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    Novel rhodium on carbon catalysts for the oxidation of benzyl alcohol to benzaldehyde: A study of the modification of metal/support interactions by acid pre-treatments

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    wilde_et_al_2019.pdf (2.405Mb)
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    Publication date
    2019-01-25
    Author
    Wilde, C.A.
    Ryabenkova, Yulia
    Firth, I.M.
    Pratt, L.
    Railton, J.
    Bravo-Sanchez, M.
    Sano, N.
    Cumpson, P.J.
    Coates, Philip D.
    Liu, X.
    Conte, M.
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    Keyword
    Rhodium
    Nanoparticles
    Organometallic complexes
    Carbon catalysts
    Benzaldehyde
    Acid pre-treatments
    Rights
    (c) 2019 The Authors. This is an Open Access article distributed under the Creative Commons CC-BY license (http://creativecommons.org/licenses/by/4.0/)
    Peer-Reviewed
    Yes
    
    Metadata
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    Abstract
    Rhodium nanoparticles or rhodium organometallic complexes are mainly used in catalysis for reduction or hydroformylation reactions. In this work instead, we explored the capabilities of Rh nanoparticles as an oxidation catalyst, applied to the oxidation of benzyl alcohol to benzaldehyde under very mild conditions (100 °C, and atmospheric pressure) as a model reaction. Here we report the preparation of novel Rh/C catalysts by using an impregnation protocol, with particular emphasis on the pre-treatment of the carbon supports by using HNO3 and HCl, as well as the characterization of these materials by using an array of methods involving TEM, XPS and XRPD. Our preparation method led to a wide Rh particle size distribution ranging from 20 to 100 nm, and we estimate an upper limit diameter of Rh nanoparticles for their activity towards benzyl alcohol oxidation to be ca. 30 nm. Furthermore, a HNO3 pre-treatment of the activated carbon support was able to induce a smaller and narrower particle size distribution of Rh nanoparticles, whereas a HCl pre-treatment had no effect or sintered the Rh nanoparticles. We rationalise these results by HNO3 as an acid able to create new nucleation sites for Rh on the carbon surface, with the final effect of smaller nanoparticles, whereas for HCl the effect of sintering was most likely due to site blocking of the nucleation sites over the carbon surface. The roles of acid centres on the carbon surfaces for the oxidation reaction was also investigated, and the larger their amounts the larger the amounts of by-products. However, by treatment with HNO3 we were able to convert neutral or basic carbons into supports capable to enhance the catalytic activity of Rh, and yet minimised detrimental effects on the selectivity of the oxidation to benzaldehyde.
    URI
    http://hdl.handle.net/10454/17007
    Version
    Published version
    Citation
    Wilde CA, Ryabenkova Y, Firth IM et al (2019) Novel rhodium on carbon catalysts for the oxidation of benzyl alcohol to benzaldehyde: A study of the modification of metal/support interactions by acid pre-treatments. 570: 271-282.
    Link to publisher’s version
    https://doi.org/10.1016/j.apcata.2018.11.006
    Type
    Article
    Collections
    Engineering and Informatics Publications

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