Research Papers

Effect of Flow Rates on Operation of a Solar Thermochemical Reactor for Splitting CO2 Via the Isothermal Ceria Redox Cycle

[+] Author and Article Information
Brandon J. Hathaway

Department of Mechanical Engineering,
University of Minnesota,
Minneapolis, MN 55455
e-mail: hatha050@umn.edu

Rohini Bala Chandran

Department of Mechanical Engineering,
University of Minnesota,
Minneapolis, MN 55455
e-mail: bala0137@umn.edu

Stephen Sedler

Department of Mechanical Engineering,
University of Minnesota,
Minneapolis, MN 55455
e-mail: sedl0033@umn.edu

Daniel Thomas

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

Adam Gladen

Department of Mechanical Engineering,
University of Minnesota,
Minneapolis, MN 55455
e-mail: glad0092@umn.edu

Thomas Chase

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

Jane H. Davidson

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

1Corresponding author.

Contributed by the Solar Energy Division of ASME for publication in the JOURNAL OF SOLAR ENERGY ENGINEERING: INCLUDING WIND ENERGY AND BUILDING ENERGY CONSERVATION. Manuscript received July 29, 2015; final manuscript received October 26, 2015; published online December 8, 2015. Assoc. Editor: Prof. Nesrin Ozalp.

J. Sol. Energy Eng 138(1), 011007 (Dec 08, 2015) (12 pages) Paper No: SOL-15-1238; doi: 10.1115/1.4032019 History: Received July 29, 2015; Revised October 26, 2015

A prototype 4 kW solar thermochemical reactor for the continuous splitting of carbon dioxide via the isothermal ceria redox cycle is demonstrated. These first tests of the new reactor showcase both the innovation of continuous on-sun fuel production in a single reactor and remarkably effective heat recovery of the sensible heat of the reactant and product gases. The impact of selection of gas flow rates is explored with respect to reactor fuel productivity and external energy costs of gas separation and pumping. Thermal impacts of gas flow selection are explored by coupling measured temperatures with a computational fluid dynamics (CFD) model to calculate internal temperature distributions and estimate heat recovery. Optimized gas flows selected for operation provide a 75% increase in fuel productivity and reduction in parasitic energy costs by 10% with respect to the design case.

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Eyring, L. , 1991, “ The Binary Lanthanide Oxides: Synthesis and Identification,” Synthesis of Lanthanide and Actinide Compounds, G. Meyer and L. R. Morss , eds., Kluwer Academic Publishers, Dordrecht, The Netherlands, p. 201.
Chueh, W. C. , and Haile, S. M. , 2010, “ A Thermochemical Study of Ceria: Exploiting an Old Material for New Modes of Energy Conversion and CO2 Mitigation,” Philos. Trans. A Math. Phys. Eng. Sci., 368(1923), pp. 3269–3294. [CrossRef] [PubMed]
Ackermann, S. , Scheffe, J. R. , and Steinfeld, A. , 2014, “ Diffusion of Oxygen in Ceria at Elevated Temperatures and Its Application to H2O/CO2 Splitting Thermochemical Redox Cycles,” J. Phys. Chem. C, 118(10), pp. 5216–5225. [CrossRef]
Millot, F. , and Mierry, P. D. , 1985, “ A New Method for the Study of Chemical Diffusion in Oxides With Application to Cerium Oxide CeO2−x,” J. Phys. Chem. Solids, 46(7), pp. 797–801. [CrossRef]
Chueh, W. C. , Falter, C. , Abbott, M. , Scipio, D. , Furler, P. , Haile, S. M. , and Steinfeld, A. , 2010, “ High-Flux Solar-Driven Thermochemical Dissociation of CO2 and H2O Using Nonstoichiometric Ceria,” Science, 330(6012), pp. 1797–1801. [CrossRef] [PubMed]
Furler, P. , Scheffe, J. R. , and Steinfeld, A. , 2012, “ Syngas Production by Simultaneous Splitting of H2O and CO2 Via Ceria Redox Reactions in a High-Temperature Solar Reactor,” Energy Environ. Sci., 5(3), pp. 6098–6103. [CrossRef]
Furler, P. , Scheffe, J. , Marxer, D. , Gorbar, M. , Bonk, A. , Vogt, U. , and Steinfeld, A. , 2014, “ Thermochemical CO2 Splitting Via Redox Cycling of Ceria Reticulated Foam Structures With Dual-Scale Porosities,” Phys. Chem. Chem. Phys., 16(22), pp. 10503–10511. [CrossRef] [PubMed]
Venstrom, L. J. , De Smith, R. M. , Hao, Y. , Haile, S. M. , and Davidson, J. H. , 2014, “ Efficient Splitting of CO2 in an Isothermal Redox Cycle Based on Ceria,” Energy Fuels, 28(4), pp. 2732–2742. [CrossRef]
Panlener, R. J. , Blumenthal, R. N. , and Garnier, J. E. , 1975, “ A Thermodynamic Study of Nonstoichiometric Cerium Dioxide,” J. Phys. Chem. Solids, 36(11), pp. 1213–1222. [CrossRef]
Bader, R. , Venstrom, L. J. , Davidson, J. H. , and Lipiński, W. , 2013, “ Thermodynamic Analysis of Isothermal Redox Cycling of Ceria for Solar Fuel Production,” Energy Fuels, 27(9), pp. 5533–5544. [CrossRef]
Hao, Y. , Yang, C.-K. , and Haile, S. M. , 2013, “ High-Temperature Isothermal Chemical Cycling for Solar-Driven Fuel Production.,” Phys. Chem. Chem. Phys., 15(40), pp. 17084–17092. [CrossRef] [PubMed]
Ermanoski, I. , Miller, J. E. , and Allendorf, M. D. , 2014, “ Efficiency Maximization in Solar-Thermochemical Fuel Production: Challenging the Concept of Isothermal Water Splitting,” Phys. Chem. Chem. Phys., 16(18), pp. 8418–8427. [CrossRef] [PubMed]
Krenzke, P. T. , and Davidson, J. H. , 2015, “ On the Efficiency of Solar H2 and CO Production Via the Thermochemical Cerium Oxide Redox Cycle: The Option of Inert-Swept Reduction,” Energy Fuels, 29(2), pp. 1045–1054.
Bader, R. , Bala Chandran, R. , Venstrom, L. J. , Sedler, S. J. , Krenzke, P. T. , De Smith, R. M. , Banerjee, A. , Chase, T. R. , Davidson, J. H. , and Lipinski, W. , 2015, “ Design of a Solar Reactor to Split CO2 Via Isothermal Redox Cycling of Ceria,” ASME J. Sol. Energy Eng., 137(3), p. 031007. [CrossRef]
Banerjee, A. , Bala Chandran, R. , and Davidson, J. H. , 2015, “ Experimental Investigation of a Reticulated Porous Alumina Heat Exchanger for High Temperature Gas Heat Recovery,” Appl. Therm. Eng., 75, pp. 889–895. [CrossRef]
Bala Chandran, R. , De Smith, R. M. , and Davidson, J. H. , 2015, “ Model of an Integrated Solar Thermochemical Reactor/Reticulated Ceramic Foam Heat Exchanger for Gas-Phase Heat Recovery,” Int. J. Heat Mass Transfer, 81, pp. 404–414. [CrossRef]
Krueger, K. R. , Davidson, J. H. , and Lipiński, W. , 2011, “ Design of a New 45 kWe High-Flux Solar Simulator for High-Temperature Solar Thermal and Thermochemical Research,” ASME J. Sol. Energy Eng., 133(1), p. 011013. [CrossRef]
Krueger, K. R. , Lipiński, W. , and Davidson, J. H. , 2013, “ Operational Performance of the University of Minnesota 45 kW e High-Flux Solar Simulator,” ASME J. Sol. Energy Eng., 135(4), p. 044501. [CrossRef]
Steinfeld, A. , and Schubnell, M. , 1993, “ Optimum Aperture Size and Operating Temperature of a Solar Cavity-Receiver,” Sol. Energy, 50(1), pp. 19–25. [CrossRef]
Kaviany, M. , 1995, Principles of Heat Transfer in Porous Media, Springer-Verlag, New York, pp. 13–109.
Modest, M. F. , 2003, “ The Method of Spectral Harmonics (PN-Approximation),” Radiative Heat Transfer, Academic Press, San Diego, CA, pp. 465–492.
Markham, J. R. , Solomon, P. R. , and Best, P. E. , 1990, “ An FT-IR Based Instrument for Measuring Spectral Emittance of Material at High Temperature,” Rev. Sci. Instrum., 61(12), p. 3700. [CrossRef]
Yaws, C. , 2010, Transport Properties of Chemicals and Hydrocarbons, Knovel, New York.
Binnewies, M. , and Milke, E. , 2002, Thermochemical Data of Elements and Compounds, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim, Germany.
Cussler, E. L. , 1997, “ Values of Diffusion Coefficients,” Diffusion Mass Transfer in Fluid Systems, Cambridge University Press, Cambridge, UK, pp. 117–126.
ANSYS® Academic Research, 2011, Ansys Fluent Users Guide, Release 14.0, ANSYS, Inc., Canonsburg, PA, pp. 1715–1762.
De Smith, R. M. , 2014, “ Improving the Efficiency of a Ceria Reduction-Oxidation Cycle Through the Choice of Operating Conditions and Ceria Morphology,” M.S. thesis, Department of Mechanical Engineering, University of Minnesota, Minneapolis, MN.
Venstrom, L. J. , De Smith, R. M. , Bala Chandran, R. , Boman, D. B. , Krenzke, P. T. , and Davidson, J. H. , 2015, “ Applicability of an Equilibrium Model To Predict the Conversion of CO2 to CO Via the Reduction and Oxidation of a Fixed Bed of Cerium Dioxide,” Energy Fuels, Article ASAP.


Grahic Jump Location
Fig. 2

Contours of relative heat capacity rate, Crel, for massspecific oxidizer and sweep gas flow rates from 0.83 to 2.5 std mL s−1 g−1. The dashed line represents the locus of flow combinations that result in a normalized average heat capacity rate of 1.

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Fig. 1

Cutaway views of the solar reactor and heat exchanger: (a) CAD model of the reactor showing the various functional components and (b) details of the reactive element and heat exchanger assembly (aspect ratio distorted to clarify structure of reactive element)

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Fig. 3

Instantaneous gas yield rates for (a) fuel during the oxidation half-cycle and (b) oxygen during the reduction half-cycle at the equal flows condition

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Fig. 4

Average yield rate of (a) carbon monoxide and (b) oxygen during cycling for varied flow configurations

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Fig. 5

Measured temperature profiles in the outer tube wall of RE1 for gas flow rates listed in Table 2: (a) spatially averaged surface temperatures during redox cycling and (b) axial profile of wall temperatures at the end of oxidation. Oxidation and reduction half cycles are abbreviated as “Ox” and “Rd.”

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Fig. 6

Temperatures in RE1 for two cycles of steady-periodic reactor operation with 1.67 mL s−1 g−1 of sweep gas and CO2. Spatially averaged, measured wall surface temperatures, modelpredicted bulk gas temperatures, and measured cavity temperature are shown. Oxidation and reduction half cycles are abbreviated as Ox and Rd.

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Fig. 7

Axial variation of model predicted bulk gas temperatures along its flow path in the central channel and the annulus at the onset of reduction with a sweep gas flow rate of 1.67 mL s−1 g−1. Subplot zooms into the axial temperature variation in the packed bed of ceria.

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Fig. 8

Cycle-averaged power requirements for the various gas flow rates listed in Table 1

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Fig. 9

Cycle-average O2 and CO yield rates per unit mass of ceria during the steady-periodic cycling. Open markers are for RE1, and solid markers are for RE2. Note the stability between cycles and similarity in performance between elements.

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Fig. 10

Instantaneous yield rate of fuel from both reactive elements, demonstrating the ability for the reactor to produce a continuous stream of fuel during cycling with multiple elements




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