Iron porphyrin-based cathode catalysts for polymer electrolyte membrane fuel cells: Effect of NH3 and Ar mixtures as pyrolysis gases on catalytic activity and stability

Meng, Hui; Larouche, Nicholas; Lefèvre, Michel; Jaouen, Frédéric; Stansfield, B.L.; Dodelet, Jean‐Pol

doi:10.1016/j.electacta.2010.06.039

Cited by 109 publications

(72 citation statements)

References 70 publications

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“…The Tafel slopes of the more-active catalysts show values of about 70 mV dec −1 . This value is in good agreement with the values that were observed for other catalysts prepared by the (oxalate supported) pyrolysis of porphyrins [15,24,29] as well as alternatively prepared catalysts (without the use of a reactive gas heat-treatment) [19]. When the fraction of oxalic acid goes down the Tafel slope increases, getting closer to 100 mV dec −1 .…”

Section: Resultssupporting

confidence: 79%

Influence of the Structure-Forming Agent on the Performance of Fe-N-C Catalysts

et al. 2018

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Abstract:In this work, the influence of the structure-forming agent on the composition, morphology and oxygen reduction reaction (ORR) activity of Fe-N-C catalysts was investigated. As structure-forming agents (SFAs), dicyandiamide (DCDA) (nitrogen source) or oxalic acid (oxygen source) or mixtures thereof were used. For characterization, cyclic voltammetry and rotating disc electrode (RDE) experiments were performed in 0.1 M H 2 SO 4 . In addition to this, N 2 sorption measurements and Raman spectroscopy were performed for the structural, and elemental analysis for chemical characterization. The role of metal, nitrogen and carbon sources within the synthesis of Fe-N-C catalysts has been pointed out before. Here, we show that the optimum in terms of ORR activity is achieved if both N-and O-containing SFAs are used in almost similar fractions. All catalysts display a redox couple, where its position depends on the fractions of SFAs. The SFA has also a strong impact on the morphology: Catalysts that were prepared with a larger fraction of N-containing SFA revealed a higher order in graphitization, indicated by bands in the 2nd order range of the Raman spectra. Nevertheless, the optimum in terms of ORR activity is obtained for the catalyst with highest D/G band ratio. Therefore, the results indicate that the presence of an additional oxygen-containing SFA is beneficial within the preparation.

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Section: Resultssupporting

confidence: 79%

Influence of the Structure-Forming Agent on the Performance of Fe-N-C Catalysts

et al. 2018

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“…The Tafel slopes of the more-active catalysts give values of about 70 mV dec -1 . This value is in good agreement with the values that were observed for other catalysts prepared by the (oxalate supported) pyrolysis of porphyrins [15,[24][25] as well as alternatively prepared catalysts (without the use of a reactive gas heat-treatment) [19]. When the fraction of oxalic acid goes down the Tafel slope increases, getting closer to 100 mV dec -1 .…”

Section: Resultssupporting

confidence: 79%

Influence of the Structure Forming Agent on the Performance of Fe-N-C Catalysts

Schardt¹,

Weidler²,

Wallace³

et al. 2018

Preprint

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Abstract:In this work the influence of the structure forming agent on the composition, morphology and oxygen reduction reaction (ORR) activity of Fe-N-C catalysts was investigated. As structure forming agent (SFA), dicyandiamide (DCDA) (nitrogen source) or oxalic acid (oxygen source) or mixtures thereof were used. For characterization, cyclic voltammetry and rotating disc electrode (RDE) experiments were performed in 0.1 M H2SO4. In addition to this, N2 sorption measurements and Raman spectroscopy were performed for the structural characterization. The role of metal, nitrogen and carbon sources within the synthesis of Fe-N-C catalysts has been pointed out before. Here, we show that the optimum in terms of ORR activity is achieved if both N-and O-containing SFAs are used in almost similar fractions. All catalysts display a redox couple, whereat its position depends on the fractions of SFAs. The SFA has also a strong impact on the morphology: Catalysts that were prepared with a larger fraction of N-containing SFA revealed a higher order in graphitization, indicated by bands in the 2 nd order range of the Raman spectra. Nevertheless, the optimum in terms of ORR activity is obtained for the catalyst with highest D/G band ratio. Therefore, the results indicate that the presence of an additional oxygen-containing SFA is beneficial within the preparation.

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“…This assignment of Fe-containing particles to iron nitrides also agrees with the mainly spherical shape of most of the individual (non-aggregated) particles seen in Figs. 7B and 8B, as iron nitrides particles have been found to evolve from a quenched liquid iron nitride phase rich in nitrogen [41][42][43]. Furthermore, iron nitride particles are not surrounded by a protecting carbon layer as are iron carbides [42].…”

Section: Transmission Electronic Microscopy (Tem) and Catalyst Stabilitymentioning

confidence: 98%

Activity, Performance, and Durability for the Reduction of Oxygen in PEM Fuel Cells, of Fe/N/C Electrocatalysts Obtained from the Pyrolysis of Metal-Organic-Framework and Iron Porphyrin Precursors

Yang

Larouche

Chenitz

et al. 2015

Electrochimica Acta

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133

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Iron porphyrin-based cathode catalysts for polymer electrolyte membrane fuel cells: Effect of NH3 and Ar mixtures as pyrolysis gases on catalytic activity and stability

Cited by 109 publications

References 70 publications

Influence of the Structure-Forming Agent on the Performance of Fe-N-C Catalysts

Influence of the Structure-Forming Agent on the Performance of Fe-N-C Catalysts

Influence of the Structure Forming Agent on the Performance of Fe-N-C Catalysts

Activity, Performance, and Durability for the Reduction of Oxygen in PEM Fuel Cells, of Fe/N/C Electrocatalysts Obtained from the Pyrolysis of Metal-Organic-Framework and Iron Porphyrin Precursors

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Iron porphyrin-based cathode catalysts for polymer electrolyte membrane fuel cells: Effect of NH3 and Ar mixtures as pyrolysis gases on catalytic activity and stability

Cited by 109 publications

References 70 publications

Influence of the Structure-Forming Agent on the Performance of Fe-N-C Catalysts

Influence of the Structure-Forming Agent on the Performance of Fe-N-C Catalysts

Influence of the Structure&nbsp;Forming Agent on the Performance of Fe-N-C Catalysts

Activity, Performance, and Durability for the Reduction of Oxygen in PEM Fuel Cells, of Fe/N/C Electrocatalysts Obtained from the Pyrolysis of Metal-Organic-Framework and Iron Porphyrin Precursors

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Influence of the Structure Forming Agent on the Performance of Fe-N-C Catalysts