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Nickel Speciation and Methane Dry Reforming Performance of Ni/CexZr1–xO2 Prepared by Different Synthesis Methods

  • Yimeng Lyu
    Yimeng Lyu
    School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Yimeng Lyu
  • Jennifer Jocz
    Jennifer Jocz
    School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
  • Rui Xu
    Rui Xu
    School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    More by Rui Xu
  • Eli Stavitski
    Eli Stavitski
    National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, United States
  • , and 
  • Carsten Sievers*
    Carsten Sievers
    School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    *Email: [email protected]
Cite this: ACS Catal. 2020, 10, 19, 11235–11252
Publication Date (Web):September 3, 2020
https://doi.org/10.1021/acscatal.0c02426
Copyright © 2020 American Chemical Society
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Abstract

Ceria–zirconia-supported Ni catalysts (Ni/Ce0.83Zr0.17O2 or Ni/CZ) are prepared by dry impregnation, strong electrostatic adsorption, coprecipitation (CP), and combustion synthesis (CS). The nature and abundance of Ni species in these samples are characterized by X-ray adsorption spectroscopy, temperature-programmed reduction, and CO chemisorption. The bulk synthesis methods (i.e., CP and CS) produce Ni cations that are incorporated into the CZ lattice forming mixed-metal oxides with Ni3+ species at low Ni content. The formation of mixed-metal oxides increases the reducibility of CZ and increases the abundance of active surface oxygen. All NiO/CZ catalysts are active for methane dry reforming and retain some of their activity at a steady state. The initial methane conversion correlates linearly with the fraction of accessible Ni after reduction. The predominant path of catalyst deactivation strongly depends on the structure of the catalyst and, thus, on the synthesis method used. All catalysts experience agglomeration of Ni particles under reaction conditions. Improving the Ni dispersion to isolated species embedded in a support does not improve resistance to Ni particle growth. Coke formation is inversely related to the concentration of active surface oxygen. The dominant deactivation mechanism for catalysts made by CS is the encapsulation of Ni particles by the support.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.0c02426.

  • Adsorption/desorption isotherms and pore size distribution for unreduced samples; linear combination fitting of XANES spectra for unreduced catalysts; standards used for LCF XANES fittings; EXAFS fits and fitted parameters for unreduced samples; XPS survey scans and XPS Ni 2p spectra for unreduced samples; XPS fits and fitted parameters for unreduced samples; deconvoluted TPR patterns; reactivity performance for all samples; adsorption/desorption isotherms and pore size distribution for spent samples; TGA of spent samples; SEM images of spent samples; and relationship between the initial CO2 conversion and the surface Ni concentration (PDF)

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