Abstract
Hierarchical beta zeolites obtained in the concentrated reaction mixtures (H2O/Si = 2.5) and micromesoporous materials synthesized using a dual-template approach from a zeolite beta precursor were rigorously characterized and tested in a sustainable and environmentally friendly process of α-pinene oxide isomerization. The highest yield of trans-carveol (42%) with chemopreventive activity of mammary carcinogenesis was achieved over low crystalline micromesoporous materials characterized by well-developed mesoporosity, an increased fraction of weak-to-medium Brønsted acid sites and low Brønsted and Lewis acid sites (BAS/LAS) ratio. In turn, highly crystalline hierarchical beta zeolites with a lower mesopore volume and the mesopore surface area, stronger Brønsted acidity, and a higher BAS/LAS ratio favored the formation of campholenic aldehyde (31% yield). The mechanism of the desired product and byproducts formation was discussed and its feasibility was confirmed by kinetic modeling.
| Original language | English |
|---|---|
| Pages (from-to) | 6642-6656 |
| Number of pages | 15 |
| Journal | ACS Sustainable Chemistry and Engineering |
| Volume | 10 |
| Issue number | 20 |
| DOIs | |
| Publication status | Published - 23 May 2022 |
| MoE publication type | A1 Journal article-refereed |
Funding
R.B. and N.S. acknowledge the support of the National Research Foundation of Ukraine to the Project “New effective zeolite catalysts for environmentally friendly processes of the conversion of renewable raw materials into valuable organic compounds” (Project Number 2020.02/0335). N.S. also acknowledges the support of the Verkhovna Rada of Ukraine to a personal scholarship for young scientists - doctors of sciences for 2021. The authors express their gratitude to Valentina Tsyrina (L.V. Pisarzhevsky Institute of Physical Chemistry) for NH-TPD. 3
Keywords
- Campholenic aldehyde
- Hierarchical beta zeolites
- Kinetic modeling
- trans-Carveol
- α-Pinene oxide isomerization