Oxygen reduction on nanocrystalline ruthenia-local structure effects

Daniel F. Abbott, Sanjeev Mukerjee, Valery Petrykin, Zdeněk Bastl, Niels Bendtsen Halck, Jan Rossmeisl, Petr Krtil

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Nanocrystalline ruthenium dioxide and doped ruthenia of the composition Ru1-xMxO2 (M = Co, Ni, Zn) with 0 ≤ x ≤ 0.2 were prepared by the spray-freezing freeze-drying technique. The oxygen reduction activity and selectivity of the prepared materials were evaluated in alkaline media using the RRDE methodology. All ruthenium based oxides show a strong preference for a 2-electron oxygen reduction pathway at low overpotentials. The catalysts' selectivity shifts towards the 4-electron reduction pathway at high overpotentials (i.e. at potentials below 0.4 V vs. RHE). This trend is particularly noticeable on non-doped and Zn-doped catalysts; the materials containing Ni and Co produce a significant fraction of hydrogen peroxide even at high overpotentials. The suppression of the 4-electron reduction pathway on Ni and Co-doped catalysts can be accounted for by the presence of the Ni and Co cations in the cus binding sites as shown by the DFT-based analyses on non-doped and doped catalysts.
Original languageEnglish
JournalRSC Advances
Issue number2
Pages (from-to)1235-1243
Number of pages9
Publication statusPublished - 2015


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