Electron microscopy has been used to study the mesoscopic (nanometer-level) and
microscopic (micrometer-level) structural evolution of mesoscopic silica thin films grown at
the air−water interface under dilute, acidic (pH < 2) conditions. Transmission electron
microscope observations reveal that the film begins with a disordered (amorphous) structure.
Over time, mesoscopically ordered regions (hexagonally packed cylindrical channels) nucleate
and grow within the film. Scanning electron microscopy reveals microscopic structural
features such as ribbons, protrusions, domain boundaries, microindentations, and pits. Our
work shows that mesoscopic order develops within the film through a “disorder to order
transition.” Our observations also clarify the role of the air−water interface in confining
film growth to two dimensions during the initial stages. We note that a two-dimensional
(in-plane) to three-dimensional (unconstrained) growth transition occurs when the film
exceeds a critical thickness. We extend the current understanding of the structural evolution
of the film by providing a detailed mechanism for the development of mesoscopic order and
microscopic features and consider the possibility of a universal growth mechanism for films
and particles.
Porous ceramics are of great interest for filtration, catalysis, and reactive separation processes. Performance in these applications is highly dependent on features such as pore size distribution and connectivity and wall composition. Here, we describe a method allowing the rational design and synthesis of mesoporous silica composites with controlled heterogeneous pore architectures and demonstrate its validity by producing structures with predetermined placement of regions having different pore size and pore organization.
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