Highly active platinum nanoparticles supported by nitrogen/sulfur functionalized graphene composite for ethanol electro-oxidation

•Graphene modified with cystamine and DWCNT forms a superior Pt catalyst support.•CO electro-oxidation onset potential is lowered by the cystamine modification.•Ethanol electro-oxidation activity, stability and poisoning resistance increases.•Activation energy for ethanol oxidation is higher with cystamine modification.

In this study, Pt nanoparticles are deposited on the surface of nitrogen-sulfur functionalized reduced graphene oxide and mixed with double wall carbon nanotubes (Pt/NS-rGO/DWCNT). The obtained nanocomposite is used as an electrocatalyst for the ethanol electro-oxidation reaction (EOR). CO oxidation studies with differential electrochemical mass spectroscopy (DEMS) show a lower onset potential indicating higher poisoning tolerance of these materials. The electrocatalytic activity of the Pt/NS-rGO/DWCNT nanocomposite is studied at different temperatures (40, 50, 60, and 70 °C) and compared with that of Pt/rGO, Pt/rGO/DWCNT composites and commercial carbon-supported Pt catalyst. Pt/rGO/DWCNT and Pt/NS-rGO/DWCNT display significantly higher ethanol electro-oxidation currents especially at low potentials relevant to fuel cell applications. At high temperatures (>50 °C), Pt/NS-rGO/DWCNT is the most active catalyst in concordance with its higher apparent activation energy. Pt/NS-rGO/DWCNT is also the most durable of the catalysts after a 500 potential cycle test and suffers the least from poisoning effects during chronopotentiometric testing. These results allow to conclude that combining NS-functionalized graphene catalyst support with DWCNT to form a composite provides excellent performances due to enhanced Pt electrocatalytic activity from NS-functionalization and enhanced mass transfer from the DWCNT filler.

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