Nanoframe alloy structures represent a class of high-performance catalysts for the oxygen reduction reaction (ORR), owing to their high active surface area, efficient molecular accessibility, and nanoconfinement effect. However, structural and chemical instabilities of nanoframes remain an important challenge. Here, we report the synthesis of PtCu nanoframes constructed with an atomically ordered intermetallic structure (-PtCuNF/C) showing high ORR activity, durability, and chemical stability. We rationally designed the -PtCuNF/C catalyst by combining theoretical composition predictions with a silica-coating-mediated synthesis. The -PtCuNF/C combines intensified strain and ligand effects from the intermetallic PtCu L1 structure and advantages of the nanoframes, resulting in superior ORR activity to disordered alloy PtCu nanoframes (-PtCuNF/C) and commercial Pt/C catalysts. Importantly, the -PtCuNF/C showed the highest ORR mass activity among PtCu-based catalysts. Furthermore, the -PtCuNF/C exhibited higher ORR durability and far less etching of constituent atoms than -PtCuNF/C and Pt/C, attesting to the chemically stable nature of the intermetallic structure.
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