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Identify the Activity Origin of Pt Single-Atom Catalyst via Atom-by-Atom Counting.

Atom dispersion in metal supported catalysts is vital as it structurally accounts for their catalytic performances. Since practical catalysts normally present structural diversity, such as the coexistence of single atoms, clusters, and particles, traditional spectroscopy methods including chemisorption, titration, and X-ray absorption, however, provide only an averaged description about the atom dispersion but are not able to distinguish localized structural divergence. In this work, through developing a methodology of electron-microscopy-based atom recognition statistics (EMARS), catalyst dispersion has been redefined at atomic precision in real space via the statistically counting 18 000+ Pt atoms for a Pt/Al2O3 industrial reforming catalyst. The EMARS results combined with in situ microscopy evidence disclose that the activity for aromatics production quantitatively correlates with the density of Pt single-atoms, while Pt clusters contribute no direct activity but could kinetically transform into single-atoms when being heated under an oxidative atmosphere. Compared to EMARS, the traditional hydrogen-oxygen titration method is found to induce serious bias in the Pt dispersion in reference to actual activity. This distinctive capability of EMARS for metal dispersion quantification offers a possibility of directly identifying the catalysis roles of different metal species in a practical catalyst via atom-resolved statistics.