Facile heterogeneously catalyzed nitrogen rixation by MXenes

The rate-limiting step for ammonia (NH3) production via the Haber-Bosch process is the dissociation of molecular nitrogen (N2), which requires quite harsh working conditions, even when using appropriate heterogeneous catalysts. Here, motivated by the demonstrated enhanced chemical activity of MXenes...

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Autores: Gouveia, José D., Morales García, Ángel, Viñes Solana, Francesc, Gomes, José R. B., Illas i Riera, Francesc
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2020
País:España
Institución:Universidad de Barcelona
Repositorio:Dipòsit Digital de la UB
OAI Identifier:oai:diposit.ub.edu:2445/165778
Acceso en línea:https://hdl.handle.net/2445/165778
Access Level:acceso abierto
Palabra clave:Carburs
Adsorció
Amoníac
Teoria del funcional de densitat
Catàlisi heterogènia
Carbides
Adsorption
Ammonia
Density functionals
Heterogeneus catalysis
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repository_id_str
spelling Facile heterogeneously catalyzed nitrogen rixation by MXenesGouveia, José D.Morales García, ÁngelViñes Solana, FrancescGomes, José R. B.Illas i Riera, FrancescCarbursAdsorcióAmoníacTeoria del funcional de densitatCatàlisi heterogèniaCarbidesAdsorptionAmmoniaDensity functionalsHeterogeneus catalysisThe rate-limiting step for ammonia (NH3) production via the Haber-Bosch process is the dissociation of molecular nitrogen (N2), which requires quite harsh working conditions, even when using appropriate heterogeneous catalysts. Here, motivated by the demonstrated enhanced chemical activity of MXenes¿ a class of two-dimensional inorganic materials¿ toward the adsorption of quite stable molecules such as CO2 and H2O, we use density functional theory including dispersion, to investigate the suitability of such MXene materials to catalyze N2 dissociation. Results show that MXenes exothermically adsorb N2, with rather large adsorption energies ranging from −1.11 to −3.45 eV and elongation of the N2 bond length by ∼20%, greatly facilitating their dissociation with energy barriers below 1 eV, reaching 0.28 eV in the most favorable studied case of W2N. Microkinetic simulations indicate that the first hydrogenation of adsorbed atomic nitrogen is feasible at low pressures and moderate temperatures, and that the production of NH3 may occur above 800 K on most studied MXenes, in particular, in W2N. These results reinforce the promising capabilities of MXenes to dissociate nitrogen and suggest combining them co-catalytically with Ru nanoparticles to further improve the efficiency of ammonia synthesis.American Chemical Society2020info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionapplication/pdfhttps://hdl.handle.net/2445/165778Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Dipòsit Digital de la UBinstname:Universidad de BarcelonaInglésVersió postprint del document publicat a: https://doi.org/10.1021/acscatal.0c00935ACS Catalysis, 2020, vol. 10, num. 9, p. 5049-5056https://doi.org/10.1021/acscatal.0c00935info:eu-repo/grantAgreement/EC/H2020/730897(c) American Chemical Society , 2020info:eu-repo/semantics/openAccessoai:diposit.ub.edu:2445/1657782026-05-27T06:46:51Z
dc.title.none.fl_str_mv Facile heterogeneously catalyzed nitrogen rixation by MXenes
title Facile heterogeneously catalyzed nitrogen rixation by MXenes
spellingShingle Facile heterogeneously catalyzed nitrogen rixation by MXenes
Gouveia, José D.
Carburs
Adsorció
Amoníac
Teoria del funcional de densitat
Catàlisi heterogènia
Carbides
Adsorption
Ammonia
Density functionals
Heterogeneus catalysis
title_short Facile heterogeneously catalyzed nitrogen rixation by MXenes
title_full Facile heterogeneously catalyzed nitrogen rixation by MXenes
title_fullStr Facile heterogeneously catalyzed nitrogen rixation by MXenes
title_full_unstemmed Facile heterogeneously catalyzed nitrogen rixation by MXenes
title_sort Facile heterogeneously catalyzed nitrogen rixation by MXenes
dc.creator.none.fl_str_mv Gouveia, José D.
Morales García, Ángel
Viñes Solana, Francesc
Gomes, José R. B.
Illas i Riera, Francesc
author Gouveia, José D.
author_facet Gouveia, José D.
Morales García, Ángel
Viñes Solana, Francesc
Gomes, José R. B.
Illas i Riera, Francesc
author_role author
author2 Morales García, Ángel
Viñes Solana, Francesc
Gomes, José R. B.
Illas i Riera, Francesc
author2_role author
author
author
author
dc.subject.none.fl_str_mv Carburs
Adsorció
Amoníac
Teoria del funcional de densitat
Catàlisi heterogènia
Carbides
Adsorption
Ammonia
Density functionals
Heterogeneus catalysis
topic Carburs
Adsorció
Amoníac
Teoria del funcional de densitat
Catàlisi heterogènia
Carbides
Adsorption
Ammonia
Density functionals
Heterogeneus catalysis
description The rate-limiting step for ammonia (NH3) production via the Haber-Bosch process is the dissociation of molecular nitrogen (N2), which requires quite harsh working conditions, even when using appropriate heterogeneous catalysts. Here, motivated by the demonstrated enhanced chemical activity of MXenes¿ a class of two-dimensional inorganic materials¿ toward the adsorption of quite stable molecules such as CO2 and H2O, we use density functional theory including dispersion, to investigate the suitability of such MXene materials to catalyze N2 dissociation. Results show that MXenes exothermically adsorb N2, with rather large adsorption energies ranging from −1.11 to −3.45 eV and elongation of the N2 bond length by ∼20%, greatly facilitating their dissociation with energy barriers below 1 eV, reaching 0.28 eV in the most favorable studied case of W2N. Microkinetic simulations indicate that the first hydrogenation of adsorbed atomic nitrogen is feasible at low pressures and moderate temperatures, and that the production of NH3 may occur above 800 K on most studied MXenes, in particular, in W2N. These results reinforce the promising capabilities of MXenes to dissociate nitrogen and suggest combining them co-catalytically with Ru nanoparticles to further improve the efficiency of ammonia synthesis.
publishDate 2020
dc.date.none.fl_str_mv 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/2445/165778
url https://hdl.handle.net/2445/165778
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/acscatal.0c00935
ACS Catalysis, 2020, vol. 10, num. 9, p. 5049-5056
https://doi.org/10.1021/acscatal.0c00935
info:eu-repo/grantAgreement/EC/H2020/730897
dc.rights.none.fl_str_mv (c) American Chemical Society , 2020
info:eu-repo/semantics/openAccess
rights_invalid_str_mv (c) American Chemical Society , 2020
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 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:Dipòsit Digital de la UB
instname:Universidad de Barcelona
instname_str Universidad de Barcelona
reponame_str Dipòsit Digital de la UB
collection Dipòsit Digital de la UB
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,300719

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