Charge
transfer from the supports to nanoparticles at the interface
is one of the key factors to determine the catalytic performances
of supported nanoparticles. In this work, we showed in a systematic
way that the charge transfer from semiconductor supports to Au nanoparticle
catalysts can lower the onset temperature toward CO oxidation. For
this study, a novel Au/SiO2/Si composite system synthesized
by the helium droplet deposition method with precisely tuned SiO2 layer thickness was fabricated to control the magnitude of
interfacial charge transfer. With the support of X-ray photoelectron
spectroscopy and numerical simulations, it was demonstrated that the
Schottky barrier formed across the Au/SiO2/Si heterojunction
led to a negative charge accumulation on the surface of Au nanoparticles.
In turn, this additional charge can be transferred to the antibonding
orbital of adsorbed O2 molecules to activate the O–O
bonds, leading to enhanced CO oxidation. In addition to the charge
transfer mechanism, the role of a strong electric field arising from
the formation of the Schottky barrier was also explored to explain
the observed enhancement of catalytic reactivity. Overall, this work
highlights an important pathway for systematically tuning metal–support
interactions to accelerate catalytic reactions and designing the next
generation of nanocatalysts.