Cascade Reactions in Nanozymes: Spatially Separated Active Sites inside Ag-Core-Porous-Cu-Shell Nanoparticles for Multistep Carbon Dioxide Reduction to Higher Organic Molecules
File version
Accepted Manuscript (AM)
Author(s)
Wilde, Patrick
Benedetti, Tania M
Andronescu, Corina
Cheong, Soshan
Gooding, J Justin
Tilley, Richard D
Schuhmann, Wolfgang
Griffith University Author(s)
Primary Supervisor
Other Supervisors
Editor(s)
Date
Size
File type(s)
Location
License
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.
Journal Title
Journal of the American Chemical Society
Conference Title
Book Title
Edition
Volume
141
Issue
36
Thesis Type
Degree Program
School
Publisher link
Patent number
Funder(s)
Grant identifier(s)
Rights Statement
Rights Statement
This document is the Accepted Manuscript version of a Published Work that appeared in final form in the Journal of the American Chemical Society, copyright 2019 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/jacs.9b07310
Item Access Status
Note
Access the data
Related item(s)
Subject
Chemical sciences
Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Chemistry
ELECTROCHEMICAL REDUCTION
Persistent link to this record
Citation
O'Mara, PB; Wilde, P; Benedetti, TM; Andronescu, C; Cheong, S; Gooding, JJ; Tilley, RD; Schuhmann, W, 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, 2019, 141 (36), pp. 14093-14097