The paramount challenge of current chemical technology, including catalysis, is meeting the ecological sustainability requirements. The feasible production of zeolites is crucial because they constitute the principal group of heterogeneous catalysts. However, current zeolite manufacturing via hydrothermal synthesis is connected with considerable consumption of water resources, generation of wastewater, and significant equipment costs. Solvent-free strategies have attracted great attention as high-yielding methods for sustainable synthesis, particularly beneficial in terms of water consumption minimization and an outstanding increase in production due to the efficient use of synthesis space capacity. So far, the solvent-free preparation of numerous zeolite materials has been performed with the preceding grinding of reagents in a mortar. The proposed article describes recent advances in the application of automatized milling instead of manual work. Pretreatment automatization makes the entire process well-controlled, less sensitive to human factors, and is significantly more relevant to industrial scale-up. Moreover, the automatized milling activation unlocks opportunities for solvent-free synthesis from a broader range of common reagents, where the manual treatment is not efficient. Possibilities and limitations of the milling methods are discussed on the basis of a comprehensive analysis of parameter optimization, activation mechanisms, and applicability of common reagents used for zeolite production.

The effect of particle size and support on the catalytic performance of supported subnanometer copper clusters was investigated in the oxidative dehydrogenation of cyclohexene. From among the investigated seven size-selected subnanometer copper particles between a single atom and clusters containing 2 to 7 atoms, the highest activity was observed for the titania-supported copper tetramer with 100 % selectivity towards benzene production, and being about an order of magnitude more active than all the other investigated cluster sizes on the same support, but also the same tetramer on the other supports Al₂O₃, SiO₂, and SnO₂. In addition to the profound effect of clusters size on activity and with Cu₄ outstanding from the studied series, Cu₄ clusters supported on SiO₂ provide an example of tuning selectivity through support effects when this particular catalyst produces also cyclohexadiene with about 30% selectivity. Titania-supported Cu₅ and Cu₇ clusters supported on TiO₂ produce a high fraction of cyclohexadiene in contrary to their neighbors, while Cu₄ and Cu₆ produce solely benzene without any combustion, thus representing odd-even oscillation of selectivity with the number of atoms in the cluster.

Beta zeolites with Si/Al around 14 were prepared using three new alkali-free synthesis methods based on the application of amorphous aluminosilicate precursor and calcined in ammonia or air. All samples exhibit structural and textural properties of standard beta zeolite. Comprehensive study by ²⁷Al and ²⁹Si MAS NMR, together with FTIR adsorption of d₃-acetonitrile and pyridine were used to characterize the influence of both the synthesis and calcination procedure on the framework Al atoms and related Brønsted and Lewis acid sites. While calcination in ammonia preserves all framework Al atoms, calcination in air results in 15% release of framework Al, but without restrictions of the accessibility of the beta zeolite channel system for bulky pyridine molecules. Terminal (SiO)₃AlOH groups present in the hydrated zeolites were suggested as a precursor of framework Al-Lewis sites. Surprisingly, the mild dealumination of the air-calcined zeolites result in an increase of the concentration of Brønsted acid sites and a decrease of the total concentration of Lewis sites with the formation of the extra-framework ones.