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| Naji, M. |
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| Motta, Antonella |
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| Aletan, Dirar |
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| Mohamed, Tarek |
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| Ertürk, Emre |
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| Taccardi, Nicola |
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| Kononenko, Denys |
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| Petrov, R. H. | Madrid |
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| Alshaaer, Mazen | Brussels |
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| Bih, L. |
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| Casati, R. |
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| Muller, Hermance |
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| Kočí, Jan | Prague |
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| Šuljagić, Marija |
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| Kalteremidou, Kalliopi-Artemi | Brussels |
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| Azam, Siraj |
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| Ospanova, Alyiya |
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| Blanpain, Bart |
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| Ali, M. A. |
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| Popa, V. |
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| Rančić, M. |
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| Ollier, Nadège |
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| Azevedo, Nuno Monteiro |
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| Landes, Michael |
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| Rignanese, Gian-Marco |
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Pérez-Gallent, Elena
in Cooperation with on an Cooperation-Score of 37%
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Publications (3/3 displayed)
- 2019Mechanistic study of the electrosynthesis of propylene carbonate from propylene oxide and CO2 on copper electrodescitations
- 2017Spectroscopic observation of a hydrogenated CO dimer intermediate during CO reduction on Cu(100) electrodescitations
- 2017Structure- and potential-dependent cation effects on CO reduction at copper single-crystal electrodescitations
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article
Structure- and potential-dependent cation effects on CO reduction at copper single-crystal electrodes
Abstract
<p>The complexity of the electrocatalytic reduction of CO to CH<sub>4</sub> and C<sub>2</sub>H<sub>4</sub> on copper electrodes prevents a straightforward elucidation of the reaction mechanism and the design of new and better catalysts. Although structural and electrolyte effects have been separately studied, there are no reports on structure-sensitive cation effects on the catalyst's selectivity over a wide potential range. Therefore, we investigated CO reduction on Cu(100), Cu(111), and Cu(polycrystalline) electrodes in 0.1 M alkaline hydroxide electrolytes (LiOH, NaOH, KOH, RbOH, CsOH) between 0 and -1.5 V vs RHE. We used online electrochemical mass spectrometry and high-performance liquid chromatography to determine the product distribution as a function of electrode structure, cation size, and applied potential. First, cation effects are potential dependent, as larger cations increase the selectivity of all electrodes toward ethylene at E > -0.45 V vs RHE, but methane is favored at more negative potentials. Second, cation effects are structure-sensitive, as the onset potential for C<sub>2</sub>H<sub>4</sub> formation depends on the electrode structure and cation size, whereas that for CH<sub>4</sub> does not. Fourier Transform infrared spectroscopy (FTIR) and density functional theory help to understand how cations favor ethylene over methane at low overpotentials on Cu(100). The rate-determining step to methane and ethylene formation is CO hydrogenation, which is considerably easier in the presence of alkaline cations for a CO dimer compared to a CO monomer. For Li<sup>+</sup> and Na<sup>+</sup>, the stabilization is such that hydrogenated dimers are observable with FTIR at low overpotentials. Thus, potential-dependent, structure-sensitive cation effects help steer the selectivity toward specific products.</p>