Fine‐Tuning Intrinsic Strain in Penta‐Twinned Pt–Cu–Mn Nanoframes Boosts Oxygen Reduction Catalysis

Abstract Tuning the intrinsic strain of Pt‐based nanomaterials has shown great promise for improving the oxygen reduction reaction (ORR) performance. Herein, reported is a tunable surface strain in penta‐twinned ternary Pt–Cu–Mn nanoframes (NFs). Pt–Cu–Mn ultrafine NFs (UNFs) exhibit ≈1.5% compressive strain compared to Pt–Cu–Mn pentagonal NFs (PNFs) and show the superior activity toward ORR in an alkaline environment. Specifically, the specific and mass activity of Pt–Cu–Mn UNFs are 3.38 mA cm−2 and 1.45 A mg−1, respectively, which is 1.45 and 1.71 times higher than that of Pt–Cu–Mn PNFs, demonstrating that compressive strain in NFs structure can effectively enhance the catalytic activity of ORR. Impressively, Pt–Cu–Mn UNFs exhibit 8.67 and 9.67 times enhanced specific and mass activity compared with commercial Pt/C. Theoretical calculations reveal that compression on the surface of Pt–Cu–Mn UNFs can weaken the bonding strengths and adsorption of oxygen‐containing intermediates, resulting in an optimal condition for ORR.