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

Abstract

Herein, 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 themore » support.« less

Authors:
 [1]; ORCiD logo [1];  [1];  [2]; ORCiD logo [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Publication Date:
Research Org.:
Georgia Institute of Technology, Atlanta, GA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II) and Center for Functional Nanomaterials (CFN)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1706600
Alternate Identifier(s):
OSTI ID: 1659329
Report Number(s):
BNL-220571-2020-JAAM
Journal ID: ISSN 2155-5435
Grant/Contract Number:  
SC0016486; SC0012704; ECCS-1542174
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 10; Journal Issue: 19; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; nickel catalyst; X-ray absorption spectroscopy; deactivation; sintering; coke formation; encapsulation

Citation Formats

Lyu, Yimeng, Jocz, Jennifer, Xu, Rui, Stavitski, Eli, and Sievers, Carsten. Nickel Speciation and Methane Dry Reforming Performance of Ni/CexZr1-xO2 Prepared by Different Synthesis Methods. United States: N. p., 2020. Web. https://doi.org/10.1021/acscatal.0c02426.
Lyu, Yimeng, Jocz, Jennifer, Xu, Rui, Stavitski, Eli, & Sievers, Carsten. Nickel Speciation and Methane Dry Reforming Performance of Ni/CexZr1-xO2 Prepared by Different Synthesis Methods. United States. https://doi.org/10.1021/acscatal.0c02426
Lyu, Yimeng, Jocz, Jennifer, Xu, Rui, Stavitski, Eli, and Sievers, Carsten. Thu . "Nickel Speciation and Methane Dry Reforming Performance of Ni/CexZr1-xO2 Prepared by Different Synthesis Methods". United States. https://doi.org/10.1021/acscatal.0c02426. https://www.osti.gov/servlets/purl/1706600.
@article{osti_1706600,
title = {Nickel Speciation and Methane Dry Reforming Performance of Ni/CexZr1-xO2 Prepared by Different Synthesis Methods},
author = {Lyu, Yimeng and Jocz, Jennifer and Xu, Rui and Stavitski, Eli and Sievers, Carsten},
abstractNote = {Herein, 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.},
doi = {10.1021/acscatal.0c02426},
journal = {ACS Catalysis},
number = 19,
volume = 10,
place = {United States},
year = {2020},
month = {9}
}

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