G. Lalande et al., IS NITROGEN IMPORTANT IN THE FORMULATION OF FE-BASED CATALYSTS FOR OXYGEN REDUCTION IN SOLID POLYMER FUEL-CELLS, Electrochimica acta, 42(9), 1997, pp. 1379-1388
The role of nitrogen and iron in the generation of catalysts for oxyge
n reduction in acidic media has been investigated by using two indepen
dent organic precursors. The Fe and N precursors were polyvinylferroce
ne adsorbed on carbon black and acetonitrile vapor, respectively. Thes
e precursors were pyrolyzed at 1000 degrees C. A catalyst is obtained
only if Fe and N are present together in the reactor during pyrolysis.
Inactive Fe clusters surrounded by a protective graphitic envelope ar
e produced when adsorbed polyvinylferrocene is pyrolyzed alone at 1000
degrees C. The latter material may, however, be activated by a second
pyrolysis in acetonitrile vapor. The characterization of the catalyst
indicates that the iron is oxidized (Fe-II and Fe-III), but no strong
Fe-N-x bonds were unequivocally detected by ToF SIMS. Lifetime testin
g of the catalyst in a polymer electrolyte fuel cell demonstrated stab
le currents for at least 300 h. The current density measured with a ca
talyst containing 1 wt% Fe was about 1/3 of that measured with a comme
rcial Pt-based catalyst containing 2 wt% metal loading. (C) 1997 Publi
shed by Elsevier Science Ltd.