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Title: Evaluation of the Redox Performance and Characterization of Fe2O3/CeO2/ZrO2 Oxygen Carriers under High Temperature in Situ Gasification Chemical-Looping Combustion Conditions

Abstract

Iron-based oxygen carriers with a CeO2 support have interesting redox applications in chemical-looping combustion (CLC). CeO2 behaves as an active support for many oxygen carrier applications because of the reversible release of lattice oxygen. High temperature processes may lead to improved process efficiency; however, the poor thermal stability of CeO2 gives rise to a need for oxygen carriers that can resist sintering and agglomeration and maintain reactivity after multiple reduction and oxidation (redox) cycles during in situ gasification chemical-looping combustion (iG-CLC) at 1100 °C. In this work, Fe-based oxygen carriers on CeO2, ZrO2, and Ce0.75Zr0.25O2 supports were prepared by a coprecipitation method. The redox stability, reactivity, and sintering of the oxygen carriers were evaluated to investigate the effect of the CeO2–ZrO2 solid solution support. The oxygen transport capability was evaluated in a drop tube fixed-bed reactor under iG-CLC conditions with coal char at 1100 °C for 10 redox cycles. The CeO2–ZrO2 solid solution improved the oxygen mobility of the support from the creation of more oxygen defects. The Fe–Ce oxygen carrier had the highest oxygen transport capability because of the formation of cerium orthoferrite (CeFeO3) during high temperature reduction. The Fe–Ce–Zr oxygen carrier showed improved reactivity over the Fe–Ce oxygenmore » carrier as the number of redox cycles increased. The oxygen carriers, before and after multiple redox cycles, were characterized by X-ray diffraction, scanning electron microscopy, and surface/pore analysis.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [2];  [3]
  1. National Energy Technology Laboratory (NETL), Pittsburgh, PA (United States); Leidos Research Support Team, Pittsburgh, PA (United States)
  2. National Energy Technology Laboratory (NETL), Pittsburgh, PA (United States)
  3. National Energy Technology Laboratory (NETL), Morgantown, WV (United States)
Publication Date:
Research Org.:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1635625
Grant/Contract Number:  
89243318CFE000003
Resource Type:
Accepted Manuscript
Journal Name:
Energy and Fuels
Additional Journal Information:
Journal Volume: 34; Journal Issue: 1; Journal ID: ISSN 0887-0624
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Means, Nicholas C., Hammache, Sonia, Burgess, Ward A., Howard, Bret H., and Smith, Mark W.. Evaluation of the Redox Performance and Characterization of Fe2O3/CeO2/ZrO2 Oxygen Carriers under High Temperature in Situ Gasification Chemical-Looping Combustion Conditions. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.energyfuels.9b03018.
Means, Nicholas C., Hammache, Sonia, Burgess, Ward A., Howard, Bret H., & Smith, Mark W.. Evaluation of the Redox Performance and Characterization of Fe2O3/CeO2/ZrO2 Oxygen Carriers under High Temperature in Situ Gasification Chemical-Looping Combustion Conditions. United States. https://doi.org/10.1021/acs.energyfuels.9b03018
Means, Nicholas C., Hammache, Sonia, Burgess, Ward A., Howard, Bret H., and Smith, Mark W.. Wed . "Evaluation of the Redox Performance and Characterization of Fe2O3/CeO2/ZrO2 Oxygen Carriers under High Temperature in Situ Gasification Chemical-Looping Combustion Conditions". United States. https://doi.org/10.1021/acs.energyfuels.9b03018. https://www.osti.gov/servlets/purl/1635625.
@article{osti_1635625,
title = {Evaluation of the Redox Performance and Characterization of Fe2O3/CeO2/ZrO2 Oxygen Carriers under High Temperature in Situ Gasification Chemical-Looping Combustion Conditions},
author = {Means, Nicholas C. and Hammache, Sonia and Burgess, Ward A. and Howard, Bret H. and Smith, Mark W.},
abstractNote = {Iron-based oxygen carriers with a CeO2 support have interesting redox applications in chemical-looping combustion (CLC). CeO2 behaves as an active support for many oxygen carrier applications because of the reversible release of lattice oxygen. High temperature processes may lead to improved process efficiency; however, the poor thermal stability of CeO2 gives rise to a need for oxygen carriers that can resist sintering and agglomeration and maintain reactivity after multiple reduction and oxidation (redox) cycles during in situ gasification chemical-looping combustion (iG-CLC) at 1100 °C. In this work, Fe-based oxygen carriers on CeO2, ZrO2, and Ce0.75Zr0.25O2 supports were prepared by a coprecipitation method. The redox stability, reactivity, and sintering of the oxygen carriers were evaluated to investigate the effect of the CeO2–ZrO2 solid solution support. The oxygen transport capability was evaluated in a drop tube fixed-bed reactor under iG-CLC conditions with coal char at 1100 °C for 10 redox cycles. The CeO2–ZrO2 solid solution improved the oxygen mobility of the support from the creation of more oxygen defects. The Fe–Ce oxygen carrier had the highest oxygen transport capability because of the formation of cerium orthoferrite (CeFeO3) during high temperature reduction. The Fe–Ce–Zr oxygen carrier showed improved reactivity over the Fe–Ce oxygen carrier as the number of redox cycles increased. The oxygen carriers, before and after multiple redox cycles, were characterized by X-ray diffraction, scanning electron microscopy, and surface/pore analysis.},
doi = {10.1021/acs.energyfuels.9b03018},
journal = {Energy and Fuels},
number = 1,
volume = 34,
place = {United States},
year = {2019},
month = {12}
}

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