Entropy-driven expansion of the thermodynamic stability of compositionally complex spinel oxides

Abstract

High-entropy ceramics have sparked renewed interest in compositionally complex ceramics since the first introduction in 2015. The kaleidoscopic array of compositions and structures harnessed by this idea has unlocked an unprecedented opportunity to tailor materials for specific applications, including catalysis, thermal barriers, and electrochemical energy storage. Within the family of oxides, a competition exists between rock-salt and spinel structures. The rock-salt structure is highly symmetrical, consisting of a single cation sublattice, while the spinel structure offers more flexibility to accommodate various cations in two distinct sublattices. Herein, we aimed at stabilizing and expanding the thermal stability range of the spinel-structured oxide, successfully synthesizing novel, single-phase, compositionally complex materials by capitalizing on entropy stabilization, all while avoiding the ubiquitous use of nickel and chrome, notorious for their negative environmental impact. The right combination of cations resulted in the synthesis of a seven-metal oxide that is thermally stable up to the remarkable temperature of 1473 K.