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Two new high-entropy ceramics (HECs) in the weberite and fergusonitestructures, along with unexpected formation of ordered pyrochlore phases withultrahigh-entropy compositions and an abrupt pyrochlore-weberite transition,are discovered in a 21-component oxide system. While the Gibbs phase ruleallows 21 equilibrium phases, nine out of the 13 compositions examined possesssingle HEC phases (with ultrahigh ideal configurational entropies: ~2.7kB percation or higher on one sublattice in most cases). Notably,(15RE1/15)(Nb1/2Ta1/2)O4 possess a single monoclinic fergusonite (C2/c) phaseand (15RE1/15)3(Nb1/2Ta1/2)1O7 form a single orthorhombic (C2221) weberitephase, where 15RE1/15 representsSc1/15Y1/15La1/15Pr1/15Nd1/15Sm1/15Eu1/15Gd1/15Tb1/15Dy1/15Ho1/15Er1/15Tm1/15Yb1/15Lu1/15.Moreover, a series of eight(15RE1/15)2+x(Ti1/4Zr1/4Ce1/4Hf1/4)2-2x(Nb1/2Ta1/2)xO7 specimens all exhibitsingle phases, where a pyrochlore-weberite transition occurs within 0.75 < x <0.8125. This cubic-to-orthorhombic transition does not change thetemperature-dependent thermal conductivity appreciably, as the amorphous limitmay have already been achieved in the ultrahigh-entropy 21-component oxides.These discoveries expand the diversity and complexity of HECs, towardsmany-component compositionally complex ceramics (CCCs) and ultrahigh-entropyceramics.

21-Component Compositionally Complex Ceramics: Discovery of Ultrahigh-Entropy Weberite and Fergusonite Phases and a Pyrochlore-Weberite Transition