Symmetry‐Induced Regulation of Pt Strain Derived from Pt3Ga Intermetallic for Boosting Oxygen Reduction Reaction

Pt‐based fuel cell catalysts with excellent activity and stability for proton‐exchange membrane fuel cells (PEMFCs) have been developed through strain regulation in recent years. Herein, this work demonstrates that symmetry‐induced strain regulation of Pt surface of PtGa intermetallic compounds can greatly enhance the catalytic performance of the oxygen reduction reaction (ORR). With the strain environment varies derived from the lattice mismatch of analogous PtGa core but different symmetry, the Pt surface of the PtGa alloy and the Pt3Ga (Pm3¯$\bar{3}$m) precisely realize 0.58% and 2.7% compressive strain compared to the Pt3Ga (P4/mmm). Experimental and theoretical results reveal that when the compressive stress of the Pt lattice increases, the desorption process of O* intermediates becomes accelerated, which is conducive to oxygen reduction. The Pt3Ga (Pm3¯$\bar{3}$m) with high symmetry and compressive Pt surface exhibit the highest mass and specific activities of 2.18 A mgPt−1 and 5.36 mA cm−2, respectively, which are more than one order of magnitude higher than those of commercial Pt/C catalysts. This work demonstrates that material symmetry can be used to precisely modulate Pt surface stress to enhance the ORR, as well as provide a distinct platform to investigate the relationship between Pt compressibility and catalytic activity. In this work, by altering the symmetry of the PtGa‐intermetallic structure, the stress environment in the surface Pt layer is precisely modified. By increasing strain, the key intermediate desorption step accelerates, resulting Pt3Ga (Pm3¯$\bar{\it 3}$m) with high symmetry exhibiting 10 times higher mass activity than commercial PtC and other samples with stretched surface.