: Supported noble metal cluster catalysts are typically operated under severe conditions involving switches between reducing and oxidizing atmospheres, causing irreversible transformation of catalyst structure and thereby leading to permanent deactivation. We discovered that various Pt precursors spontaneously disperse in Ge-MFI zeolite, which opposes the Ostwald ripening phenomenon, producing self-regenerating Pt/Ge-MFI catalysts for propane dehydrogenation. These catalysts reversibly switch between Pt clusters and Pt single-atoms in response to reducing reaction and oxidizing regeneration conditions. This environmental adaptability allows them to completely self-regenerate over 110 reaction-regeneration cycles in propane dehydrogenation. They exhibited unprecedented sintering-resistance when exposed to air at 800 °C for 10 days. Such spontaneous metal dispersion in Ge-zeolites is a robust and versatile methodology for fabricating various Rh, Ru, Ir and Pd cluster catalysts.
