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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.

著者 O'Mara PB , Wilde P , Benedetti T , Andronescu C , Cheong S , Gooding JJ , Tilley RD , Schuhmann W
J Am Chem Soc.2019 Aug 25 ; ():.
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Enzymes can perform complex multi-step cascade reactions by linking multiple distinct catalytic sites via substrate chan-neling. We mimic this feature in a generalized approach with an electrocatalytic nanoparticle for the carbon dioxide reduc-tion reaction comprising a Ag-core surrounded by a porous Cu shell providing different active sites in nano-confined volumes. The architecture of the nanozyme provides the basis for a cascade reaction, which promotes C-C coupling reac-tions. 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.
PMID: 31448598 [PubMed - as supplied by publisher]
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