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Tailoring the Local Environment of Platinum in Single-Atom Pt1 /CeO2 Catalysts for Robust Low-Temperature CO Oxidation.
Jiang, Dong; Yao, Yonggang; Li, Tangyuan; Wan, Gang; Pereira-Hernández, Xavier Isidro; Lu, Yubing; Tian, Jinshu; Khivantsev, Konstantin; Engelhard, Mark H; Sun, Chengjun; García-Vargas, Carlos E; Hoffman, Adam S; Bare, Simon R; Datye, Abhaya K; Hu, Liangbing; Wang, Yong.
Afiliación
  • Jiang D; The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, 99164, USA.
  • Yao Y; Department of Materials Science and Engineering, University of Maryland, College Park, MD, 20742, USA.
  • Li T; Current address: State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China.
  • Wan G; Department of Materials Science and Engineering, University of Maryland, College Park, MD, 20742, USA.
  • Pereira-Hernández XI; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
  • Lu Y; The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, 99164, USA.
  • Tian J; Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, WA, 99354, USA.
  • Khivantsev K; Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, WA, 99354, USA.
  • Engelhard MH; Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, WA, 99354, USA.
  • Sun C; Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, WA, 99354, USA.
  • García-Vargas CE; X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Lemont, IL, 60439, USA.
  • Hoffman AS; The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, 99164, USA.
  • Bare SR; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
  • Datye AK; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
  • Hu L; Department of Chemical and Biological Engineering and Center for Micro-Engineered Materials, University of New Mexico, Albuquerque, NM, 87131, USA.
  • Wang Y; Department of Materials Science and Engineering, University of Maryland, College Park, MD, 20742, USA.
Angew Chem Int Ed Engl ; 60(50): 26054-26062, 2021 Dec 06.
Article en En | MEDLINE | ID: mdl-34346155
ABSTRACT
A single-atom Pt1 /CeO2 catalyst formed by atom trapping (AT, 800 °C in air) shows excellent thermal stability but is inactive for CO oxidation at low temperatures owing to over-stabilization of Pt2+ in a highly symmetric square-planar Pt1 O4 coordination environment. Reductive activation to form Pt nanoparticles (NPs) results in enhanced activity; however, the NPs are easily oxidized, leading to drastic activity loss. Herein we show that tailoring the local environment of isolated Pt2+ by thermal-shock (TS) synthesis leads to a highly active and thermally stable Pt1 /CeO2 catalyst. Ultrafast shockwaves (>1200 °C) in an inert atmosphere induced surface reconstruction of CeO2 to generate Pt single atoms in an asymmetric Pt1 O4 configuration. Owing to this unique coordination, Pt1 δ+ in a partially reduced state dynamically evolves during CO oxidation, resulting in exceptional low-temperature performance. CO oxidation reactivity on the Pt1 /CeO2 _TS catalyst was retained under oxidizing conditions.
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Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2021 Tipo del documento: Article País de afiliación: Estados Unidos
Texto completo
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2021 Tipo del documento: Article País de afiliación: Estados Unidos