The traditional deposition–precipitation (DP)
method is
common but not universal in manipulating Au nanoparticles’
spatial locations in propene epoxidation catalysts, especially for
hierarchical hydrophilic TS-1 supports. Directional loading of Au
nanoparticles to hierarchical hydrophilic TS-1 pores is challenging
because the strong hydrophilicity of the hierarchical TS-1 zeolite
would make Au nanoparticles loaded by the DP method tend to be deposited
on the hydrophilic support surface, thus blocking the pore mouths
and leading to deactivation. Therefore, manipulating Au nanoparticles’
spatial locations on hierarchical hydrophilic TS-1 supports is of
great significance to enhance the catalytic performance but is a bottleneck
problem. In this work, taking hierarchical hydrophilic HTS-1 supports
as an example, we propose a new modified isometric impregnation (NIMG)
method to manipulate the spatial location of Au nanoparticles. Moreover,
the Au spatial location inside HTS-1 pores is quantitatively reflected
by introducing the V
na parameter. Combined
with the N2 physisorption, high-angle annular dark-field
scanning transmission electron microscopy, inductively coupled plasma,
and X-ray photoelectron spectroscopy, it is found that the Au nanoparticles
loaded by the NIMG method tend to be uniformly distributed inside
the pores of HTS-1 due to the capillary effect. As expected, the Au/HTS-1(NIMG)
catalyst (with the Au nanoparticles inside the pores) exhibits a much
higher propylene oxide (PO) formation rate, PO selectivity, and H2 efficiency than the Au/HTS-1(DP) catalyst (with the Au nanoparticles
on the outer surface). This is possibly because loading Au nanoparticles
inside the pores is conducive to the transfer of H2O2 from Au to the nearby abundant Ti active sites, thus weakening
the decomposition of H2O2 to H2O,
avoiding the ring-opening side reactions, and promoting propene epoxidation
into PO. This work sheds new light for controlling the spatial location
of Au in hierarchically structured hydrophilic catalysts for direct
propene epoxidation.