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Kinetics of oxygen uncoupling of a copper based oxygen carrier

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  • Hu, Wenting
  • Donat, Felix
  • Scott, S.A.
  • Dennis, J.S.

Abstract

Here, an oxygen carrier consisting of 60wt% CuO supported on a mixture of Al2O3 and CaO (23wt% and 17wt% respectively) was synthesised by wet-mixing powdered CuO, Al(OH)3 and Ca(OH)2, followed by calcination at 1000°C. Its suitability for chemical looping with oxygen uncoupling (CLOU) was investigated. After 25 repeated redox cycles in either a thermogravimetric analyser (TGA) or a laboratory-scale fluidised bed, (with 5vol% H2 in N2 as the fuel, and air as the oxidant) no significant change in either the oxygen uncoupling capacity or the overall oxygen availability of the carrier was found. In the TGA, it was found that the rate of oxygen release from the material was controlled by intrinsic chemical kinetics and external transfer of mass from the surface of the particles to the bulk gas. By modelling the various resistances, values of the rate constant for the decomposition were obtained. The activation energy of the reaction was found to be 59.7kJ/mol (with a standard error of 5.6kJ/mol) and the corresponding pre-exponential factor was 632m3/mol/s. The local rate of conversion within a particle was assumed to occur either (i) by homogeneous chemical reaction, or (ii) in uniform, non-porous grains, each reacting as a kinetically-controlled shrinking core. Upon cross validation against a batch fluidised bed experiment, the homogeneous reaction model was found to be more plausible. By accurately accounting for the various artefacts (e.g. mass transfer resistances) present in both TGA and fluidised bed experiments, it was possible to extract a consistent set of kinetic parameters which reproduced the rates of oxygen release in both experiments.

Suggested Citation

  • Hu, Wenting & Donat, Felix & Scott, S.A. & Dennis, J.S., 2016. "Kinetics of oxygen uncoupling of a copper based oxygen carrier," Applied Energy, Elsevier, vol. 161(C), pages 92-100.
    • Handle: RePEc:eee:appene:v:161:y:2016:i:c:p:92-100
    DOI: 10.1016/j.apenergy.2015.10.006
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    References listed on IDEAS

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    1. Rydén, Magnus & Leion, Henrik & Mattisson, Tobias & Lyngfelt, Anders, 2014. "Combined oxides as oxygen-carrier material for chemical-looping with oxygen uncoupling," Applied Energy, Elsevier, vol. 113(C), pages 1924-1932.
    2. Imtiaz, Qasim & Broda, Marcin & Müller, Christoph R., 2014. "Structure–property relationship of co-precipitated Cu-rich, Al2O3- or MgAl2O4-stabilized oxygen carriers for chemical looping with oxygen uncoupling (CLOU)," Applied Energy, Elsevier, vol. 119(C), pages 557-565.
    3. Moldenhauer, Patrick & Rydén, Magnus & Mattisson, Tobias & Younes, Mourad & Lyngfelt, Anders, 2014. "The use of ilmenite as oxygen carrier with kerosene in a 300W CLC laboratory reactor with continuous circulation," Applied Energy, Elsevier, vol. 113(C), pages 1846-1854.
    4. Clayton, Christopher K. & Whitty, Kevin J., 2014. "Measurement and modeling of decomposition kinetics for copper oxide-based chemical looping with oxygen uncoupling," Applied Energy, Elsevier, vol. 116(C), pages 416-423.
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    1. Ping Wang & Bret Howard & Nicholas Means & Dushyant Shekhawat & David Berry, 2019. "Coal Chemical-Looping with Oxygen Uncoupling (CLOU) Using a Cu-Based Oxygen Carrier Derived from Natural Minerals," Energies, MDPI, vol. 12(8), pages 1-13, April.
    2. Saman Setoodeh Jahromy & Felix Birkelbach & Christian Jordan & Clemens Huber & Michael Harasek & Andreas Werner & Franz Winter, 2019. "Impact of Partial Pressure, Conversion, and Temperature on the Oxidation Reaction Kinetics of Cu 2 O to CuO in Thermochemical Energy Storage," Energies, MDPI, vol. 12(3), pages 1-15, February.
    3. Saghafifar, Mohammad & Schnellmann, Matthias A. & Scott, Stuart A., 2020. "Chemical looping electricity storage," Applied Energy, Elsevier, vol. 279(C).
    4. Adánez-Rubio, Iñaki & Abad, Alberto & Gayán, Pilar & García-Labiano, Francisco & de Diego, Luis F. & Adánez, Juan, 2017. "Coal combustion with a spray granulated Cu-Mn mixed oxide for the Chemical Looping with Oxygen Uncoupling (CLOU) process," Applied Energy, Elsevier, vol. 208(C), pages 561-570.

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