The isotopic substitution in chemistry is characterized by two main effects, i.e., the kinetic isotope effect (KIE), associated with differences in the reaction rates, and the geometric isotope effect (GIE) related to crystallographic features. In this work, considering the difference in the weight of deuterium (D) compared to the weight of hydrogen (H), we use the isotopic substitution to investigate the crystallisation mechanism of template-free nanosized faujasite (FAU) type zeolite in colloidal precursors. Тhe basic hydrothermal synthesis solvent - water (H2O), is substituted with heavy water (D2O), aiming to understand the isotopic influence and the effect of H-bond networks on the zeolite crystallisation. The crystallinity, viscosity, conductivity, chemical composition, morphology and local order of the FAU zeolites synthesized in both hydrated (H) and deuterated (D) medium are evaluated with X-ray diffraction, TEM microscopy, EDX and ICP analysis, FT-IR and solid-state NMR spectroscopy. The structural directing agent - Na+, exhibits a lower mobility in the deuterated medium, because of a characteristic higher viscosity compared to hydrated medium. This leads to a slower nucleation and crystallisation in the initial stages of hydrothermal treatment in the colloidal suspensions but also to a significant difference in the Al distribution.
The influence of deuterium on sodium mobility and viscosity of colloidal precursor suspensions yielding template-free nanosized zeolites
Dalena, Francesco;Mintova, Svetlana
2023-01-01
Abstract
The isotopic substitution in chemistry is characterized by two main effects, i.e., the kinetic isotope effect (KIE), associated with differences in the reaction rates, and the geometric isotope effect (GIE) related to crystallographic features. In this work, considering the difference in the weight of deuterium (D) compared to the weight of hydrogen (H), we use the isotopic substitution to investigate the crystallisation mechanism of template-free nanosized faujasite (FAU) type zeolite in colloidal precursors. Тhe basic hydrothermal synthesis solvent - water (H2O), is substituted with heavy water (D2O), aiming to understand the isotopic influence and the effect of H-bond networks on the zeolite crystallisation. The crystallinity, viscosity, conductivity, chemical composition, morphology and local order of the FAU zeolites synthesized in both hydrated (H) and deuterated (D) medium are evaluated with X-ray diffraction, TEM microscopy, EDX and ICP analysis, FT-IR and solid-state NMR spectroscopy. The structural directing agent - Na+, exhibits a lower mobility in the deuterated medium, because of a characteristic higher viscosity compared to hydrated medium. This leads to a slower nucleation and crystallisation in the initial stages of hydrothermal treatment in the colloidal suspensions but also to a significant difference in the Al distribution.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.
