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Looking inside a Ni-Fe/MgAl2O4 catalyst for methane dry reforming via Mössbauer spectroscopy and in situ QXAS

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Abstract
The evolution of the constituents of an 8 wt%Ni-5 wt%Fe/MgAl2O4 catalyst for dry reforming of methane (DRM) is monitored by in situ quick X-ray absorption spectroscopy (QXAS) and Fe-57 Mossbauer spectroscopy. In as prepared state, Fe is present as NiFe2O4 at the surface and as MgFex3+Al2-xO4 within the support, whereas Ni is mainly present as NiO. During H-2-TPR, NiFe2O4 and NiO form an alloy from 500 degrees C on and (MgFex+Al2-xO4)-Al-3 is partially reduced to MgFex2+Al2-xO4, such that Ni-Fe alloy, MgFex2+Al2-xO4 and MgFex3+Al2-xO4 are the prevalent phases in the reduced catalyst. During DRM, dominantly oxidizing environments (CH4/CO2 = 1/2, 1/1.5) lead to formation of FeOx nanoparticles at the surface of the Ni-Fe alloy, thereby affecting the DRM activity, and possibly to some reincorporation of Fe into the support. For CH4/CO2 = 1/1, no significant changes occur in the catalyst's activated state, as a consequence of reduction by CH4 dissociation species counteracting oxidation by CO2. However, Mossbauer analysis detects continued extraction of Fe from the support, sustaining ongoing NiFe alloying.
Keywords
Process Chemistry and Technology, General Environmental Science, Catalysis, Ni-Fe alloy, X-ray absorption spectroscopy, MCR-ALSCO2 re-oxidation, METAL-SUPPORT INTERACTION, LOOPING PARTIAL OXIDATION, PRE-EDGE FEATURES, FE-NI, NI/MGAL2O4 CATALYST, CO2 CONVERSION, NICKEL, STEAM, STABILITY, MGAL2O4

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MLA
De Coster, Valentijn, et al. “Looking inside a Ni-Fe/MgAl2O4 Catalyst for Methane Dry Reforming via Mössbauer Spectroscopy and in Situ QXAS.” APPLIED CATALYSIS B-ENVIRONMENTAL, vol. 300, 2022, doi:10.1016/j.apcatb.2021.120720.
APA
De Coster, V., Nadadur Veeraraghavan Srinath, Theofanidis, S.-A., Pirro, L., Van Alboom, A., Poelman, H., … Galvita, V. (2022). Looking inside a Ni-Fe/MgAl2O4 catalyst for methane dry reforming via Mössbauer spectroscopy and in situ QXAS. APPLIED CATALYSIS B-ENVIRONMENTAL, 300. https://doi.org/10.1016/j.apcatb.2021.120720
Chicago author-date
De Coster, Valentijn, Nadadur Veeraraghavan Srinath, Stavros-Alexandros Theofanidis, Laura Pirro, Antoine Van Alboom, Hilde Poelman, Maarten Sabbe, Guy Marin, and Vladimir Galvita. 2022. “Looking inside a Ni-Fe/MgAl2O4 Catalyst for Methane Dry Reforming via Mössbauer Spectroscopy and in Situ QXAS.” APPLIED CATALYSIS B-ENVIRONMENTAL 300. https://doi.org/10.1016/j.apcatb.2021.120720.
Chicago author-date (all authors)
De Coster, Valentijn, Nadadur Veeraraghavan Srinath, Stavros-Alexandros Theofanidis, Laura Pirro, Antoine Van Alboom, Hilde Poelman, Maarten Sabbe, Guy Marin, and Vladimir Galvita. 2022. “Looking inside a Ni-Fe/MgAl2O4 Catalyst for Methane Dry Reforming via Mössbauer Spectroscopy and in Situ QXAS.” APPLIED CATALYSIS B-ENVIRONMENTAL 300. doi:10.1016/j.apcatb.2021.120720.
Vancouver
1.
De Coster V, Nadadur Veeraraghavan Srinath, Theofanidis S-A, Pirro L, Van Alboom A, Poelman H, et al. Looking inside a Ni-Fe/MgAl2O4 catalyst for methane dry reforming via Mössbauer spectroscopy and in situ QXAS. APPLIED CATALYSIS B-ENVIRONMENTAL. 2022;300.
IEEE
[1]
V. De Coster et al., “Looking inside a Ni-Fe/MgAl2O4 catalyst for methane dry reforming via Mössbauer spectroscopy and in situ QXAS,” APPLIED CATALYSIS B-ENVIRONMENTAL, vol. 300, 2022.
@article{8733304,
  abstract     = {{The evolution of the constituents of an 8 wt%Ni-5 wt%Fe/MgAl2O4 catalyst for dry reforming of methane (DRM) is monitored by in situ quick X-ray absorption spectroscopy (QXAS) and Fe-57 Mossbauer spectroscopy. In as prepared state, Fe is present as NiFe2O4 at the surface and as MgFex3+Al2-xO4 within the support, whereas Ni is mainly present as NiO. During H-2-TPR, NiFe2O4 and NiO form an alloy from 500 degrees C on and (MgFex+Al2-xO4)-Al-3 is partially reduced to MgFex2+Al2-xO4, such that Ni-Fe alloy, MgFex2+Al2-xO4 and MgFex3+Al2-xO4 are the prevalent phases in the reduced catalyst. During DRM, dominantly oxidizing environments (CH4/CO2 = 1/2, 1/1.5) lead to formation of FeOx nanoparticles at the surface of the Ni-Fe alloy, thereby affecting the DRM activity, and possibly to some reincorporation of Fe into the support. For CH4/CO2 = 1/1, no significant changes occur in the catalyst's activated state, as a consequence of reduction by CH4 dissociation species counteracting oxidation by CO2. However, Mossbauer analysis detects continued extraction of Fe from the support, sustaining ongoing NiFe alloying.}},
  articleno    = {{120720}},
  author       = {{De Coster, Valentijn and Nadadur Veeraraghavan Srinath and Theofanidis, Stavros-Alexandros and Pirro, Laura and Van Alboom, Antoine and Poelman, Hilde and Sabbe, Maarten and Marin, Guy and Galvita, Vladimir}},
  issn         = {{0926-3373}},
  journal      = {{APPLIED CATALYSIS B-ENVIRONMENTAL}},
  keywords     = {{Process Chemistry and Technology,General Environmental Science,Catalysis,Ni-Fe alloy,X-ray absorption spectroscopy,MCR-ALSCO2 re-oxidation,METAL-SUPPORT INTERACTION,LOOPING PARTIAL OXIDATION,PRE-EDGE FEATURES,FE-NI,NI/MGAL2O4 CATALYST,CO2 CONVERSION,NICKEL,STEAM,STABILITY,MGAL2O4}},
  language     = {{eng}},
  pages        = {{13}},
  title        = {{Looking inside a Ni-Fe/MgAl2O4 catalyst for methane dry reforming via Mössbauer spectroscopy and in situ QXAS}},
  url          = {{http://dx.doi.org/10.1016/j.apcatb.2021.120720}},
  volume       = {{300}},
  year         = {{2022}},
}

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