Zeolites have been well known for decades as catalytic materials and adsorbents and are traditionally prepared using the bottom-up synthesis method. Although it was productive for more than 250 zeolite frameworks, the conventional solvothermal synthesis approach provided limited control over the structural characteristics of the formed materials. In turn, the discovery and development of the Assembly-Disassembly-Organization-Reassembly (ADOR) strategy for the regioselective manipulation of germanosilicates enabled the synthesis of previously unattainable zeolites with predefined structures. To date, the family tree of ADOR materials has included the topological branches of UTL, UOV, IWW, *CTH, and IWV zeolites. Herein, we report on the expansion of ADOR zeolites with a new branch related to the IWR topology, which is yet unattainable experimentally but theoretically predicted as highly promising adsorbents for CO2 separation applications. The optimization of not only the chemical composition but also the dimensions of the crystalline domain in the parent IWR zeolite in the Assembly step was found to be the key to the success of its ADOR transformation into previously unknown IPC-17 zeolite with an intersecting 12 × 8 × 8-ring pore system. The structure of the as-prepared IPC-17 zeolite was verified by a combination of microscopic and diffraction techniques, while the results on the epichlorohydrin ring-opening with alcohols of variable sizes proved the molecular sieving ability of IPC-17 with potential application in heterogeneous catalysis. The proposed synthesis strategy may facilitate the discovery of zeolite materials that are difficult or yet impossible to achieve using a traditional bottom-up synthesis approach.

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Zeolites are key materials in both basic research and industrial applications. However, their synthesis is neither diverse nor applicable to labile frameworks because classical procedures require harsh hydrothermal conditions, whereas post-synthesis methods are limited to a few suitable parent materials. Remaining frameworks can fail due to amorphization, dissolution, and other decomposition processes. Nevertheless, stopping degradation at intermediate structures could yield new zeolites. Here, by optimizing the design and synthesis parameters of the parent zeolite IWV, we "caught" a new, highly crystalline, and siliceous zeolite during its degradation. IWV seed-assisted crystallization followed by gentle transformation into the water-alcohol system yielded the highly crystalline daughter zeolite IPC-20, whose structure was solved by precession-assisted three-dimensional electron diffraction. Without additional requirements, as in conventional (direct or post-synthesis) strategies, our approach may be applied to any chemically labile material with a staged structure.

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Zeolites are a class of microporous materials with tremendous value for large scale industrial applications such as catalysis, ion exchange, or gas separation. In addition to naturally ocurring variants, zeolites are made synthetically using hydrothermal synthesis, requiring temperatures beyond 100 °C and long reaction times up to weeks. Furthermore, specific applications may require more sophisticated synthesis conditions, expensive reagents, or post-synthetic modifications. Some of these issues can be tackled by using the reemerged technique of mechanochemistry. In 2014, Majano et al. reviewed the space and outlined several possibilities for the usage of mechanical forces in zeolite chemistry. Since then the field has seen many more publications employing mechanochemical methodology to further and improve the synthesis and properties of zeolite materials. The usage ranges from the activation of raw materials, rendering the synthesis of the widely used catalysts much more economical in terms of duration, atom efficiency, and production of waste, to post-synthetic modification of the materials leading to improved properties for target aplications. We present a short review of the advances that have been reported recently, highlight promising work and important studies, and give a perspective of potential future endeavours.

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The assembly-disassembly-organisation-reassembly (ADOR) process has led to the discovery of numerous zeolite structures, albeit limited to materials with decreased pore size in relation to the parent germanosilicate zeolite. This limitation stems from the rapid decrease in d-spacing upon hydrolysis (disassembly). Nevertheless, we have artificially increased the d-spacing of layered IPC-1P by intercalating organic species. Furthermore, we have reconstructed double four rings (D4R) between layers, thus transforming IPC-1P back into the parent UTL zeolite. This reconstruction has provided not only germanosilicate but also a new, high-silica UTL zeolite (Si/Ge = 481). Therefore, our "reverse ADOR" opens up new synthetic routes towards promising extra-large-pore zeolite-based materials with new chemical compositions.

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The ADOR (Assembly-Disassembly-Organisation-Reassembly) process for zeolites has been shown to produce a number of previously unknown frameworks inaccessible through conventional synthesis methods. Here, we present successful mechanochemically assisted hydrolysis of germanosilicate zeolite UTL leading to ADOR products under mild conditions, low amounts of solvent and in short reaction times. The expansion of zeolite synthesis into the realm of mechanochemistry opens up feasible pathways regarding the production of these materials, especially for industrial purposes, as well as an exciting application for economical enrichment of materials with the low natural abundance NMR-active isotope of oxygen, 17O. The results from mechanochemically assisted hydrolysis differ from those seen in the traditional ADOR approach: differences that can be attributed to a change in solvent availability.

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