Electrochemical Reduction of CO2 at Functionalized Au Electrodes
| Autor: | Yuxin Fang, John C. Flake |
|---|---|
| Rok vydání: | 2017 |
| Předmět: |
Chemistry
Inorganic chemistry 02 engineering and technology General Chemistry Electrolyte 010402 general chemistry 021001 nanoscience & nanotechnology Electrochemistry 01 natural sciences Biochemistry Redox Catalysis 0104 chemical sciences chemistry.chemical_compound Colloid and Surface Chemistry Desorption Electrode Formate 0210 nano-technology Selectivity Faraday efficiency |
| Zdroj: | Journal of the American Chemical Society. 139:3399-3405 |
| ISSN: | 1520-5126 0002-7863 |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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