Research Papers: Radiative Heat Transfer

A Model of Transient Heat and Mass Transfer in a Heterogeneous Medium of Ceria Undergoing Nonstoichiometric Reduction

[+] Author and Article Information
Wojciech Lipiński

e-mail: lipinski@umn.edu
Department of Mechanical Engineering,
University of Minnesota,
Minneapolis, MN 55455

1Corresponding author.

Contributed by the Heat Transfer Division of ASME for publication in the JOURNAL OF HEAT TRANSFER. Manuscript received March 28, 2012; final manuscript received January 22, 2013; published online April 11, 2013. Assoc. Editor: Oronzio Manca.

J. Heat Transfer 135(5), 052701 (Apr 11, 2013) (9 pages) Paper No: HT-12-1134; doi: 10.1115/1.4023494 History: Received March 28, 2012; Revised January 22, 2013

The redox chemistry of nonstoichiometric metal oxides can be used to produce chemical fuels by harnessing concentrated solar energy to split water and/or carbon dioxide. In such a process, it is desirable to use a porous reactive substrate for increased surface area and improved gas transport. The present study develops a macroscopic-scale model of porous ceria undergoing thermal reduction. The model captures the coupled interactions between the heat and mass transfer and the heterogeneous chemistry using a local thermal nonequilibrium (LTNE) formulation of the volume-averaged conservation of mass and energy equations in an axisymmetric cylindrical domain. The results of a representative test case simulation demonstrate strong coupling between gas phase mass transfer and the chemical kinetics as well as the pronounced impact of optical thickness on the temperature distribution and thus global solar-to-chemical energy conversion.

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Abanades, S., and Flamant, G., 2006, “Thermochemical Hydrogen Production From a Two-Step Solar-Driven Water-Splitting Cycle Based on Cerium Oxides,” Sol. Energy, 80, pp. 1611−1623. [CrossRef]
Chueh, W., and Haile, S., 2009, “Ceria as a Thermochemical Reaction Medium for Selectively Generating Syngas or Methane From H2O and CO2,” ChemSusChem, 2, pp. 735−739. [CrossRef] [PubMed]
Cheuh, W., and Haile, S., 2010, “A Thermochemical Study of Ceria: Exploiting an Old Material for New Modes of Energy Conversion and CO2 Mitigation,” Philos. Trans. R. Soc. A, 368, pp. 3269−3294. [CrossRef]
Lapp, J., Davidson, J., and Lipinski, W., 2012, “Efficiency of Two-Step Solar Thermochemical Non-Stoichiometric Redox Cycles With Heat Recovery,” Energy, 37, pp. 591−600. [CrossRef]
Venstrom, L., Petkovich, N., Rudisill, S., Stein, A., and Davidson, J., 2012, “The Effects of Morphology on the Oxidation of Ceria by Water and Carbon Dioxide,” ASME J. Sol. Energ., 134(1), p. 011005. [CrossRef]
Petkovich, N., Rudisill, S., Venstrom, L., Davidson, J., and Stein, A., 2011, “Control of Heterogeneity in Nanostructured Ce1xZrxO2 Binary Oxides for Enhanced Thermal Stability and Water Splitting Activity,” J. Phys. Chem. C, 115(43), pp. 21022−21033. [CrossRef]
Miller, J., Allendorf, M., Diver, R., Evans, L., Siegel, N., and Stuecker, J., 2008, “Metal Oxide Composites and Structures for Ultra-High Temperature Solar Thermochemical Cycles,” J. Mater. Sci., 43, pp. 4714−4728. [CrossRef]
Chueh, W., Falter, C., Abbot, M., Scipio, D., Furler, P., Haile, S., and Steinfeld, A., 2010, “High-Flux Solar-Driven Thermochemical Dissociation of CO2 and H2O Using Nonstoichiometric Ceria,” Science, 330, pp. 1797−1801. [CrossRef] [PubMed]
Whitaker, S., 1999, The Method of Volume Averaging, Kluwer Academic, Boston.
Liang, Z., Chueh, W., Ganesan, K., Haile, S., and Lipinski, W., 2011, “Experimental Determination of Transmittance of Porous Cerium Dioxide Media in the Spectral Range of 300−1100 nm,” Exp. Heat Transfer, 24(4), pp. 285–299. [CrossRef]
Ganesan, K., and Lipinski, W., 2011, “Experimental Determination of Spectral Transmittance of Porous Cerium Dioxide in the Range 900-1700 nm,” ASME J. Heat Trans., 133(10), p. 104501. [CrossRef]
Dombrovsky, L. A., Ganesan, K., and Lipiński, W., 2012, “Combined Two-Flux Approximation and Monte Carlo Model for Identification of Radiative Properties of Highly Scattering Dispersed Materials,” Comput. Therm. Sci., 4, pp. 365–378. [CrossRef]
Ganesan, K., Dombrovsky, L. A., and Lipiński, W., 2013, “Visible and Near-Infrared Optical Properties of Ceria Ceramics,” Infrared Phys. Technol., 57, pp. 101–109. [CrossRef]
Cussler, E., 2009, Diffusion: Mass Transfer in Fluid Systems, Cambridge University Press, Cambridge.
Yaws, C., 2009, Transport Properties of Chemicals and Hydrocarbons: Viscosity, Thermal Conductivity, and Diffusivity of C1 to C100 Organics and Ac to Zr Inorganics, Elsevier, New York.
Binnewies, M., and Milke, E., 2002, Thermochemical Data of Elements and Compounds, Wiley-VCH, Weinheim, Germany.
Chekhovskoy, V., and Stavrovsky, G., 1970, “Thermal Conductivity of Cerium Dioxide,” 9th Conference on Thermal Conductivity, pp. 295−298.
Panlener, R., Blumenthal, R., and Garnier, J., 1975, “A Thermodynamic Study of Nonstoichiometric Cerium Dioxide,” J. Phys. Chem. Solids, 36, pp. 1213−1222. [CrossRef]
Modest, M., 2003, Radiative Heat Transfer, Academic Press, New York.
Kaviany, M., 1995, Principles of Heat Transfer in Porous Media, Springer, New York.
Wakao, N., Kaguei, S., and Funazkri, T., 1979, “Effect of Fluid Dispersion Coefficients on Particle-to-Fluid Heat Transfer Coefficients in Packed Beds. Correlation of Nusselt Numbers,” Chem. Eng. Sci., 34, pp. 325−336. [CrossRef]
Kuwahara, F., Yang, C., Ando, K., and Nakayama, A., 2011, “Exact Solutions for a Thermal Nonequilibrium Model of Fluid Saturated Porous Media Based on an Effective Porosity,” ASME J. Heat Trans., 133(11), p. 112602. [CrossRef]
Haussener, S., and Steinfeld, A., 2012, “Effective Heat and Mass Transport Properties of Anisotropic Porous Ceria for Solar Thermochemical Fuel Generation,” Materials, 5, pp. 192−209. [CrossRef]
Patankar, S., 1980, Numerical Heat Transfer and Fluid Flow, Taylor & Francis, London.
Ferziger, J., and Peric, M., 2001, Computational Methods for Fluid Dynamics, Springer, New York.


Grahic Jump Location
Fig. 1

Schematic of the axisymmetric cylindrical two-phase solid–gas reacting medium under direct irradiation

Grahic Jump Location
Fig. 2

Boundary conditions for mass and energy Eqs. (22), (23), (25), and (27)

Grahic Jump Location
Fig. 3

Time evolution of the terms identified in the global energy balance described by Eq. (37)

Grahic Jump Location
Fig. 4

The axial distributions of (a) solid temperature, (b) fluid temperature, (c) nonstoichiometry, (d) oxygen partial pressure, and (e) reaction rate are plotted at r = 0 for selected times



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