Nejvíce citovaný článek - PubMed ID 26489452
Layer like porous materials with hierarchical structure
Direct exfoliation of layered zeolites into solutions of monolayers has remained unresolved since the 1990s. Recently, zeolite MCM-56 with the MWW topology (layers denoted mww) has been exfoliated directly in high yield by soft-chemical treatment with tetrabutylammonium hydroxide (TBAOH). This has enabled preparation of zeolite-based hierarchical materials and intimate composites with other active species that are unimaginable via the conventional solid-state routes. The extension to other frameworks, which provides broader benefits, diversified activity, and functionality, is not routine and requires finding suitable synthesis formulations, viz. compositions and conditions, of the layered zeolites themselves. This article reports exfoliation and characterization of layers with ferrierite-related structure, denoted bifer, having rectangular lattice constants like those of the FER and CDO zeolites, and thickness of approximately 2 nm, which is twice that of the so-called fer layer. Several techniques were combined to prove the exfoliation, supported by simulations: AFM; in-plane, in situ, and powder X-ray diffraction; TEM; and SAED. The results confirmed (i) the structure and crystallinity of the layers without unequivocal differentiation between the FER and CDO topologies and (ii) uniform thickness in solution (monodispersity), ruling out significant multilayered particles and other impurities. The bifer layers are zeolitic with Brønsted acid sites, demonstrated catalytic activity in the alkylation of mesitylene with benzyl alcohol, and intralayer pores visible in TEM. The practical benefits are demonstrated by the preparation of unprecedented intimately mixed zeolite composites with the mww, with activity greater than the sum of the components despite high content of inert silica as pillars.
- Publikační typ
- časopisecké články MeSH
The most effective approach to practical exploitation of the layered solids that often have unique valuable properties-such as graphene, clays, and other compounds-is by dispersion into colloidal suspensions of monolayers, called liquid exfoliation. This fundamentally expected behavior can be used to deposit monolayers on supports or to reassemble into hierarchical materials to produce, by design, catalysts, nanodevices, films, drug delivery systems, and other products. Zeolites have been known as extraordinary catalysts and sorbents with three-dimensional structures but emerged as an unexpected new class of layered solids contributing previously unknown valuable features: catalytically active layers with pores inside or across. The self-evident question of layered zeolite exfoliation has remained unresolved for three decades. Here, we report the first direct exfoliation of zeolites into suspension of monolayers as proof of the concept, which enables diverse applications including membranes and hierarchical catalysts with improved access.
- Publikační typ
- časopisecké články MeSH