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Abstract Two new high-entropy ceramics (HECs) in the weberite and fergusonite structures, along with the unexpected formation of ordered pyrochlore phases with ultrahigh-entropy compositions and an abrupt pyrochlore-weberite transition, are discovered in a 21-component oxide system. While the Gibbs phase rule allows 21 equilibrium phases, 9 out of the 13 compositions examined possess single HEC phases (with ultrahigh ideal configurational entropies: ∼2.7 k B per cation or higher on one sublattice in most cases). Notably, (15RE 1/15 )(Nb 1/2 Ta 1/2 )O 4 possess a single monoclinic fergusonite (C2/ c ) phase, and (15RE 1/15 ) 3 (Nb 1/2 Ta 1/2 ) 1 O 7 form a single orthorhombic (C222 1 ) weberite phase, where 15RE 1/15 represents Sc 1/15 Y 1/15 La 1/15 Pr 1/15 Nd 1/15 Sm 1/15 Eu 1/15 Gd 1/15 Tb 1/15 Dy 1/15 Ho 1/15 Er 1/15 Tm 1/15 Yb 1/15 Lu 1/15 . Moreover, a series of eight (15RE 1/15 ) 2+ x (Ti 1/4 Zr 1/4 Ce 1/4 H 1/4 ) 2−2 x (Nb 1/2 Ta 1/2 ) x O 7 specimens all exhibit single phases, where a pyrochlore-weberite transition occurs within 0.75 < x < 0.8125. This cubic-to-orthorhombic transition does not change the temperature-dependent thermal conductivity appreciably, as the amorphous limit may have already been achieved in the ultrahigh-entropy 21-component oxides. These discoveries expand the diversity and complexity of HECs, towards many-component compositionally complex ceramics (CCCs) and ultrahigh-entropy ceramics.
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Phase stability and cation partitioning in compositionally complex rare earth aluminates and aluminate‐zirconate mixtures
Abstract Multicomponent oxides have received significant recent attention due to their potential for improved property tunability. In simple structures, compositionally complex oxides can be stabilized by increased configurational entropy and are sometimes called “high entropy” ceramics. In phases with multiple cation sublattices or complex stoichiometries, it is more difficult to achieve high configurational entropy. However, there is limited knowledge about the factors influencing stability and solubility limits in many systems. This study investigated the limits on the stability of rare earth (RE) aluminates containing mixtures of RE cations including Gd, La, Nd, Yb, and Y in cases where (i) a fixed RE:Al ratio attempts to constrain the material into a single‐phase aluminate or (ii) a two‐phase aluminate, and in equilibrium with RE zirconates that readily dissolve multiple RE3+. The results show that it is difficult to form single‐phase, equimolar mixed‐RE aluminates encompassing a range of RE3+sizes. Instead, the RE3+selectively partition into specific phases based on RE‐size trends in the constituent binary systems. The results are discussed in terms of the phase stability and cation partition trends and potential applications.
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- Award ID(s):
- 2011401
- PAR ID:
- 10444050
- Publisher / Repository:
- Wiley-Blackwell
- Date Published:
- Journal Name:
- Journal of the American Ceramic Society
- Volume:
- 107
- Issue:
- 3
- ISSN:
- 0002-7820
- Format(s):
- Medium: X Size: p. 1760-1775
- Size(s):
- p. 1760-1775
- Sponsoring Org:
- National Science Foundation
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