Templating with organic substances is known as a primary
step for
synthesizing silica-based porous materials, e.g., porous clay nanoheterostructures,
but the shrinkage dynamics of template substances in response to temperatures
and its influence on micro- and mesopore formation has not been the
subject of extensive research. Here, the shrinkage of hexadecyltrimethylammonium
(HDTMA+) monomers with long alkyl chains perceptible to
temperatures is studied by means of molecular simulations coupled
with angstrom-scale open-space analysis using positronium. The HDTMA+ monomers are deviated from trans conformation concomitantly
forming ∼6 Å open spaces in the agglomerate upon coexisting
with propanol molecules. Pore texture properties in view of micro-
and mesopores, studied by N2 adsorption/desorption experiments
at −196 °C, are found to be improved at low temperatures
owing to efficient pillaring between two adjacent nanosheets resultant
from less shrinkage of HDTMA+ monomers.