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dc.contributor.authorWang, Jiayue
dc.contributor.authorKalaev, Dmitri
dc.contributor.authorYang, Jing
dc.contributor.authorWaluyo, Iradwikanari
dc.contributor.authorHunt, Adrian
dc.contributor.authorSadowski, Jerzy T
dc.contributor.authorTuller, Harry L
dc.contributor.authorYildiz, Bilge
dc.date.accessioned2023-01-25T19:21:00Z
dc.date.available2023-01-25T19:21:00Z
dc.date.issued2023-01-10
dc.identifier.urihttps://hdl.handle.net/1721.1/147714
dc.description.abstractExsolution is a recent advancement for fabricating oxide-supported metal nanoparticle catalysts via phase precipitation out of a host oxide. A fundamental understanding and control of the exsolution kinetics are needed to engineer exsolved nanoparticles to obtain higher catalytic activity toward clean energy and fuel conversion. Since oxygen release via oxygen vacancy formation in the host oxide is behind oxide reduction and metal exsolution, we hypothesize that the kinetics of metal exsolution should depend on the kinetics of oxygen release, in addition to the kinetics of metal cation diffusion. Here, we probe the surface exsolution kinetics both experimentally and theoretically using thin-film perovskite SrTi0.65Fe0.35O3 (STF) as a model system. We quantitatively demonstrated that in this system the surface oxygen release governs the metal nanoparticle exsolution kinetics. As a result, by increasing the oxygen release rate in STF, either by reducing the sample thickness or by increasing the surface reactivity, one can effectively accelerate the Fe0 exsolution kinetics. Fast oxygen release kinetics in STF not only shortened the prereduction time prior to the exsolution onset, but also increased the total quantity of exsolved Fe0 over time, which agrees well with the predictions from our analytical kinetic modeling. The consistency between the results obtained from in situ experiments and analytical modeling provides a predictive capability for tailoring exsolution, and highlights the importance of engineering host oxide surface oxygen release kinetics in designing exsolved nanocatalysts.en_US
dc.language.isoen
dc.publisherAmerican Chemical Society (ACS)en_US
dc.relation.isversionof10.1021/jacs.2c10256en_US
dc.rightsCreative Commons Attribution-Noncommercial-Share Alikeen_US
dc.rights.urihttp://creativecommons.org/licenses/by-nc-sa/4.0/en_US
dc.sourceMIT web domainen_US
dc.titleFast Surface Oxygen Release Kinetics Accelerate Nanoparticle Exsolution in Perovskite Oxidesen_US
dc.typeArticleen_US
dc.identifier.citationWang, Jiayue, Kalaev, Dmitri, Yang, Jing, Waluyo, Iradwikanari, Hunt, Adrian et al. 2023. "Fast Surface Oxygen Release Kinetics Accelerate Nanoparticle Exsolution in Perovskite Oxides." Journal of the American Chemical Society.
dc.contributor.departmentMassachusetts Institute of Technology. Department of Nuclear Science and Engineeringen_US
dc.relation.journalJournal of the American Chemical Societyen_US
dc.eprint.versionAuthor's final manuscripten_US
dc.type.urihttp://purl.org/eprint/type/JournalArticleen_US
eprint.statushttp://purl.org/eprint/status/PeerRevieweden_US
dc.date.updated2023-01-25T18:38:17Z
dspace.orderedauthorsWang, J; Kalaev, D; Yang, J; Waluyo, I; Hunt, A; Sadowski, JT; Tuller, HL; Yildiz, Ben_US
dspace.date.submission2023-01-25T18:38:22Z
mit.licenseOPEN_ACCESS_POLICY
mit.metadata.statusAuthority Work and Publication Information Neededen_US


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