A well-defined catalyst with platinum (Pt) and gold (Au) encapsulated in
micropore and mesopore of micro-mesoporous zeolite (TMSN), respectively,
was designed to investigate the original active sites and kinetics of
semi-hydrogenation. Specifically, hydrogen molecules are dissociated on
Pt nanoclusters (NCs) to form hydrogen atoms that migrate to the
surfaces of TMSN zeolite and Au nanoparticles (NPs). Meanwhile, the Au
NPs with inferior H dissociation capability in the
mesopore can be served as the detector and controller of hydrogen
spillover. The Pt NCs in micropore act as H
dissociation sites while both the Au NPs and zeolite surface are
identified as the semi-hydrogenation sites. Noteworthy, the Pt-Au/TMSN
catalyst with double active sites exhibits higher selectivity and rate
constant ratio for semi-hydrogenation than Pt/TMSN, as well as higher
turnover frequency (TOF) than Au/MSN. This work creates an effective
regulation strategy of hydrogen spillover for improving active sites and
kinetics of semi-hydrogenation.