Scale up for the win! Hierarchically structured zeolites are prepared on a large scale by desilication followed by forming into mm‐sized bodies. Extrapolation of the superior catalytic properties is proven by the remarkable similarity between pilot and laboratory scale results. The binder and the shaping process does not alter the enhanced porous properties of the mesoporous zeolite. These results unlock the door towards the study of further key steps in the design of mesoporous zeolite catalysts for large scale applications.

Summary: A new approach for the production of macroporous polymer materials is presented. Cross‐linked polystyrene particles are first produced by emulsion polymerization. This latex is then swollen by a further addition of monomer and it is successively destabilized, by addition of salt, in such a way that a controlled aggregation is achieved. The system is left aggregating until a gel is obtained. Although polymer gels have their own consistency, latex particles are kept together by weak interactions only, e.g. Van der Waals' forces. In order to impart enough mechanical resistance to the material, the residual monomer is polymerized, thus bridging the polymer particles with cross‐linked polymer. Accordingly, the process has been named “reactive gelation”. In this work, it is shown how it is possible to obtain an accurate control upon the pore structure of the material by properly tuning each step of the process. An application of the obtained material as stationary phase in a separation carried out by high performance liquid chromatography is presented.SEM picture of the macroporous material obtained by reactive gelation.magnified imageSEM picture of the macroporous material obtained by reactive gelation.

Engineering levels of porosity in hierarchical zeolites is a vibrant area of research with remarkable application potential. To gain practical relevance, the superior properties observed for the as‐synthesized powders have to be preserved when they are shaped into suitable technical geometries. Herein, mechanically stable millimeter‐sized bodies are prepared by granulation of mesoporous ZSM‐5 zeolite powders using an attapulgite clay binder. Alkaline treatment of conventional zeolite granules is demonstrated to be unsuitable for this purpose. Multiple techniques are applied to characterize mesoporous zeolite granules with respect to their conventional zeolite counterparts, thus establishing the impact of binder inclusion and granulation on their respective properties. The intrinsic structure and acidity of the zeolite are retained post‐structuring. Gas adsorption and mercury porosimetry confirm the presence of interconnected micro‐, meso‐, and macropores. A wide range of imaging techniques permits visualization of the particle properties, phase distribution, and consequent origins of the distinct levels of porosity within the zeolite granules. The superior adsorption properties of the hierarchical ZSM‐5 zeolite granules are demonstrated using cyclohexane, toluene, and isopropyl alcohol as probe molecules.

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