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Research Papers

Design and Characterization of a Novel Upward Flow Reactor for the Study of High-Temperature Thermal Reduction for Solar-Driven Processes

[+] Author and Article Information
H. Evan Bush, Robert J. Gill, Sheldon M. Jeter

George W. Woodruff School of
Mechanical Engineering,
Georgia Institute of Technology,
Atlanta, GA 30332-0405

Karl-Philipp Schlichting

Department of Mechanical and
Process Engineering,
ETH Zurich,
Zurich 8092, Switzerland

Peter G. Loutzenhiser

George W. Woodruff School of
Mechanical Engineering,
Georgia Institute of Technology,
Atlanta, GA 30332-0405
e-mail: peter.loutzenhiser@me.gatech.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 February 13, 2017; final manuscript received May 18, 2017; published online July 18, 2017. Assoc. Editor: Marc Röger.

J. Sol. Energy Eng 139(5), 051004 (Jul 18, 2017) (11 pages) Paper No: SOL-17-1056; doi: 10.1115/1.4037191 History: Received February 13, 2017; Revised May 18, 2017

The design and characterization of an upward flow reactor (UFR) coupled to a high flux solar simulator (HFSS) under vacuum is presented. The UFR was designed to rapidly heat solid samples with concentrated irradiation to temperatures greater than 1000 °C at heating rates in excess of 50 K/s. Such conditions are ideal for examining high-temperature thermal reduction kinetics of reduction/oxidation-active materials by temporally monitoring O2 evolution. A steady-state, computational fluid dynamics (CFD) model was employed in the design to minimize the formation of eddies and recirculation, and lag and dispersion were characterized through a suite of O2 tracer experiments using deconvolution and the continuously stirred tank reactors (CSTR) in series models. A transient, CFD and heat transfer model of the UFR was combined with Monte Carlo ray tracing (MCRT) to determine radiative heat fluxes on the sample from the HFSS to model spatial and temporal sample temperatures. The modeled temperatures were compared with those measured within the sample during an experiment in which Co3O4 was thermally reduced to CoO and O2. The measured temperatures within the bed were bounded by the average top and bottom modeled bed temperatures for the duration of the experiment. Small variances in the shape of the modeled versus experimental temperatures were due to contact resistance between the thermocouple and particles in the bed and changes in the spectral absorptivity and emissivity as the Co3O4 was reduced to CoO and O2.

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References

Parida, B. , Iniyan, S. , and Goic, R. , 2011, “ A Review of Solar Photovoltaic Technologies,” Renewable Sustainable Energy Rev., 15(3), pp. 1625–1636. [CrossRef]
Zhang, H. L. , Baeyens, J. , Degrève, J. , and Cacères, G. , 2013, “ Concentrated Solar Power Plants: Review and Design Methodology,” Renewable Sustainable Energy Rev., 22, pp. 466–481. [CrossRef]
Ho, C. K. , and Iverson, B. D. , 2014, “ Review of High-Temperature Central Receiver Designs for Concentrating Solar Power,” Renewable Sustainable Energy Rev., 29, pp. 835–846. [CrossRef]
Steinfeld, A. , 2005, “ Solar Thermochemical Production of Hydrogen—A Review,” Sol. Energy, 78(5), pp. 603–615. [CrossRef]
Loutzenhiser, P. G. , Meier, A. , and Steinfeld, A. , 2010, “ Review of the Two-Step H2O/CO2-Splitting Solar Thermochemical Cycle Based on Zn/ZnO Redox Reactions,” Materials, 3(11), pp. 4922–4938. [CrossRef]
Miller, J. E. , Ambrosini, A. , Coker, E. N. , Allendorf, M. D. , and McDaniel, A. H. , 2014, “ Advancing Oxide Materials for Thermochemical Production of Solar Fuels,” Energy Procedia, 49, pp. 2019–2026. [CrossRef]
Agrafiotis, C. , Roeb, M. , and Sattler, C. , 2015, “ A Review on Solar Thermal Syngas Production Via Redox Pair-Based Water/Carbon Dioxide Splitting Thermochemical Cycles,” Renewable Sustainable Energy Rev., 42, pp. 254–285. [CrossRef]
Dry, M. E. , 2002, “ The Fischer–Tropsch Process: 1950–2000,” Catal. Today, 71(3–4), pp. 227–241. [CrossRef]
Schrader, A. J. , Muroyama, A. P. , and Loutzenhiser, P. G. , 2015, “ Solar Electricity Via an Air Brayton Cycle With an Integrated Two-Step Thermochemical Cycle for Heat Storage Based on Co3O4/CoO Redox Reactions: Thermodynamic Analysis,” Sol. Energy, 118, pp. 485–495. [CrossRef]
Carrillo, A. J. , Serrano, D. P. , Pizarro, P. , and Coronado, J. M. , 2014, “ Thermochemical Heat Storage Based on the Mn2O3/Mn3O4 Redox Couple: Influence of the Initial Particle Size on the Morphological Evolution and Cyclability,” J. Mater. Chem. A, 2(45), pp. 19435–19443. [CrossRef]
Pagkoura, C. , Karagiannakis, G. , Zygogianni, A. , Lorentzou, S. , Kostoglou, M. , Konstandopoulos, A. G. , Rattenburry, M. , and Woodhead, J. W. , 2014, “ Cobalt Oxide Based Structured Bodies as Redox Thermochemical Heat Storage Medium for Future CSP Plants,” Sol. Energy, 108, pp. 146–163. [CrossRef]
Marxer, D. , Furler, P. , Scheffe, J. , Geerlings, H. , Falter, C. , Batteiger, V. , Sizmann, A. , and Steinfeld, A. , 2015, “ Demonstration of the Entire Production Chain to Renewable Kerosene Via Solar Thermochemical Splitting of H2O and CO2,” Energy Fuels, 29(5), pp. 3241–3250. [CrossRef]
Neises, M. , Tescari, S. , de Oliveira, L. , Roeb, M. , Sattler, C. , and Wong, B. , 2012, “ Solar-Heated Rotary Kiln for Thermochemical Energy Storage,” Sol. Energy, 86(10), pp. 3040–3048. [CrossRef]
Loutzenhiser, P. G. , Gálvez, M. E. , Hischier, I. , Stamatiou, A. , Frei, A. , and Steinfeld, A. , 2009, “ CO2 Splitting Via Two-Step Solar Thermochemical Cycles With Zn/ZnO and FeO/Fe3O4 Redox Reactions II: Kinetic Analysis,” Energy Fuels, 23(5), pp. 2832–2839. [CrossRef]
Wong, B. , 2011, “ Thermochemical Heat Storage for Concentrated Solar Power,” U.S. Department of Energy, San Diego, CA, Report No. DOE/GO18145. https://www.osti.gov/scitech/servlets/purl/1039304/
Muroyama, A. P. , Schrader, A. J. , and Loutzenhiser, P. G. , 2015, “ Solar Electricity Via an Air Brayton Cycle With an Integrated Two-Step Thermochemical Cycle for Heat Storage Based on Co3O4/CoO Redox Reactions II: Kinetic Analyses,” Sol. Energy, 122, pp. 409–418. [CrossRef]
Abu Hamed, T. , Venstrom, L. , Alshare, A. , Brulhart, M. , and Davidson, J. H. , 2009, “ Study of a Quench Device for the Synthesis and Hydrolysis of Zn Nanoparticles: Modeling and Experiments,” ASME J. Sol. Energy Eng., 131(3), p. 031018. [CrossRef]
McDaniel, A. H. , Ambrosini, A. , Coker, E. N. , Miller, J. E. , Chueh, W. C. , O'Hayre, R. , and Tong, J. , 2014, “ Nonstoichiometric Perovskite Oxides for Solar Thermochemical H2 and CO Production,” Energy Procedia, 49, pp. 2009–2018. [CrossRef]
Mizusaki, J. , 1992, “ Nonstoichiometry, Diffusion, and Electrical Properties of Perovskite-Type Oxide Electrode Materials,” Solid State Ionics, 52(1), pp. 79–91. [CrossRef]
Schunk, L. O. , and Steinfeld, A. , 2009, “ Kinetics of the Thermal Dissociation of ZnO Exposed to Concentrated Solar Irradiation Using a Solar-Driven Thermogravimeter in the 1800–2100 K Range,” AIChE J., 55(6), pp. 1497–1504. [CrossRef]
Alonso, E. , Hutter, C. , Romero, M. , Steinfeld, A. , and Gonzalez-Aguilar, J. , 2013, “ Kinetics of Mn2O3–Mn3O4 and Mn3O4–MnO Redox Reactions Performed Under Concentrated Thermal Radiative Flux,” Energy Fuels, 27(8), pp. 4884–4890. [CrossRef]
Takacs, M. , Ackermann, S. , Bonk, A. , Neises-von Puttkamer, M. , Haueter, P. , Scheffe, J. R. , Vogt, U. F. , and Steinfeld, A. , 2017, “ Splitting CO2 With a Ceria-Based Redox Cycle in a Solar-Driven Thermogravimetric Analyzer,” AIChE J., 63(4), pp. 1263–1271. [CrossRef] [PubMed]
Scheffe, J. R. , McDaniel, A. H. , Allendorf, M. D. , and Weimer, A. W. , 2013, “ Kinetics and Mechanism of Solar-Thermochemical H2 Production by Oxidation of a Cobalt Ferrite-Zirconia Composite,” Energy Environ. Sci., 6(3), pp. 963–973. [CrossRef]
Alonso, E. , and Romero, M. , 2015, “ A Directly Irradiated Solar Reactor for Kinetic Analysis of Non-Volatile Metal Oxides Reductions,” Int. J. Energy Res., 39(9), pp. 1217–1228. [CrossRef]
ANSYS, 2013, “ ANSYS Fluent,” ANSYS, Inc., Canonsburg, PA.
NETZSCH, 2012, “ Operating Instructions: Simultaneous TG-DTA/DSC Apparatus, STA 449 F3 Jupiter,” NETZSCH-Gerätebau GmbH, Selb, Germany, p. 3.30.
McMaster-Carr, 2015, “ Extreme-Chemical O-Ring FEP With Viton® Core,” McMaster-Carr, Elmhurst, IL.
Gill, R. , Bush, E. , Haueter, P. , and Loutzenhiser, P. , 2015, “ Characterization of a 6 kW High-Flux Solar Simulator With an Array of Xenon Arc Lamps Capable of Concentrations of Nearly 5000 Suns,” Rev. Sci. Instrum., 86(12), p. 125107. [CrossRef] [PubMed]
Andraka, C. E. , Sadlon, S. , Myer, B. , Trapeznikov, K. , and Liebner, C. , 2013, “ Rapid Reflective Facet Characterization Using Fringe Reflection Techniques,” ASME J. Sol. Energy Eng., 136(1), p. 011002. [CrossRef]
Smith, D. , Shiles, E. , and Inokuti, M. , 1985, “ The Optical Properties of Metallic Aluminum,” Handbook of Optical Constants of Solids, Vol. 1, Academic Press, Cambridge, MA, pp. 369–406.
TGP, 2010, “ Fused Quartz Average Transmittance Curves,” Technical Glass Products, Lake County, OH, accessed Mar. 9, 2017, https://www.technicalglass.com/fused_quartz_transmission.html
NIST, 2016, “ Tricobalt Tetraoxide,” NIST Chemistry WebBook, P. J. Linstrom and W. G. Mallard , eds., National Institute of Standards and Technology, Gaithersburg, MD.
Tsotsas, E. , and Martin, H. , 1987, “ Thermal Conductivity of Packed Beds: A Review,” Chem. Eng. Process., 22(1), pp. 19–37. [CrossRef]
Modest, M. F. , 2013, Radiative Heat Transfer, Academic Press, Oxford, UK.
Kim, S. J. , and Jang, S. P. , 2002, “ Effects of the Darcy Number, the Prandtl Number, and the Reynolds Number on Local Thermal Non-Equilibrium,” Int. J. Heat Mass Transfer, 45(19), pp. 3885–3896. [CrossRef]
Lapp, J. , Davidson, J. H. , and Lipiński, W. , 2013, “ Heat Transfer Analysis of a Solid-Solid Heat Recuperation System for Solar-Driven Nonstoichiometric Redox Cycles,” ASME J. Sol. Energy Eng., 135(3), p. 031004. [CrossRef]
Singh, B. P. , and Kaviany, M. , 1992, “ Modelling Radiative Heat Transfer in Packed Beds,” Int. J. Heat Mass Transfer, 35(6), pp. 1397–1405. [CrossRef]
Zehner, P. , and Schlünder, E. U. , 1972, “ Einfluß der Wärmestrahlung und des Druckes auf den Wärmetransport in nicht durchströmten Schüttungen,” Chem. Ing. Tech., 44(23), pp. 1303–1308. [CrossRef]
Sahoo, P. , Djieutedjeu, H. , and Poudeu, P. F. P. , 2013, “ Co3O4 Nanostructures: The Effect of Synthesis Conditions on Particles Size, Magnetism and Transport Properties,” J. Mater. Chem. A, 1(47), pp. 15022–15030. [CrossRef]
Lewis, F. B. , and Saunders, N. H. , 1973, “ The Thermal Conductivity of NiO and CoO at the Neel Temperature,” J. Phys. C, 6(15), p. 2525. [CrossRef]
Ghiaasiaan, S. M. , 2011, Convective Heat and Mass Transfer, Cambridge University Press, New York. [CrossRef]
LeFevre, E. J. , 1956, “ Laminar Free Convection From a Vertical Plane Surface,” The Ninth International Congress on Applied Mechanics, Brussels, Belgium, Sept. 5–13, pp. 175–183.
Cook, J. G. , and van der Meer, M. P. , 1986, “ The Optical Properties of Sputtered Co3O4 Films,” Thin Solid Films, 144(2), pp. 165–176. [CrossRef]
Sumin Sih, S. , and Barlow, J. W. , 2004, “ The Prediction of the Emissivity and Thermal Conductivity of Powder Beds,” Part. Sci. Technol., 22(3), pp. 291–304. [CrossRef]
Levenspiel, O. , 1999, Chemical Reaction Engineering, Wiley, Hoboken, NJ. [PubMed] [PubMed]
MathWorks, 2016, “ FFT: Fast Fourier Transform,” MathWorks, Natick, MA.

Figures

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Fig. 1

Exploded wireframe view of the UFR with (1) domed quartz tube, (2) alumina crucible, (3) o-rings, (4) stainless steel adapter, (5) stainless steel body, (6) cast clamps, and (7) gas/thermocouple feedthrough

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Fig. 2

Schematic of experimental setup: O2 and Ar tanks supplied gas to the reactor via flow controllers, driven by a pump downstream of the reactor outlet. A pressure transducer was used to monitor reactor operating pressure and products of reduction were measured via a mass spectrometer (MS) and gas chromatograph (GC). Labels A and B indicate locations at which the O2 flow controller and supply were connected for dispersion testing.

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Fig. 3

Mesh for UFR CFD and heat transfer modeling. The outer surface (left), outlet stem (top right), and sample crucible inside the reactor (bottom right) are depicted with annotations matching the boundary conditions in Table 3.

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Fig. 4

Average input (solid) and output (dash-dotted) dimensionless O2 concentration curves for dispersion tracer step tests. Gray regions indicate 95% confidence intervals. Curves were measured for step changes (a) from 0 to 0.2 LN/min and (b) from 0.2 to 0 LN/min flow controller settings with 60 s between changes to reach steady flow.

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Fig. 5

Residence time distribution of the reactor determined via the method of deconvolution (solid) and the CSTR in series model (dashed)

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Fig. 6

Three-dimensional streamlines originating from the three reactor inlets, as predicted by steady-state heat and mass transfer modeling of the UFR. Fluid velocity is defined by a logarithmic gradient on the streamlines and is higher near the inlets and outlet

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Fig. 7

Experimental results of Co3O4 reduction performed in UFR for HFSS input power (dashed), thermocouple temperature, (dashed), and Ar (solid, light) and O2 (solid, heavy) ion current

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Fig. 8

Modeled, smoothed sample surface heat fluxes for the center lamp of the HFSS in kW m−2, produced from the MCRT model modified for beam down configuration

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Fig. 9

Modeled steady-state temperature contours for a cross-sectional detail view of the crucible, sample, and neighboring fluid field for temperatures between 1100 and 1500 K

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Fig. 10

Modeled temporal temperature evolution averaged over the top surface (dotted), bottom surface (dashed), and bed (solid) compared with measured temporal temperatures (circles) for (a) the entire test and (b) the first 60 s of the test

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Fig. 11

Thermal reduction of Co3O4 as measured by mass spectrometer and gas chromatographer (solid) and corrected for dispersion (dashed), presented as (a) O2 molar flow rates and (b) Co3O4 to CoO conversion

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