Strong Metal–Support Interaction in Platinum Group Metal Heterostructured Catalysts

Constructing heterostructured catalysts has emerged as an effective strategy to enhance the activity and durability of platinum group metal (PGM) catalysts. At heterointerfaces, strong metal–support interactions (SMSI) can profoundly regulate catalytic behavior by restructuring metal active sites, modulating interfacial charge transfer, and altering the local chemical environment, thereby influencing reaction pathways and kinetics. Despite extensive progress, a unified framework for interpreting the diverse manifestations of SMSI and correlating them with catalytic performance remains lacking. In this review, we introduce the concept of SMSI descriptors, which translate coupled interfacial structural and electronic evolutions into quantifiable parameters that enable cross-system comparison and structure–performance analysis. We first trace the historical development and mechanistic understanding of SMSI, followed by a systematic discussion of recent advances in constructing and regulating PGM-based heterostructured catalysts. Particular emphasis is placed on how in situ/operando characterization techniques, together with density functional theory (DFT) and emerging machine-learning approaches, reveal the dynamic evolution of SMSI under working conditions. Finally, we outline descriptor-guided design principles for engineering next-generation catalysts with improved activity, selectivity, and stability for energy and environmental applications.