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Active sites of atomically dispersed Pt supported on Gd-doped ceria with improved low temperature performance for CO oxidation

Li, Yuanyuan (författare)
Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook NY 11794 USA; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge TN 37831 USA
Wang, Haodong (författare)
Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook NY 11794 USA
Song, Haohong (författare)
Interdisciplinary Materials Science, Vanderbilt University, Nashville TN 37235 USA
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Rui, Ning (författare)
Chemistry Division, Brookhaven National Laboratory, Upton NY 11973 USA
Kottwitz, Matthew (författare)
Department of Chemistry, University of Illinois, Urbana IL 61801 USA
Senanayake, Sanjaya D. (författare)
Chemistry Division, Brookhaven National Laboratory, Upton NY 11973 USA
Nuzzo, Ralph G. (författare)
KTH,Yt- och korrosionsvetenskap,Department of Chemistry, University of Illinois, Urbana IL 61801 USA
Wu, Zili (författare)
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge TN 37831 USA
Jiang, De En (författare)
Interdisciplinary Materials Science, Vanderbilt University, Nashville TN 37235 USA; Department of Chemical and Biomolecular Engineering, Vanderbilt University, Nashville TN 37235 USA
Frenkel, Anatoly I. (författare)
Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook NY 11794 USA; Chemistry Division, Brookhaven National Laboratory, Upton NY 11973 USA
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 (creator_code:org_t)
Royal Society of Chemistry (RSC), 2023
2023
Engelska.
Ingår i: Chemical Science. - : Royal Society of Chemistry (RSC). - 2041-6520 .- 2041-6539. ; 14:44, s. 12582-12588
  • Tidskriftsartikel (refereegranskat)
Abstract Ämnesord
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  • “Single-atom” catalysts (SACs) have been the focus of intense research, due to debates about their reactivity and challenges toward determining and designing “single-atom” (SA) sites. To address the challenge, in this work, we designed Pt SACs supported on Gd-doped ceria (Pt/CGO), which showed improved activity for CO oxidation compared to its counterpart, Pt/ceria. The enhanced activity of Pt/CGO was associated with a new Pt SA site which appeared only in the Pt/CGO catalyst under CO pretreatment at elevated temperatures. Combined X-ray and optical spectroscopies revealed that, at this site, Pt was found to be d-electron rich and bridged with Gd-induced defects via an oxygen vacancy. As explained by density functional theory calculations, this site opened a new path via a dicarbonyl intermediate for CO oxidation with a greatly reduced energy barrier. These results provide guidance for rationally improving the catalytic properties of SA sites for oxidation reactions.

Ämnesord

NATURVETENSKAP  -- Fysik -- Den kondenserade materiens fysik (hsv//swe)
NATURAL SCIENCES  -- Physical Sciences -- Condensed Matter Physics (hsv//eng)

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