In situ Raman spectroscopy studies of single-atom catalysis

In situ Raman spectroscopy enables real-time identification of key reaction intermediates and pathways in single-atom catalysis. This Perspective highlights recent methodological advances and mechanistic insights achieved through its application in electrocatalysis and organocatalysis over single-atom catalysts (SACs). We discuss the strengths and limitations of conventional and surface-enhanced Raman approaches in SACs’ mechanistic studies, and outline emerging opportunities for probing catalytic processes at the single-atom limit. We hope this summary will advance insights into single-atom catalysis and promote the rational design of SACs for real-world applications.