posted on 2021-12-07, 19:07authored byZhiyang Zhang, Gui Liu, Liping Ding, Mi Hu, Jing Gu, Wenlong Xu, Qingbo Xiao
The
microenvironment surrounding the metal clusters on a carrier
produces a tremendous influence on its catalytic performance. In this
work, the promotion effect of the zeolitic inner host on catalytic
performance of encapsulated platinum nanoclusters is reported. In
the reaction of phenylacetylene semihydrogenation to styrene, Pt@X-zeolite,
where platinum nanoclusters are encapsulated into the inner microporosity
of the X-zeolite, exhibits an ∼3.37 times increased turnover
frequency and a much better selectivity of 87.6% in comparison to
the referenced Pt/X-zeolite of 79.3% selectivity to styrene at the
same reaction conditions, in which the platinum nanoclusters are located
at the exterior of the zeolite. Meanwhile, the Pt@X-zeolite displays
a higher stability after 10 cycles of the reaction. Through the detailed
characteristics, the excellent performance of Pt@X-zeolite is mainly
due to the promotion of the zeolitic framework on the encapsulated
Pt clusters, resulting in “electron-deficient” Pt clusters,
leading to a stronger interaction with the π* molecular orbitals
of phenylacetylene and thus enhancing the activation and conversion
of phenylacetylene. The zeolite cavity wrapped with encapsulated Pt
clusters regulates the adsorption trend of phenylacetylene through
the acetylene group on it, promotes the desorption of styrene, and
strengthens its selectivity. Meanwhile, Pt@X-zeolite has an excellent
stability through the zeolite framework, which protects the Pt species
from being lost. This investigation reveals the importance of the
zeolitic microenvironment on the catalytic performance of encapsulated
metal species and deepens the cognition for this type of catalyst.