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Journal Article
Research Support, U.S. Gov't, Non-P.H.S.
Electrochemical Reduction of CO 2 at Functionalized Au Electrodes.
Journal of the American Chemical Society 2017 March 9
Electrochemical reduction of CO2 provides an opportunity to store renewable energy as fuels with much greater energy densities than batteries. Product selectivity of the reduction reaction is known to be a function of the electrolyte and electrode; however, electrodes modified with functional ligands may offer new methods to control selectivity. Here, we report the electrochemical reduction of CO2 at functionalized Au surfaces with three thiol-tethered ligands: 2-mercaptopropionic acid, 4-pyridinylethanemercaptan, and cysteamine. Remarkably, Au electrodes modified with 4-pyridinylethanemercaptan show a 2-fold increase in Faradaic efficiency and 3-fold increase in formate production relative to Au foil. Conversely, electrodes with 2-mercaptopropionic acid ligands show nearly 100% Faradaic efficiency toward the hydrogen evolution reaction, while cystemine-modified electrodes show 2-fold increases in both CO and H2 production. We propose a proton-induced desorption mechanism associated with pKa of the functionalized ligand as responsible for the dramatic selectivity changes.
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