Synergistic effect between few layer graphene and carbon nanotube supports for palladium catalyzing electrochemical oxidation of alcohols

能源化学(英文) ›› 2013, Vol. 22 ›› Issue (2): 296-304.

Synergistic effect between few layer graphene and carbon nanotube supports for palladium catalyzing electrochemical oxidation of alcohols

Bruno F. Machado^a, Andrea Marchionni^b, Revathi R. Bacsa^a, Marco Bellini^b, Julien Beausoleil^a,c, Werner Oberhauser^b, Francesco Vizza^b, Philippe Serp^a

a. Laboratoire de Chimie de Coordination, UPR CNRS 8241, Composante ENSIACET, Université de Toulouse UPS-INP-LCC, 4 allée Emile Monso, BP 44362, 31432 Toulouse Cedex 4, France;
b. Istituto di Chimica dei Composti Organometallici (ICCOM-CNR), Via Madonna del Piano 10, 50019 Sesto Fiorentino, Italy;
c. Arkema, Groupement de Recherches de Lacq, BP 34, RD 817, 64170 Lacq, France

收稿日期:2012-11-01 修回日期:2013-01-11 出版日期:2013-03-20 发布日期:2013-04-04
通讯作者: Francesco Vizza, Philippe Serp
基金资助:
This work was supported by the MATTM (Italy) for the PIRODE Project No 94, the MSE for the PRIT Project Industria 2015, the MIUR (Italy) for the FIRB 2010 Project RBFR10J4H7 002 and HYDROLAB2.

Synergistic effect between few layer graphene and carbon nanotube supports for palladium catalyzing electrochemical oxidation of alcohols

Bruno F. Machado^a, Andrea Marchionni^b, Revathi R. Bacsa^a, Marco Bellini^b, Julien Beausoleil^a,c, Werner Oberhauser^b, Francesco Vizza^b, Philippe Serp^a

a. Laboratoire de Chimie de Coordination, UPR CNRS 8241, Composante ENSIACET, Université de Toulouse UPS-INP-LCC, 4 allée Emile Monso, BP 44362, 31432 Toulouse Cedex 4, France;
b. Istituto di Chimica dei Composti Organometallici (ICCOM-CNR), Via Madonna del Piano 10, 50019 Sesto Fiorentino, Italy;
c. Arkema, Groupement de Recherches de Lacq, BP 34, RD 817, 64170 Lacq, France

Received:2012-11-01 Revised:2013-01-11 Online:2013-03-20 Published:2013-04-04
Supported by:
This work was supported by the MATTM (Italy) for the PIRODE Project No 94, the MSE for the PRIT Project Industria 2015, the MIUR (Italy) for the FIRB 2010 Project RBFR10J4H7 002 and HYDROLAB2.

摘要/Abstract

摘要： Few layer graphene (FLG), multi-walled carbon nanotubes (CNTs) and a nanotube-graphene composite (CNT-FLG) were used as supports for palladium nanoparticles. The catalysts, which were characterized by transmission electron microscopy, Raman spectroscopy and X-ray diffraction, were used as anodes in the electrooxidation of ethanol, ethylene glycol and glycerol in half cells and in passive direct ethanol fuel cells. Upon Pd deposition, a stronger interaction was found to occur between the metal and the nanotube-graphene composite and the particle size was significantly smaller in this material (6.3 nm), comparing with nanotubes and graphene alone (8 and 8.4 nm, respectively). Cyclic voltammetry experiments conducted with Pd/CNT, Pd/FLG and Pd/CNT-FLG in 10 wt% ethanol and 2 M KOH solution, showed high specific currents of 1.48, 2.29 and 2.51 mA·μg_Pd^-1, respectively. Moreover, the results obtained for ethylene glycol and glycerol oxidation highlighted the excellent electrocatalytic activity of Pd/CNT-FLG in terms of peak current density (up to 3.70 mA·μg_Pd^-1 for ethylene glycol and 1.84 mA·μg_Pd^-1 for glycerol, respectively). Accordingly, Pd/CNT-FLG can be considered as the best performing one among the electrocatalysts ever reported for ethylene glycol oxidation, especially considering the low metal loading used in this work. Direct ethanol fuel cells at room temperature were studied by obtaining power density curves and undertaking galvanostatic experiments. The power density outputs using Pd/CNT, Pd/FLG and Pd/CNT-FLG were 12.1, 16.3 and 18.4 mW·cm^-2, respectively. A remarkable activity for ethanol electrooxidation was shown by Pd/CNT-FLG anode catalyst. In a constant current experiment, the direct ethanol fuel cell containing Pd/CNT-FLG could continuously deliver 20 mA·cm^-2 for 9.5 h during the conversion of ethanol into acetate of 30%, and the energy released from the cell was about 574 J.

关键词: electrooxidation, alcohols, fuel cells, palladium, graphene, nanotube-graphene composites

Abstract: Few layer graphene (FLG), multi-walled carbon nanotubes (CNTs) and a nanotube-graphene composite (CNT-FLG) were used as supports for palladium nanoparticles. The catalysts, which were characterized by transmission electron microscopy, Raman spectroscopy and X-ray diffraction, were used as anodes in the electrooxidation of ethanol, ethylene glycol and glycerol in half cells and in passive direct ethanol fuel cells. Upon Pd deposition, a stronger interaction was found to occur between the metal and the nanotube-graphene composite and the particle size was significantly smaller in this material (6.3 nm), comparing with nanotubes and graphene alone (8 and 8.4 nm, respectively). Cyclic voltammetry experiments conducted with Pd/CNT, Pd/FLG and Pd/CNT-FLG in 10 wt% ethanol and 2 M KOH solution, showed high specific currents of 1.48, 2.29 and 2.51 mA·μg_Pd^-1, respectively. Moreover, the results obtained for ethylene glycol and glycerol oxidation highlighted the excellent electrocatalytic activity of Pd/CNT-FLG in terms of peak current density (up to 3.70 mA·μg_Pd^-1 for ethylene glycol and 1.84 mA·μg_Pd^-1 for glycerol, respectively). Accordingly, Pd/CNT-FLG can be considered as the best performing one among the electrocatalysts ever reported for ethylene glycol oxidation, especially considering the low metal loading used in this work. Direct ethanol fuel cells at room temperature were studied by obtaining power density curves and undertaking galvanostatic experiments. The power density outputs using Pd/CNT, Pd/FLG and Pd/CNT-FLG were 12.1, 16.3 and 18.4 mW·cm^-2, respectively. A remarkable activity for ethanol electrooxidation was shown by Pd/CNT-FLG anode catalyst. In a constant current experiment, the direct ethanol fuel cell containing Pd/CNT-FLG could continuously deliver 20 mA·cm^-2 for 9.5 h during the conversion of ethanol into acetate of 30%, and the energy released from the cell was about 574 J.

Key words: electrooxidation, alcohols, fuel cells, palladium, graphene, nanotube-graphene composites

Bruno F. Machado, Andrea Marchionni, Revathi R. Bacsa, Marco Bellini, Julien Beausoleil, Werner Oberhauser, Francesco Vizza, Philippe Serp. Synergistic effect between few layer graphene and carbon nanotube supports for palladium catalyzing electrochemical oxidation of alcohols[J]. 能源化学(英文), 2013, 22(2): 296-304.

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Synergistic effect between few layer graphene and carbon nanotube supports for palladium catalyzing electrochemical oxidation of alcohols

Synergistic effect between few layer graphene and carbon nanotube supports for palladium catalyzing electrochemical oxidation of alcohols

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