Flexible Mesopores in Nanoscrolls: Extraordinarily Large Alteration of Pore Sizes and Their Reversibility

Abstract Flexible porous materials have gained considerable interest for their potential applications in selective absorption and controlled release/storage of specific molecules or compounds. Here, nanoscrolls are proposed as a type of inorganic solids with reversibly flexible mesopores. Nanoscrolls exhibit a rolled‐up structure composed of nanosheets with a 1D rod‐like morphology, possessing two distinct nanospaces. The first space comprises 1D tubular mesopores located at the center of the rod, while the second space exists in the interlayer regions on the wall of the mesopore, resulting from the layer stacking caused by the scrolling of nanosheets. By replacing the interlayer cations on the nanoscroll walls with other cations, a drastic alteration in the size of the 1D mesopores is observed. For instance, exchanging bulky dodecylammonium cations with small NH ₄ ⁺ cations leads to a substantial change in pore size, with differences ranging from 10 to 20 nm—a notably larger variation compared to previous reports on flexible porous materials. Importantly, the alteration of pore size induced by the exchange reaction is found to be reversible. This reversible alteration in pore size holds promise for applications in host–guest chemistry involving large moieties such as nanoparticles and enzymes.