Abstract
An accurate understanding of the surface structure–activity relationship is essential to rational designing highly efficient electrocatalysts for methanol oxidation reaction (MOR). Here, L11-ordered PtCu/C with rough and smooth Pt shells were obtained by electrochemically (ED) and chemically dealloying (CD) methods to investigate the difference in their MOR performances. The rough Pt shells (PtCu/C-700-ED) exhibited mass activity (MA) of 1625.2 mA mgPt−1 at peak potential, 2.19 and 2.74 times higher than smooth Pt shells (PtCu/C-700-CD) (743.1 mA mgPt−1) and commercial Pt/C (593.5 mA mgPt−1), respectively. DFT calculations indicate that PtCu with rough surfaces has a weaker CO binding energy than that with smooth surfaces, leading to better CO resistance and MOR activity. However, accelerated durability tests exhibit that the PtCu/C-700-CD catalysts obtained activity above the initial current density after 2000 cycles compared to PtCu/C-700-ED (36.48% loss) and commercial Pt/C (67.35% loss), indicating that smooth Pt shells have prominent structural stability. In addition, similar results were found simultaneously for other ordered Pt-based binary catalysts.
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