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    Cascade Reactions in Nanozymes: Spatially Separated Active Sites inside Ag-Core−Porous-Cu-Shell Nanoparticles for Multistep Carbon Dioxide Reduction to Higher Organic Molecules

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    Article (2.615Mb)
    Date
    2019
    Author
    O’Mara, Peter B.
    Wilde, Patrick
    Benedetti, Tania M.
    Andrones, Corina
    Cheong, Soshan
    Gooding, Justin
    Tilley, Richard D.
    Schuhmann, Wolfgang
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    Abstract
    Enzymes can perform complex multistep cascade reactions by linking multiple distinct catalytic sites via substrate channeling. We mimic this feature in a generalized approach with an electrocatalytic nanoparticle for the carbon dioxide reduction reaction comprising a Ag core surrounded by a porous Cu shell, providing different active sites in nanoconfined volumes. The architecture of the nanozyme provides the basis for a cascade reaction, which promotes C−C coupling reactions. The first step occurs on the Ag core, and the subsequent steps on the porous copper shell, where a sufficiently high CO concentration due to the nanoconfinement facilitates C−C bond formation. The architecture yields the formation of n-propanol and propionaldehyde at potentials as low as −0.6 V vs RHE.
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    https://nru.uncst.go.ug/handle/123456789/6203
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