Examining and Modeling Oxygen Uncoupling Kinetics of Cu-Based Oxygen Carriers for Chemical Looping with Oxygen Uncoupling (CLOU) in a Drop Tube Fluidized Bed Reactor
Abstract
Chemical looping combustion with oxygen uncoupling (CLOU) is a promising carbon capture and storage (CCS) technology for conversion of gaseous and solid hydrocarbon fuels where the release of gaseous O2 from an oxygen carrier is favored at high temperature and low O2 partial pressure. One promising CLOU material is the copper oxide redox system (CuO–Cu2O). The primary objective of this study was to examine the use of a drop tube fluidized bed reactor (DT-FBR) for evaluating the kinetics of oxygen uncoupling with Cu-based oxygen carriers. Appropriate rate expressions from redox experiments are needed to model and scale up CLOU systems. Additionally, the determined oxygen uncoupling kinetic parameters were validated using a computational fluid dynamic model. Two oxygen carriers consisting of 20 wt % CuO/Al2O3 and 9 wt % CuO/Al2O3 were prepared by physical mixing. A third oxygen carrier sample was prepared at 9 wt % CuO/Al2O3 by incipient wetness impregnation. The reaction rates of the copper oxide redox system are strongly dependent on thermodynamic effects of the oxygen partial pressure relative to the equilibrium oxygen partial pressure. The results presented in this paper offer an alternative and simplified kinetic analysis compared to that traditionally presented in the literature for themore »
- Authors:
-
[1];
[1];
- National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
- National Energy Technology Lab. (NETL), Morgantown, WV (United States)
- Publication Date:
- Research Org.:
- National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
- Sponsoring Org.:
- USDOE Office of Fossil Energy (FE)
- OSTI Identifier:
- 1569815
- Report Number(s):
- RSS010
Journal ID: ISSN 0887-0624
- Grant/Contract Number:
- 89243318CFE000003
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Energy and Fuels
- Additional Journal Information:
- Journal Volume: 33; Journal Issue: 6; Journal ID: ISSN 0887-0624
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Means, Nicholas C., Burgess, Ward A., Howard, Bret H., Smith, Mark W., Wang, Ping, and Shekhawat, Dushyant. Examining and Modeling Oxygen Uncoupling Kinetics of Cu-Based Oxygen Carriers for Chemical Looping with Oxygen Uncoupling (CLOU) in a Drop Tube Fluidized Bed Reactor. United States: N. p., 2019.
Web. doi:10.1021/acs.energyfuels.9b00338.
Means, Nicholas C., Burgess, Ward A., Howard, Bret H., Smith, Mark W., Wang, Ping, & Shekhawat, Dushyant. Examining and Modeling Oxygen Uncoupling Kinetics of Cu-Based Oxygen Carriers for Chemical Looping with Oxygen Uncoupling (CLOU) in a Drop Tube Fluidized Bed Reactor. United States. https://doi.org/10.1021/acs.energyfuels.9b00338
Means, Nicholas C., Burgess, Ward A., Howard, Bret H., Smith, Mark W., Wang, Ping, and Shekhawat, Dushyant. Mon .
"Examining and Modeling Oxygen Uncoupling Kinetics of Cu-Based Oxygen Carriers for Chemical Looping with Oxygen Uncoupling (CLOU) in a Drop Tube Fluidized Bed Reactor". United States. https://doi.org/10.1021/acs.energyfuels.9b00338. https://www.osti.gov/servlets/purl/1569815.
@article{osti_1569815,
title = {Examining and Modeling Oxygen Uncoupling Kinetics of Cu-Based Oxygen Carriers for Chemical Looping with Oxygen Uncoupling (CLOU) in a Drop Tube Fluidized Bed Reactor},
author = {Means, Nicholas C. and Burgess, Ward A. and Howard, Bret H. and Smith, Mark W. and Wang, Ping and Shekhawat, Dushyant},
abstractNote = {Chemical looping combustion with oxygen uncoupling (CLOU) is a promising carbon capture and storage (CCS) technology for conversion of gaseous and solid hydrocarbon fuels where the release of gaseous O2 from an oxygen carrier is favored at high temperature and low O2 partial pressure. One promising CLOU material is the copper oxide redox system (CuO–Cu2O). The primary objective of this study was to examine the use of a drop tube fluidized bed reactor (DT-FBR) for evaluating the kinetics of oxygen uncoupling with Cu-based oxygen carriers. Appropriate rate expressions from redox experiments are needed to model and scale up CLOU systems. Additionally, the determined oxygen uncoupling kinetic parameters were validated using a computational fluid dynamic model. Two oxygen carriers consisting of 20 wt % CuO/Al2O3 and 9 wt % CuO/Al2O3 were prepared by physical mixing. A third oxygen carrier sample was prepared at 9 wt % CuO/Al2O3 by incipient wetness impregnation. The reaction rates of the copper oxide redox system are strongly dependent on thermodynamic effects of the oxygen partial pressure relative to the equilibrium oxygen partial pressure. The results presented in this paper offer an alternative and simplified kinetic analysis compared to that traditionally presented in the literature for the thermal reduction of copper oxide or other CLOU oxygen carriers. The reactor system used in this study allows for operating parameters to be adjusted, minimizing thermodynamic and mass transfer limitations, which eliminates the need for more complex kinetic/thermodynamic reaction models. The reaction kinetics measured in this study is compared based on the preparation method and the CuO weight percent loading. These results may aid in the development of CLOU technologies during reactor design and process modeling.},
doi = {10.1021/acs.energyfuels.9b00338},
journal = {Energy and Fuels},
number = 6,
volume = 33,
place = {United States},
year = {Mon Apr 22 00:00:00 EDT 2019},
month = {Mon Apr 22 00:00:00 EDT 2019}
}
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