| Sumario: | Herein we report the synthesis, structure solution, and catalytic properties of PST-31, which has an unprecedented framework topology. This high-silica (Si/Al=16) zeolite was synthesized using a pyrazolium-based dication with a tetramethylene linker as an organic structure-directing agent (OSDA) in hydroxide media. The PST-31 structure is built from new building layers containing four-, five-, six-, and seven-membered rings, which are connected by single four-membered rings in the interlayer region to form a two-dimensional pore system. Its channels consist of [4.56.6.9.11] and [5.6.7.9.10.11] cavities and are thus delimited by nine-, ten-, and eleven-membered rings. The OSDA cations in as-synthesized PST-31 were determined to reside without disorder in the large [42.514.64.72.94] cavities composed of smaller [4.56.6.9.11] and [5.6.7.9.10.11] ones, leading to a symmetry coincidence between the OSDA and the surrounding zeolite cavity. The proton form of PST-31 was found to be selective for the cracking of n-hexane to light olefins.
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