Surface activity of early transition-metal oxycarbides: CO2 adsorption case study

Theoretical studies and experiments have suggested that transition metal carbides (TMCs) can be useful materials for carbon capture and storage or use technologies from air sources. However, TMCs are known to become easily oxidized in the presence of molecular oxygen, and their properties jeopardize...

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Autores: Kunkel, Christian, Viñes Solana, Francesc, Illas i Riera, Francesc
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2019
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2445/165637
Acceso en línea:https://hdl.handle.net/2445/165637
Access Level:acceso abierto
Palabra clave:Carburs
Metalls de transició
Adsorció
Carbides
Transition metals
Adsorption
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spelling Surface activity of early transition-metal oxycarbides: CO2 adsorption case studyKunkel, ChristianViñes Solana, FrancescIllas i Riera, FrancescCarbursMetalls de transicióAdsorcióCarbidesTransition metalsAdsorptionTheoretical studies and experiments have suggested that transition metal carbides (TMCs) can be useful materials for carbon capture and storage or use technologies from air sources. However, TMCs are known to become easily oxidized in the presence of molecular oxygen, and their properties jeopardized while being transformed into transition metal oxycarbides (TMOCs), which can affect the TMCs chemical activity, e.g. towards CO2. Here, by means of density functional theory (DFT) based calculations including dispersion we address the possible effect of oxycarbide formation in the CO2 capture course. A careful analysis of different models show that for group 4 TMCs (TM = Ti, Zr, Hf), their oxidation into TMOCs involves a negligible structural distortion of the outermost oxide surface layer, whereas severe rumplings are predicted for group 5 and 6 TMOCs (TM = V, Nb, Ta, Mo). The large surface distortion in the latter TMOCs results in a weak interaction with CO2 with adsorption energies below -0.27 eV. On the contrary, on group 4 TMOCs surfaces CO2 adsorption becomes stronger, with the adsorption values strengthening by 0.44-1.2 eV, a fact that, according to adsorption/desorption rates estimates, increments the air CO2 capture temperature window by 175-400 K. The present DFT results point to group 4 TMCs, TiC in particular, as promising materials for air CO2 capture and storage/conversion, even in the presence of oxygen and the possible formation of transition metal oxycarbides.American Chemical Society2020202020192020info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersion8 p.application/pdfhttps://hdl.handle.net/2445/165637Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésVersió postprint del document publicat a: https://doi.org/10.1021/acs.jpcc.8b11942Journal of Physical Chemistry C, 2019, vol. 123, num. 6, p. 3664-3671https://doi.org/10.1021/acs.jpcc.8b11942(c) American Chemical Society , 2019info:eu-repo/semantics/openAccessoai:recercat.cat:2445/1656372026-05-29T05:05:01Z
dc.title.none.fl_str_mv Surface activity of early transition-metal oxycarbides: CO2 adsorption case study
title Surface activity of early transition-metal oxycarbides: CO2 adsorption case study
spellingShingle Surface activity of early transition-metal oxycarbides: CO2 adsorption case study
Kunkel, Christian
Carburs
Metalls de transició
Adsorció
Carbides
Transition metals
Adsorption
title_short Surface activity of early transition-metal oxycarbides: CO2 adsorption case study
title_full Surface activity of early transition-metal oxycarbides: CO2 adsorption case study
title_fullStr Surface activity of early transition-metal oxycarbides: CO2 adsorption case study
title_full_unstemmed Surface activity of early transition-metal oxycarbides: CO2 adsorption case study
title_sort Surface activity of early transition-metal oxycarbides: CO2 adsorption case study
dc.creator.none.fl_str_mv Kunkel, Christian
Viñes Solana, Francesc
Illas i Riera, Francesc
author Kunkel, Christian
author_facet Kunkel, Christian
Viñes Solana, Francesc
Illas i Riera, Francesc
author_role author
author2 Viñes Solana, Francesc
Illas i Riera, Francesc
author2_role author
author
dc.subject.none.fl_str_mv Carburs
Metalls de transició
Adsorció
Carbides
Transition metals
Adsorption
topic Carburs
Metalls de transició
Adsorció
Carbides
Transition metals
Adsorption
description Theoretical studies and experiments have suggested that transition metal carbides (TMCs) can be useful materials for carbon capture and storage or use technologies from air sources. However, TMCs are known to become easily oxidized in the presence of molecular oxygen, and their properties jeopardized while being transformed into transition metal oxycarbides (TMOCs), which can affect the TMCs chemical activity, e.g. towards CO2. Here, by means of density functional theory (DFT) based calculations including dispersion we address the possible effect of oxycarbide formation in the CO2 capture course. A careful analysis of different models show that for group 4 TMCs (TM = Ti, Zr, Hf), their oxidation into TMOCs involves a negligible structural distortion of the outermost oxide surface layer, whereas severe rumplings are predicted for group 5 and 6 TMOCs (TM = V, Nb, Ta, Mo). The large surface distortion in the latter TMOCs results in a weak interaction with CO2 with adsorption energies below -0.27 eV. On the contrary, on group 4 TMOCs surfaces CO2 adsorption becomes stronger, with the adsorption values strengthening by 0.44-1.2 eV, a fact that, according to adsorption/desorption rates estimates, increments the air CO2 capture temperature window by 175-400 K. The present DFT results point to group 4 TMCs, TiC in particular, as promising materials for air CO2 capture and storage/conversion, even in the presence of oxygen and the possible formation of transition metal oxycarbides.
publishDate 2019
dc.date.none.fl_str_mv 2019
2020
2020
2020
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/165637
url https://hdl.handle.net/2445/165637
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Versió postprint del document publicat a: https://doi.org/10.1021/acs.jpcc.8b11942
Journal of Physical Chemistry C, 2019, vol. 123, num. 6, p. 3664-3671
https://doi.org/10.1021/acs.jpcc.8b11942
dc.rights.none.fl_str_mv (c) American Chemical Society , 2019
info:eu-repo/semantics/openAccess
rights_invalid_str_mv (c) American Chemical Society , 2019
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 8 p.
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,811543

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