Publication date: 10th April 2024
In situ exsolution has emerged as an outstanding route for producing oxide-supported metal nanoparticles. A variety of transition-metal cations can be incorporated into the host lattice – typically a perovskite-oxide – under oxidising conditions and exsolved as metallic nanoclusters after reduction. Consistent and comprehensive descriptions of the thermodynamics and kinetics of this phenomenon are lacking, however.
Herein, supported by hybrid Density-Functional-Theory calculations, we propose a single model that explains diverse experimental observations; why transition-metal cations (but not host cations) exsolve from perovskite lattices upon reduction; why different transition-metal cations exsolve under different conditions; why the metal nanoparticles are embedded at the surface; why the oxide’s surface orientation affect behaviour; why exsolution occurs surprisingly rapidly at relatively low temperatures; and why the re-incorporation of exsolved species involves far longer times and much higher temperatures. Our model’s foundation is that the transition-metal cations are completely reduced within the perovskite lattice as the Fermi level is shifted upwards within the bandgap.[1] The calculations also emphasise the importance of oxygen vacancies and A-site vacancies. Our model provides a fundamental basis for improving existing, and creating new, exsolution catalysts.
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