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Reactivity of Hydrosilanes with the CrII/SiO2 Phillips Catalyst: Observation of Intermediates and Properties of the Modified CrII Sites

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Abstract

The reaction of hydrosilanes (both silane and triethylsilane) with CrII/SiO2 catalyst has been investigated in detail by analysis of the gaseous by-products, temperature- and pressure- resolved FT-IR spectroscopy and deuterium exchanges. We found that the reaction proceeds via two steps, passing through intermediates characterized by elongated Si–H bonds and transient Cr-hydride species leading to the release of H2 in the gas phase. These experimental evidence allowed us to advance an hypothesis of the reaction mechanism, which validates our previous proposal for the structure of the modified chromium sites. Furthermore, based on the intermediates of the reaction mechanism, we have also tested the ability of the modified “homogeneous-like” CrII sites toward H2 (D2) activation, demonstrating that, contrarily to the unmodified CrII species, such reactivity is present.

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Acknowledgments

The authors are grateful to the organizing committee of ISHHC Conference held in Utrecht in July 2015. The laboratory COMS and LCPP in Lyon are kindly acknowledged for the support in the collection of gas-chromatographic data. This work has been supported by the Progetto di Ateneo/CSP 2014 (Torino_call2014_L1_73) and by the Grant VINCI from Université Franco-Italienne.

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Authors and Affiliations

  1. Department of Chemistry, NIS Centre and INSTM, University of Torino, Via G. Quarello 15A, Torino, I10135, Italy

    Caterina Barzan, Silvia Bordiga & Elena Groppo

  2. CNRS—CPE Lyon—Universite´ Lyon 1 (C2P2 UMR 5265), Universite´ de Lyon, Bât 308F, 43 B. du 11 Novembre 1918, Villeurbanne, 69616, France

    Elsje Alessandra Quadrelli

Authors
  1. Caterina Barzan
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  2. Silvia Bordiga
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  3. Elsje Alessandra Quadrelli
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  4. Elena Groppo
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Correspondence to Elsje Alessandra Quadrelli or Elena Groppo.

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Barzan, C., Bordiga, S., Quadrelli, E.A. et al. Reactivity of Hydrosilanes with the CrII/SiO2 Phillips Catalyst: Observation of Intermediates and Properties of the Modified CrII Sites. Top Catal 59, 1732–1739 (2016). https://doi.org/10.1007/s11244-016-0694-8

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  • DOI: https://doi.org/10.1007/s11244-016-0694-8

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