Abstract

In this experimental study, we determine the size dependent activity as well as accelerated voltage cycling stability of various carbon supported palladium electrocatalysts for the oxygen reduction in acidic medium. Furthermore, ex-situ transmission electron microscopy studies before and after accelerated voltage cycles provide a deeper understanding regarding particle stability during operating conditions. Regarding oxygen reduction, a particle size effect on the specific activity is observed, with bulky Pd-black (≈4 m2/gPd) exhibiting ≈x6 times higher activity than Pd supported on Vulcan carbon (≈190 m2/gPd). Mass activities, however exhibit a strong correlation with catalyst surface area at small values, but are observed to be weakly dependent only between ≈50-200 m2/gPd. As stability tests during voltage cycling reveal a benefit for smaller surface areas, i.e. bigger particles, a limited gain in stability can be achieved by increasing catalyst particle size at a negligible cost of electrocatalytic mass-based activity.

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