Average turn-over frequency of O2 electro-reduction for Fe/N/C and Co/N/C catalysts in PEFCs

This work aims to evaluate the average turn-over frequency of 02 electro-reduction for the catalytic sites resulting from the heat-treatment of iron- or cobalt-acetate and carbon black in ammonia at high temperature. This task is complex because at least three factors may control the activity of such catalysts: their metal content, nitrogen content and micropore specific area. In this work, the activity was measured for metal contents from 0.005 to 5 wt.%. The time of heat-treatment was tuned to keep the micropore specific area constant. At Fe content <= 0.2 wt.% the activity increases linearly with Fe content, thus enabling the average turn-over frequency of the Fe/N/C site to be determined. At Co content <= 1.0 wt.% the activity increases approximately as the square root of the Co content. Because no linear relation was found, the turn-over frequency of the Co/N/C site could not be determined. For both Fe and Co catalysts, the activity drops dramatically at contents >1 wt.%. This is concurrent with a drop in the micropore specific area of the catalysts. (C) 2007 Elsevier Ltd. All rights reserved.