Authors: Genlei Zhang, Dongjie Cao, Shiyu Guo, Yan Fang, Qi Wang, Sheng Cheng, Wansheng Zuo, Zhenzhen Yang, Peng Cui
Published: 2022-07-25
Source: Full article
AbstractDevelopment 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 (Ir1) onhcp‐PtPb/fcc‐Pt core–shell hexagonal nanoplates (PtPb@PtIr1HNPs) 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 Ir1sites, the PtPb@PtIr1HNPs 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@PtIr1HNPs 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 Ir1sites. Density functional theory calculations indicate that the strong synergy on the PtPb@PtIr1HNPs surface significantly promotes the breaking of CC bond of CH2CO* 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.