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

Li, Yuanyuan; Wang, Haodong; Song, Haohong; Rui, Ning; Kottwitz, Matthew; Senanayake, Sanjaya D.; Nuzzo, Ralph G.; Wu, Zili; Jiang, De-en; Frenkel, Anatoly I.

doi:10.1039/D3SC03988A

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

Journal Article · Wed Nov 15 00:00:00 EST 2023 · Chemical Science

DOI:https://doi.org/10.1039/D3SC03988A· OSTI ID:2203963

^[1]; Wang, Haodong ^[2];

^[3]; Rui, Ning ^[4];

^[5];

^[4]; Nuzzo, Ralph G. ^[6];

^[7];

^[8];

^[9]

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
Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, NY 11794, USA
Interdisciplinary Materials Science, Vanderbilt University, Nashville, TN 37235, USA
Chemistry Division, Brookhaven National Laboratory, Upton, NY 11973, USA
Department of Chemistry, University of Illinois, Urbana, IL 61801, USA
Department of Chemistry, University of Illinois, Urbana, IL 61801, USA, Surface and Corrosion Science, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of Technology, Drottning Kristinasväg 51, 10044, Stockholm, Sweden
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
Interdisciplinary Materials Science, Vanderbilt University, Nashville, TN 37235, USA, Department of Chemical and Biomolecular Engineering, Vanderbilt University, Nashville, TN 37235, USA
Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, NY 11794, USA, Chemistry Division, Brookhaven National Laboratory, Upton, NY 11973, USA

“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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0012335, DE-SC0012704; SC0012704; SC0022199; SC0012335; AC02-05CH11231

OSTI ID:: 2203963

Alternate ID(s):: OSTI ID: 2222386

Report Number(s):: BNL-225032-2023-JAAM; CSHCBM

Journal Information:: Chemical Science, Journal Name: Chemical Science Vol. 14 Journal Issue: 44; ISSN 2041-6520

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

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