In Situ High-Temperature Structural Analysis of High-Entropy Rare-Earth Sesquioxides

Matheus Pianassola; Kaden Anderson; Can Agca; Chris J. Benmore; Jake W. McMurray; Jöerg C. Neuefeind; Charles Melcher; Mariya Zhuravleva

doi:10.1021/acs.chemmater.2c03088

In Situ High-Temperature Structural Analysis of High-Entropy Rare-Earth Sesquioxides

Matheus Pianassola, Kaden Anderson, Can Agca, Chris J. Benmore, Jake W. McMurray, Jöerg C. Neuefeind, Charles Melcher, Mariya Zhuravleva

Powder Diffraction

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Abstract

High-entropy rare-earth (RE) sesquioxides (RE₂O₃) containing five cations in equimolar amounts have been investigated for a variety of applications, but little is known about their polymorphic behavior and coefficient of thermal expansion. Here, we evaluate the effect of the average ionic radius (AIR) on the polymorphism of high-entropy RE₂O₃. Powder samples of compositions 1 (Lu,Y,Ho,Nd,La)₂O₃ (AIR = 0.938 Å) and 2 (Gd,Eu,Sm,Nd,La)₂O₃ (AIR = 0.982 Å) were synthesized via a wet chemical method, and bead samples were prepared for aerodynamic levitation by melting the powders in a copper hearth. Structural transitions were monitored upon cooling from the melt to 1000 °C via in situ X-ray diffraction on aerodynamically levitated samples. The phase evolution was liquid, hexagonal H-type, and monoclinic B-type for composition 1 and liquid, cubic X-type, H-type, and B-type for composition 2. Based on their AIR, the general polymorphic transformations of the high-entropy RE₂O₃ follow the trend of single-RE RE₂O₃, but the transition temperatures differ from those of single-RE RE₂O₃.

Original language	English
Pages (from-to)	1116-1124
Number of pages	9
Journal	Chemistry of Materials
Volume	35
Issue number	3
DOIs	https://doi.org/10.1021/acs.chemmater.2c03088
State	Published - Feb 14 2023

Funding

This work was supported by the National Science Foundation (DMR 1846935). This material is partially based upon work supported by the U.S. Department of Homeland Security under grant award number 20CWDARI00037-01-00. The views and conclusions contained in this document are those of the authors and should not be interpreted as necessarily representing the official policies, either expressed or implied, of the U.S. Department of Homeland Security. Powder XRD was performed at the Institute for Advanced Materials & Manufacturing (IAMM) Diffraction Facility, located at the University of Tennessee, Knoxville. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under contract no. DE-AC02-06CH11357.

Funders	Funder number
Institute for Advanced Materials & Manufacturing
National Science Foundation	DMR 1846935
U.S. Department of Energy	DE-AC02-06CH11357
U.S. Department of Homeland Security	20CWDARI00037-01-00
Office of Science
Argonne National Laboratory
Oak Ridge National Laboratory
University of Tennessee

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title = "In Situ High-Temperature Structural Analysis of High-Entropy Rare-Earth Sesquioxides",

abstract = "High-entropy rare-earth (RE) sesquioxides (RE2O3) containing five cations in equimolar amounts have been investigated for a variety of applications, but little is known about their polymorphic behavior and coefficient of thermal expansion. Here, we evaluate the effect of the average ionic radius (AIR) on the polymorphism of high-entropy RE2O3. Powder samples of compositions 1 (Lu,Y,Ho,Nd,La)2O3 (AIR = 0.938 {\AA}) and 2 (Gd,Eu,Sm,Nd,La)2O3 (AIR = 0.982 {\AA}) were synthesized via a wet chemical method, and bead samples were prepared for aerodynamic levitation by melting the powders in a copper hearth. Structural transitions were monitored upon cooling from the melt to 1000 °C via in situ X-ray diffraction on aerodynamically levitated samples. The phase evolution was liquid, hexagonal H-type, and monoclinic B-type for composition 1 and liquid, cubic X-type, H-type, and B-type for composition 2. Based on their AIR, the general polymorphic transformations of the high-entropy RE2O3 follow the trend of single-RE RE2O3, but the transition temperatures differ from those of single-RE RE2O3.",

author = "Matheus Pianassola and Kaden Anderson and Can Agca and Benmore, {Chris J.} and McMurray, {Jake W.} and Neuefeind, {J{\"o}erg C.} and Charles Melcher and Mariya Zhuravleva",

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AU - Anderson, Kaden

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AU - McMurray, Jake W.

AU - Neuefeind, Jöerg C.

AU - Melcher, Charles

AU - Zhuravleva, Mariya

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N2 - High-entropy rare-earth (RE) sesquioxides (RE2O3) containing five cations in equimolar amounts have been investigated for a variety of applications, but little is known about their polymorphic behavior and coefficient of thermal expansion. Here, we evaluate the effect of the average ionic radius (AIR) on the polymorphism of high-entropy RE2O3. Powder samples of compositions 1 (Lu,Y,Ho,Nd,La)2O3 (AIR = 0.938 Å) and 2 (Gd,Eu,Sm,Nd,La)2O3 (AIR = 0.982 Å) were synthesized via a wet chemical method, and bead samples were prepared for aerodynamic levitation by melting the powders in a copper hearth. Structural transitions were monitored upon cooling from the melt to 1000 °C via in situ X-ray diffraction on aerodynamically levitated samples. The phase evolution was liquid, hexagonal H-type, and monoclinic B-type for composition 1 and liquid, cubic X-type, H-type, and B-type for composition 2. Based on their AIR, the general polymorphic transformations of the high-entropy RE2O3 follow the trend of single-RE RE2O3, but the transition temperatures differ from those of single-RE RE2O3.

AB - High-entropy rare-earth (RE) sesquioxides (RE2O3) containing five cations in equimolar amounts have been investigated for a variety of applications, but little is known about their polymorphic behavior and coefficient of thermal expansion. Here, we evaluate the effect of the average ionic radius (AIR) on the polymorphism of high-entropy RE2O3. Powder samples of compositions 1 (Lu,Y,Ho,Nd,La)2O3 (AIR = 0.938 Å) and 2 (Gd,Eu,Sm,Nd,La)2O3 (AIR = 0.982 Å) were synthesized via a wet chemical method, and bead samples were prepared for aerodynamic levitation by melting the powders in a copper hearth. Structural transitions were monitored upon cooling from the melt to 1000 °C via in situ X-ray diffraction on aerodynamically levitated samples. The phase evolution was liquid, hexagonal H-type, and monoclinic B-type for composition 1 and liquid, cubic X-type, H-type, and B-type for composition 2. Based on their AIR, the general polymorphic transformations of the high-entropy RE2O3 follow the trend of single-RE RE2O3, but the transition temperatures differ from those of single-RE RE2O3.

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In Situ High-Temperature Structural Analysis of High-Entropy Rare-Earth Sesquioxides

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