“…Surface reactions on nanomaterials are important for many modern industrial processes because of the large variety of surface transformations involved, including (de)hydrogenation, redox, carbon-based bond coupling, and cleavage reactions. − Tremendous work had been done with traditional ensemble methods. − However, because of the inherent heterogeneity among nanoparticles in size, shape, morphology, surface composition, and so on, it is challenging to determine the precise structure–reactivity relationship from such ensemble measurements. For a deeper and more precise understanding of structure–reactivity relationships, it is highly desirable to study surface reactions in situ at the single-molecule/single-particle level in real time with sufficiently high spatiotemporal resolution.…”