Using ultrasound to improve the sequential post-synthesis modification method for making mesoporous Y zeolites

Abstract

Mesoporous Y zeolites were prepared by the sequential chemical dealumination (using chelating agents such as ethylenediaminetetraacetic acid, H₄EDTA, and citric acid aqueous solutions) and alkaline desilication (using sodium hydroxide, NaOH, aqueous solutions) treatments. Specifically, the ultrasound-assisted alkaline treatment (i.e., ultrasonic treatment) was proposed as the alternative to conventional alkaline treatments which are performed under hydrothermal conditions. In comparison with the hydrothermal alkaline treatment, the ultrasonic treatment showed the comparatively enhanced efficiency (with the reduced treatment time, i.e., 5 min vs. 30 min, all with 0.2 mol·L⁻¹ NaOH at 65°C) in treating the dealuminated Y zeolites for creating mesoporosity. For example, after the treatment of a dealuminated zeolite Y (using 0.1 mol·L⁻¹ H₄EDTA at 100°C for 6 h), the ultrasonic treatment produced the mesoporous zeolite Y with the specific external surface area (S_external) of 160 m²·g⁻¹ and mesopore volume (V_meso) of 0.22 cm³·g⁻¹, being slightly higher than that by the conventional method (i.e., S_external = 128 m²·g⁻¹ and V_meso = 0.19 cm³·g⁻¹). The acidic property and catalytic activity (in catalytic cracking of n-octane) of mesoporous Y zeolites obtained by the two methods were comparable. The ultrasonic desilication treatment was found to be generic, also being effective to treat the dealuminated Y zeolites by citric acid. Additionally, the first step of chemical dealumination treatment was crucial to enable the effective creation of mesopores in the parent Y zeolite (with a silicon-to-aluminium ratio, Si/Al= 2.6) regardless of the subsequent alkaline desilication treatment (i.e., ultrasonic or hydrothermal). Therefore, appropriate selection of the condition of the chemical dealumination treatment based on the property of parent zeolites, such as Si/Al ratio and crystallinity, is important for making mesoporous zeolites effectively.

Graphical abstract

Keywords

zeolite Y / mesoporous zeolite / post-synthesis treatment / ultrasound / chemical dealumination treatment / alkaline desilication treatment

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Acknowledgements

Yilai Jiao thanks the China Scholarship Council for his academic visiting fellowship in the UK (File No. 201604910181). Na Wang thanks the National Natural Science Foundation of China (Grant No. 51973124) for supporting her research.

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