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Research Papers

The Effects of Morphology on the Oxidation of Ceria by Water and Carbon Dioxide

[+] Author and Article Information
Luke J. Venstrom

Department of Mechanical Engineering,  University of Minnesota-Twin Cities, 111 Church St. S.E., Minneapolis, MN 55455lvenstro@me.umn.edu

Nicholas Petkovich, Stephen Rudisill

Andreas Stein1

Department of Chemistry,  University of Minnesota-Twin Cities, 207 Pleasant St. S.E., Minneapolis, MN 55455a-stein@umn.edu

Jane H. Davidson1

Department of Mechanical Engineering,  University of Minnesota-Twin Cities, 111 Church St. S.E., Minneapolis, MN 55455jhd@me.umn.edu

1

Corresponding authors.

J. Sol. Energy Eng 134(1), 011005 (Nov 01, 2011) (8 pages) doi:10.1115/1.4005119 History: Received May 03, 2011; Revised September 01, 2011; Published November 01, 2011; Online November 01, 2011

The oxidation of three-dimensionally ordered macroporous (3DOM) CeO2 (ceria) by H2 O and CO2 at 1100 K is presented in comparison to the oxidation of nonordered mesoporous and sintered, low porosity ceria. 3DOM ceria, which features interconnected and ordered pores, increases the maximum H2 and CO production rates over the low porosity ceria by 125% and 260%, respectively, and increases the maximum H2 and CO production rates over the nonordered mesoporous cerium oxide by 75% and 175%, respectively. The increase in the kinetics of H2 O and CO2 splitting with 3DOM ceria is attributed to its enhanced specific surface area and to its interconnected pore system that facilitates the transport of reacting species to and from oxidation sites.

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Copyright © 2012 by American Society of Mechanical Engineers
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Figures

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Figure 1

Vertical fixed bed tubular flow reactor. The terms “oxidation” and “reduction” are used with respect to the ceria

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Figure 2

SEM images of the as-synthesized (first column) and chemically cycled (second column) commercial CeO2 (a and b), DS CeO2 (c and d), and 3DOM CeO2 (e and f)

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Figure 3

TEM images of the as-synthesized (first column) and chemically cycled (second column) DS CeO2 (a and b) and 3DOM CeO2 (c and d)

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Figure 4

Pore size distribution of the as-synthesized DS CeO2

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Figure 5

The rate of production of H2 during the oxidation of 3DOM CeO2 at 1100 K over 6 isothermal chemical redox cycles

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Figure 6

The rate of production of fuel as a function of time at 1100 K for the CeO2 samples for (a) H2 O and (b) CO2 splitting and the rate of production of fuel as a function of the reaction extent for (c) H2 O and (d) CO2 splitting. The conditions for (a) and (c) are yH2O = 2.7 ± 0.1 mol% and Qtotal  = 200–1000 cm3 min − 1 . The conditions for (b) and (d) are yCO2 = 4.0 ± 0.2 mol% and Qtotal  = 550 cm3 min−1 . A mass spectrometer was used to analyze the gas composition in the H2 O splitting experiments. A Raman laser gas analyzer was used to analyze the gas composition in the CO2 splitting experiments.

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Figure 7

SEM images of 3DOM CeO2 thermally treated at (a) 1273 K for 4 h and (b) 1523 K for 1 h

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