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    Photochemical Processes in a Rhenium(I) Tricarbonyl N-Heterocyclic Carbene Complex Studied by Time-Resolved Measurements

    250592.pdf (1.267Mb)
    Access Status
    Open access
    Authors
    Mukuta, T.
    Simpson, Peter
    Vaughan, Jamila
    Skelton, B.
    Stagni, S.
    Massi, Massimiliano
    Koike, K.
    Ishitani, O.
    Onda, K.
    Date
    2017
    Type
    Journal Article
    
    Metadata
    Show full item record
    Citation
    Mukuta, T. and Simpson, P. and Vaughan, J. and Skelton, B. and Stagni, S. and Massi, M. and Koike, K. et al. 2017. Photochemical Processes in a Rhenium(I) Tricarbonyl N-Heterocyclic Carbene Complex Studied by Time-Resolved Measurements. Inorganic Chemistry. 56 (6): pp. 3404-3413.
    Source Title
    Inorganic Chemistry
    DOI
    10.1021/acs.inorgchem.6b02936
    ISSN
    1520-510X
    School
    Nanochemistry Research Institute
    Funding and Sponsorship
    http://purl.org/au-research/grants/arc/FT130100033
    Remarks

    This document is the Accepted Manuscript version of a Published Work that appeared in final form in Inorganic Chemistry, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see 10.1021/acs.inorgchem.6b02936, see http://pubs.acs.org/page/policy/articlesonrequest/index.html.

    URI
    http://hdl.handle.net/20.500.11937/51356
    Collection
    • Curtin Research Publications
    Abstract

    We carried out time-resolved infrared (TR-IR) and emission lifetime measurements on a Re(I) carbonyl complex having an N-heterocyclic carbene ligand, namely, fac-[Re(CO)3(PyImPh)Br], under photochemically reactive (in solution in acetonitrile) and nonreactive (in solution in dichloromethane) conditions to investigate the mechanism of photochemical ligand substitution reactions. The TR-IR measurements revealed that no reaction occurs on a picosecond time scale and the cationic product, namely, fac-[Re(CO)3(PyImPh)(MeCN)](+), is produced on a nanosecond time scale only in solution in acetonitrile, which indicates that the reaction proceeds thermally from the excited state. Because no other products were observed by TR-IR, we concluded that this cationic product is an intermediate species for further reactions. The measurements of the temperature-dependent emission lifetime and analysis using transition-state theory revealed that the photochemical substitution reaction proceeds from a metal-to-ligand charge transfer excited state, the structure of which allows the potential coordination of a solvent molecule. Thus, the coordinating capacity of the solvent determines whether the reaction proceeds or not. This mechanism is different from those of photochemical reactions of other types of Re(I) carbonyl complexes owing to the unique characteristics of the carbene ligand.

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