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Zeolite mordenite (MOR) is one of the most studied zeolites for the stepwise direct conversion of methane to methanol, but it also can exist in two forms: large port and small port. Here we report that the synthesis and selection of the parent mordenite is critical for optimizing productivity, and that large-port mordenite outperforms small-port mordenite for the stepwise conversion of methane to methanol., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

A family of Al-rich ZSM-5 zeolites with Si/Al = 8 ± 0.5 was prepared according to a biomass-mediated supramolecular approach. A combination of advanced characterisation techniques and periodic density functional theory (DFT) calculations unraveled the purity and stability of un-expected Al-enriched ZSM-5 structures, hence allowing to cross the frontier of Si/Al lower limit. In addition, these Al-rich ZSM-5 zeolites demonstrated high catalytic activity in n -hexane cracking and methanol conversion into hydrocarbons, being in line with the presence of numerous Brønsted acid sites.

Advances in materials synthesis bring about many opportunities for technological applications, but are often accompanied by unprecedented complexity. This is clearly illustrated by the case of hierarchically organized zeolite catalysts, a class of crystalline microporous solids that has been revolutionized by the engineering of multilevel pore architectures, which combine unique chemical functionality with efficient molecular transport. Three key attributes, the crystal, the pore and the active site structure, can be expected to dominate the design process. This review examines the adequacy of the palette of techniques applied to characterize these distinguishing features and their catalytic impact.