Effect of Fe/N-doped carbon nanotube (CNT) wall thickness on CO<sub>2</sub> conversion: A DFT study

<p dir="ltr">Many researches on CO<sub>2</sub> adsorption using carbon nanotubes (CNTs) have been actively studied, but experimental and theoretical studies on CO<sub>2</sub> conversion are still in demand. In particular, the effect of CNT wall thickness on CO...

وصف كامل

محفوظ في:
التفاصيل البيبلوغرافية
المؤلف الرئيسي: Sun Hee Yoon (7179263) (author)
مؤلفون آخرون: Hyunwoong Park (1521754) (author), Nimir O. Elbashir (1850563) (author), Dong Suk Han (1748989) (author)
منشور في: 2020
الموضوعات:
الوسوم: إضافة وسم
لا توجد وسوم, كن أول من يضع وسما على هذه التسجيلة!
_version_ 1864513558932357120
author Sun Hee Yoon (7179263)
author2 Hyunwoong Park (1521754)
Nimir O. Elbashir (1850563)
Dong Suk Han (1748989)
author2_role author
author
author
author_facet Sun Hee Yoon (7179263)
Hyunwoong Park (1521754)
Nimir O. Elbashir (1850563)
Dong Suk Han (1748989)
author_role author
dc.creator.none.fl_str_mv Sun Hee Yoon (7179263)
Hyunwoong Park (1521754)
Nimir O. Elbashir (1850563)
Dong Suk Han (1748989)
dc.date.none.fl_str_mv 2020-12-01T00:00:00Z
dc.identifier.none.fl_str_mv 10.1016/j.susmat.2020.e00224
dc.relation.none.fl_str_mv https://figshare.com/articles/journal_contribution/Effect_of_Fe_N-doped_carbon_nanotube_CNT_wall_thickness_on_CO_sub_2_sub_conversion_A_DFT_study/24242596
dc.rights.none.fl_str_mv CC BY 4.0
info:eu-repo/semantics/openAccess
dc.subject.none.fl_str_mv Engineering
Chemical engineering
Materials engineering
Carbon nanotube
CO2 conversion
Density functional theory
Wall thickness
Formate
dc.title.none.fl_str_mv Effect of Fe/N-doped carbon nanotube (CNT) wall thickness on CO<sub>2</sub> conversion: A DFT study
dc.type.none.fl_str_mv Text
Journal contribution
info:eu-repo/semantics/publishedVersion
text
contribution to journal
description <p dir="ltr">Many researches on CO<sub>2</sub> adsorption using carbon nanotubes (CNTs) have been actively studied, but experimental and theoretical studies on CO<sub>2</sub> conversion are still in demand. In particular, the effect of CNT wall thickness on CO<sub>2</sub> conversion is not yet established clearly. This study employed two different-walled CNT catalysts doped with iron and nitrogen, single-walled CNT (Fe-N-SWCNT) and double-walled CNT (Fe-N-DWCNT). The structural and electrical properties of these CNTs and their influences on CO<sub>2</sub> conversion were characterized and compared using density functional theory (DFT) calculations. As a result, Fe-N-DWCNT was shown to improve catalyst stability with higher formation energy and adsorption energy for CO<sub>2</sub> adsorption than Fe-N-SWCNT. Also, the CO<sub>2</sub> molecules were found to be highly delocalized and strongly hybridized with Fe-N-DWCNT, leading to more active charge transfer in the catalyst. These findings demonstrate the potential of selective CO<sub>2</sub> conversion, as wall thickness differences can lead to different electrical properties of CNTs by showing that the larger the thicknesses, the lower the energy barrier required for CO<sub>2</sub> conversion. Specifically, Fe-N-DWCNT is easier to convert CO<sub>2</sub> to HCOOH than Fe-N-SWCNT at lower overpotential (0.15 V) obtained with limiting potentials and free energies calculated by understanding the possible reaction pathways in the proton-electron transfer process. Therefore, these results support the hypothesis that the wall thickness of CNT influences CO<sub>2</sub> conversion by showing that the double-walled heterogeneous CNT (Fe-N-DWCNT) is a potential catalyst to selectively produce HCOOH from CO<sub>2</sub> conversion.</p><h2>Other Information</h2><p dir="ltr">Published in: Sustainable Materials and Technologies<br>License: <a href="http://creativecommons.org/licenses/by/4.0/" target="_blank">http://creativecommons.org/licenses/by/4.0/</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.1016/j.susmat.2020.e00224" target="_blank">https://dx.doi.org/10.1016/j.susmat.2020.e00224</a></p>
eu_rights_str_mv openAccess
id Manara2_0b7ccef4085548a71e449f8b99cebed4
identifier_str_mv 10.1016/j.susmat.2020.e00224
network_acronym_str Manara2
network_name_str Manara2
oai_identifier_str oai:figshare.com:article/24242596
publishDate 2020
repository.mail.fl_str_mv
repository.name.fl_str_mv
repository_id_str
rights_invalid_str_mv CC BY 4.0
spelling Effect of Fe/N-doped carbon nanotube (CNT) wall thickness on CO<sub>2</sub> conversion: A DFT studySun Hee Yoon (7179263)Hyunwoong Park (1521754)Nimir O. Elbashir (1850563)Dong Suk Han (1748989)EngineeringChemical engineeringMaterials engineeringCarbon nanotubeCO2 conversionDensity functional theoryWall thicknessFormate<p dir="ltr">Many researches on CO<sub>2</sub> adsorption using carbon nanotubes (CNTs) have been actively studied, but experimental and theoretical studies on CO<sub>2</sub> conversion are still in demand. In particular, the effect of CNT wall thickness on CO<sub>2</sub> conversion is not yet established clearly. This study employed two different-walled CNT catalysts doped with iron and nitrogen, single-walled CNT (Fe-N-SWCNT) and double-walled CNT (Fe-N-DWCNT). The structural and electrical properties of these CNTs and their influences on CO<sub>2</sub> conversion were characterized and compared using density functional theory (DFT) calculations. As a result, Fe-N-DWCNT was shown to improve catalyst stability with higher formation energy and adsorption energy for CO<sub>2</sub> adsorption than Fe-N-SWCNT. Also, the CO<sub>2</sub> molecules were found to be highly delocalized and strongly hybridized with Fe-N-DWCNT, leading to more active charge transfer in the catalyst. These findings demonstrate the potential of selective CO<sub>2</sub> conversion, as wall thickness differences can lead to different electrical properties of CNTs by showing that the larger the thicknesses, the lower the energy barrier required for CO<sub>2</sub> conversion. Specifically, Fe-N-DWCNT is easier to convert CO<sub>2</sub> to HCOOH than Fe-N-SWCNT at lower overpotential (0.15 V) obtained with limiting potentials and free energies calculated by understanding the possible reaction pathways in the proton-electron transfer process. Therefore, these results support the hypothesis that the wall thickness of CNT influences CO<sub>2</sub> conversion by showing that the double-walled heterogeneous CNT (Fe-N-DWCNT) is a potential catalyst to selectively produce HCOOH from CO<sub>2</sub> conversion.</p><h2>Other Information</h2><p dir="ltr">Published in: Sustainable Materials and Technologies<br>License: <a href="http://creativecommons.org/licenses/by/4.0/" target="_blank">http://creativecommons.org/licenses/by/4.0/</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.1016/j.susmat.2020.e00224" target="_blank">https://dx.doi.org/10.1016/j.susmat.2020.e00224</a></p>2020-12-01T00:00:00ZTextJournal contributioninfo:eu-repo/semantics/publishedVersiontextcontribution to journal10.1016/j.susmat.2020.e00224https://figshare.com/articles/journal_contribution/Effect_of_Fe_N-doped_carbon_nanotube_CNT_wall_thickness_on_CO_sub_2_sub_conversion_A_DFT_study/24242596CC BY 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/242425962020-12-01T00:00:00Z
spellingShingle Effect of Fe/N-doped carbon nanotube (CNT) wall thickness on CO<sub>2</sub> conversion: A DFT study
Sun Hee Yoon (7179263)
Engineering
Chemical engineering
Materials engineering
Carbon nanotube
CO2 conversion
Density functional theory
Wall thickness
Formate
status_str publishedVersion
title Effect of Fe/N-doped carbon nanotube (CNT) wall thickness on CO<sub>2</sub> conversion: A DFT study
title_full Effect of Fe/N-doped carbon nanotube (CNT) wall thickness on CO<sub>2</sub> conversion: A DFT study
title_fullStr Effect of Fe/N-doped carbon nanotube (CNT) wall thickness on CO<sub>2</sub> conversion: A DFT study
title_full_unstemmed Effect of Fe/N-doped carbon nanotube (CNT) wall thickness on CO<sub>2</sub> conversion: A DFT study
title_short Effect of Fe/N-doped carbon nanotube (CNT) wall thickness on CO<sub>2</sub> conversion: A DFT study
title_sort Effect of Fe/N-doped carbon nanotube (CNT) wall thickness on CO<sub>2</sub> conversion: A DFT study
topic Engineering
Chemical engineering
Materials engineering
Carbon nanotube
CO2 conversion
Density functional theory
Wall thickness
Formate