Mechanistic Insights Gained by High Spatial Resolution Reactivity Mapping of Homogeneous and Heterogeneous (Electro)Catalysts

[Image: see text] The recent development of high spatial resolution microscopy and spectroscopy tools enabled reactivity analysis of homogeneous and heterogeneous (electro)catalysts at previously unattainable resolution and sensitivity. These techniques revealed that catalytic entities are more heterogeneous than expected and local variations in reaction mechanism due to divergences in the nature of active sites, such as their atomic properties, distribution, and accessibility, occur both in homogeneous and heterogeneous (electro)catalysts. In this review, we highlight recent insights in catalysis research that were attained by conducting high spatial resolution studies. The discussed case studies range from reactivity detection of single particles or single molecular catalysts, inter- and intraparticle communication analysis, and probing the influence of catalysts distribution and accessibility on the resulting reactivity. It is demonstrated that multiparticle and multisite reactivity analyses provide unique knowledge about reaction mechanism that could not have been attained by conducting ensemble-based, averaging, spectroscopy measurements. It is highlighted that the integration of spectroscopy and microscopy measurements under realistic reaction conditions will be essential to bridge the gap between model-system studies and real-world high spatial resolution reactivity analysis.