Dual d– p hybridization in Ternary PtGaGe Enables Concurrent Activity and Stability Enhancement for Alkaline Oxygen Reduction

Abstract

ABSTRACT The activity–stability trade‐off in oxygen reduction reactions (ORR) fundamentally limits the practical development of Zinc–air batteries (ZABs) and fuel cells. Here, we address this long‐standing challenge through spatial electronic engineering that enables dual d–p orbital hybridization within a Pt‐based ternary alloy. The resulting PtGaGe catalyst exhibits exceptional alkaline ORR performance, achieving a mass activity of 1.79 A·mg Pt −1 and a half‐wave potential of 0.90 V (vs. RHE)—both surpassing commercial Pt/C and most previously reported Pt‐based catalysts. When integrated into a ZAB, it reaches a peak power density of 207.6 mW·cm −2 and maintains steady operation for over 200 h at 10 mA·cm −2 , highlighting outstanding durability under practical operating conditions. Density functional theory (DFT) calculations reveal that dual d–p hybridization induces spatial electron redistribution between Pt and Ga/Ge sites, modulating the Pt d ‐band center and facilitating O─O bond activation while suppressing catalyst degradation. This synergistic electronic regulation simultaneously improves catalytic activity, stability, and Pt utilization efficiency. This work establishes a mechanistic paradigm for electronic‐structure engineering in high‐performance ORR electrocatalysts.