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    Unearthing a Well-Defined Highly Active Bimetallic W/Ti Precatalyst Anchored on a Single Silica Surface for Metathesis of Propane

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    Type
    Article
    Authors
    Samantaray, Manoja
    Kavitake, Santosh Giridhar
    Morlanes, Natalia Sanchez cc
    Abou-Hamad, Edy cc
    Hamieh, Ali Imad Ali cc
    Dey, Raju cc
    Basset, Jean-Marie cc
    KAUST Department
    Ali I. Al-Naimi Petroleum Engineering Research Center (ANPERC)
    Chemical Science Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Date
    2017-02-23
    Online Publication Date
    2017-02-23
    Print Publication Date
    2017-03-08
    Permanent link to this record
    http://hdl.handle.net/10754/623929
    
    Metadata
    Show full item record
    Abstract
    Two compatible organometallic complexes, W(Me)(6) (1) and TiNp4 (2), were successively anchored on a highly dehydroxylated single silica support (SiO2-700) to synthesize the well-defined bimetallic precatalyst [(equivalent to Si-O-)W(Me)(5)(equivalent to Si-O-)Ti(Np)(3)] (4). Precatalyst 4 was characterized at the molecular level using advanced surface organometallic chemistry (SOMC) characterization techniques. The strong autocorrelation observed between methyl of W and Ti in H-1-H-1 multiple-quantum NMR spectra demonstrates that W and Ti species are in close proximity to each other. The bimetallic precatalyst 4, with a turnover number (TON) of 9784, proved to be significantly more efficient than the silica-supported monometallic catalyst [(equivalent to Si-O-)W(Me)(5)] (3), with a TON of 98, for propane metathesis at 150 degrees C in a flow reactor. The dramatic improvement in the activity signifies the cooperativity between Ti and W and indicates that the key step of alkane metathesis (C-H bond activation followed by beta-H elimination) occurs on Ti, followed by olefin metathesis, which occurs on W. We have demonstrated the influence and importance of proximity of Ti to W for achieving such a significantly high activity. This is the first report demonstrating the considerably high activity (TON = 9784) in propane metathesis at moderate temperature (150 degrees C) using a well-defined bimetallic system prepared via the SOMC approach.
    Citation
    Samantaray MK, Kavitake S, Morlanés N, Abou-Hamad E, Hamieh A, et al. (2017) Unearthing a Well-Defined Highly Active Bimetallic W/Ti Precatalyst Anchored on a Single Silica Surface for Metathesis of Propane. Journal of the American Chemical Society 139: 3522–3527. Available: http://dx.doi.org/10.1021/jacs.6b12970.
    Sponsors
    The authors acknowledge the KAUST Nuclear Magnetic Resonance Core Lab and Analytical Core Lab (ACL) for the analysis of the sample. This publication is based upon work supported by the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR).
    Publisher
    American Chemical Society (ACS)
    Journal
    Journal of the American Chemical Society
    DOI
    10.1021/jacs.6b12970
    Additional Links
    http://pubs.acs.org/doi/abs/10.1021/jacs.6b12970
    ae974a485f413a2113503eed53cd6c53
    10.1021/jacs.6b12970
    Scopus Count
    Collections
    Articles; Ali I. Al-Naimi Petroleum Engineering Research Center (ANPERC); Physical Science and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

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