Super-Resolution Electrogenerated Chemiluminescence Microscopy for Single-Nanocatalyst Imaging.

Abstract

Electrogenerated chemiluminescence microscopy (ECLM) provides a real-time imaging approach to visualize the surface-dependent catalytic activity of nanocatalysts, which helps to rationalize the design of catalysts. In this study, we first propose super-resolution ECLM that could measure the facet- and site-specific activities of a single nanoparticle with nanometer resolution. The stochastic nature of the ECL emission makes the generation of photons obey Poisson statistics, which fits the requirement of super-resolution radial fluctuation (SRRF). By processing an SRRF algorithm, the spatial resolution of ECL images achieved ca. 100 nm, providing more abundant details on electrocatalytic reactivities at the subparticle level. Beyond conventional wide-field ECL imaging, super-resolution ECLM provided the spatial distribution of catalytic activities at a Au nanorod and nanoplate with scales of a few hundred nanometers. It helped uncover the facet- and defect-dependent surface activity, as well as the dynamic fluctuation of reactivity patterns on single nanoparticles. The super-resolution ECLM provides high spatiotemporal resolution, which shows great potential in the field of catalysis, biological imaging, and single-entity analysis.