Abstract
The practice of direct ethanol fuel cells (DEFCs) is hindered by insufficient activity of anode Pt-based catalyst for ethanol oxidation reaction (EOR), while alloying Rh and Ru to Pt is hopeful to solve the problem by simultaneously enhancing CC cleavage and decreasing poisoning; and Ru owning better stability and activity than usually doped Sn in alkaline electrolyte. Nevertheless, Pt-Rh-Ru catalysts were rarely reported. In this work, to avoid random trials, the “composition engineering” strategy was applied to design PtxRhRu catalysts. The optimal x range was predicted by DFT. Then, carbon nanotubes supported PtxRhRu ultrafine nanoparticles (PtxRhRu/CNTs) were synthesized and characterized. The synthetic mechanism was also studied. EOR tests show that, in line with the forecast, Pt4RhRu/CNTs (∼1.9 nm) exhibit the highest activity (5.85 mA·cm−2), 6.97 times of commercial Pt/C, and higher than most reports. The selectivity, stability and durability are also excellent. DFT analysis reveals the role of Pt-Rh-Ru site for the first time, that the optimal route on PtxRhRu is changed. New route clearly enhances complete ethanol oxidation and reduces poisoning. Bifunctional mechanism on Pt-Rh-Ru site was also confirmed. This study may provide new perspective for material design; the products are also promotive for DEFCs into practice.
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