Functional Motif Directed Decoupling‐Recoupling Strategy for Constructing Multi‐Site Pt‐Based Catalyst Toward Efficient Hydrogen Oxidation in Fuel Cells

ABSTRACT Hydrogen oxidation reaction (HOR) in alkaline media suffers from multiple challenges of sluggish kinetics, CO poisoning, and active‐site degradation. Multi‐metallic catalysts with multiple active sites hold promise for addressing the issues; however, they are thwarted by structural heterogeneity at the atomic level and reliance on empirical trial‐and‐error screening. Herein, we introduce a novel functional motif directed decoupling‐recoupling strategy for the design of multi‐site catalysts capable of super‐active and durable HOR electrocatalysis. Leveraging the well‐defined atomic coordinates for each element and superlattice ordering structure of the PtM intermetallic compound (IMC), the development of a multi‐functional Pt‐based HOR catalyst is decoupled into the independent screening of discrete Pt–M functional motifs. These optimally selected Pt–M motifs were subsequently recoupled into an L1 0 ‐PtFe framework, constructing the designed PtRuFeGaMo‐I catalyst. PtRuFeGaMo‐I integrates the multifunctionality of Pt–Ru/Ga/Mo motifs to simultaneously overcome the key limitations of alkaline HOR. Consequently, the engineered PtRuFeGaMo‐I exhibits exceptional HOR performance. In an anion exchange membrane fuel cell (AEMFC), PtRuFeGaMo‐I achieves a remarkable mass activity of 0.84 A mg total PGM −1 , surpassing commercial Pt/C and most reported noble‐metal‐based catalysts. This work provides a new platform to design advanced catalysts tailored to diverse electrocatalytic demands.