Despite their enormous impact in modern heterogeneous catalysis, single-atom catalysts (SACs) continue to puzzle the catalysis community, which often struggles to draw correct conclusions in SAC-catalyzed experiments. In many cases, the reasons for such an uncertainty originate from the lack of knowledge of the exact single-atom evolution under operative conditions and the fundamental factors controlling the fate of the single atom in relation to the catalytic mechanism. This has led to confusion also about correct definition and terminology, where the coined term single-site catalysts reflects the difficulty in defining the true active species as well as in obtaining long-range ordered homogeneous supports [Chi, S.; et al. J. Catal. 2023, 419, 49-57. DOI: 10.1016/j.jcat.2023.02.003]. Most recent studies have attempted to clarify several of the key aspects that are in play during SAC catalysis. However, one largely overlooked opportunity is to take advantage of all the dynamic phenomena occurring at the single metal site to turn the conventional catalytic sequences into a smart, stimulus-responsive, and controllable evolution of the single atom under operative conditions. Such “smartness” could potentially unleash pathways that mitigate some of the typical drawbacks of SACs, such as selectivity and stability. Here we present our vision on these yet-unexplored opportunities for exploiting the dynamicity of SACs, and we discuss various examples that could be the cornerstones for the advent of a next generation of SACs, that we term here “smart” single-atom catalysts (SSACs). Despite smart-behaving SACs still being far from realization, the clues provided here suggest pathways to achieve this goal.
