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A family of zeolites with controlled pore size prepared using a top-down method

Abstract

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.

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Figure 1: The structures of zeolites UTL, IPC-2 and IPC-4.
Figure 2: The pore windows and sizes for zeolites IPC-2 and IPC-4.
Figure 3: Characterization of zeolites IPC-2 and IPC-4.
Figure 4: The ADOR strategy for the preparation of zeolites.

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Acknowledgements

The authors acknowledge the Grant Agency of the Czech Republic (Center of Excellence – P106/12/G015). R.E.M. is a Royal Society Industry Fellow. We also thank the Leverhulme Trust and the Engineering and Physical Sciences Research Council (EP/K005499/1 and EP/K039210/1) for funding. J.Č. thanks Micromeritics for an Instrument Award.

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Authors and Affiliations

Authors

Contributions

W.J.R., P.C. and O.S. completed the synthesis work, P.N., L.G. and M.P. the calculations, P.S.W. the Rietveld refinement, V.R.S. and S.E.A. the NMR spectroscopy and A.Z. the adsorption experiments. W.J.R., P.N., J.Č. and R.E.M. co-wrote the paper.

Corresponding authors

Correspondence to Russell E. Morris or Jiří Čejka.

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The authors declare no competing financial interests.

Supplementary information

Supplementary information

Supplementary information (PDF 1406 kb)

Supplementary information

Atomic positions of experimental IPC-2 structure (CIF 5 kb)

Supplementary information

Atomic positions of experimental IPC-4 structure (CIF 5 kb)

Supplementary information

Calculated atomic positions for IPC-2 (equivalent to structure a in Figure S3) (CIF 5 kb)

Supplementary information

Calculated atomic positions for structure b in Figure S3 (CIF 5 kb)

Supplementary information

Calculated atomic positions for structure c in Figure S3 (CIF 9 kb)

Supplementary information

Calculated atomic positions for structure d in Figure S3 (CIF 5 kb)

Supplementary information

Calculated atomic positions for IPC-4 (equivalent to structure a in Figure S1) (CIF 7 kb)

Supplementary information

Calculated atomic positions for structure b in Figure S1 (CIF 4 kb)

Supplementary information

Calculated atomic positions for structure c in Figure S1 (CIF 7 kb)

Supplementary information

Calculated atomic positions for structure d in Figure S1 (CIF 4 kb)

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Roth, W., Nachtigall, P., Morris, R. et al. A family of zeolites with controlled pore size prepared using a top-down method. Nature Chem 5, 628–633 (2013). https://doi.org/10.1038/nchem.1662

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