2025 AIChE Annual Meeting

(7g) Fine-Tuning SSZ-39 Zeolite Properties for Catalytic Applications Via Ultrafast Mixed Interzeolite Conversion.

Authors

Gleb Ivanushkin, KU Leuven
Raquel Simancas, The University of Tokyo
Toru Wakihara, The University of Tokyo
Simon Kuhn, KU Leuven
SSZ-39 (AEI framework) zeolite is a promising catalyst candidate [1], however, its synthesis is time intensive and requires fine-tuned reactant compositions [2]. Interzeolite conversion (IZC), which uses crystalline Si and Al sources, offers an alternative approach to synthesize zeolites with optimal features: it provides a faster kinetic route to access zeolites synthesis within hours or even minutes [3].

A mixture of two commercial FAU zeolites (Si/Al=385, 15) is employed as source to achieve complete synthesis of pure AEI. Starting with Si/Al=25, AEI zeolite is synthesized in 30 min in a tubular reactor, using 2wt% milled seeds (synthesized in autoclave, 170 °C, 5 days), at 210 °C, obtaining Si/Al=11. The reactants molar ratio is (TMP+=tetramethylpyperidinium): 1SiO2:25-1Al:0.25TMP+:0.25Na+:0.5OH-:10.5H2O. It has been observed that only milled seeds can significantly accelerate the synthesis, whereas as-made seeds do not influence the kinetics.

In contrast to other IZC systems, this transformation does not proceed via any amorphous intermediate: XRD patterns show a simultaneous decrease in FAU peaks intensities and formation of AEI peaks. This results in a solid yield that never decreases below 30%, with a final value of 44%.

To unravel the intrinsic mechanism of the FAU-AEI transformation, operando IZC at 210 °C and 190 °C is analyzed via SAXS/WAXS, where the role of the milled seeds is also investigated. Moreover, the fast-synthesized AEI is tested for NH3-SCR, while the as-made seeds are tested for methanol-mediated CO2 conversion. Two different crystal sizes are obtained: 500 nm for the fast-synthesized and 3-4 μm for the autoclave-synthesized seeds, respectively, which play an important role in the different catalytic processes. The opportunity to control the Si/Al and the crystal size via mixed IZC and fast crystallization leads towards the synthesis of versatile zeolites which can be fine tuned to be applied in several catalytic processes.

[1]- 10.1021/acs.chemrev.7b00738.

[2]-10.1016/j.apcatb.2023.122395.

[3]-10.1039/d1ra02887a.