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Synthesis of ‘unfeasible’ zeolites

Abstract

Zeolites are porous aluminosilicate materials that have found applications in many different technologies. However, although simulations suggest that there are millions of possible zeolite topologies, only a little over 200 zeolite frameworks of all compositions are currently known, of which about 50 are pure silica materials. This is known as the zeolite conundrum—why have so few of all the possible structures been made? Several criteria have been formulated to explain why most zeolites are unfeasible synthesis targets. Here we demonstrate the synthesis of two such ‘unfeasible’ zeolites, IPC-9 and IPC-10, through the assembly–disassembly–organization–reassembly mechanism. These new high-silica zeolites have rare characteristics, such as windows that comprise odd-membered rings. Their synthesis opens up the possibility of preparing other zeolites that have not been accessible by traditional solvothermal synthetic methods. We envisage that these findings may lead to a step change in the number and types of zeolites available for future applications.

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Figure 1: Synthesis of ‘unfeasible’ zeolites.
Figure 2: The role of choline cations in organizing IPC-1P layers.
Figure 3: Structures of IPC-9 and IPC-10.
Figure 4: The energetics of IPC-9 and IPC-10.

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Acknowledgements

R.E.M. thanks the Royal Society and the Engineering and Physical Sciences Research Council (Grants EP/L014475/1, EP/K025112/1 and EP/K005499/1) for funding work in this area. J.Č. and P.N. acknowledge the Czech Science Foundation for the project of the Centre of Excellence (P106/12/G015) and the European Union Seventh Framework Programme (FP7/ 2007–2013) under Grant Agreement No. 604307. The research leading to these results has received funding from the European Union Seventh Framework Programme under Grant Agreement No. 312483—ESTEEM2 (Integrated Infrastructure Initiative–I3). W.J.R. thanks his current institution, Jagiellonian University in Krakow, Faculty of Chemistry. We thank W. Zhou and F. Yu for their expertise in TEM and D. Dawson for help with NMR spectroscopy.

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M.M., P.E. and W.J.R. completed the synthesis aspects of the work and P.S.W. coordinated the characterization of the prepared materials. M.P. completed the computational modelling under the supervision of P.N. M.N. and A.M. completed the aberration-corrected electron microscopy studies. J.Č. and R.E.M. coordinated the project as a whole and wrote the paper.

Corresponding authors

Correspondence to Jiří Čejka or Russell E. Morris.

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The authors declare no competing financial interests.

Supplementary information

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Supplementary Movie 1 (MOV 6549 kb)

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Supplementary Movie 2 (MOV 9144 kb)

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Supplementary Movie 3 (MOV 12673 kb)

Supplementary information

Crystallographic data for compound IPC9 (CIF 22 kb)

Supplementary information

Crystallographic data for compound IPC10 (CIF 12 kb)

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Mazur, M., Wheatley, P., Navarro, M. et al. Synthesis of ‘unfeasible’ zeolites. Nature Chem 8, 58–62 (2016). https://doi.org/10.1038/nchem.2374

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