Methodological aspects of producing aluminosilicalites with typological structure of HZSM-5. Rational design and catalytic properties
摘要
In this work, the analysis and generalization of data on the elemental, phase and surface composition, crystal structure and microstructure of MFI-type HZSM-5 with Si/Al = 12, 25, 40, 300 were presented. Relationships between the composition of zeolite in HZSM-5 samples with different Si/Al and pore volume, specific surface, and framework voids area were established. Data obtained by electron microscopy and energy dispersive X-ray microanalysis explained the discrepancy between HZSM-5 real composition and the initial (as synthesized) one. Samples with the maximum content of Brønsted (HZSM-5 with Si/Al = 25) and Lewis (HZSM-5 with Si/Al = 12) acid sites responsible for the catalytic activity were identified using diffuse reflectance Fourier transform infrared spectroscopy. N2O decomposition reaction rate was found to decrease in the row HZSM-5(25) > HZSM-5(12) > HZSM-5(40) > HZSM-5(40)C > > HZSM-5(300). The high N2O decomposition rate demonstrated by HZSM-5(25) makes it promising catalyst. The second phase of iron oxides, found in all studied HZSM-5 as an impurity of the initial components, and the presence of faceted particles {001} oriented in HZSM-5(25) were shown to contribute to its maximum catalytic activity in N2O decomposition. The applied methodology for studying aluminosilicalites with different silicon to aluminum ratio and the revealed correlations can provide a fundamental perspective in studying other zeolites.