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Size and stoichiometry effects on the reactivity of mocynanoparticles toward ethylene

dc.contributor.authorJimenez-Orozco C
dc.contributor.authorFigueras M
dc.contributor.authorFlórez E
dc.contributor.authorViñes F
dc.contributor.authorRodriguez J.A
dc.contributor.authorIllas F.
dc.date.accessioned2022-09-14T14:34:06Z
dc.date.available2022-09-14T14:34:06Z
dc.date.created2021
dc.identifier.issn19327447
dc.identifier.urihttp://hdl.handle.net/11407/7565
dc.descriptionMolybdenum carbides are promising alternative catalysts to Pt-group metals for the hydrogenation of unsaturated hydrocarbons. Nanostructuring has been shown to be an efficient way to boost the catalytic activity of these materials with MoCy nanoparticles (NPs) exhibiting a good performance when encapsulated inside zeolites or dispersed on inert supports such as carbon or gold. Hereby, we focus on a systematic DFT study of the interaction of MoCy NPs with ethylene (C2H4) as a general and simple approach for examining binding and activation of C═C bonds. Models for 14 NPs, with a Mo/C ratio in the 0.67-2.00 range, have been built following a cascade procedure. Several chemical descriptors, including the adsorption energy, structural NPs distortion, C═C deformation, and C2H4 attachment energy, have been analyzed along with a meticulous geometric and electronic characterization of bare NPs and C2H4 binding. The present results show that 1:1 stoichiometric Mo6C6, Mo12C12, and Mo24C24 and the nonstochiometric Mo4C6, Mo8C12 (MetCar), and Mo14C13 (nanocube) are excellent systems for the binding and activation of ethylene, exhibiting a much larger reactivity than a bulk δ-MoC(001) surface with a similar Mo/C ratio. In addition, C2H4 binding on the NPs with a Mo/C < 1.08 is advantageous because, apart from a rather large adsorption energy, it implies low energy values for NPs deformation (from 0.00 to 0.31 eV), C═C distortion (from 0.30 to 0.52 eV), and C2H4 attachment (from -2.12 to -2.58 eV). These theoretical results point to the ideal MoCy size and composition for C2H4 binding, providing a background for further experimental studies aimed at the preparation of MoCy NPs as hydrogenation catalysts. © 2021 American Chemical Society.eng
dc.language.isoeng
dc.publisherAmerican Chemical Society
dc.relation.isversionofhttps://www.scopus.com/inward/record.uri?eid=2-s2.0-85103436929&doi=10.1021%2facs.jpcc.0c10689&partnerID=40&md5=488d412533b73160a9c371782486e7bf
dc.sourceJournal of Physical Chemistry C
dc.titleSize and stoichiometry effects on the reactivity of mocynanoparticles toward ethylene
dc.typeArticle
dc.rights.accessrightsinfo:eu-repo/semantics/restrictedAccess
dc.publisher.programCiencias Básicas
dc.type.spaArtículo
dc.identifier.doi10.1021/acs.jpcc.0c10689
dc.subject.keywordAliphatic compoundseng
dc.subject.keywordBinding energyeng
dc.subject.keywordCarbideseng
dc.subject.keywordCatalyst activityeng
dc.subject.keywordChemical activationeng
dc.subject.keywordChemical analysiseng
dc.subject.keywordDeformationeng
dc.subject.keywordHydrogenationeng
dc.subject.keywordMolybdenum compoundseng
dc.subject.keywordZeoliteseng
dc.subject.keywordAdsorption energieseng
dc.subject.keywordAlternative catalystseng
dc.subject.keywordChemical descriptorseng
dc.subject.keywordElectronic characterizationeng
dc.subject.keywordHydrogenation catalysteng
dc.subject.keywordMolybdenum carbideeng
dc.subject.keywordNanoparticle (NPs)eng
dc.subject.keywordUnsaturated ydrocarbonseng
dc.subject.keywordEthyleneeng
dc.publisher.facultyFacultad de Ciencias Básicas
dc.affiliationJimenez-Orozco, C., Facultad de Ciencias Básicas, Grupo de Materiales con Impacto (Matandmpac), Universidad de Medellín, Carrera 87 No. 30-65, Medellín, Colombia
dc.affiliationFigueras, M., Departament de Ciència de Materials i Química Física, Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona, c/Martí i Franquès 1-11, Barcelona, 08028, Spain
dc.affiliationFlórez, E., Facultad de Ciencias Básicas, Grupo de Materiales con Impacto (Matandmpac), Universidad de Medellín, Carrera 87 No. 30-65, Medellín, Colombia
dc.affiliationViñes, F., Departament de Ciència de Materials i Química Física, Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona, c/Martí i Franquès 1-11, Barcelona, 08028, Spain
dc.affiliationRodriguez, J.A., Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973, United States
dc.affiliationIllas, F., Departament de Ciència de Materials i Química Física, Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona, c/Martí i Franquès 1-11, Barcelona, 08028, Spain
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dc.type.coarhttp://purl.org/coar/resource_type/c_6501
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dc.type.driverinfo:eu-repo/semantics/article
dc.identifier.reponamereponame:Repositorio Institucional Universidad de Medellín
dc.identifier.repourlrepourl:https://repository.udem.edu.co/
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