Electrochemical Promotion of Catalysis for CO<sub>2</sub> Hydrogenation on Ru-Based Catalyst Using Ionically Conducting Ceramics
Notice bibliographique
Résumé
The release of carbon dioxide (CO 2 ) into the atmosphere has led to effects of climate change resulting in an increase in global temperature, ocean acidification and many other environmental issues. Hydrogenation of CO 2 into synthetic hydrocarbons is a promising solution in decreasing anthropogenic dependence on fossil fuels and providing an energy source that is carbon-neutral. The reverse water gas shift (RWGS) reaction is a feasible hydrogenation reaction that requires a 2-electron transfer to yield syngas (CO + H 2 ) to be used in the Fischer-Tropsch reaction to synthesize synthetic hydrocarbons. In previous work (submitted to the Journal of CO 2 Utilization), the conversion of CO 2 into CO using Ru-nanostructured metal nanoparticles dispersed on ionically conducting ceramic supports like ceria (CeO 2 ), doped-ceria (x-CeO 2 ) and yttria-stabilized zirconia (YSZ) was studied with promising results. The activity of the Ru-based nanoparticles was improved due to the ionically conductive properties of the support, which contain oxygen (O δ- ) ionic species that promote the reaction. This promotional effect is known as the metal-support interaction (MSI) where nanoparticles are dispersed on a powder support, allowing O δ- species to migrate from support to nanoparticle by an increase in temperature [1,2]. The MSI effect has been observed using the best Ru-based powder catalyst supported on samarium-doped ceria (SDC) - Ru 45 Fe 55 /SDC (2 wt.%), which yielded high CO amounts between 300-750°C. Current research aims at improving the overall RWGS reaction at lower temperatures through the utilization of the electrochemical promotion of catalysis (EPOC) or non-faradaic electrochemical modification of catalytic activity (NEMCA) effect [3,4]. EPOC allows to control in-situ the migration of ionic species to and from the metal surface through the application of a potential difference or current between the catalyst-working electrode and an inert counter electrode. This migration of species leads to the formation of a neutral double layer encapsulating Ru nanoparticles, promoting the reaction. The catalyst setup resembles an electrocatalytic cell where metal nanoparticles act as the working electrode deposited on a solid support in the form of a disc. The support (YSZ in this case) represents a fixed layer of electrolytes that conducts O δ- ions to migrate to and from the active catalyst. As shown in Fig. 1, a promotional effect is observed for Ru on YSZ at 350°C under constant potential of 0.25 V, favoring the formation of CO through an enhancement ratio of ~2 and Faradaic efficiency of ~19, which is attributed to the synergistic effect between the metal and promoted ionic species O δ- . Additionally, density functional theory (DFT) calculations are being conducted for the hydrogenation of CO 2 on Ru nanoparticles and will be discussed in correlation with the experimental findings to confirm the mechanisms occurring during the reaction. [1] P. Vernoux, M. Guth, X. Li, Ionically Conducting Ceramics as Alternative Catalyst Supports, Electrochem. Solid-State Lett . 12 (2009) E9–E11. [2] S. Ntais, R.J. Isaifan, E.A. Baranova, An X-ray photoelectron spectroscopy study of platinum nanoparticles on yttria-stabilized zirconia ionic support: Insight into metal support interaction, Mater. Chem. Phys. 148 (2014) 673–679. [3] D. Vayenas, C.G., Bebelis, S., Pliangos, C., Brosda, S., Tsiplakides, Electrochemical Activation of Catalysis, Springer US , (2001). [4] P. Vernoux, L. Lizarraga, M.N. Tsampas, F.M. Sapountzi, A. De Lucas-Consuegra, J.L. Valverde, S. Souentie, C.G. Vayenas, D. Tsiplakides, S. Balomenou, E.A. Baranova, Ionically Conducting Ceramics as Active Catalyst Supports, Chem. Rev. 113 (2013) 8192–8260. Figure 1
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Prédiction distillée sur la base complète
Imitation des enseignantsNi prévalence calibrée, ni vérité terrain. Validation humaine à venir. Apprise à partir de 10 348 étiquettes directes de Codex et de 10 348 étiquettes directes de Gemma. Le mode candidate est l'union des têtes enseignantes seuillées; le consensus est leur intersection. Ces sorties portent le statut machine_predicted_unvalidated et ne sont ni des étiquettes humaines ni des étiquettes directes de modèles de pointe.
Scores Codex et Gemma par catégorie
| Catégorie | Codex | Gemma |
|---|---|---|
| Métarecherche | 0,001 | 0,003 |
| Méta-épidémiologie (sens strict) | 0,000 | 0,000 |
| Méta-épidémiologie (sens large) | 0,000 | 0,000 |
| Bibliométrie | 0,000 | 0,000 |
| Études des sciences et des technologies | 0,000 | 0,000 |
| Communication savante | 0,000 | 0,000 |
| Science ouverte | 0,000 | 0,000 |
| Intégrité de la recherche | 0,000 | 0,000 |
| Charge utile insuffisante (le modèle a refusé de juger) | 0,000 | 0,000 |
Scores machine (provisoires)
Les deux têtes enseignantes du modèle étudiant, lues sur ce travail. Un score ordonne la base pour la relecture; il n'affirme jamais une catégorie, et le statut de validation accompagne chaque rangée tel quel.
Scores de référence d'un modèle non mature (critères de maturité non atteints, 7 itérations). Un score ordonne; il n'affirme jamais une catégorie.
score_only:v0-immature-baseline · tel quel depuis la passe de notation : score_only signifie que le nombre peut ordonner les travaux, et qu'aucune étiquette de catégorie n'en découleClassification
machine, non validéePrédiction automatique; un appel candidat d’une seule tête enseignante, pas un consensus.
Le détail, modèle par modèle et score par score, se trouve en fin de page sous « Comment cette classification a été obtenue ».