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Local environment of Fe dopants in nanoscale Fe: CeO2-x oxygen storage material

(2015) NANOSCALE. 7(7). p.3196-3204
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Abstract
Nanoscale Fe : CeO2-x oxygen storage material for the process of chemical looping has been investigated by advanced transmission electron microscopy and electron energy-loss spectroscopy before and after a model looping procedure, consisting of redox cycles at heightened temperature. Separately, the activity of the nanomaterial has been tested in a toluene total oxidation reaction. The results show that the material consists of ceria nanoparticles, doped with single Fe atoms and small FeOx clusters. The iron ion is partially present as Fe3+ in a solid solution within the ceria lattice. Furthermore, enrichment of reduced Fe2+ species is observed in nanovoids present in the ceria nanoparticles, as well as at the ceria surface. After chemical looping, agglomeration occurs and reduced nanoclusters appear at ceria grain boundaries formed by sintering. These clusters originate from surface Fe2+ aggregation, and from bulk Fe3+, which "leaks out" in reduced state after cycling to a slightly more agglomerated form. The activity of Fe : CeO2 during the toluene total oxidation part of the chemical looping cycle is ensured by the dopant Fe in the Fe1-xCexO2 solid solution, and by surface Fe species. These measurements on a model Fe : CeO2-x oxygen storage material give a unique insight into the behavior of dopants within a nanosized ceria host, and allow to interpret a plethora of (doped) cerium oxide-based reactions.
Keywords
TRANSITION-METAL, SHALLOW TRENCH ISOLATION, SOLID-SOLUTIONS, TOTAL OXIDATION, CERIUM OXIDE, NANOPARTICLES, COMBUSTION, METHANE, ENERGY, WATER

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Chicago
Meledina, M, S Turner, Vladimir Galvita, Hilde Poelman, Guy Marin, and G Van Tendeloo. 2015. “Local Environment of Fe Dopants in Nanoscale Fe: CeO2-x Oxygen Storage Material.” Nanoscale 7 (7): 3196–3204.
APA
Meledina, M, Turner, S., Galvita, V., Poelman, H., Marin, G., & Van Tendeloo, G. (2015). Local environment of Fe dopants in nanoscale Fe: CeO2-x oxygen storage material. NANOSCALE, 7(7), 3196–3204.
Vancouver
1.
Meledina M, Turner S, Galvita V, Poelman H, Marin G, Van Tendeloo G. Local environment of Fe dopants in nanoscale Fe: CeO2-x oxygen storage material. NANOSCALE. 2015;7(7):3196–204.
MLA
Meledina, M, S Turner, Vladimir Galvita, et al. “Local Environment of Fe Dopants in Nanoscale Fe: CeO2-x Oxygen Storage Material.” NANOSCALE 7.7 (2015): 3196–3204. Print.
@article{6880185,
  abstract     = {Nanoscale Fe : CeO2-x oxygen storage material for the process of chemical looping has been investigated by advanced transmission electron microscopy and electron energy-loss spectroscopy before and after a model looping procedure, consisting of redox cycles at heightened temperature. Separately, the activity of the nanomaterial has been tested in a toluene total oxidation reaction. The results show that the material consists of ceria nanoparticles, doped with single Fe atoms and small FeOx clusters. The iron ion is partially present as Fe3+ in a solid solution within the ceria lattice. Furthermore, enrichment of reduced Fe2+ species is observed in nanovoids present in the ceria nanoparticles, as well as at the ceria surface. After chemical looping, agglomeration occurs and reduced nanoclusters appear at ceria grain boundaries formed by sintering. These clusters originate from surface Fe2+ aggregation, and from bulk Fe3+, which {\textacutedbl}leaks out{\textacutedbl} in reduced state after cycling to a slightly more agglomerated form. The activity of Fe : CeO2 during the toluene total oxidation part of the chemical looping cycle is ensured by the dopant Fe in the Fe1-xCexO2 solid solution, and by surface Fe species. These measurements on a model Fe : CeO2-x oxygen storage material give a unique insight into the behavior of dopants within a nanosized ceria host, and allow to interpret a plethora of (doped) cerium oxide-based reactions.},
  author       = {Meledina, M and Turner, S and Galvita, Vladimir and Poelman, Hilde and Marin, Guy and Van Tendeloo, G},
  issn         = {2040-3364},
  journal      = {NANOSCALE},
  keyword      = {TRANSITION-METAL,SHALLOW TRENCH ISOLATION,SOLID-SOLUTIONS,TOTAL OXIDATION,CERIUM OXIDE,NANOPARTICLES,COMBUSTION,METHANE,ENERGY,WATER},
  language     = {eng},
  number       = {7},
  pages        = {3196--3204},
  title        = {Local environment of Fe dopants in nanoscale Fe: CeO2-x oxygen storage material},
  url          = {http://dx.doi.org/10.1039/c4nr06060a},
  volume       = {7},
  year         = {2015},
}

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