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Synthesis, Structure, Gas-Phase Reactivity, and Catalytic Relevance of Trinuclear Mo3S4 Clusters Bearing Terminal Hydroxo and Hydrosulfido Groups

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Synthesis, Structure, Gas-Phase Reactivity, and Catalytic Relevance of Trinuclear Mo3S4 Clusters Bearing Terminal Hydroxo and Hydrosulfido Groups

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dc.contributor.author Beltran, Tomas F. es_ES
dc.contributor.author Feliz Rodriguez, Marta es_ES
dc.contributor.author Llusar, Rosa es_ES
dc.contributor.author Safont, Vicent S. es_ES
dc.contributor.author Vicent, Cristian es_ES
dc.date.accessioned 2016-05-12T07:38:23Z
dc.date.available 2016-05-12T07:38:23Z
dc.date.issued 2013-11-12
dc.identifier.issn 1434-1948
dc.identifier.uri http://hdl.handle.net/10251/63948
dc.description.abstract Molybdenum(IV) hydroxo [Mo3S4(dmpe)3(OH)3]+ (1+) and hydrosulfido [Mo3S4(dmpe)3(SH)3]+ (2+) [dmpe = 1,2-bis(dimethylphosphanyl)ethane] trimetallic cuboidal cluster complexes have been isolated in high yields by treating their chloride precursors with sodium hydroxide or sodium hydrosulfide, respectively. The crystal structures of [1]BPh4 and [2]PF6 confirm that QH (Q = O, S) groups are coordinated to metal centers. Both hydroxo and hydrosulfido Mo3S4 cluster complexes are fully characterized by spectroscopic, mass spectrometric, and X-ray techniques. A comparative study of the gas-phase dissociation of 1+ and 2+ cations using ESI tandem mass spectrometry is presented, and the results are compared with those already reported for the hydroxo tungsten analogue. The gas-phase reactivity of 1+ and 2+ species towards ethanol and 1-penthanethiol have been explored. The gas-phase-generated [Mo3S4(dmpe)2(O)(OH)]+ cation activates ethanol molecules through a similar mechanism to that proposed for its tungsten congener. The main differences in aldehyde elimination under collision-induced dissociation (CID) conditions between molybdenum and tungsten cluster sulfides are discussed. es_ES
dc.description.sponsorship The financial support of the Spanish Ministerio de Economia y Competitividad (MEC) (grant number CTQ2011-23157, research project MAT2011-28009), Fundacio Bancaixa-UJI (research project P1.1B2010-46), Universitat Politecnica de Valencia (PAID-06-12/SP20120740), and the Generalitat Valenciana (Prometeo/2009/053 and ACOMP/2013/2013/215) is gratefully acknowledged. The authors also thank the Serveis Central d'Instrumentacio Cientifica (SCIC) of the Universitat Jaume I for providing mass spectrometry, NMR spectroscopy, infrared, and X-ray facilities. T. B. thanks the Spanish Ministerio de Ciencia e Innovacion (MICINN) for a doctoral fellowship (FPI). en_EN
dc.language Inglés es_ES
dc.publisher Wiley-VCH Verlag es_ES
dc.relation.ispartof European Journal of Inorganic Chemistry es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject Molybdenum es_ES
dc.subject Cluster compounds es_ES
dc.subject Mass spectrometry es_ES
dc.subject Gas-phase reactions es_ES
dc.subject Density functional calculations es_ES
dc.title Synthesis, Structure, Gas-Phase Reactivity, and Catalytic Relevance of Trinuclear Mo3S4 Clusters Bearing Terminal Hydroxo and Hydrosulfido Groups es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1002/ejic.201300890
dc.relation.projectID info:eu-repo/grantAgreement/MICINN//CTQ2011-23157/ES/FUNCIONALIZACION DE CALCOGENUROS CLUSTER DE METALES DE LOS GRUPOS 6 Y 7 DIRIGIDA AL DESARROLLO DE MATERIALES MOLECULARES Y SOPORTADOS CON APLICACIONES EN CATALISIS ORGANICA/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MICINN//MAT2011-28009/ES/CATALIZADORES MONO- Y MULTIFUNCIONALES BASADOS EN NANOPARTICULAS METALICAS DIRIGIDOS A TRANSFORMACIONES SECUENCIALES O REACCIONES EN CASCADA/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/UJI//P1·1B2010-46/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/UPV//PAID-06-12-SP20120740/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/GVA//PROMETEO09%2F2009%2F053/ES/Química teórica y computacional de sistemas biológicos, sólidos y de materiales moleculares (Quitecobismm)/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/GVA//ACOMP%2F2013%2F215/ es_ES
dc.rights.accessRights Cerrado es_ES
dc.contributor.affiliation Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química es_ES
dc.description.bibliographicCitation Beltran, TF.; Feliz Rodriguez, M.; Llusar, R.; Safont, VS.; Vicent, C. (2013). Synthesis, Structure, Gas-Phase Reactivity, and Catalytic Relevance of Trinuclear Mo3S4 Clusters Bearing Terminal Hydroxo and Hydrosulfido Groups. European Journal of Inorganic Chemistry. 33:5797-5805. https://doi.org/10.1002/ejic.201300890 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion http://dx.doi.org/10.1002/ejic.201300890 es_ES
dc.description.upvformatpinicio 5797 es_ES
dc.description.upvformatpfin 5805 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 33 es_ES
dc.relation.senia 260175 es_ES
dc.contributor.funder Ministerio de Ciencia e Innovación es_ES
dc.contributor.funder Universitat Jaume I; Fundació Caixa Castelló - Bancaixa es_ES
dc.contributor.funder Universitat Politècnica de València es_ES
dc.contributor.funder Generalitat Valenciana es_ES
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