Articles producció científica> Química Física i Inorgànica

Investigating the Transformations of Polyoxoanions Using Mass Spectrometry and Molecular Dynamics

  • Dades identificatives

    Identificador: PC:1905
    Handle: https://hdl.handle.net/20.500.11797/PC1905
    Autors:
    Antonio Rodríguez-ForteaJamie M. CameronLaia Vilà-NadalRoss S. WinterFumichika IijimaJuan Carlos MurilloHiroki OshioJosep M. PobletLeroy Cronin
    Resum:
    The reactions of [¿-SiW10O36]8- represent one of the most important synthetic gateways into a vast array of polyoxotungstate chemistry. Herein, we set about exploring the transformation of the lacunary polyoxoanion [¿2-SiW11O39]8- into [¿-SiW10O36]8- using high-resolution electrospray mass spectrometry, density functional theory, and molecular dynamics. We show that the reaction proceeds through an unexpected {SiW9} precursor capable of undertaking a direct ¿ ¿ ¿ isomerization via a rotational transformation. The remarkably low-energy transition state of this transformation could be identified through theoretical calculations. Moreover, we explore the significant role of the countercations for the first time in such studies. This combination of experimental and the theoretical studies can now be used to understand the complex chemical transformations of oxoanions, leading to the design of reactivity by structural control.

  • Altres:

    Autor segons l'article: Antonio Rodríguez-Fortea; Jamie M. Cameron; Laia Vilà-Nadal; Ross S. Winter; Fumichika Iijima; Juan Carlos Murillo; Hiroki Oshio; Josep M. Poblet; Leroy Cronin
    Departament: Química Física i Inorgànica
    Autor/s de la URV: RODRÍGUEZ FORTEA, ANTONIO; Jamie M. Cameron; Laia Vilà-Nadal; Ross S. Winter; Fumichika Iijima; Juan Carlos Murillo; Hiroki Oshio; POBLET RIUS, JOSEP MARIA; Leroy Cronin
    Paraules clau: mass spectrometry molecular dynamics
    Resum: The reactions of [¿-SiW10O36]8- represent one of the most important synthetic gateways into a vast array of polyoxotungstate chemistry. Herein, we set about exploring the transformation of the lacunary polyoxoanion [¿2-SiW11O39]8- into [¿-SiW10O36]8- using high-resolution electrospray mass spectrometry, density functional theory, and molecular dynamics. We show that the reaction proceeds through an unexpected {SiW9} precursor capable of undertaking a direct ¿ ¿ ¿ isomerization via a rotational transformation. The remarkably low-energy transition state of this transformation could be identified through theoretical calculations. Moreover, we explore the significant role of the countercations for the first time in such studies. This combination of experimental and the theoretical studies can now be used to understand the complex chemical transformations of oxoanions, leading to the design of reactivity by structural control.
    Grup de recerca: Química Quàntica
    Àrees temàtiques: Chemistry Química Química
    Accès a la llicència d'ús: https://creativecommons.org/licenses/by/3.0/es/
    ISSN: 0002-7863
    Identificador de l'autor: 0000-0001-5884-5629; 0000-0003-0138-933X; 0000-0002-7718-7227; n/a; n/a; n/a; n/a; 0000-0002-4533-0623; n/a
    Data d'alta del registre: 2016-09-13
    Pàgina final: 8773
    Volum de revista: 138
    Versió de l'article dipositat: info:eu-repo/semantics/publishedVersion
    Enllaç font original: http://pubs.acs.org/doi/abs/10.1021/jacs.6b02245
    URL Document de llicència: https://repositori.urv.cat/ca/proteccio-de-dades/
    DOI de l'article: https://doi.org/10.1021/jacs.6b02245
    Entitat: Universitat Rovira i Virgili
    Any de publicació de la revista: 2016
    Pàgina inicial: 8765
    Tipus de publicació: Article Artículo Article

  • Paraules clau:

    Espectrometria de masses
    Dinàmica molecular
    mass spectrometry
    molecular dynamics
    Chemistry
    Química
    Química
    0002-7863

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