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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Date
2019Author
O’Mara, Peter B.
Wilde, Patrick
Benedetti, Tania M.
Andrones, Corina
Cheong, Soshan
Gooding, Justin
Tilley, Richard D.
Schuhmann, Wolfgang
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Show full item recordAbstract
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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