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Surface Refaceting Mechanism on Cubic Ceria

  • Chengwu Yang
    Chengwu Yang
    Beijing Key Laboratory of Bio-inspired Energy Materials and Devices, School of Space and Environment, Beihang University, Beijing 102206, China
    Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein-Leopoldshafen, Germany
    More by Chengwu Yang
  • Marçal Capdevila-Cortada
    Marçal Capdevila-Cortada
    Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, 43007 Tarragona, Spain
  • Chunyan Dong
    Chunyan Dong
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
    University of Chinese Academy of Sciences, Beijing 100049, China
    More by Chunyan Dong
  • Yan Zhou*
    Yan Zhou
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
    *Email: [email protected]
    More by Yan Zhou
  • Junjun Wang
    Junjun Wang
    Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein-Leopoldshafen, Germany
    More by Junjun Wang
  • Xiaojuan Yu
    Xiaojuan Yu
    Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein-Leopoldshafen, Germany
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  • Alexei Nefedov
    Alexei Nefedov
    Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein-Leopoldshafen, Germany
  • Stefan Heißler
    Stefan Heißler
    Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein-Leopoldshafen, Germany
  • Núria López*
    Núria López
    Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, 43007 Tarragona, Spain
    *Email: [email protected]
  • Wenjie Shen
    Wenjie Shen
    State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
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  • Christof Wöll*
    Christof Wöll
    Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein-Leopoldshafen, Germany
    *Email: [email protected]
  • , and 
  • Yuemin Wang*
    Yuemin Wang
    Institute of Functional Interfaces (IFG), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein-Leopoldshafen, Germany
    *Email: [email protected]
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Cite this: J. Phys. Chem. Lett. 2020, 11, 18, 7925–7931
Publication Date (Web):September 1, 2020
https://doi.org/10.1021/acs.jpclett.0c02409
Copyright © 2020 American Chemical Society
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Abstract

Polar surfaces of solid oxides are intrinsically unstable and tend to reconstruct due to the diverging electrostatic energy and thus often exhibit unique physical and chemical properties. However, a quantitative description of the restructuring mechanism of these polar surfaces remains challenging. Here we provide an atomic-level picture of the refaceting process that governs the surface polarity compensation of cubic ceria nanoparticles based on the accurate reference data acquired from the well-defined model systems. The combined results from advanced infrared spectroscopy, atomic-resolved transmission electron microscopy, and density functional theory calculations identify a two-step scenario where an initial O-terminated (2 × 2) reconstruction is followed by a severe refaceting via massive mass transport at elevated temperatures to yield {111}-dominated nanopyramids. This significant surface restructuring promotes the redox properties of ceria nanocubes, which account for the enhanced catalytic activity for CO oxidation.

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  • Experimental and computational details; additional results obtained from HRTEM/STEM/SEM, catalytic evaluation, DFT calculations, XPS, LEED, as well as IR investigations (PDF)

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Cited By


This article is cited by 9 publications.

  1. Wen-Zhu Yu, Mei-Yao Wu, Wei-Wei Wang, Chun-Jiang Jia. In Situ Generation of the Surface Oxygen Vacancies in a Copper–Ceria Catalyst for the Water–Gas Shift Reaction. Langmuir 2021, 37 (35) , 10499-10509. https://doi.org/10.1021/acs.langmuir.1c01428
  2. Yuxin Zhao, Ahsan Jalal, Alper Uzun. Interplay between Copper Nanoparticle Size and Oxygen Vacancy on Mg-Doped Ceria Controls Partial Hydrogenation Performance and Stability. ACS Catalysis 2021, 11 (13) , 8116-8131. https://doi.org/10.1021/acscatal.1c01471
  3. Farahnaz Maleki, Gianfranco Pacchioni. Steric and Orbital Effects Induced by Isovalent Dopants on the Surface Chemistry of ZrO2. ACS Catalysis 2021, 11 (2) , 554-567. https://doi.org/10.1021/acscatal.0c04553
  4. Junjun Wang, Weijia Wang, Zhiying Fan, Shuang Chen, Alexei Nefedov, Stefan Heißler, Roland A. Fischer, Christof Wöll, Yuemin Wang. Defect-Engineered Metal–Organic Frameworks: A Thorough Characterization of Active Sites Using CO as a Probe Molecule. The Journal of Physical Chemistry C 2021, 125 (1) , 593-601. https://doi.org/10.1021/acs.jpcc.0c09738
  5. Patricia Pérez-Bailac, Pablo G Lustemberg, M Verónica Ganduglia-Pirovano. Facet-dependent stability of near-surface oxygen vacancies and excess charge localization at CeO 2 surfaces. Journal of Physics: Condensed Matter 2021, 33 (50) , 504003. https://doi.org/10.1088/1361-648X/ac238b
  6. Dong Jiang, Yonggang Yao, Tangyuan Li, Gang Wan, Xavier Isidro Pereira‐Hernández, Yubing Lu, Jinshu Tian, Konstantin Khivantsev, Mark H. Engelhard, Chengjun Sun, Carlos E. García‐Vargas, Adam S. Hoffman, Simon R. Bare, Abhaya K. Datye, Liangbing Hu, Yong Wang. Tailoring the Local Environment of Platinum in Single‐Atom Pt 1 /CeO 2 Catalysts for Robust Low‐Temperature CO Oxidation. Angewandte Chemie 2021, 133 (50) , 26258-26266. https://doi.org/10.1002/ange.202108585
  7. Dong Jiang, Yonggang Yao, Tangyuan Li, Gang Wan, Xavier Isidro Pereira‐Hernández, Yubing Lu, Jinshu Tian, Konstantin Khivantsev, Mark H. Engelhard, Chengjun Sun, Carlos E. García‐Vargas, Adam S. Hoffman, Simon R. Bare, Abhaya K. Datye, Liangbing Hu, Yong Wang. Tailoring the Local Environment of Platinum in Single‐Atom Pt 1 /CeO 2 Catalysts for Robust Low‐Temperature CO Oxidation. Angewandte Chemie International Edition 2021, 60 (50) , 26054-26062. https://doi.org/10.1002/anie.202108585
  8. Xènia Garcia, Lluís Soler, Albert Casanovas, Carlos Escudero, Jordi Llorca. X-ray photoelectron and Raman spectroscopy of nanostructured ceria in soot oxidation under operando conditions. Carbon 2021, 178 , 164-180. https://doi.org/10.1016/j.carbon.2021.03.009
  9. Pablo G. Lustemberg, Philipp N. Plessow, Yuemin Wang, Chengwu Yang, Alexei Nefedov, Felix Studt, Christof Wöll, M. Verónica Ganduglia-Pirovano. Vibrational Frequencies of Cerium-Oxide-Bound CO: A Challenge for Conventional DFT Methods. Physical Review Letters 2020, 125 (25) https://doi.org/10.1103/PhysRevLett.125.256101