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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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Wicks, Joshua
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Publications (3/3 displayed)
- 2022High-Rate and Selective CO2 Electrolysis to Ethylene via Metal–Organic-Framework-Augmented CO2 Availabilitycitations
- 2020CO2 electrolysis to multicarbon products at activities greater than 1 A cm−2citations
- 2020High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layercitations
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article
High-Rate and Selective CO2 Electrolysis to Ethylene via Metal–Organic-Framework-Augmented CO2 Availability
Abstract
High-rate conversion of carbon dioxide (CO<sub>2</sub>) to ethylene (C<sub>2</sub>H<sub>4</sub>) in the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) requires fine control over the phase boundary of the gas diffusion electrode (GDE) to overcome the limit of CO<sub>2</sub> solubility in aqueous electrolytes. Here, a metal–organic framework (MOF)-functionalized GDE design is presented, based on a catalysts:MOFs:hydrophobic substrate materials layered architecture, that leads to high-rate and selective C<sub>2</sub>H<sub>4</sub> production in flow cells and membrane electrode assembly (MEA) electrolyzers. It is found that using electroanalysis and operando X-ray absorption spectroscopy (XAS), MOF-induced organic layers in GDEs augment the local CO<sub>2</sub> concentration near the active sites of the Cu catalysts. MOFs with different CO<sub>2</sub> adsorption abilities are used, and the stacking ordering of MOFs in the GDE is varied. While sputtering Cu on poly(tetrafluoroethylene) (PTFE) (Cu/PTFE) exhibits 43% C<sub>2</sub>H<sub>4</sub> Faradaic efficiency (FE) at a current density of 200 mA cm<sup>−</sup><sup>2</sup> in a flow cell, 49% C<sub>2</sub>H<sub>4</sub> FE at 1 A cm<sup>−</sup><sup>2</sup> is achieved on MOF-augmented GDEs in CO<sub>2</sub>RR. MOF-augmented GDEs are further evaluated in an MEA electrolyzer, achieving a C<sub>2</sub>H<sub>4</sub> partial current density of 220 mA cm<sup>−2</sup> for CO<sub>2</sub>RR and 121 mA cm<sup>−2</sup> for the carbon monoxide reduction reaction (CORR), representing 2.7-fold and 15-fold improvement in C<sub>2</sub>H<sub>4</sub> production rate, compared to those obtained on bare Cu/PTFE.