Controlling the stability of a Fe–Ni reforming catalyst: Structural organization of the active components
[Display omitted] •Enhanced control of the stability of carbon resistant Fe–Ni/MgAl2O4.•Formation of a core shell alloy with Fe–Ni in the core and Fe–Ni–Pd in the shell.•Catalyst with Ni:Pd molar ratio of 75:1 showed the best performance.•The addition of Pd to Fe–Ni reduces the tendency of Fe to seg...
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| Vydáno v: | Applied catalysis. B, Environmental Ročník 209; s. 405 - 416 |
|---|---|
| Hlavní autoři: | , , , , , |
| Médium: | Journal Article |
| Jazyk: | angličtina |
| Vydáno: |
Amsterdam
Elsevier B.V
15.07.2017
Elsevier BV |
| Témata: | |
| ISSN: | 0926-3373, 1873-3883 |
| On-line přístup: | Získat plný text |
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| Abstract | [Display omitted]
•Enhanced control of the stability of carbon resistant Fe–Ni/MgAl2O4.•Formation of a core shell alloy with Fe–Ni in the core and Fe–Ni–Pd in the shell.•Catalyst with Ni:Pd molar ratio of 75:1 showed the best performance.•The addition of Pd to Fe–Ni reduces the tendency of Fe to segregate from the alloy.
Fe–Ni catalysts present high activity in dry reforming of methane, with high carbon resistance, but suffer from deactivation via sintering and Fe segregation. Enhanced control of the stability and activity of Fe–Ni/MgAl2O4 was achieved by means of Pd addition. The evolution of the catalyst structure during H2 Temperature Programmed Reduction (TPR) and CO2 Temperature Programmed Oxidation (TPO) was investigated using time-resolved in situ X-ray diffraction (XRD). During reduction of Fe–Ni–Pd supported on MgAl2O4, a core shell alloy forms at the surface, where Fe–Ni is in the core and Fe–Ni–Pd in the shell. A 0.2wt% Pd loading or Ni:Pd molar ratio as high as 75:1 showed the best performance in terms of both activity and stability of the catalyst at 1023K and total pressure of 101.3kPa. Experimental results and DFT calculations showed that Pd addition to bimetallic Fe–Ni reduces the tendency of Fe to segregate to the surface of the alloy particles under methane dry reforming (DRM) conditions, due to the formation of a thin Fe–Ni–Pd surface layer. The latter acts as a barrier for Fe segregation from the core. Segregation of Fe from the trimetallic shell still occurs, but to a lesser extent as the Fe concentration is lower. This Ni:Pd molar ratio is capable of controlling the carbon formation and hence ensure high catalyst activity of 24.8mmols−1gmetals−1 after 21h time-on-stream. |
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| AbstractList | [Display omitted]
•Enhanced control of the stability of carbon resistant Fe–Ni/MgAl2O4.•Formation of a core shell alloy with Fe–Ni in the core and Fe–Ni–Pd in the shell.•Catalyst with Ni:Pd molar ratio of 75:1 showed the best performance.•The addition of Pd to Fe–Ni reduces the tendency of Fe to segregate from the alloy.
Fe–Ni catalysts present high activity in dry reforming of methane, with high carbon resistance, but suffer from deactivation via sintering and Fe segregation. Enhanced control of the stability and activity of Fe–Ni/MgAl2O4 was achieved by means of Pd addition. The evolution of the catalyst structure during H2 Temperature Programmed Reduction (TPR) and CO2 Temperature Programmed Oxidation (TPO) was investigated using time-resolved in situ X-ray diffraction (XRD). During reduction of Fe–Ni–Pd supported on MgAl2O4, a core shell alloy forms at the surface, where Fe–Ni is in the core and Fe–Ni–Pd in the shell. A 0.2wt% Pd loading or Ni:Pd molar ratio as high as 75:1 showed the best performance in terms of both activity and stability of the catalyst at 1023K and total pressure of 101.3kPa. Experimental results and DFT calculations showed that Pd addition to bimetallic Fe–Ni reduces the tendency of Fe to segregate to the surface of the alloy particles under methane dry reforming (DRM) conditions, due to the formation of a thin Fe–Ni–Pd surface layer. The latter acts as a barrier for Fe segregation from the core. Segregation of Fe from the trimetallic shell still occurs, but to a lesser extent as the Fe concentration is lower. This Ni:Pd molar ratio is capable of controlling the carbon formation and hence ensure high catalyst activity of 24.8mmols−1gmetals−1 after 21h time-on-stream. Fe-Ni catalysts present high activity in dry reforming of methane, with high carbon resistance, but suffer from deactivation via sintering and Fe segregation. Enhanced control of the stability and activity of Fe-Ni/MgAl2O4 was achieved by means of Pd addition. The evolution of the catalyst structure during H2 Temperature Programmed Reduction (TPR) and CO2 Temperature Programmed Oxidation (TPO) was investigated using time-resolved in situ X-ray diffraction (XRD). During reduction of Fe-Ni-Pd supported on MgAl2O4, a core shell alloy forms at the surface, where Fe-Ni is in the core and Fe-Ni-Pd in the shell. A 0.2 wt% Pd loading or Ni:Pd molar ratio as high as 75:1 showed the best performance in terms of both activity and stability of the catalyst at 1023 K and total pressure of 101.3 kPa. Experimental results and DFT calculations showed that Pd addition to bimetallic Fe-Ni reduces the tendency of Fe to segregate to the surface of the alloy particles under methane dry reforming (DRM) conditions, due to the formation of a thin Fe-Ni-Pd surface layer. The latter acts as a barrier for Fe segregation from the core. Segregation of Fe from the trimetallic shell still occurs, but to a lesser extent as the Fe concentration is lower. This Ni:Pd molar ratio is capable of controlling the carbon formation and hence ensure high catalyst activity of 24.8 mmol s-1 gmetals-1 after 21 h time-on-stream. |
| Author | Theofanidis, Stavros Alexandros Marin, Guy B. Detavernier, Christophe Sabbe, Maarten Galvita, Vladimir V. Poelman, Hilde |
| Author_xml | – sequence: 1 givenname: Stavros Alexandros surname: Theofanidis fullname: Theofanidis, Stavros Alexandros organization: Laboratory for Chemical Technology, Ghent University, Technologiepark 914, B-9052 Ghent, Belgium – sequence: 2 givenname: Vladimir V. surname: Galvita fullname: Galvita, Vladimir V. email: Vladimir.Galvita@UGent.be organization: Laboratory for Chemical Technology, Ghent University, Technologiepark 914, B-9052 Ghent, Belgium – sequence: 3 givenname: Maarten surname: Sabbe fullname: Sabbe, Maarten organization: Laboratory for Chemical Technology, Ghent University, Technologiepark 914, B-9052 Ghent, Belgium – sequence: 4 givenname: Hilde surname: Poelman fullname: Poelman, Hilde organization: Laboratory for Chemical Technology, Ghent University, Technologiepark 914, B-9052 Ghent, Belgium – sequence: 5 givenname: Christophe surname: Detavernier fullname: Detavernier, Christophe organization: Department of Solid State Sciences, Ghent University, Krijgslaan 281, S1, B-9000 Ghent, Belgium – sequence: 6 givenname: Guy B. surname: Marin fullname: Marin, Guy B. organization: Laboratory for Chemical Technology, Ghent University, Technologiepark 914, B-9052 Ghent, Belgium |
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| Keywords | Catalyst stability Methane reforming Synthesis gas In situ XRD Fe–Ni alloy |
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•Enhanced control of the stability of carbon resistant Fe–Ni/MgAl2O4.•Formation of a core shell alloy with Fe–Ni in the core and Fe–Ni–Pd in... Fe-Ni catalysts present high activity in dry reforming of methane, with high carbon resistance, but suffer from deactivation via sintering and Fe segregation.... |
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| SubjectTerms | Bimetals Carbon dioxide Catalyst stability Catalysts Control stability Deactivation Fe–Ni alloy In situ XRD Iron Methane Methane reforming Nickel Oxidation Reduction Reforming Sintering Surface layers Synthesis gas Temperature effects X-ray diffraction |
| Title | Controlling the stability of a Fe–Ni reforming catalyst: Structural organization of the active components |
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