Tuning the Selective Ethanol Oxidation on Tensile‐Trained Pt(110) Surface by Ir Single Atoms

Abstract

Abstract Development of efficient and robust electrocatalysts for complete oxidation of ethanol is critical for the commercialization of direct ethanol fuel cells. However, the complete oxidation of ethanol suffers from poor efficiency due to the low C1 pathway selectivity. Herein, single‐atomic Ir (Ir 1 ) on hcp ‐PtPb/ fcc ‐Pt core–shell hexagonal nanoplates (PtPb@PtIr 1 HNPs) enclosed by Pt(110) surface with a 7.2% tensile strain is constructed to drive complete electro‐oxidation of ethanol. Benefiting from the construction of Ir 1 sites, the PtPb@PtIr 1 HNPs exhibit a Faraday efficiency of 57.93% for the C1 pathway, which is ≈8.3 times higher than that of the commercial Pt/C‐JM. Furthermore, the PtPb@PtIr 1 HNPs show a top‐ranked electro‐activity achieving 45.1‐fold and 56.3‐fold higher than the specific and mass activities of Pt/C‐JM, respectively. Meanwhile, the durability can be significantly enhanced by the construction of Ir 1 sites. Density functional theory calculations indicate that the strong synergy on the PtPb@PtIr 1 HNPs surface significantly promotes the breaking of CC bond of CH 2 CO* and facilitates CO oxidation and suppresses the deactivation of the catalyst. This work offers a unique single‐atom approach using low‐coordination active sites on shape‐controlled nanocrystals to tune the selectivity and activity toward complicated catalytic reactions.