Reducing the Irreducible : Dispersed Metal Atoms Facilitate Reduction of Irreducible Oxides
Korpelin, V., Melander, M. M., & Honkala, K. (2022). Reducing the Irreducible : Dispersed Metal Atoms Facilitate Reduction of Irreducible Oxides. Journal of Physical Chemistry C, 126(2), 933-945. https://doi.org/10.1021/acs.jpcc.1c08979
Published inJournal of Physical Chemistry C
DisciplineNanoscience CenterFysikaalinen kemiaResurssiviisausyhteisöNanoscience CenterPhysical ChemistrySchool of Resource Wisdom
© 2022 the Authors
Oxide reducibility is a central concept quantifying the role of the support in catalysis. While reducible oxides are often considered catalytically active, irreducible oxides are seen as inert supports. Enhancing the reducibility of irreducible oxides has, however, emerged as an effective way to increase their catalytic activity while retaining their inherent thermal stability. In this work, we focus on the prospect of using single metal atoms to increase the reducibility of a prototypical irreducible oxide, zirconia. Based on extensive self-consistent DFT+U calculations, we demonstrate that single metal atoms significantly improve and tune the surface reducibility of zirconia. Detailed analysis of the observed single atom induced reducibility allows us to attribute the enhanced reducibility to strong interactions between the metal atom and the electrons trapped in the vacancy and d–p orbital interactions between the metal atom and oxygen. This analysis enables transferring the obtained theoretical understanding to other irreducible oxides as well. The detailed understanding of how oxide reducibility can be tuned offers precise control over the catalytic properties of metal oxides. ...
PublisherAmerican Chemical Society (ACS)
Publication in research information system
MetadataShow full item record
Related funder(s)Academy of Finland
Funding program(s)Academy Project, AoF; Postdoctoral Researcher, AoF
Additional information about fundingThe work was supported by the Academy of Finland through Projects 277222 (V.K. and K.H.), 307853 (M.M.M.), and 317739 (M.M.M. and K.H.).
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