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Sustainable iron-based oxygen carriers for hydrogen production : real-time operando investigation

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Abstract
In this work, a spray-dried Fe-based oxygen carrier with an in situ generated Mg1-xAl2-yFex+yO4-support was investigated during packed-bed chemical looping operation with methane at 900 degrees C. The evolution of the solid-state chemistry taking place in the oxygen carrier material was investigated in real-time with synchrotron X-ray diffraction while the spatial distribution of the phases was investigated using X-ray diffraction computed tomography (XRD-CT). These measurements revealed that some Fe-cations were systematically taken up and released from the spinel support. This take-up and release was shown to be strongly related with the oxidation state of the active phase. Although this take-up and release of Fe-cations decreased the amount of Fe-oxides active in the chemical looping process, the oxygen transfer capacity was still sufficiently high. The microstructure of the oxygen carriers along the length of the packed reactor bed was also investigated with scanning electron microscopy (SEM). The experiments indicate that the MgFeAlOx support with an extra Fe-based active phase is a promising material for oxygen carriers, as it forms a sustainable non-toxic, stable and green alternative to the typical Ni-based oxygen carriers, for hydrogen generation by chemical looping.
Keywords
Chemical looping, Oxygen carrier, Iron oxide, Diffraction tomography, CHEMICAL-LOOPING COMBUSTION, PACKED-BED, CO2 CONVERSION, NATURAL-GAS, METHANE, STABILITY, SUPPORT, CLC, SYNGAS, PROGRESS

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MLA
De Vos, Yoran, et al. “Sustainable Iron-Based Oxygen Carriers for Hydrogen Production : Real-Time Operando Investigation.” INTERNATIONAL JOURNAL OF GREENHOUSE GAS CONTROL, vol. 88, 2019, pp. 393–402, doi:10.1016/j.ijggc.2019.06.016.
APA
De Vos, Y., Vamvakeros, A., Matras, D., Jacobs, M., Van Der Voort, P., Van Driessche, I., … Verberckmoes, A. (2019). Sustainable iron-based oxygen carriers for hydrogen production : real-time operando investigation. INTERNATIONAL JOURNAL OF GREENHOUSE GAS CONTROL, 88, 393–402. https://doi.org/10.1016/j.ijggc.2019.06.016
Chicago author-date
De Vos, Yoran, Antonis Vamvakeros, Dorota Matras, Marijke Jacobs, Pascal Van Der Voort, Isabel Van Driessche, Simon Jacques, Vesna Middelkoop, and An Verberckmoes. 2019. “Sustainable Iron-Based Oxygen Carriers for Hydrogen Production : Real-Time Operando Investigation.” INTERNATIONAL JOURNAL OF GREENHOUSE GAS CONTROL 88: 393–402. https://doi.org/10.1016/j.ijggc.2019.06.016.
Chicago author-date (all authors)
De Vos, Yoran, Antonis Vamvakeros, Dorota Matras, Marijke Jacobs, Pascal Van Der Voort, Isabel Van Driessche, Simon Jacques, Vesna Middelkoop, and An Verberckmoes. 2019. “Sustainable Iron-Based Oxygen Carriers for Hydrogen Production : Real-Time Operando Investigation.” INTERNATIONAL JOURNAL OF GREENHOUSE GAS CONTROL 88: 393–402. doi:10.1016/j.ijggc.2019.06.016.
Vancouver
1.
De Vos Y, Vamvakeros A, Matras D, Jacobs M, Van Der Voort P, Van Driessche I, et al. Sustainable iron-based oxygen carriers for hydrogen production : real-time operando investigation. INTERNATIONAL JOURNAL OF GREENHOUSE GAS CONTROL. 2019;88:393–402.
IEEE
[1]
Y. De Vos et al., “Sustainable iron-based oxygen carriers for hydrogen production : real-time operando investigation,” INTERNATIONAL JOURNAL OF GREENHOUSE GAS CONTROL, vol. 88, pp. 393–402, 2019.
@article{8623086,
  abstract     = {{In this work, a spray-dried Fe-based oxygen carrier with an in situ generated Mg1-xAl2-yFex+yO4-support was investigated during packed-bed chemical looping operation with methane at 900 degrees C. The evolution of the solid-state chemistry taking place in the oxygen carrier material was investigated in real-time with synchrotron X-ray diffraction while the spatial distribution of the phases was investigated using X-ray diffraction computed tomography (XRD-CT). These measurements revealed that some Fe-cations were systematically taken up and released from the spinel support. This take-up and release was shown to be strongly related with the oxidation state of the active phase. Although this take-up and release of Fe-cations decreased the amount of Fe-oxides active in the chemical looping process, the oxygen transfer capacity was still sufficiently high. The microstructure of the oxygen carriers along the length of the packed reactor bed was also investigated with scanning electron microscopy (SEM). The experiments indicate that the MgFeAlOx support with an extra Fe-based active phase is a promising material for oxygen carriers, as it forms a sustainable non-toxic, stable and green alternative to the typical Ni-based oxygen carriers, for hydrogen generation by chemical looping.}},
  author       = {{De Vos, Yoran and Vamvakeros, Antonis and Matras, Dorota and Jacobs, Marijke and Van Der Voort, Pascal and Van Driessche, Isabel and Jacques, Simon and Middelkoop, Vesna and Verberckmoes, An}},
  issn         = {{1750-5836}},
  journal      = {{INTERNATIONAL JOURNAL OF GREENHOUSE GAS CONTROL}},
  keywords     = {{Chemical looping,Oxygen carrier,Iron oxide,Diffraction tomography,CHEMICAL-LOOPING COMBUSTION,PACKED-BED,CO2 CONVERSION,NATURAL-GAS,METHANE,STABILITY,SUPPORT,CLC,SYNGAS,PROGRESS}},
  language     = {{eng}},
  location     = {{Park City, UT, USA}},
  pages        = {{393--402}},
  title        = {{Sustainable iron-based oxygen carriers for hydrogen production : real-time operando investigation}},
  url          = {{http://dx.doi.org/10.1016/j.ijggc.2019.06.016}},
  volume       = {{88}},
  year         = {{2019}},
}

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