Synthesis and crystal structures of a novel layered silicate SSA-1 and its microporous derivatives by topotactic transformation.

ABSTRACT

The synthesis of a novel layered silicate SSA-1 (SSA silicate synthesized with a quaternary amine) was achieved in the SiO2-H2O-TEAOH (TEAOH tetraethylammonium hydroxide - as an organic structural directing agent) system. The crystal structure of SSA-1 involved two silicate layers composed of bre [10T]-type CBU (Composite Building Unit) and TEAOH in interlayers. The topotactic transformation of SSA-1 by calcination was examined, resulting in a porous material (PML-1 porous material transformed from a layered silicate) with a 108 m2 g-1 BET surface area and 0.035 cm3 g-1 pore volume. PML-1 is a siliceous microporous material with silanols in the framework and possesses unique properties, such as hydrophilicity, in spite of all its silica composition. The most reasonable crystal structure of PML-1 was successfully determined on the basis of the crystal structure of SSA-1 by a combination of manual modelling, PXRD pattern simulation, DFT optimization and Rietveld analysis. Additionally, an interlayer expanded siliceous zeolite SSA-1 (IEZ-SSA-1) was also successfully prepared by silylation using trichloro(methyl)silane under acidic conditions. IEZ-SSA-1 showed hydrophilicity or hydrophobicity properties by changing the functional group of the pillar part in the interlayer. Additionally, IEZ-SSA-1 showed a large gas adsorption property (537 m2 g-1 and 0.21 cm3 g-1).