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Tiny Species with Big Impact: High Activity of Cu Single Atoms on CeO2–TiO2 Deciphered by Operando Spectroscopy

  • Jawaher Mosrati
    Jawaher Mosrati
    Leibniz-Institut für Katalyse, Albert-Einstein-Str. 29A, 18059 Rostock, Germany
    Laboratoire de chimie des matériaux et catalyse, Département de chimie, Faculté des sciences de Tunis, Université de Tunis el Manar, Tunis 1092, Tunisie
  • Ali M. Abdel-Mageed
    Ali M. Abdel-Mageed
    Institute of Surface Chemistry and Catalysis, Ulm University, Albert-Einstein-Allee 47, D-89081 Ulm, Germany
    Department of Chemistry, Faculty of Science, Cairo University, Giza 12613, Egypt
  • Thanh Huyen Vuong
    Thanh Huyen Vuong
    Leibniz-Institut für Katalyse, Albert-Einstein-Str. 29A, 18059 Rostock, Germany
  • Reni Grauke
    Reni Grauke
    Leibniz-Institut für Katalyse, Albert-Einstein-Str. 29A, 18059 Rostock, Germany
    More by Reni Grauke
  • Stephan Bartling
    Stephan Bartling
    Leibniz-Institut für Katalyse, Albert-Einstein-Str. 29A, 18059 Rostock, Germany
  • Nils Rockstroh
    Nils Rockstroh
    Leibniz-Institut für Katalyse, Albert-Einstein-Str. 29A, 18059 Rostock, Germany
  • Hanan Atia
    Hanan Atia
    Leibniz-Institut für Katalyse, Albert-Einstein-Str. 29A, 18059 Rostock, Germany
    More by Hanan Atia
  • Udo Armbruster
    Udo Armbruster
    Leibniz-Institut für Katalyse, Albert-Einstein-Str. 29A, 18059 Rostock, Germany
  • Sebastian Wohlrab
    Sebastian Wohlrab
    Leibniz-Institut für Katalyse, Albert-Einstein-Str. 29A, 18059 Rostock, Germany
  • Jabor Rabeah*
    Jabor Rabeah
    Leibniz-Institut für Katalyse, Albert-Einstein-Str. 29A, 18059 Rostock, Germany
    *Email: [email protected]
    More by Jabor Rabeah
  • , and 
  • Angelika Brückner*
    Angelika Brückner
    Leibniz-Institut für Katalyse, Albert-Einstein-Str. 29A, 18059 Rostock, Germany
    *Email: [email protected]
Cite this: ACS Catal. 2021, 11, 17, 10933–10949
Publication Date (Web):August 18, 2021
https://doi.org/10.1021/acscatal.1c02349
Copyright © 2021 The Authors. Published by American Chemical Society
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Abstract

Cu single-atom catalysts (SACs) supported on CeO2–TiO2 were prepared by a sol–gel method and tested for CO oxidation between 120 and 350 °C. Operando and in situ spectroscopic methods including diffuse reflectance infrared Fourier transform (DRIFT), electron paramagnetic resonance (EPR), and near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) combined with other basic characterizations were applied to identify active sites and to derive reliable structure–reactivity relationships. Rising the Cu content from 0.06 to 0.86 wt % resulted in a significant decrease of the Cu-mass normalized CO2 formation rate from 690 to 310 μmolCO2·gCu–1·s–1 at 250 °C, which was attributed to the formation of the less active CuOx species. The catalysts showed high stability during time on stream for more than 1000 min with negligible agglomeration of Cu single sites. Spectroscopic results revealed that active sites are single Cu ions on the surface of highly dispersed ceria particles, shuttling between −Cu2+–O–Ce4+– and −Cu+–□–Ce3+– by supplying active oxygen for oxidation of CO to CO2. The highest concentrations of Cu single sites and O vacancies associated with Ce3+ species correlated with the highest CO oxidation activity.

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  • Additional data including FTIR, EPR, ESI-MS, EPR of pure supports and supported Cu CeO2–TiO2 catalysts (PDF)

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