DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Fluidized-bed and fixed-bed reactor testing of methane chemical looping combustion with MgO-promoted hematite

Abstract

In this article MgO-promoted Fe2O3 hematite oxygen carriers were synthesized from various Mg sources and evaluated for methane chemical looping combustion. Particles suitable for fluidized bed flow reactor studies were prepared in the lab. Cyclic CLC tests conducted in the fluidized bed with MgO promoted hematite showed better performance than that with hematite. Attrition resistance of laboratory prepared MgO promoted hematite was excellent. Reactivity and stability of the oxygen carrier materials were also tested in the thermogravimetric analyzer and bench-scale reactors. Scanning electron microscopy and energy-dispersive X-ray spectroscopy, and X-ray diffraction were used to study the morphology and elemental compositions present in the hematite and promoted hematite oxygen carriers prior to and following the multi-cycle chemical looping reaction. The incorporation of 5 wt% MgO led to an increased reaction rate and an increase in oxygen utilized as compared to the pure hematite oxygen carrier. Possible reasons for the promotion effect by MgO were evaluated. These studies reveal that the best performing oxygen carrier was the 5 wt% MgO/Fe2O3 which exhibited no observed degradation in the kinetics and conversion performance in the methane step over 15 reduction and oxidation cycles. The Mg promoted oxygen carrier also showed reduced coke formation asmore » compared to the pure hematite carrier.« less

Authors:
 [1];  [2];  [2]
  1. National Energy Technology Lab. (NETL), Morgantown, WV (United States); URS Corp., Morgantown, WV (United States)
  2. 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:
1225713
Alternate Identifier(s):
OSTI ID: 1247577
Report Number(s):
A-CONTR-PUB-050
Journal ID: ISSN 0306-2619; PII: S030626191500224X
Grant/Contract Number:  
FE0004000
Resource Type:
Accepted Manuscript
Journal Name:
Applied Energy
Additional Journal Information:
Journal Volume: 146; Journal Issue: C; Journal ID: ISSN 0306-2619
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemical looping; fluidized bed; fixed bed; MgO promoted hematite

Citation Formats

Miller, Duane D., Siriwardane, Ranjani, and Poston, James. Fluidized-bed and fixed-bed reactor testing of methane chemical looping combustion with MgO-promoted hematite. United States: N. p., 2015. Web. doi:10.1016/j.apenergy.2015.02.047.
Miller, Duane D., Siriwardane, Ranjani, & Poston, James. Fluidized-bed and fixed-bed reactor testing of methane chemical looping combustion with MgO-promoted hematite. United States. https://doi.org/10.1016/j.apenergy.2015.02.047
Miller, Duane D., Siriwardane, Ranjani, and Poston, James. Thu . "Fluidized-bed and fixed-bed reactor testing of methane chemical looping combustion with MgO-promoted hematite". United States. https://doi.org/10.1016/j.apenergy.2015.02.047. https://www.osti.gov/servlets/purl/1225713.
@article{osti_1225713,
title = {Fluidized-bed and fixed-bed reactor testing of methane chemical looping combustion with MgO-promoted hematite},
author = {Miller, Duane D. and Siriwardane, Ranjani and Poston, James},
abstractNote = {In this article MgO-promoted Fe2O3 hematite oxygen carriers were synthesized from various Mg sources and evaluated for methane chemical looping combustion. Particles suitable for fluidized bed flow reactor studies were prepared in the lab. Cyclic CLC tests conducted in the fluidized bed with MgO promoted hematite showed better performance than that with hematite. Attrition resistance of laboratory prepared MgO promoted hematite was excellent. Reactivity and stability of the oxygen carrier materials were also tested in the thermogravimetric analyzer and bench-scale reactors. Scanning electron microscopy and energy-dispersive X-ray spectroscopy, and X-ray diffraction were used to study the morphology and elemental compositions present in the hematite and promoted hematite oxygen carriers prior to and following the multi-cycle chemical looping reaction. The incorporation of 5 wt% MgO led to an increased reaction rate and an increase in oxygen utilized as compared to the pure hematite oxygen carrier. Possible reasons for the promotion effect by MgO were evaluated. These studies reveal that the best performing oxygen carrier was the 5 wt% MgO/Fe2O3 which exhibited no observed degradation in the kinetics and conversion performance in the methane step over 15 reduction and oxidation cycles. The Mg promoted oxygen carrier also showed reduced coke formation as compared to the pure hematite carrier.},
doi = {10.1016/j.apenergy.2015.02.047},
journal = {Applied Energy},
number = C,
volume = 146,
place = {United States},
year = {Thu Mar 05 00:00:00 EST 2015},
month = {Thu Mar 05 00:00:00 EST 2015}
}

Journal Article:

Citation Metrics:
Cited by: 29 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Chemical-looping combustion of solid fuels in a 10kW reactor system using natural minerals as oxygen carrier
journal, January 2013


Synergetic effects of mixed copper–iron oxides oxygen carriers in chemical looping combustion
journal, June 2013


Methane combustion by moving bed fuel reactor with Fe2O3/Al2O3 oxygen carriers
journal, January 2014


Iron-Based Coal Direct Chemical Looping Combustion Process: 200-h Continuous Operation of a 25-kW th Subpilot Unit
journal, March 2013

  • Bayham, Samuel C.; Kim, Hyung R.; Wang, Dawei
  • Energy & Fuels, Vol. 27, Issue 3
  • DOI: 10.1021/ef400010s

Progress in Chemical-Looping Combustion and Reforming technologies
journal, April 2012

  • Adanez, Juan; Abad, Alberto; Garcia-Labiano, Francisco
  • Progress in Energy and Combustion Science, Vol. 38, Issue 2, p. 215-282
  • DOI: 10.1016/j.pecs.2011.09.001

Activity of NiCuAl catalyst in methane decomposition studied using a thermobalance and the structural changes in the Ni and the deposited carbon
journal, May 2008


The use of NiO as an oxygen carrier in chemical-looping combustion
journal, March 2006


Chemical-Looping Combustion with NiO and Fe 2 O 3 in a Thermobalance and Circulating Fluidized Bed Reactor with Double Loops
journal, April 2006

  • Son, Sung Real; Kim, Sang Done
  • Industrial & Engineering Chemistry Research, Vol. 45, Issue 8
  • DOI: 10.1021/ie050919x

Catalytic decomposition of methane on Raney-type catalysts
journal, September 2008


Integrated Hydrogen and Power Production with CO2 Capture Using Chemical-Looping ReformingRedox Reactivity of Particles of CuO, Mn2O3, NiO, and Fe2O3 Using SiO2 as a Support
journal, May 2005

  • Zafar, Qamar; Mattisson, Tobias; Gevert, Börje
  • Industrial & Engineering Chemistry Research, Vol. 44, Issue 10, p. 3485-3496
  • DOI: 10.1021/ie048978i

Reducible Supports for Ni-based Oxygen Carriers in Chemical Looping Combustion
journal, March 2013

  • Bhavsar, Saurabh; Veser, Götz
  • Energy & Fuels, Vol. 27, Issue 4
  • DOI: 10.1021/ef400184b

Particle characterisation in chemical looping combustion
journal, February 2012


Catalyst development for thermocatalytic decomposition of methane to hydrogen
journal, January 2008


Catalytic decomposition of methane over Ni-Al2O3 coprecipitated catalysts
journal, October 2003


Investigation of Fe 2 O 3 with MgAl 2 O 4 for Chemical-Looping Combustion
journal, October 2004

  • Johansson, Marcus; Mattisson, Tobias; Lyngfelt, Anders
  • Industrial & Engineering Chemistry Research, Vol. 43, Issue 22
  • DOI: 10.1021/ie049813c

NiO particles with Ca and Mg based additives produced by spray- drying as oxygen carriers for chemical-looping combustion
journal, February 2009


Ionic diffusion in the oxidation of iron—effect of support and its implications to chemical looping applications
journal, January 2011

  • Li, Fanxing; Sun, Zhenchao; Luo, Siwei
  • Energy & Environmental Science, Vol. 4, Issue 3, p. 876-880
  • DOI: 10.1039/c0ee00589d

Kinetics of Copper Oxidation in the Air Reactor of a Chemical Looping Combustion System using the Law of Additive Reaction Times
journal, November 2011

  • Sahir, Asad H.; Lighty, JoAnn S.; Sohn, Hong Yong
  • Industrial & Engineering Chemistry Research, Vol. 50, Issue 23
  • DOI: 10.1021/ie201577g

Methane decomposition over Ni–MgO–Al2O3 catalysts
journal, April 2009


Catalytic decomposition of CH4 over Ni-Al2O3-SiO2 catalysts: Influence of pretreatment conditions for the production of H2
journal, June 2008


Evaluation of Novel Ceria-Supported Metal Oxides As Oxygen Carriers for Chemical-Looping Combustion
journal, September 2012

  • Hedayati, Ali; Azad, Abdul-Majeed; Rydén, Magnus
  • Industrial & Engineering Chemistry Research, Vol. 51, Issue 39
  • DOI: 10.1021/ie300168j

Reactivity of a NiO/Al2O3 oxygen carrier prepared by impregnation for chemical-looping combustion
journal, November 2010


Testing of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for a SR–CLC system in a continuous CLC unit
journal, April 2012


NiO supported on Mg–ZrO2 as oxygen carrier for chemical-looping combustion and chemical-looping reforming
journal, January 2009

  • Rydén, Magnus; Johansson, Marcus; Lyngfelt, Anders
  • Energy & Environmental Science, Vol. 2, Issue 9
  • DOI: 10.1039/b904370e

Interaction of Iron Oxide with Alumina in a Composite Oxygen Carrier during the Production of Hydrogen by Chemical Looping
journal, December 2011

  • Kidambi, Piran R.; Cleeton, Jason P. E.; Scott, Stuart A.
  • Energy & Fuels, Vol. 26, Issue 1
  • DOI: 10.1021/ef200859d

Investigation of Combined Supports for Cu-Based Oxygen Carriers for Chemical-Looping with Oxygen Uncoupling (CLOU)
journal, June 2013

  • Adánez-Rubio, Iñaki; Arjmand, Mehdi; Leion, Henrik
  • Energy & Fuels, Vol. 27, Issue 7
  • DOI: 10.1021/ef401161s

Ilmenite and Nickel as Catalysts for Upgrading of Raw Gas Derived from Biomass Gasification
journal, February 2013

  • Lind, Fredrik; Berguerand, Nicolas; Seemann, Martin
  • Energy & Fuels, Vol. 27, Issue 2
  • DOI: 10.1021/ef302091w

Multicycle Reduction and Oxidation of Different Types of Iron Oxide ParticlesApplication to Chemical-Looping Combustion
journal, May 2004

  • Mattisson, Tobias; Johansson, Marcus; Lyngfelt, Anders
  • Energy & Fuels, Vol. 18, Issue 3
  • DOI: 10.1021/ef0301405

Thermogravimetric Analysis of Modified Hematite by Methane (CH 4 ) for Chemical-Looping Combustion: A Global Kinetics Mechanism
journal, October 2013

  • Monazam, Esmail R.; Breault, Ronald W.; Siriwardane, Ranjani
  • Industrial & Engineering Chemistry Research, Vol. 52, Issue 42
  • DOI: 10.1021/ie4024116

Oxidation and reduction characteristics of oxygen carrier particles and reaction kinetics by unreacted core model
journal, November 2001

  • Ryu, Ho-Jung; Bae, Dal-Hee; Han, Keun-Hee
  • Korean Journal of Chemical Engineering, Vol. 18, Issue 6
  • DOI: 10.1007/BF02705604

The Reduction of Mg–Fe–O and Mg–Fe–Al–O Complex Oxides Studied by Temperature-Programmed Reduction Combined with in Situ Mössbauer Spectroscopy
journal, October 2001

  • Ge, Xin; Li, Mingshi; Shen, Jianyi
  • Journal of Solid State Chemistry, Vol. 161, Issue 1
  • DOI: 10.1006/jssc.2001.9264

Effects of Support on the Performance of NiO-Based Oxygen Carriers
journal, March 2011

  • Baek, J. -I.; Kim, J. -W.; Lee, J. B.
  • Oil & Gas Science and Technology – Revue d’IFP Energies nouvelles, Vol. 66, Issue 2
  • DOI: 10.2516/ogst/2011003

Hydrogen and syngas production from two-step steam reforming of methane using CeO2 as oxygen carrier
journal, May 2011


Mapping of the range of operational conditions for Cu-, Fe-, and Ni-based oxygen carriers in chemical-looping combustion
journal, January 2007

  • Abad, Alberto; Adánez, Juan; García-Labiano, Francisco
  • Chemical Engineering Science, Vol. 62, Issue 1-2
  • DOI: 10.1016/j.ces.2006.09.019

Redox Investigation of Some Oxides of Transition-State Metals Ni, Cu, Fe, and Mn Supported on SiO 2 and MgAl 2 O 4
journal, January 2006

  • Zafar, Qamar; Mattisson, Tobias; Gevert, Börje
  • Energy & Fuels, Vol. 20, Issue 1
  • DOI: 10.1021/ef0501389

Evaluation of a Spray-Dried CuO/MgAl 2 O 4 Oxygen Carrier for the Chemical Looping with Oxygen Uncoupling Process
journal, December 2011

  • Adánez-Rubio, Iñaki; Gayán, Pilar; Abad, Alberto
  • Energy & Fuels, Vol. 26, Issue 5
  • DOI: 10.1021/ef3002229

Experimental comparison of two different ilmenites in fluidized bed and fixed bed chemical-looping combustion
journal, January 2014


Hydrogen production by thermocatalytic decomposition of methane over Ni-Al and Ni-Cu-Al catalysts: Effect of calcination temperature
journal, June 2007


Enhanced Performance of Alkali Metal Doped Fe2O3 and Fe2O3/Al2O3 Composites As Oxygen Carrier Material in Chemical Looping Combustion
journal, July 2013

  • Liu, Lu; Zachariah, Michael R.
  • Energy & Fuels, Vol. 27, Issue 8, p. 4977-4983
  • DOI: 10.1021/ef400748x

Reaction Kinetics of Freeze-Granulated NiO/MgAl2O4 Oxygen Carrier Particles for Chemical-Looping Combustion
journal, February 2007

  • Zafar, Qamar; Abad, Alberto; Mattisson, Tobias
  • Energy & Fuels, Vol. 21, Issue 2
  • DOI: 10.1021/ef060450y

Hydrogen production by catalytic decomposition of methane over Ni/SiO2Ni/SiO2☆
journal, August 2007


Reduction Kinetics of Cu-, Ni-, and Fe-Based Oxygen Carriers Using Syngas (CO + H2) for Chemical-Looping Combustion
journal, July 2007

  • Abad, Alberto; García-Labiano, Francisco; de Diego, Luis F.
  • Energy & Fuels, Vol. 21, Issue 4, p. 1843-1853
  • DOI: 10.1021/ef070025k

Redox Characteristics of Fe–Ni/SiO 2 Bimetallic Oxygen Carriers in CO under Conditions Pertinent to Chemical Looping Combustion
journal, October 2011

  • Song, Hui; Doroodchi, Elham; Moghtaderi, Behdad
  • Energy & Fuels, Vol. 26, Issue 1
  • DOI: 10.1021/ef201152u

Reactivity of Some Metal Oxides Supported on Alumina with Alternating Methane and Oxygen - Application for Chemical-Looping Combustion
journal, May 2003

  • Mattisson, Tobias; Järdnäs, Anders; Lyngfelt, Anders
  • Energy & Fuels, Vol. 17, Issue 3, p. 643-651
  • DOI: 10.1021/ef020151i

Mechanism of Methane Chemical Looping Combustion with Hematite Promoted with CeO 2
journal, March 2013

  • Miller, Duane D.; Siriwardane, Ranjani
  • Energy & Fuels, Vol. 27, Issue 8
  • DOI: 10.1021/ef302132e

A 300W laboratory reactor system for chemical-looping combustion with particle circulation
journal, July 2006


Studies on the redox reaction kinetics of Fe2O3–CuO/Al2O3 and Fe2O3/TiO2 oxygen carriers
journal, February 2014


The use of iron oxide as oxygen carrier in a chemical-looping reactor
journal, May 2007


Combustion of Syngas and Natural Gas in a 300 W Chemical-Looping Combustor
journal, September 2006

  • Johansson, E.; Mattisson, T.; Lyngfelt, A.
  • Chemical Engineering Research and Design, Vol. 84, Issue 9, p. 819-827
  • DOI: 10.1205/cherd05024

Iron-based syngas chemical looping process and coal-direct chemical looping process development at Ohio State University
journal, January 2014


Ilmenite with addition of NiO as oxygen carrier for chemical-looping combustion
journal, November 2010


Chemical-Looping Combustion and Chemical-Looping Reforming in a Circulating Fluidized-Bed Reactor Using Ni-Based Oxygen Carriers
journal, July 2008

  • Rydén, Magnus; Lyngfelt, Anders; Mattisson, Tobias
  • Energy & Fuels, Vol. 22, Issue 4
  • DOI: 10.1021/ef800065m