21-Component compositionally complex ceramics: Discovery of ultrahigh-entropy weberite and fergusonite phases and a pyrochlore-weberite transition

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 rul...

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Bibliographic Details
Published in:Journal of advanced ceramics 2022-04, Vol.11 (4), p.641-655
Main Authors: Qin, Mingde, Vega, Heidy, Zhang, Dawei, Adapa, Sarath, Wright, Andrew J., Chen, Renkun, Luo, Jian
Format: Article
Language:English
Subjects:
Ceramic materials
Ceramics
Characterization and Evaluation of Materials
Chemistry and Materials Science
Complexity
Composites
Composition
Electric properties
Entropy
Equilibrium
Fluorides
Glass
Materials Science
Nanotechnology
Natural Materials
Phase rule
Phases
Pyrochlores
Research Article
Structural Materials
Temperature dependence
Thermal conductivity
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Summary: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.
ISSN:2226-4108
2227-8508
DOI:10.1007/s40145-022-0575-5