Mesoporous materials
with large surface area and chemical inertness
are of great importance, and currently prevailing synthetic approaches
involve usages of micelles as pore-directing agents to create such
mesopores. In this work, allophanes, which are hollow aluminosilicate
spherules of 3.5–5.5 nm in size, have been synthesized and
assembled simultaneously for the first time in a controlled manner
to generate mesoporous spherical allophane assemblages (MSAAs) with
diameters of 445 ± 40 nm, specific surface area as high as 1032
m2/g, pore volume 1.104 mL/g at P/P
0 = 0.975, and average mesopore size at 3.4
nm. Furthermore, the thus-prepared MSAA could be doped with transition
metal ions to create a series of isomorphous derivatives; they could
also be converted to aluminum-based hierarchical assemblages of layered
double hydroxide easily. Different from the conventional channel-like
mesopores, the new mesoporosity attained in MSAA is easily accessible
because their mesopores are generated from the interparticle spaces
of spherical building units of hollow spherules. Therefore, the mesoporous
MSAA provides an excellent platform for construction of integrated
nanocatalysts. Highly dispersed noble metal nanoclusters such as Pt,
Au, and Pd could be deposited on the surface or in the interior mesopores
of the MSAA. Excellent activity and stability of MSAA-based catalysts
for Suzuki couplings and electrochemical sensing of H2O2 have been demonstrated using Pd/MSAA and Au/MSAA nanocomposites,
respectively.