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
2019
Journal Title
Journal ISSN
Volume Title
Publisher
Journal of the American Chemical Society
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.
Description
Keywords
Cascade Reactions, Nanozymes, Ag-Core−Porous-Cu-Shell Nanoparticles, Carbon Dioxide, Organic Molecules
Citation
O’Mara, P. B., Wilde, P., Benedetti, T. M., Andronescu, C., Cheong, S., Gooding, J. J., ... & Schuhmann, W. (2019). Cascade reactions in nanozymes: Spatially separated active sites inside Ag-Core–Porous-Cu-shell nanoparticles for multistep carbon dioxide reduction to higher organic molecules. Journal of the American Chemical Society, 141(36), 14093-14097. DOI: 10.1021/jacs.9b07310