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Confined Catalysis in the g‑C3N4/Pt(111) Interface: Feasible Molecule Intercalation, Tunable Molecule–Metal Interaction, and Enhanced Reaction Activity of CO Oxidation
journal contribution
posted on 2017-09-06, 00:00 authored by Shujiao Wang, Yingxin Feng, Ming’an Yu, Qiang Wan, Sen LinThe
deposition of a two-dimensional (2D) atomic nanosheet on a
metal surface has been considered as a new route for tuning the molecule–metal
interaction and surface reactivity in terms of the confinement effect.
In this work, we use first-principles calculations to systematically
explore a novel nanospace constructed by placing a 2D graphitic carbon
nitride (g-C3N4) nanosheet
over a Pt(111) surface. The confined catalytic activity in this nanospace
is investigated using CO oxidation as a model reaction. With the inherent
triangular pores in the g-C3N4 overlayer being taken advantage of, molecules such as CO and O2 can diffuse to adsorb on the Pt(111) surface underneath the g-C3N4 overlayer. Moreover, the mechanism
of intercalation is also elucidated, and the results reveal that the
energy barrier depends mainly on the properties of the molecule and
the channel. Importantly, the molecule–catalyst interaction
can be tuned by the g-C3N4 overlayer,
considerably reducing the adsorption energy of CO on Pt(111) and leading
to enhanced reactivity in CO oxidation. This work will provide important
insight for constructing a promising nanoreactor in which the following
is observed: The molecule intercalation is facile; the molecule–metal
interaction is efficiently tuned; the metal-catalyzed reaction is
promoted.