A Macroscopically Relevant 3D-Metrology Approach for Nanocatalysis Research

A 3D nanometrological approach, which considers as an unbiased validation criterion the quantitative match between values of properties determined by macroscopic characterization techniques and those determined from the nanoscopic results, is developed to unveil the details of complex nanocatalysts. This approach takes into account both the peculiar characteristics of this type of materials and the large influence of noise in the tilt series. It combines, in an optimized way, the latest experimental developments in high angle annular dark field scanning transmission electron microscopy mode (HAADF-STEM) tomography, such as batch tomography, image denoising by undecimated wavelet transforms, improved reconstructions by total variation minimization and a more efficient, user-independent, segmentation scheme. To illustrate the use of this novel approach, the 3D structural characterization of a model nanocatalyst comprising gold nanoparticles dispersed on the surface of CeO2 nanocubes is performed, and the obtained results used to compute the values of different macroscopic chemical and textural properties. Comparison with values obtained by macroscopic characterization techniques match very closely those obtained by 3D nanometrology. Importantly, the new approach described in this work also illustrates a pipeline for nearly fully automated HAADF-STEM tomography studies, guaranteeing reliable correlations between nanoscopic and macroscopic properties.