PtNi alloy and hybrid structures have shown impressive catalytic activities toward the cathodic oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). However, such promise does not often translate into improved electrode performances in PEMFC devices. In this contribution, a Ni impregnation and subsequent annealing method, translatable to vertically aligned nanowire gas diffusion electrodes (GDEs), is shown in thin-film rotating disk electrode measurements (TFRDE) to enhance the ORR mass activity of Pt nanowires (NWs) supported on carbon (Pt NWs/C) by around 1.78 times. Physical characterisation results indicate that this improvement can be attributed to a combination of Ni alloying of the nanowires with retention of the morphology, while demonstrating that Ni can also help improve the thermal stability of Pt NWs. These catalysts are then tested in single PEMFCs. Lower power performances are achieved for PtNi NWs/C than Pt NWs/C. A further investigation confirms the different surface behaviour between Pt NWs and PtNi NWs when in contact with electrolyte ionomer in the electrodes in PEMFC operation. Indications are that this interaction exacerbates reactant mass transport limitations not seen with TFRDE measurements.
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