Geometry-assisted three-dimensional superlocalization imaging of single-molecule catalysis on modular multilayer nanocatalysts

Angew Chem Int Ed Engl. 2014 Nov 17;53(47):12865-9. doi: 10.1002/anie.201407140. Epub 2014 Sep 26.

Abstract

To establish the structure-catalytic property relationships of heterogeneous catalysts, a detailed characterization of the three-dimensional (3D) distribution of active sites on a single catalyst is essential. Single-particle catalysis of a modular multilayer catalytic platform that consists of a solid silica core, a mesoporous silica shell, and uniformly distributed Pt nanoparticles sandwiched in between these layers is presented. The first 3D high-resolution super-localization imaging of single fluorescent molecules produced at active sites on the core-shell model nanocatalysts is demonstrated. The 3D mapping is aided by the well-defined geometry and a correlation study in scanning electron microscopy and total internal reflection fluorescence and scattering microscopy. This approach can be generalized to study other nano- and mesoscale structures.

Keywords: heterogeneous catalysis; mesoporous silica; multilayer nanocatalysts; platinum; three-dimensional imaging.