysis temperature. Since the early 1970s, PDCs have attracted widespread attention due to their unique microstructures, and the benefits of polymeric precursors for advanced manufacturing techniques. Depending on various doping elements, molecular configurations, and microstructures, PDCs may also be beneficial for electrochemical applications at elevated temperatures that exceed the applicability of other materials. However, the microstructural evolution, or the conversion, segregation, and decomposition of amorphous nanodomain structures, decreases the reliability of PDC products at temperatures above 1400 °C. This review investigates structure-related properties of PDC products at elevated temperatures close to or higher than 1000 °C, including manufacturing production, and challenges of high-temperature PDCs. Analysis and future outlook of high-temperature structural and electrical applications, such as fibers, ceramic matrix composites (CMCs), microelectromechanical systems (MEMSs), and sensors, within high-temperature regimes are also discussed.more » « less
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Abstract Developing stable and efficient electrocatalysts is vital for boosting oxygen evolution reaction (OER) rates in sustainable hydrogen production. High-entropy oxides (HEOs) consist of five or more metal cations, providing opportunities to tune their catalytic properties toward high OER efficiency. This work combines theoretical and experimental studies to scrutinize the OER activity and stability for spinel-type HEOs. Density functional theory confirms that randomly mixed metal sites show thermodynamic stability, with intermediate adsorption energies displaying wider distributions due to mixing-induced equatorial strain in active metal-oxygen bonds. The rapid sol-flame method is employed to synthesize HEO, comprising five 3d-transition metal cations, which exhibits superior OER activity and durability under alkaline conditions, outperforming lower-entropy oxides, even with partial surface oxidations. The study highlights that the enhanced activity of HEO is primarily attributed to the mixing of multiple elements, leading to strain effects near the active site, as well as surface composition and coverage.
