Catalytic complete
oxidation is an efficient approach to reducing
methane emissions, a significant contributor to global warming. This
approach requires active catalysts that are highly resistant to sintering
and water vapor. In this work, we demonstrate that Pd nanoparticles
confined within silicalite-1 zeolites (Pd@S-1), fabricated using a
facile in situ encapsulation strategy, are highly active and stable
in catalyzing methane oxidation and are superior to those supported
on the S-1 surface due to a confinement effect. The activity of the
confined Pd catalysts was further improved by co-confining a suitable
amount of Ce within the S-1 zeolite (PdCe0.4@S-1), which
is attributed to confinement-reinforced Pd–Ce interactions
that promote the formation of oxygen vacancies and highly reactive
oxygen species. Furthermore, the introduction of Ce improves the hydrophobicity
of the S-1 zeolite and, by forming Pd–Ce mixed oxides, inhibits
the transformation of the active PdO phase to inactive Pd(OH)2 species. Overall, the bimetallic PdCe0.4@S-1 catalyst
delivers exceptional outstanding activity and durability in complete
methane oxidation, even in the presence of water vapor. This study
may provide new prospects for the rational design of high-performance
and durable Pd catalysts for complete methane oxidation.