Effect of the pre-treatment of carbon black supports on the activity of Fe-based electrocatalysts for the reduction of oxygen

Journal Article · Thu Mar 25 04:00:00 EST 1999 · Journal of Physical Chemistry B: Materials, Surfaces, Interfaces, amp Biophysical

DOI:https://doi.org/10.1021/jp9821735· OSTI ID:349855

Wang, H; Cote, R; Faubert, G; Guay, D; Dodelet, J P ^[1]

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1. INRS-Energie et Materiaux, Varennes, Quebec (Canada)

A method involving HNO{sub 3}/NH{sub 3} treatments of a carbon support (Vulcan XC-72R), addition of Fe from inorganic precursors, and a thermal treatment at 900 C under an inert atmosphere for the preparation of Fe-based oxygen reduction electrocatalysts for use in polymer electrolyte fuel cells has been investigated. The prepared materials were evaluated in acidic medium by the rotating disk electrode technique using the potential at the oxygen reduction peak, E{sub p}, as a measure of the electrocatalytic activity. Two sets of experiments were performed: (i) varying the conditions of the HNO{sub 3} and NH{sub 3} treatments of Vulcan XC-72R, and (ii) varying Fe loadings added to the HNO{sub 3}/NH{sub 3} pretreated C samples. In the first set of experiments, no Fe was adsorbed on the C support. It was shown that a combined HNO{sub 3} and NH{sub 3} treatment of the carbon support gave higher activity for oxygen reduction than either HNO{sub 3} or NH{sub 3} treatment alone. In the second set of experiments, it was shown that the activity of the HNO{sub 3}/NH{sub 3}-modified C support increases steadily as the iron content is increased from 10 to about 1000 ppm. Above that Fe content, the activity of the materials first levels off and then decreases for even larger Fe concentrations. The value of E{sub p} at saturation increases with the total N surface content of HNO{sub 3}/NH{sub 3}-pretreated C support. X-ray photoelectron spectroscopy reveals that at maximal electrochemical activity, there is only 1 Fe atom per 100 N atoms at the surface of the carbon support. For larger Fe contents another mechanism, i.e., the aggregation of small iron-containing particles, probably accounts for all additional Fe ions adsorbed on the modified carbon black during the preparation procedure.

• OSTI ID: 349855
• Journal Information: Journal of Physical Chemistry B: Materials, Surfaces, Interfaces, amp Biophysical, Journal Name: Journal of Physical Chemistry B: Materials, Surfaces, Interfaces, amp Biophysical Journal Issue: 12 Vol. 103; ISSN 1089-5647; ISSN JPCBFK
• Country of Publication: United States
• Language: English

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