This study made use of a recently developed combination of advanced methods to reveal the atomic structure of a disordered nanocrystalline zeolite using exit wave reconstruction, automated diffraction tomography, disorder modelling and diffraction pattern simulation. By applying these methods, it was possible to determine the so far unknown structures of the hydrous layer silicate RUB-6 and the related zeolite-like material RUB-5. The structures of RUB-5 and RUB-6 contain the same dense layer-like building units (LLBUs). In the case of RUB-5, these building units are interconnected via additional SiO4/2 tetrahedra, giving rise to a framework structure with a 2D pore system consisting of intersecting 8-ring channels. In contrast, RUB-6 contains these LLBUs as separate silicate layers terminated by silanol/sil-oxy groups. Both RUB-6 and RUB-5 show stacking disorder with intergrowths of different polymorphs. The unique structure of RUB-6, together with the possibility for an interlayer expansion reaction to form RUB-5, make it a promising candidate for interlayer expansion with various metal sources to include catalytically active reaction centres.

Chair for Crystallography and Structural Physics Friedrich Alexander Universität Erlangen Nürnberg Staudtstrasse 3 Erlangen D 91058 Germany

Department of Materials and Geoscience Technische Universität Darmstadt Petersenstrasse 23 Darmstadt D 64287 Germany

Department of Structure Analysis of the Institute of Physics Czech Academy of Sciences Cukrovarnická 10 112 Prague 162 00 Czech Republic

Departure of Geology Mineralogy and Geophysics Ruhr University Bochum Universitätsstrasse 150 Bochum D 44801 Germany

Institute of Inorganic Chemistry and Analytical Chemistry Johannes Gutenberg University Duesbergweg 10 14 Mainz D 55128 Germany

LENS MIND IN2UB Engineer department Electronics section Universitat de Barcelona Martí i Franquès 1 Barcelona 08028 Spain

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