Liquid-phase oxidation of betulin over supported Ag NPs catalysts: Kinetic regularities, catalyst deactivation and reactivation

A. Grigoreva; E. Kolobova; E. Pakrieva; P. Mäki-Arvela; S. Kuznetsova; S. A.C. Carabineiro; N. Bogdanchikova; A. Pestryakov; D. Yu Murzin

doi:10.1016/j.mcat.2022.112461

Liquid-phase oxidation of betulin over supported Ag NPs catalysts: Kinetic regularities, catalyst deactivation and reactivation

A. Grigoreva, E. Kolobova^*, E. Pakrieva, P. Mäki-Arvela, S. Kuznetsova, S. A.C. Carabineiro, N. Bogdanchikova, A. Pestryakov, D. Yu Murzin

^*Corresponding author for this work

Laboratory of Industrial Chemistry and Reaction Engineering

Research output: Contribution to journal › Article › Scientific › peer-review

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Abstract

Betulin, being a pentacyclic triterpene alcohol and an extractive from birch bark, along with its oxo-derivatives, has a broad range of physiological properties of interest for synthesis of pharmaceuticals. Instead of oxidizing betulin with strong and toxic oxidizing agents the present study shows a possibility of using liquid-phase oxidation of betulin with air over supported Ag NPs catalysts as an alternative method for synthesis of its oxo-derivatives. Based on catalytic studies, high resolution transmission electron microscopy, X-ray photoelectron spectroscopy and ultraviolet-visible diffuse reflectance spectroscopy, the evolution of the surface of nanosilver catalysts during the catalysis was demonstrated, as well as under the impact of reactant gas composition. The kinetic regularities and causes of deactivation of supported Ag NPs catalysts were revealed. An approach to the regeneration of silver catalysts was proposed. Kinetic analysis with numerical data fitting was performed resulting in an adequate description of the concentration dependencies.

Original language	English
Article number	112461
Number of pages	15
Journal	Molecular Catalysis
Volume	528
DOIs	https://doi.org/10.1016/j.mcat.2022.112461
Publication status	Published - Aug 2022
MoE publication type	A1 Journal article-refereed

Funding

The research is funded from Ministry of Education and Science of the Russian Federation Program No. 075–03–2021–287/6 (Russia). XPS measurements were carried out at the Central laboratories of Tomsk Polytechnic University (Analytical Center). HRTEM was carried out at the Innovation centre for Nanomaterials and Nanotechnologies of Tomsk Polytechnic University. The ICP-OES analysis was carried out using the core facilities of “Physics and Chemical methods of analysis” of Tomsk Polytechnic University. Fundação para a Ciência e a Tecnologia for Scientific Employment Stimulus Institutional Call (CEECINST/00102/2018), UIDB/50006/2020 and UIDP/50006/2020 (LAQV), UIDB/00100/2020 and UIDP/00100/2020 (Centro de Química Estrutural).

Keywords

Betulin oxidation
Deactivation
Kinetics
Reactivation
Silver catalyst

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10.1016/j.mcat.2022.112461

1-s2.0-S2468823122003479-mainFinal published version, 4.12 MBLicence: CC BY

https://urn.fi/URN:NBN:fi-fe2022112266393

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Grigoreva, A., Kolobova, E., Pakrieva, E., Mäki-Arvela, P., Kuznetsova, S., Carabineiro, S. A. C., Bogdanchikova, N., Pestryakov, A., & Murzin, D. Y. (2022). Liquid-phase oxidation of betulin over supported Ag NPs catalysts: Kinetic regularities, catalyst deactivation and reactivation. Molecular Catalysis, 528, Article 112461. https://doi.org/10.1016/j.mcat.2022.112461

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title = "Liquid-phase oxidation of betulin over supported Ag NPs catalysts: Kinetic regularities, catalyst deactivation and reactivation",

abstract = "Betulin, being a pentacyclic triterpene alcohol and an extractive from birch bark, along with its oxo-derivatives, has a broad range of physiological properties of interest for synthesis of pharmaceuticals. Instead of oxidizing betulin with strong and toxic oxidizing agents the present study shows a possibility of using liquid-phase oxidation of betulin with air over supported Ag NPs catalysts as an alternative method for synthesis of its oxo-derivatives. Based on catalytic studies, high resolution transmission electron microscopy, X-ray photoelectron spectroscopy and ultraviolet-visible diffuse reflectance spectroscopy, the evolution of the surface of nanosilver catalysts during the catalysis was demonstrated, as well as under the impact of reactant gas composition. The kinetic regularities and causes of deactivation of supported Ag NPs catalysts were revealed. An approach to the regeneration of silver catalysts was proposed. Kinetic analysis with numerical data fitting was performed resulting in an adequate description of the concentration dependencies.",

keywords = "Betulin oxidation, Deactivation, Kinetics, Reactivation, Silver catalyst",

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year = "2022",

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doi = "10.1016/j.mcat.2022.112461",

language = "English",

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T2 - Kinetic regularities, catalyst deactivation and reactivation

AU - Grigoreva, A.

AU - Kolobova, E.

AU - Pakrieva, E.

AU - Mäki-Arvela, P.

AU - Kuznetsova, S.

AU - Carabineiro, S. A.C.

AU - Bogdanchikova, N.

AU - Pestryakov, A.

AU - Murzin, D. Yu

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N2 - Betulin, being a pentacyclic triterpene alcohol and an extractive from birch bark, along with its oxo-derivatives, has a broad range of physiological properties of interest for synthesis of pharmaceuticals. Instead of oxidizing betulin with strong and toxic oxidizing agents the present study shows a possibility of using liquid-phase oxidation of betulin with air over supported Ag NPs catalysts as an alternative method for synthesis of its oxo-derivatives. Based on catalytic studies, high resolution transmission electron microscopy, X-ray photoelectron spectroscopy and ultraviolet-visible diffuse reflectance spectroscopy, the evolution of the surface of nanosilver catalysts during the catalysis was demonstrated, as well as under the impact of reactant gas composition. The kinetic regularities and causes of deactivation of supported Ag NPs catalysts were revealed. An approach to the regeneration of silver catalysts was proposed. Kinetic analysis with numerical data fitting was performed resulting in an adequate description of the concentration dependencies.

AB - Betulin, being a pentacyclic triterpene alcohol and an extractive from birch bark, along with its oxo-derivatives, has a broad range of physiological properties of interest for synthesis of pharmaceuticals. Instead of oxidizing betulin with strong and toxic oxidizing agents the present study shows a possibility of using liquid-phase oxidation of betulin with air over supported Ag NPs catalysts as an alternative method for synthesis of its oxo-derivatives. Based on catalytic studies, high resolution transmission electron microscopy, X-ray photoelectron spectroscopy and ultraviolet-visible diffuse reflectance spectroscopy, the evolution of the surface of nanosilver catalysts during the catalysis was demonstrated, as well as under the impact of reactant gas composition. The kinetic regularities and causes of deactivation of supported Ag NPs catalysts were revealed. An approach to the regeneration of silver catalysts was proposed. Kinetic analysis with numerical data fitting was performed resulting in an adequate description of the concentration dependencies.

KW - Betulin oxidation

KW - Deactivation

KW - Kinetics

KW - Reactivation

KW - Silver catalyst

UR - https://www.scopus.com/pages/publications/85133449121

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DO - 10.1016/j.mcat.2022.112461

M3 - Article

AN - SCOPUS:85133449121

SN - 2468-8231

VL - 528

JO - Molecular Catalysis

JF - Molecular Catalysis

M1 - 112461

ER -

Liquid-phase oxidation of betulin over supported Ag NPs catalysts: Kinetic regularities, catalyst deactivation and reactivation

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