Exsolution-Driven Surface Transformation in the Host Oxide
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jiayue_nanolett_2022.pdf
Description
Accepted version
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4.33 MB
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Author(s)
Wang, Jiayue
Kumar, Abinash
Wardini, Jenna L
Zhang, Zhan
Zhou, Hua
Crumlin, Ethan J
Sadowski, Jerzy T
Woller, Kevin B
Bowman, William J
LeBeau, James M
Date Issued
2022
Journal
Nano Letters
Publisher
American Chemical Society (ACS)
Citation
Wang, Jiayue, Kumar, Abinash, Wardini, Jenna L, Zhang, Zhan, Zhou, Hua et al. 2022. "Exsolution-Driven Surface Transformation in the Host Oxide." Nano Letters, 22 (13).
Version
Author's final manuscript
Abstract
Exsolution synthesizes self-assembled metal nanoparticle catalysts via phase precipitation. An overlooked aspect in this method thus far is how exsolution affects the host oxide surface chemistry and structure. Such information is critical as the oxide itself can also contribute to the overall catalytic activity. Combining X-ray and electron probes, we investigated the surface transformation of thin-film SrTi0.65Fe0.35O3 during Fe0 exsolution. We found that exsolution generates a highly Fe-deficient near-surface layer of about 2 nm thick. Moreover, the originally single-crystalline oxide near-surface region became partially polycrystalline after exsolution. Such drastic transformations at the surface of the oxide are important because the exsolution-induced nonstoichiometry and grain boundaries can alter the oxide ion transport and oxygen exchange kinetics and, hence, the catalytic activity toward water splitting or hydrogen oxidation reactions. These findings highlight the need to consider the exsolved oxide surface, in addition to the metal nanoparticles, in designing the exsolved nanocatalysts.
MIT Department
Massachusetts Institute of Technology. Department of Nuclear Science and Engineering
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DOI of Published Version
https://doi.org/10.1021/ACS.NANOLETT.2C01439
