High-performance
zeolite-supported noble metal catalysts
with low
loading and high dispersion of active components are the most promising
materials for achieving the complete oxidation of formaldehyde (HCHO)
at room temperature. In this work, palladium nanoparticles (Pd NPs)
with different sizes were successfully encapsulated inside the silicalite-1
(S-1) zeolite framework by using diverse stabling ligands via the
one-pot method. Thereafter, the rule on selecting the coordinative
ligands for palladium was clarified: more N atoms, a short carbon
chain, a smaller branch chain, and bidentate coordination are characteristics
of an ideal ligand. Accordingly, the best-performing 0.2Pd@S-1(Ethylenediamine)
catalyst exhibited outstanding performance for HCHO oxidation, achieving
100% conversion even at room temperature. High-resolution high-angle
annular dark-field scanning transmission electron microscopy (HR HAADF-STEM)
and density functional theory (DFT) calculations indicate that the
chelate is formed by complexation of Pd2+ ions with ethylenediamine,
displaying the smallest spatial site resistance simultaneously with
the zeolite synthesis, resulting in Pd located mostly within the 5-membered
ring (5-MR) channels of S-1 after calcination, thus limiting the growth
of Pd clusters and promoting their dispersion.