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Iridium-Catalyzed Hydrogen Production from Hydrosilanes and Water

Authors

  • Dr. Karin Garcés,

    1. Departamento de Química Inorgánica, Instituto de Síntesis Química y Catálisis Homogénea (ISQCH), Universidad de Zaragoza—CSIC, Facultad de Ciencias 50009, Zaragoza (Spain)
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  • Dr. Francisco J. Fernández-Alvarez,

    Corresponding author
    1. Departamento de Química Inorgánica, Instituto de Síntesis Química y Catálisis Homogénea (ISQCH), Universidad de Zaragoza—CSIC, Facultad de Ciencias 50009, Zaragoza (Spain)
    • Departamento de Química Inorgánica, Instituto de Síntesis Química y Catálisis Homogénea (ISQCH), Universidad de Zaragoza—CSIC, Facultad de Ciencias 50009, Zaragoza (Spain)===

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  • Dr. Víctor Polo,

    1. Departamento de Química Física—Instituto de Biocomputación y Física de Sistemas complejos (BIFI), Universidad de Zaragoza, Facultad de Ciencias 50009, Zaragoza (Spain)
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  • Dr. Ralte Lalrempuia,

    1. Departamento de Química Inorgánica, Instituto de Síntesis Química y Catálisis Homogénea (ISQCH), Universidad de Zaragoza—CSIC, Facultad de Ciencias 50009, Zaragoza (Spain)
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  • Prof. Jesús J. Pérez-Torrente,

    1. Departamento de Química Inorgánica, Instituto de Síntesis Química y Catálisis Homogénea (ISQCH), Universidad de Zaragoza—CSIC, Facultad de Ciencias 50009, Zaragoza (Spain)
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  • Prof. Luis A. Oro

    Corresponding author
    1. Departamento de Química Inorgánica, Instituto de Síntesis Química y Catálisis Homogénea (ISQCH), Universidad de Zaragoza—CSIC, Facultad de Ciencias 50009, Zaragoza (Spain)
    • Departamento de Química Inorgánica, Instituto de Síntesis Química y Catálisis Homogénea (ISQCH), Universidad de Zaragoza—CSIC, Facultad de Ciencias 50009, Zaragoza (Spain)===

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Abstract

The iridium(III) complex [Ir(H)(CF3SO3)(NSiN)(coe)] (NSiN=fac-coordinated bis(pyridine-2-yloxy)methylsilyl, coe=cyclooctene) has been proven to be an effective catalyst precursor for hydrogen production from the hydrolysis of hydrosilanes at room temperature. The reaction performance depends both on the nature of the silane and the solvent. Interestingly, high turnover frequencies of around 105 h−1 were obtained by using Et2SiH2 or (Me2HSi)2O as hydrogen sources and THF as the solvent. Moreover a mechanistic insight into this Ir-catalyzed hydrogen generation process, based on both theoretical calculations and NMR spectroscopy, is reported. The overall catalytic cycle can be viewed as a two-stage process that involves water-promoted Si[BOND]H bond activation followed by water splitting by a proton transfer.

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