Catalytic oxidative transformation of betulin to its valuable oxo-derivatives over gold supported catalysts: Effect of support nature

E. Kolobova; P. Mäki-Arvela; A. Grigoreva; E. Pakrieva; S.A.C. Carabineiro; J. Peltonen; S. Kazantsev; N. Bogdanchikova; A. Pestryakov; Dmitry Murzin

doi:10.1016/j.cattod.2020.07.051

Catalytic oxidative transformation of betulin to its valuable oxo-derivatives over gold supported catalysts: Effect of support nature

E. Kolobova^*
, P. Mäki-Arvela
, A. Grigoreva
, E. Pakrieva
, S.A.C. Carabineiro
, J. Peltonen
, S. Kazantsev
, N. Bogdanchikova
, A. Pestryakov
, Dmitry Murzin

^*Corresponding author for this work

Laboratory of Industrial Chemistry and Reaction Engineering

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

8 Citations (Scopus)

108 Downloads (Pure)

Abstract

Liquid-phase oxidation of betulin extracted from birch bark was studied over gold catalysts supported on a range of supports (hydrotalcite, ZrO₂, ZnO, MgO, CeO₂, La₂O₃, HMS and various alumina) with different morphology and properties. Gold catalysts as well as the corresponding supports were characterized by XRD, BET, ICP-OES, XPS and TEM. It was found that the nature of the support plays a decisive role in betulin oxidation over gold-based catalysts, expressed in the influence on the average size and distribution of gold nanoparticles and, thereby, on their catalytic performance (activity and selectivity) in betulin oxidation. Moreover, it was revealed that betulin oxidation catalyzed by gold is a structure sensitive reaction, requiring an optimal size of gold nanoparticles of ca. 3.3 nm. The most suitable support for gold was found to be alumina. Kinetic studies allowed determination of reaction orders and conditions favorable for selective formation of a particular oxo-derivative of betulin (betulone, betulinic and betulonic aldehydes, betulinic acid).

Original language	English
Pages (from-to)	95-110
Journal	Catalysis Today
Volume	367
DOIs	https://doi.org/10.1016/j.cattod.2020.07.051
Publication status	Published - 1 May 2021
MoE publication type	A1 Journal article-refereed

Funding

The research is funded from the Russian Science Foundation project No. 18-73-00019 and Tomsk Polytechnic University Competitiveness Enhancement Program , project VIU-ISHBMT-197/2020 (Russia). This work was partially supported by Fundação para a Ciência e a Tecnologia , Portugal (2020-2023 multiannual funding to Centro de Química Estrutural). Authors thank Dr. Carlos Sá (CEMUP) for the assistance with XPS analyses and Prof. Pedro Tavares (UTAD) for assistance with XRD analyses.

Keywords

Betulin oxidation
Gold catalyst
Structure sensitivity
Support nature

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10.1016/j.cattod.2020.07.051

Catalytic oxidative transformation of betulin to its valuable oxo-derivatives over gold supported catalystsAccepted author manuscript, 1.88 MBLicence: CC BY-NC-ND

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Kolobova, E., Mäki-Arvela, P., Grigoreva, A., Pakrieva, E., Carabineiro, S. A. C., Peltonen, J., Kazantsev, S., Bogdanchikova, N., Pestryakov, A., & Murzin, D. (2021). Catalytic oxidative transformation of betulin to its valuable oxo-derivatives over gold supported catalysts: Effect of support nature. Catalysis Today, 367, 95-110. https://doi.org/10.1016/j.cattod.2020.07.051

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title = "Catalytic oxidative transformation of betulin to its valuable oxo-derivatives over gold supported catalysts: Effect of support nature",

abstract = "Liquid-phase oxidation of betulin extracted from birch bark was studied over gold catalysts supported on a range of supports (hydrotalcite, ZrO2, ZnO, MgO, CeO2, La2O3, HMS and various alumina) with different morphology and properties. Gold catalysts as well as the corresponding supports were characterized by XRD, BET, ICP-OES, XPS and TEM. It was found that the nature of the support plays a decisive role in betulin oxidation over gold-based catalysts, expressed in the influence on the average size and distribution of gold nanoparticles and, thereby, on their catalytic performance (activity and selectivity) in betulin oxidation. Moreover, it was revealed that betulin oxidation catalyzed by gold is a structure sensitive reaction, requiring an optimal size of gold nanoparticles of ca. 3.3 nm. The most suitable support for gold was found to be alumina. Kinetic studies allowed determination of reaction orders and conditions favorable for selective formation of a particular oxo-derivative of betulin (betulone, betulinic and betulonic aldehydes, betulinic acid).",

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Kolobova, E, Mäki-Arvela, P, Grigoreva, A, Pakrieva, E, Carabineiro, SAC, Peltonen, J, Kazantsev, S, Bogdanchikova, N, Pestryakov, A & Murzin, D 2021, 'Catalytic oxidative transformation of betulin to its valuable oxo-derivatives over gold supported catalysts: Effect of support nature', Catalysis Today, vol. 367, pp. 95-110. https://doi.org/10.1016/j.cattod.2020.07.051

TY - JOUR

T1 - Catalytic oxidative transformation of betulin to its valuable oxo-derivatives over gold supported catalysts

T2 - Effect of support nature

AU - Kolobova, E.

AU - Mäki-Arvela, P.

AU - Grigoreva, A.

AU - Pakrieva, E.

AU - Carabineiro, S.A.C.

AU - Peltonen, J.

AU - Kazantsev, S.

AU - Bogdanchikova, N.

AU - Pestryakov, A.

AU - Murzin, Dmitry

N1 - Corrected proof 19.2.2021 /LN tk. post-print, 24 mån embargo, CC BY-NC-ND Har mailat Päivi Mäki-Arvela [10.11.2020 LN]

PY - 2021/5/1

Y1 - 2021/5/1

N2 - Liquid-phase oxidation of betulin extracted from birch bark was studied over gold catalysts supported on a range of supports (hydrotalcite, ZrO2, ZnO, MgO, CeO2, La2O3, HMS and various alumina) with different morphology and properties. Gold catalysts as well as the corresponding supports were characterized by XRD, BET, ICP-OES, XPS and TEM. It was found that the nature of the support plays a decisive role in betulin oxidation over gold-based catalysts, expressed in the influence on the average size and distribution of gold nanoparticles and, thereby, on their catalytic performance (activity and selectivity) in betulin oxidation. Moreover, it was revealed that betulin oxidation catalyzed by gold is a structure sensitive reaction, requiring an optimal size of gold nanoparticles of ca. 3.3 nm. The most suitable support for gold was found to be alumina. Kinetic studies allowed determination of reaction orders and conditions favorable for selective formation of a particular oxo-derivative of betulin (betulone, betulinic and betulonic aldehydes, betulinic acid).

AB - Liquid-phase oxidation of betulin extracted from birch bark was studied over gold catalysts supported on a range of supports (hydrotalcite, ZrO2, ZnO, MgO, CeO2, La2O3, HMS and various alumina) with different morphology and properties. Gold catalysts as well as the corresponding supports were characterized by XRD, BET, ICP-OES, XPS and TEM. It was found that the nature of the support plays a decisive role in betulin oxidation over gold-based catalysts, expressed in the influence on the average size and distribution of gold nanoparticles and, thereby, on their catalytic performance (activity and selectivity) in betulin oxidation. Moreover, it was revealed that betulin oxidation catalyzed by gold is a structure sensitive reaction, requiring an optimal size of gold nanoparticles of ca. 3.3 nm. The most suitable support for gold was found to be alumina. Kinetic studies allowed determination of reaction orders and conditions favorable for selective formation of a particular oxo-derivative of betulin (betulone, betulinic and betulonic aldehydes, betulinic acid).

KW - Betulin oxidation

KW - Gold catalyst

KW - Structure sensitivity

KW - Support nature

UR - https://www.scopus.com/pages/publications/85089740409

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DO - 10.1016/j.cattod.2020.07.051

M3 - Article

AN - SCOPUS:85089740409

SN - 0920-5861

VL - 367

SP - 95

EP - 110

JO - Catalysis Today

JF - Catalysis Today

ER -

Catalytic oxidative transformation of betulin to its valuable oxo-derivatives over gold supported catalysts: Effect of support nature

Abstract

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Keywords

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