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Local Structure and Electronic State of Atomically Dispersed Pt Supported on Nanosized CeO2
journal contribution
posted on 2019-08-25, 20:29 authored by Matthew Kottwitz, Yuanyuan Li, Robert M. Palomino, Zongyuan Liu, Guangjin Wang, Qin Wu, Jiahao Huang, Janis Timoshenko, Sanjaya D. Senanayake, Mahalingam Balasubramanian, Deyu Lu, Ralph G. Nuzzo, Anatoly I. FrenkelSingle
atom catalysts (SACs) have shown high activity and selectivity
in a growing number of chemical reactions. Many efforts aimed at unveiling
the structure–property relationships underpinning these activities
and developing synthesis methods for obtaining SACs with the desired
structures are hindered by the paucity of experimental methods capable
of probing the attributes of local structure, electronic properties,
and interaction with supportfeatures that comprise key descriptors
of their activity. In this work, we describe a combination of experimental
and theoretical approaches that include photon and electron spectroscopy,
scattering, and imaging methods, linked by density functional theory
calculations, for providing detailed and comprehensive information
on the atomic structure and electronic properties of SACs. This characterization
toolbox is demonstrated here using a model single atom Pt/CeO2 catalyst prepared via a sol–gel-based synthesis method.
Isolated Pt atoms together with extra oxygen atoms passivate the (100)
surface of nanosized ceria. A detailed picture of the local structure
of Pt nearest environment emerges from this work involving the bonding
of isolated Pt2+ ions at the hollow sites of perturbed
(100) surface planes of the CeO2 support, as well as a
substantial (and heretofore unrecognized) strain within the CeO2 lattice in the immediate vicinity of the Pt centers. The
detailed information on structural attributes provided by our approach
is the key for understanding and improving the properties of SACs.
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Nanosized CeO 2 Single atom catalystsSACchemical reactionsimaging methodssynthesis methodsPt centersnanosized ceriaAtomically Dispersed PtMany effortsoxygen atoms passivateElectronic StateIsolated Pt atomscharacterization toolboxtheory calculationsCeO 2 latticeelectron spectroscopyCeO 2 supportLocal Structure
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