Single wall carbon nanotubes growth over cobalt-iron mesoporous MCM-41 bimetallic catalyst under methane chemical vapor deposition, an experimental and DFT evaluation
Cobalt and iron MCM-41 catalysts were synthesized through an in-situ incorporation process starting from commercial iron and cobalt nitrates. The incorporation was confirmed by diffuse reflectance UV spectroscopy (DRS-UV) inspecting the cobalt and iron silicate-like photon absorption features an...
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| Language: | English |
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Pontificia Universidad Javeriana
2020-07-01
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| Series: | Universitas Scientiarum |
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| Online Access: | https://revistas.javeriana.edu.co/index.php/scientarium/article/view/25896 |
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| author | Frank Ramírez-Rodríguez, Betty López |
| author_facet | Frank Ramírez-Rodríguez, Betty López |
| author_sort | Frank Ramírez-Rodríguez, Betty López |
| collection | DOAJ |
| description | Cobalt and iron MCM-41 catalysts were synthesized through an in-situ
incorporation process starting from commercial iron and cobalt nitrates.
The incorporation was confirmed by diffuse reflectance UV spectroscopy
(DRS-UV) inspecting the cobalt and iron silicate-like photon absorption
features and comparing with pure MCM-41-Co and MCM-41-Fe catalysts.
Additionally it was found that the incorporation of cobalt and iron does
not compromise the mesoporous structure of MCM-41 as confirmed by N2
adsorption isotherms. All catalysts showed high surface areas (∼1100 m2
g
−1
).
Catalysts performance was conducted in a simple methane chemical vapor
deposition (CVD) set up at 800 °C to produce single wall carbon nanotubes
(SWCNT) under a constant flow of methane for 30 min. CVD products were
characterized by thermogravimetric analysis (TGA) and Raman spectroscopy,
finding that the iron content in the catalysts favors the selectivity and yield
of graphitic-like structures, and confirming the presence of SWCNT by the
appearance of a characteristic radial breathing mode (RBM) signals. These
results were supported by Density Functional Theory (DFT) simulations of
the methane dissociation (CH4 +TM → H3C –TMH) over Con
(n = 1–5) and
ComFe (m = 1–4), finding a different activation energy trend where ComFe
(m = 1–4) clusters have the lower activation energy. The DFT study also
revealed a charge difference (δC − δTM) higher in the case of dissociation
over ComFe (m = 1–4) which may lead to an electrostatic stabilization of
the transition metal, diminishing the activation energy of those clusters and
leading to a faster carbon uptake. |
| format | Article |
| id | doaj-art-1082f6057a5b466faaa06eaf48485e71 |
| institution | DOAJ |
| issn | 0122-7483 2027-1352 |
| language | English |
| publishDate | 2020-07-01 |
| publisher | Pontificia Universidad Javeriana |
| record_format | Article |
| series | Universitas Scientiarum |
| spelling | doaj-art-1082f6057a5b466faaa06eaf48485e712025-08-20T03:06:12ZengPontificia Universidad JaverianaUniversitas Scientiarum0122-74832027-13522020-07-0125222724610.11144/Javeriana.SC25-2.swcnSingle wall carbon nanotubes growth over cobalt-iron mesoporous MCM-41 bimetallic catalyst under methane chemical vapor deposition, an experimental and DFT evaluationFrank Ramírez-Rodríguez, Betty López0University of Antioquia, Grupo Ciencia de los Materiales, Medellín, Colombia.Cobalt and iron MCM-41 catalysts were synthesized through an in-situ incorporation process starting from commercial iron and cobalt nitrates. The incorporation was confirmed by diffuse reflectance UV spectroscopy (DRS-UV) inspecting the cobalt and iron silicate-like photon absorption features and comparing with pure MCM-41-Co and MCM-41-Fe catalysts. Additionally it was found that the incorporation of cobalt and iron does not compromise the mesoporous structure of MCM-41 as confirmed by N2 adsorption isotherms. All catalysts showed high surface areas (∼1100 m2 g −1 ). Catalysts performance was conducted in a simple methane chemical vapor deposition (CVD) set up at 800 °C to produce single wall carbon nanotubes (SWCNT) under a constant flow of methane for 30 min. CVD products were characterized by thermogravimetric analysis (TGA) and Raman spectroscopy, finding that the iron content in the catalysts favors the selectivity and yield of graphitic-like structures, and confirming the presence of SWCNT by the appearance of a characteristic radial breathing mode (RBM) signals. These results were supported by Density Functional Theory (DFT) simulations of the methane dissociation (CH4 +TM → H3C –TMH) over Con (n = 1–5) and ComFe (m = 1–4), finding a different activation energy trend where ComFe (m = 1–4) clusters have the lower activation energy. The DFT study also revealed a charge difference (δC − δTM) higher in the case of dissociation over ComFe (m = 1–4) which may lead to an electrostatic stabilization of the transition metal, diminishing the activation energy of those clusters and leading to a faster carbon uptake.https://revistas.javeriana.edu.co/index.php/scientarium/article/view/25896dft; raman; swcnt; uv-vis. |
| spellingShingle | Frank Ramírez-Rodríguez, Betty López Single wall carbon nanotubes growth over cobalt-iron mesoporous MCM-41 bimetallic catalyst under methane chemical vapor deposition, an experimental and DFT evaluation Universitas Scientiarum dft; raman; swcnt; uv-vis. |
| title | Single wall carbon nanotubes growth over cobalt-iron mesoporous MCM-41 bimetallic catalyst under methane chemical vapor deposition, an experimental and DFT evaluation |
| title_full | Single wall carbon nanotubes growth over cobalt-iron mesoporous MCM-41 bimetallic catalyst under methane chemical vapor deposition, an experimental and DFT evaluation |
| title_fullStr | Single wall carbon nanotubes growth over cobalt-iron mesoporous MCM-41 bimetallic catalyst under methane chemical vapor deposition, an experimental and DFT evaluation |
| title_full_unstemmed | Single wall carbon nanotubes growth over cobalt-iron mesoporous MCM-41 bimetallic catalyst under methane chemical vapor deposition, an experimental and DFT evaluation |
| title_short | Single wall carbon nanotubes growth over cobalt-iron mesoporous MCM-41 bimetallic catalyst under methane chemical vapor deposition, an experimental and DFT evaluation |
| title_sort | single wall carbon nanotubes growth over cobalt iron mesoporous mcm 41 bimetallic catalyst under methane chemical vapor deposition an experimental and dft evaluation |
| topic | dft; raman; swcnt; uv-vis. |
| url | https://revistas.javeriana.edu.co/index.php/scientarium/article/view/25896 |
| work_keys_str_mv | AT frankramirezrodriguezbettylopez singlewallcarbonnanotubesgrowthovercobaltironmesoporousmcm41bimetalliccatalystundermethanechemicalvapordepositionanexperimentalanddftevaluation |