LAUSR

Ultrathin nanosheet catalysts deliver great potential in catalyzing the oxygen reduction reaction (ORR), but encounter the ceiling of the surface atomic utilizations, thus presenting a challenge associated with further boosting catalytic activity. Herein, a kind of PdPtCu ultrathin nanorings with increased numbers of electrocatalytically active sites is reported, with the purpose of breaking the activity ceiling of conventional catalysts. The as-made PdPtCu nanorings possess abundant high-index facets at the edge of both the exterior and interior surfaces. An ultrahigh electrochemical active surface area of 92.2 m2 g-1 PGM is achieved on this novel catalyst, much higher than that of the commercial Pt/C catalyst. The optimized Pd39 Pt33 Cu28 /C shows a great enhanced ORR activity with a specific activity of 2.39 mA cm-2 and a mass activity of 1.97 A mg-1 PGM at 0.9 V (versus RHE), as well as superior durability within 30 000 cycles. Density function theory calculations reveal that the high-index facets and alloying Cu atoms can optimize the oxygen adsorption energy, explaining the enhanced ORR activity. Overcoming a key technical barrier in sub-nanometer electrocatalysts, this work successfully introduces the hollow structures into the ultrathin nanosheets, heralding the exciting prospects of high-performance ORR catalysts in fuel cells.