ABSTRACT Atomic aggregates (AAs), historically deemed detrimental defects in single‐atom catalysts (SACs), are evolving from unwanted byproducts to programmable synergistic units as SAC research advances from isolated single atoms (SAs) to integrated AAs‐SAs hybrid systems. This perspective proposes that precise engineering of AAs dimension, AAs/SAs ratio, and inter‐site distance between AAs and SAs offers a paradigm‐shifting strategy to overcome the fundamental stability‐performance trade‐off plaguing SAC development. A comprehensive experimental and characterization framework for identifying and quantifying AAs‐SAs hybrid architectures is established, with their synergistic effects originating from the coupling of electronic fields, stress fields, and confinement fields. These coupled effects enable fine‐tuning of the geometric/electronic structures of SACs and intrinsic activation of reaction intermediates, thereby unlocking unparalleled catalytic activity, stability, and adaptability‐particularly in complex reaction environments such as advanced oxidation processes (AOPs). This redefined role of AAs reshapes the design principles for next‐generation high‐performance SACs.
Mo et al. (Thu,) studied this question.