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author:

Feng, Yingxin (Feng, Yingxin.) [1] | Wan, Qiang (Wan, Qiang.) [2] | Xiong, Haifeng (Xiong, Haifeng.) [3] | Zhou, Shulan (Zhou, Shulan.) [4] | Chen, Xun (Chen, Xun.) [5] | Pereira Hernandez, Xavier Isidro (Pereira Hernandez, Xavier Isidro.) [6] | Wang, Yong (Wang, Yong.) [7] | Lin, Sen (Lin, Sen.) [8] | Datye, Abhaya K. (Datye, Abhaya K..) [9] | Guo, Hua (Guo, Hua.) [10]

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EI

Abstract:

Pt/CeO2 single-atom catalysts have recently attracted increasing interest due to excellent thermal stability, high atom efficiency, and high activity in catalysis. In this study, by means of density functional theory (DFT) calculations, we systematically compare the stability and CO oxidation reactivity of Pt single atoms supported on CeO2(111) (Pt/CeO2) and Ga-doped CeO2(111) (Pt/Ga-CeO2). It was found that the formation of an oxygen vacancy (OV) is very facile near a surface Ga-doping site (Pt/Ga-CeO2-OV). Significantly, the stability of Pt single atoms anchored on the Ga site was enhanced compared with those on the bare ceria surface. In addition, our DFT results suggest a CO oxidation mechanism on Pt/Ga-CeO2-OV that differs from that on Pt/CeO2. In particular, the OV site plays an important role in activating the oxygen molecule, which then reacts with CO preadsorbed on Pt. The calculated energy barrier on Pt/Ga-CeO2-OV is about 0.43 eV lower than that on the undoped catalyst, suggesting an enhanced reactivity for CO oxidation. Experiments on CO oxidation and in situ diffuse reflectance infrared Fourier transform spectroscopy are performed to corroborate the results obtained from the DFT calculations, and a good agreement is achieved. The combination between calculations and experiments sheds light on the influence of support doping on atomically dispersed Pt/CeO2 catalysts. © 2018 American Chemical Society.

Keyword:

Atoms Catalysts Cerium oxide Density functional theory Fourier transform infrared spectroscopy Gallium compounds Oxidation Oxygen Platinum

Community:

  • [ 1 ] [Feng, Yingxin]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350002, China
  • [ 2 ] [Wan, Qiang]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350002, China
  • [ 3 ] [Xiong, Haifeng]Center for Microengineered Materials, Department of Chemical and Biological Engineering, Albuquerque; NM; 87131, United States
  • [ 4 ] [Zhou, Shulan]Department of Chemistry and Chemical Biology, University of New Mexico, Albuquerque; NM; 87131, United States
  • [ 5 ] [Zhou, Shulan]Department of Material Science and Engineering, Jingdezhen Ceramic Institute, Jingdezhen, Jiangxi; 333403, China
  • [ 6 ] [Chen, Xun]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350002, China
  • [ 7 ] [Pereira Hernandez, Xavier Isidro]Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman; WA; 99164, United States
  • [ 8 ] [Wang, Yong]Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman; WA; 99164, United States
  • [ 9 ] [Wang, Yong]Institute for Integrated Catalysis, Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, P.O. Box 999, Richland; WA; 99352, United States
  • [ 10 ] [Lin, Sen]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350002, China
  • [ 11 ] [Lin, Sen]Department of Chemistry and Chemical Biology, University of New Mexico, Albuquerque; NM; 87131, United States
  • [ 12 ] [Datye, Abhaya K.]Center for Microengineered Materials, Department of Chemical and Biological Engineering, Albuquerque; NM; 87131, United States
  • [ 13 ] [Guo, Hua]Department of Chemistry and Chemical Biology, University of New Mexico, Albuquerque; NM; 87131, United States

Reprint 's Address:

  • [xiong, haifeng]center for microengineered materials, department of chemical and biological engineering, albuquerque; nm; 87131, united states

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Source :

Journal of Physical Chemistry C

ISSN: 1932-7447

Year: 2018

Issue: 39

Volume: 122

Page: 22460-22468

4 . 3 0 9

JCR@2018

3 . 3 0 0

JCR@2023

ESI HC Threshold:209

JCR Journal Grade:1

CAS Journal Grade:2

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 93

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 2

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