Construction of Hierarchical Films via Layer‐by‐Layer Assembly of Exfoliated Unilamellar Zeolite Nanosheets

Abstract Zeolites have been widely applied as versatile catalysts, sorbents, and ion exchangers with unique porous structures showing molecular sieving capability. In these years, it is reported that some layered zeolites can be delaminated into molecularly thin 2‐dimensional (2D) nanosheets characterized by inherent porous structures and highly exposed active sites. In the present study, two types of zeolite nanosheets with distinct porous structures with MWW topology (denoted mww) and ferrierite‐related structure (denoted bifer) are deposited on a substrate through the solution process via electrostatic self‐assembly. Alternate deposition of zeolite nanosheets with polycation under optimized conditions allows the layer‐by‐layer growth of their multilayer films with a stacking distance of 2–3 nm. Furthermore, various hierarchical structures defined at the unit‐cell dimensions can be constructed simply by conducting the deposition of mww and bifer nanosheets in a designed sequence. Adsorption of a dye, Rhodamine B, in these films, is examined to show that adsorption is dependent on constituent zeolite nanosheets and their assembled nanostructures. This work has provided fundamental advancements in the fabrication of artificial zeolite‐related hierarchical structures, which may be extended to other zeolite nanosheets, broadening their functionalities, applications, and benefits.