Publication date: 10th April 2024
Metal nanoparticles on oxide surfaces hold considerable potential for application in heterogeneous catalysis and in electrocatalysis, particularly in the context of solid-state electrochemical devices such as fuel flexible fuel cells, electrolysers, and electrochemical membrane reactors. Exsolution is a process to achieve this modification of the solid support. It offers important advantages compared to conventional deposition of nanoparticles, the most prominent being the reduced tendency of the nanoparticles to agglomerate. Some insights into the structure, stoichiometry and functionality of individual material systems suitable for exsolution have already been gained, however, there is still a lack of knowledge in defect chemistry and the kinetics of exsolution.
From its size Ni2+ is expected to reside on the B-site positions of the perovskite structure of SrTiO3. However, B-site diffusion is known to be relatively slow because of the stable Ti-O-skeleton of the material which seems contradictory to the much faster exsolution process. Here, an interstitial diffusion mechanism for nickel and its dependency on different defects is investigated by density-functional theory (DFT) calculations as well as transient thermogravimetry.
Exsolution involves reduction of Ni2+ and the complementary oxidation of O2- which leaves the sample, resulting in a mass loss which can be tracked over time. With nickel diffusion being expected to be the dominant process diffusion information can be extracted from fitting this data. The studies are performed with systematic variation of several parameters, including the temperature, amount of nickel, amount of A-site and oxygen vacancies, and the particle sizes of the sample.
This approach aims to develop a more generalized understanding of the kinetics of exsolution, with the overarching goal of facilitating the tailored design of materials according to their applications.
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