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Deactivation study of Fe2O3−CeO2 during redox cycles for CO production from CO2

Naga Venkata Ranga Aditya Dharanipragada, Maria Meledina, Vladimir Galvita UGent, Hilde Poelman UGent, Stuart Turner, Gustaaf Van Tendeloo, Christophe Detavernier UGent and Guy Marin UGent (2016) INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH. 55(20). p.5911-5922
abstract
Deactivation was investigated in Fe2O3-CeO2 oxygen storage materials during repeated H-2-reduction and CO2-reoxidation. In situ XRD, XAS, and TEM were used to identify phases, crystallite sizes, and morphological changes upon cycling operation. The effect of redox cycling was investigated both in Fe-rich (80 wt % Fe2O3-CeO2) and Ce-rich (10 wt %Fe2O3-CeO2) materials. The former consisted of 100 nm Fe2O3 particles decorated with 5-10 nm Ce1-xFexO2-x. The latter presented CeO2 with incorporated Fe, i.e. a solid solution of Ce1-xFexO2-x, as the main oxygen carrier. By modeling the EXAFS Ce-K signal for as-prepared 10 wt %Fe2O3-CeO2, the amount of Fe in CeO2 was determined as 21 mol %, corresponding to 86% of the total iron content. Sintering and solid solid transformations, the latter including both new phase formation and element segregation, were identified as deactivation pathways upon redox cycling. In Ce-rich material, perovskite (CeFeO3) was identified by XRD. This phase remained inert during reduction and reoxidation, resulting in an overall lower oxygen storage capacity. Further, Fe segregated from the solid solution, thereby decreasing its reducibility. In addition, an increase in crystallite size occurred for all phases. In Fe-rich material, sintering is the main deactivation pathway, although Fe segregation from the solid solution and perovskite formation cannot be excluded.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
OXYGEN STORAGE MATERIAL, CHEMICAL-LOOPING COMBUSTION, IRON-OXIDE MATERIALS, X-RAY-DIFFRACTION, GAS SHIFT PROCESS, HYDROGEN-PRODUCTION, CARRIER, METHANE, REDUCTION, FE
journal title
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
Ind. Eng. Chem. Res.
volume
55
issue
20
pages
5911 - 5922
Web of Science type
Article
Web of Science id
000376825300013
JCR category
ENGINEERING, CHEMICAL
JCR impact factor
2.843 (2016)
JCR rank
34/135 (2016)
JCR quartile
2 (2016)
ISSN
0888-5885
DOI
10.1021/acs.iecr.6b00963
language
English
UGent publication?
yes
classification
A1
copyright statement
I have transferred the copyright for this publication to the publisher
id
8055035
handle
http://hdl.handle.net/1854/LU-8055035
date created
2016-08-25 14:28:52
date last changed
2017-03-09 12:54:27
@article{8055035,
  abstract     = {Deactivation was investigated in Fe2O3-CeO2 oxygen storage materials during repeated H-2-reduction and CO2-reoxidation. In situ XRD, XAS, and TEM were used to identify phases, crystallite sizes, and morphological changes upon cycling operation. The effect of redox cycling was investigated both in Fe-rich (80 wt \% Fe2O3-CeO2) and Ce-rich (10 wt \%Fe2O3-CeO2) materials. The former consisted of 100 nm Fe2O3 particles decorated with 5-10 nm Ce1-xFexO2-x. The latter presented CeO2 with incorporated Fe, i.e. a solid solution of Ce1-xFexO2-x, as the main oxygen carrier. By modeling the EXAFS Ce-K signal for as-prepared 10 wt \%Fe2O3-CeO2, the amount of Fe in CeO2 was determined as 21 mol \%, corresponding to 86\% of the total iron content. Sintering and solid solid transformations, the latter including both new phase formation and element segregation, were identified as deactivation pathways upon redox cycling. In Ce-rich material, perovskite (CeFeO3) was identified by XRD. This phase remained inert during reduction and reoxidation, resulting in an overall lower oxygen storage capacity. Further, Fe segregated from the solid solution, thereby decreasing its reducibility. In addition, an increase in crystallite size occurred for all phases. In Fe-rich material, sintering is the main deactivation pathway, although Fe segregation from the solid solution and perovskite formation cannot be excluded.},
  author       = {Dharanipragada, Naga Venkata Ranga Aditya and Meledina, Maria and Galvita, Vladimir and Poelman, Hilde and Turner, Stuart and Van Tendeloo, Gustaaf and Detavernier, Christophe and Marin, Guy},
  issn         = {0888-5885},
  journal      = {INDUSTRIAL \& ENGINEERING CHEMISTRY RESEARCH},
  keyword      = {OXYGEN STORAGE MATERIAL,CHEMICAL-LOOPING COMBUSTION,IRON-OXIDE MATERIALS,X-RAY-DIFFRACTION,GAS SHIFT PROCESS,HYDROGEN-PRODUCTION,CARRIER,METHANE,REDUCTION,FE},
  language     = {eng},
  number       = {20},
  pages        = {5911--5922},
  title        = {Deactivation study of Fe2O3\ensuremath{-}CeO2 during redox cycles for CO production from CO2},
  url          = {http://dx.doi.org/10.1021/acs.iecr.6b00963},
  volume       = {55},
  year         = {2016},
}

Chicago
Dharanipragada, Naga Venkata Ranga Aditya, Maria Meledina, Vladimir Galvita, Hilde Poelman, Stuart Turner, Gustaaf Van Tendeloo, Christophe Detavernier, and Guy Marin. 2016. “Deactivation Study of Fe2O3−CeO2 During Redox Cycles for CO Production from CO2.” Industrial & Engineering Chemistry Research 55 (20): 5911–5922.
APA
Dharanipragada, N. V. R. A., Meledina, M., Galvita, V., Poelman, H., Turner, S., Van Tendeloo, G., Detavernier, C., et al. (2016). Deactivation study of Fe2O3−CeO2 during redox cycles for CO production from CO2. INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 55(20), 5911–5922.
Vancouver
1.
Dharanipragada NVRA, Meledina M, Galvita V, Poelman H, Turner S, Van Tendeloo G, et al. Deactivation study of Fe2O3−CeO2 during redox cycles for CO production from CO2. INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH. 2016;55(20):5911–22.
MLA
Dharanipragada, Naga Venkata Ranga Aditya, Maria Meledina, Vladimir Galvita, et al. “Deactivation Study of Fe2O3−CeO2 During Redox Cycles for CO Production from CO2.” INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 55.20 (2016): 5911–5922. Print.