Hierarchical Beta Zeolites As Catalysts in α-Pinene Oxide Isomerization

Roman Barakov; Nataliya Shcherban; Päivi Mäki-Arvela; Pavel Yaremov; Igor Bezverkhyy; Johan Wärnå; Dmitry Yu Murzin

doi:10.1021/acssuschemeng.2c00441

Hierarchical Beta Zeolites As Catalysts in α-Pinene Oxide Isomerization

Roman Barakov
, Nataliya Shcherban
, Päivi Mäki-Arvela
, Pavel Yaremov
, Igor Bezverkhyy
, Johan Wärnå
, Dmitry Yu Murzin^*

^*Korresponderande författare för detta arbete

Teknisk kemi och reaktionsteknik

Forskningsoutput: Tidskriftsbidrag › Artikel › Vetenskaplig › Peer review

36 Citeringar (Scopus)

173 Nedladdningar (Pure)

Sammanfattning

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.

Originalspråk	Engelska
Sidor (från-till)	6642-6656
Antal sidor	15
Tidskrift	ACS Sustainable Chemistry and Engineering
Volym	10
Nummer	20
DOI	https://doi.org/10.1021/acssuschemeng.2c00441
Status	Publicerad - 23 maj 2022
MoE-publikationstyp	A1 Tidskriftsartikel-refererad

Finansiering

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

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10.1021/acssuschemeng.2c00441

acssuschemeng.2c00441Slutlig publicerad version, 9,4 MBLicens: CC BY

https://urn.fi/URN:NBN:fi-fe2023060151026

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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 Br{\o}nsted acid sites and low Br{\o}nsted 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 Br{\o}nsted 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.",

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AU - Mäki-Arvela, Päivi

AU - Yaremov, Pavel

AU - Bezverkhyy, Igor

AU - Wärnå, Johan

AU - Murzin, Dmitry Yu

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AB - 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.

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Hierarchical Beta Zeolites As Catalysts in α-Pinene Oxide Isomerization

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