The assembly-disassembly-organization-reassembly (ADOR) mechanism is a recent method for preparing inorganic framework materials and, in particular, zeolites. This flexible approach has enabled the synthesis of isoreticular families of zeolites with unprecedented continuous control over porosity, and the design and preparation of materials that would have been difficult-or even impossible-to obtain using traditional hydrothermal techniques. Applying the ADOR process to a parent zeolite with the UTL framework topology, for example, has led to six previously unknown zeolites (named IPC-n, where n = 2, 4, 6, 7, 9 and 10). To realize the full potential of the ADOR method, however, a further understanding of the complex mechanism at play is needed. Here, we probe the disassembly, organization and reassembly steps of the ADOR process through a combination of in situ solid-state NMR spectroscopy and powder X-ray diffraction experiments. We further use the insight gained to explain the formation of the unusual structure of zeolite IPC-6.

Department of Chemistry University of Oslo Sem Sælandsvei 26 0371 Oslo Norway

Department of Physical and Macromolecular Chemistry Faculty of Sciences Charles University Prague Hlavova 8 128 43 Prague 2 Czech Republic

EaStCHEM School of Chemistry University of St Andrews St Andrews KY16 9ST UK

ISIS Facility Rutherford Appleton Laboratory Harwell Oxford Didcot Oxfordshire OX11 0QX UK

J Heyrovský Institute of Physical Chemistry Academy of Sciences of the Czech Republic v v i Dolejškova 3 182 23 Prague 8 Czech Republic

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