Abstract

Surface processes of CO2 reduction on Pt(210), Pt(310), and Pt(510) electrodes were studied by cyclic voltammetry. Different surface structures of these platinum single crystal electrodes were obtained by various treatment conditions. The experimental results illustrated that the electrocatalytic activity of Pt single crystal electrodes towards CO2 reduction is decreased in an order of Pt(210)>Pt(310)>Pt(510), i.e., with the decrease of (110) step density on well-defined surfaces. When the surfaces were reconstructed due to oxygen adsorption, the catalytic activity of all the three electrodes has been enhanced to a certain extent. Although the activity order remains unchanged, the electrocatalytic activity has been enhanced more significantly as the density of (110) step sites is more intensive on the Pt single crystal surface. It has revealed that the more open the surface structure is, the more active the Pt single crystal electrode will be, and the easier for the electrode to be transformed into a surface structure that exhibits higher activity under external inductions. However, the relatively ordered surfaces of Pt single crystal electrode are comparatively stable under the same external inductions. The present study has gained knowledge on the interaction between CO2 and Pt single crystal electrode surfaces at a microscopic level, and thrown new insight into understanding the surface processes of electrocatalytic reduction of CO2.

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