Issue 4, 2013

Electrochemical reactivities of pyridinium in solution: consequences for CO2reduction mechanisms

Abstract

One of the most promising CO2 reduction processes presently known suffers from a lack of fundamental understanding of its reaction mechanism. Using first principles quantum chemistry, we report thermodynamical energies of various pyridine-derived intermediates as well as barrier heights for key homogeneous reaction mechanisms. From this work, we predict that the actual form of the co-catalyst involved in pyridinium-based CO2 reduction is not the long-proposed pyridinyl radical in solution, but is more probably a surface-bound dihydropyridine species.

Graphical abstract: Electrochemical reactivities of pyridinium in solution: consequences for CO2 reduction mechanisms

Supplementary files

Article information

Article type
Edge Article
Submitted
21 Dec 2012
Accepted
11 Feb 2013
First published
14 Feb 2013

Chem. Sci., 2013,4, 1490-1496

Electrochemical reactivities of pyridinium in solution: consequences for CO2 reduction mechanisms

J. A. Keith and E. A. Carter, Chem. Sci., 2013, 4, 1490 DOI: 10.1039/C3SC22296A

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