The simplified one‐step hydrothermal synthesis, in which SiO2 is directly reacted with aqueous NaOH in the presence or absence of tetrapropylammonium bromide (TPABr) and tetrabutylammonium bromide (TBABr) as the template compound, was investigated. The reaction in the absence of the template compounds leads to the production of pure magadiite, whereas pure Si‐ZSM‐5 is produced by the reaction in the presence of TPABr. On the other hand, crystalline magadiite/Si‐ZSM‐11 composites are synthesized by the reaction in the presence of TBABr. Furthermore, for the composites, the particle sizes of the magadiite and Si‐ZSM‐11 may be influenced by the TBABr concentrations. It was also found that the compositions of magadiite and Si‐ZSM‐11 in the composites can be controlled by regulating the NaOH concentrations.
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