The properties of zeolites, and thus their suitability for different applications, are intimately connected with their structures. Synthesizing specific architectures is therefore important, but has remained challenging. Here we report a top-down strategy that involves the disassembly of a parent zeolite, UTL, and its reassembly into two zeolites with targeted topologies, IPC-2 and IPC-4. The three zeolites are closely related as they adopt the same layered structure, and they differ only in how the layers are connected. Choosing different linkers gives rise to different pore sizes, enabling the synthesis of materials with predetermined pore architectures. The structures of the resulting zeolites were characterized by interpreting the X-ray powder-diffraction patterns through models using computational methods; IPC-2 exhibits orthogonal 12- and ten-ring channels, and IPC-4 is a more complex zeolite that comprises orthogonal ten- and eight-ring channels. We describe how this method enables the preparation of functional materials and discuss its potential for targeting other new zeolites.

We report a theoretical study of water adsorption on coordinatively unsaturated sites (cus's) in a metal−organic framework (MOF) compound CuBTC. The reliability of the density functional theory (DFT)-based methods and dispersion-corrected DFT-D schemes for the description of cus sites was investigated with respect to the accurate reference CCSD(T)/CBS data. The accuracy of both DFT and DFT-D methods was found to be insufficient. The proposed DFT/CC correction scheme gave the results in excellent agreement with the reference CCSD(T)/CBS data. DFT/CC calculations performed for the periodic CuBTC model gave R Cu−OH2 = 2.19 Å and −ΔH ads= 49 kJ mol−1, both in very good agreement with available experimental data. The interaction of the first water molecule with the paddle-wheel unit is about 5 kJ mol−1 stronger than the interaction of the second water molecule with the same paddle-wheel unit. The DFT/CC scheme provides an accurate description of the extended MOF systems, and the results obtained with periodic DFT/CC model can be used for the testing and improvement of the force fields for classical simulations.

An increased synergy between experimental and theoretical investigations in heterogeneous catalysis has become apparent during the last decade.

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