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Benzaldoxime to benzamide rearrangement catalysed by rhodium(III) hydroxocomplexes : The influence of polynuclear species. / Berdyugin, Semen; Volchek, Victoria; Asanova, Tatyana и др.

в: Applied Catalysis A: General, Том 587, 117242, 25.10.2019.

Результаты исследований: Научные публикации в периодических изданияхстатьяРецензирование

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Berdyugin S, Volchek V, Asanova T, Kolesov B, Gerasimov E, Filatov E и др. Benzaldoxime to benzamide rearrangement catalysed by rhodium(III) hydroxocomplexes: The influence of polynuclear species. Applied Catalysis A: General. 2019 окт. 25;587:117242. doi: 10.1016/j.apcata.2019.117242

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Berdyugin, Semen ; Volchek, Victoria ; Asanova, Tatyana и др. / Benzaldoxime to benzamide rearrangement catalysed by rhodium(III) hydroxocomplexes : The influence of polynuclear species. в: Applied Catalysis A: General. 2019 ; Том 587.

BibTeX

@article{38ee8ba3061d43db80f8a99a9e2a8502,
title = "Benzaldoxime to benzamide rearrangement catalysed by rhodium(III) hydroxocomplexes: The influence of polynuclear species",
abstract = "Rhodium(III) hydroxide was shown previously to possess the catalytic activity in the rearrangement reaction of primary oximes to amides. Alkaline solutions of rhodium(III) chlorocomplexes are routinely used for Rh(OH)3 preparation and allow for a diversity of rhodium hydroxocomplexes that hold a wide range of catalytic properties. In this study, two Al2O3 supported catalysts containing 1) exclusively [Rh(OH)6]3− species and 2) a mixture of rhodium hydroxocomplexes with one to four rhodium atoms ([Rh(OH)6]3–, [Rh2(μ−OH)2(OH)8]4–, [Rh3(μ−OH)3(OH)12]6–, [Rh4(μ−OH)6(OH)12]6) were prepared, characterised (XRD, Raman, EXAFS) and tested in the benzaldoxime to benzamide rearrangement. The catalyst containing polynuclear complexes possessed at least three times higher turnover frequency (TOF) and better selectivity than the [Rh(OH)6]3– based catalyst. According to the EXAFS data, the reduction of rhodium(III) took place under reaction conditions yielding small rhodium clusters (CNRh-Rh = 4), which were proposed to be the active sites of catalysts.",
keywords = "Heterogeneous catalysts, Primary amides, rhodium(III) hydroxocomplexes, MILD, ONE-POT SYNTHESIS, ACIDS, PRIMARY AMIDES, NANOPARTICLE, ALDOXIMES, HYDRATION, EXAFS, WATER",
author = "Semen Berdyugin and Victoria Volchek and Tatyana Asanova and Boris Kolesov and Evgeny Gerasimov and Evgeny Filatov and Danila Vasilchenko and Sergey Korenev",
note = "Publisher Copyright: {\textcopyright} 2019 Elsevier B.V. Copyright: Copyright 2020 Elsevier B.V., All rights reserved. Publisher Copyright: {\textcopyright} 2019 Elsevier B.V.",
year = "2019",
month = oct,
day = "25",
doi = "10.1016/j.apcata.2019.117242",
language = "English",
volume = "587",
journal = "Applied Catalysis A: General",
issn = "0926-860X",
publisher = "Elsevier",

}

RIS

TY - JOUR

T1 - Benzaldoxime to benzamide rearrangement catalysed by rhodium(III) hydroxocomplexes

T2 - The influence of polynuclear species

AU - Berdyugin, Semen

AU - Volchek, Victoria

AU - Asanova, Tatyana

AU - Kolesov, Boris

AU - Gerasimov, Evgeny

AU - Filatov, Evgeny

AU - Vasilchenko, Danila

AU - Korenev, Sergey

N1 - Publisher Copyright: © 2019 Elsevier B.V. Copyright: Copyright 2020 Elsevier B.V., All rights reserved. Publisher Copyright: © 2019 Elsevier B.V.

PY - 2019/10/25

Y1 - 2019/10/25

N2 - Rhodium(III) hydroxide was shown previously to possess the catalytic activity in the rearrangement reaction of primary oximes to amides. Alkaline solutions of rhodium(III) chlorocomplexes are routinely used for Rh(OH)3 preparation and allow for a diversity of rhodium hydroxocomplexes that hold a wide range of catalytic properties. In this study, two Al2O3 supported catalysts containing 1) exclusively [Rh(OH)6]3− species and 2) a mixture of rhodium hydroxocomplexes with one to four rhodium atoms ([Rh(OH)6]3–, [Rh2(μ−OH)2(OH)8]4–, [Rh3(μ−OH)3(OH)12]6–, [Rh4(μ−OH)6(OH)12]6) were prepared, characterised (XRD, Raman, EXAFS) and tested in the benzaldoxime to benzamide rearrangement. The catalyst containing polynuclear complexes possessed at least three times higher turnover frequency (TOF) and better selectivity than the [Rh(OH)6]3– based catalyst. According to the EXAFS data, the reduction of rhodium(III) took place under reaction conditions yielding small rhodium clusters (CNRh-Rh = 4), which were proposed to be the active sites of catalysts.

AB - Rhodium(III) hydroxide was shown previously to possess the catalytic activity in the rearrangement reaction of primary oximes to amides. Alkaline solutions of rhodium(III) chlorocomplexes are routinely used for Rh(OH)3 preparation and allow for a diversity of rhodium hydroxocomplexes that hold a wide range of catalytic properties. In this study, two Al2O3 supported catalysts containing 1) exclusively [Rh(OH)6]3− species and 2) a mixture of rhodium hydroxocomplexes with one to four rhodium atoms ([Rh(OH)6]3–, [Rh2(μ−OH)2(OH)8]4–, [Rh3(μ−OH)3(OH)12]6–, [Rh4(μ−OH)6(OH)12]6) were prepared, characterised (XRD, Raman, EXAFS) and tested in the benzaldoxime to benzamide rearrangement. The catalyst containing polynuclear complexes possessed at least three times higher turnover frequency (TOF) and better selectivity than the [Rh(OH)6]3– based catalyst. According to the EXAFS data, the reduction of rhodium(III) took place under reaction conditions yielding small rhodium clusters (CNRh-Rh = 4), which were proposed to be the active sites of catalysts.

KW - Heterogeneous catalysts

KW - Primary amides

KW - rhodium(III) hydroxocomplexes

KW - MILD

KW - ONE-POT SYNTHESIS

KW - ACIDS

KW - PRIMARY AMIDES

KW - NANOPARTICLE

KW - ALDOXIMES

KW - HYDRATION

KW - EXAFS

KW - WATER

UR - http://www.scopus.com/inward/record.url?scp=85072201658&partnerID=8YFLogxK

U2 - 10.1016/j.apcata.2019.117242

DO - 10.1016/j.apcata.2019.117242

M3 - Article

AN - SCOPUS:85072201658

VL - 587

JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

SN - 0926-860X

M1 - 117242

ER -

ID: 21538388