Tuning reduction conditions to understand and control Ni exsolution from Sr0.8La0.1Ca0.1Ti0.94Ni0.06O3−δ
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D3TA04817A.pdf
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1.8 MB
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Checksum (MD5)
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Author(s)
O'Leary, Willis
Giordano, Livia
Rupp, Jennifer L. M.
Date Issued
2023
Journal
Journal of Materials Chemistry A
Publisher
Royal Society of Chemistry (RSC)
Citation
O'Leary, Willis, Giordano, Livia and Rupp, Jennifer L. M. 2023. "Tuning reduction conditions to understand and control Ni exsolution from Sr0.8La0.1Ca0.1Ti0.94Ni0.06O3−δ." Journal of Materials Chemistry A, 11 (39).
Version
Final published version
Abstract
Ceramic-supported metal catalysts formed by exsolution of metal nanoparticles from perovskites are promising materials for energy and chemical conversion applications. However, our incomplete understanding of the exsolution mechanism presents a roadblock to engineering exsolution nanoparticle properties. We investigated the influence of reduction conditions on the properties of Ni nanoparticles exsolved on the fracture surfaces of Sr0.8La0.1Ca0.1Ti0.94Ni0.06O3−δ. We first carried out exsolution at 25 different temperatures and oxygen chemical potentials. We found that reduction at lower temperatures and moderate oxygen chemical potentials produced more numerous, smaller nanoparticles. We then fit our data to a LaMer nucleation model where the number of nanoparticles formed depends on Ni surface segregation, reduction of Ni-rich surfaces, and nanoparticle growth. Finally, we demonstrated prediction of the energetics of these processes with density functional theory calculations. Our experiments and modelling build understanding of the exsolution mechanism and are a step towards computational design of supported metal catalysts made via exsolution.
Subjects
General Materials Science
Renewable Energy, Sustainability and the Environment
General Chemistry
MIT Department
Massachusetts Institute of Technology. Department of Materials Science and Engineering
Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science
Terms of Use
Creative Commons Attribution-Noncommercial
Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1039/d3ta04817a
