Relevance of Protons in Heterolytic Activation of H2O2 over Nb(V): Insights from Model Studies on Nb-Substituted Polyoxometalates
Nataliya V. Maksimchuk
1, 2
,
Gennadii M. Maksimov
1
,
Vasilii Yu Evtushok
1, 2
,
Irina D Ivanchikova
1
,
Yuriy A Chesalov
1, 2
,
Raisa I Maksimovskaya
1
,
O.A. Kholdeeva
1, 2
,
Josep M. Poblet
3
,
Jorge Carbo
3
Тип публикации: Journal Article
Дата публикации: 2018-09-10
scimago Q1
wos Q1
БС1
SJR: 3.782
CiteScore: 19.5
Impact factor: 13.1
ISSN: 21555435
General Chemistry
Catalysis
Краткое описание
Nb-monosubstituted Lindqvist-type polyoxometalates (POM), (Bu4N)4[(NbW5O18)2O] (1) and (Bu4N)3[Nb(O)W5O18] (2), catalyze epoxidation of alkenes with hydrogen peroxide and mimic the catalytic performance of heterogeneous Nb-silicate catalysts. Dimer 1 is more active than monomer 2, but the catalytic activity of the latter increases in the presence of acid. Kinetic and spectroscopic studies suggest a mechanism that involves generation of monomer (Bu4N)2[Nb(OH)W5O18] (3), interaction of 3 with H2O2 leading to a protonated peroxo niobium species, (Bu4N)2[HNb(O2)W5O18] (4), followed by oxygen transfer to a C═C bond in alkene. The previously unknown peroxo complex 4 has been isolated and characterized by elemental analysis; UV–vis, FT-IR, Raman, 93Nb, 17O and 183W NMR spectroscopy; cyclic voltammetry; and potentiometric titration. The physicochemical techniques support a monomeric Lindqvist structure of 4 bearing one peroxo ligand attached to Nb(V) in a η2-coordination mode. While the unprotonated peroxo comple...
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Maksimchuk N. V. et al. Relevance of Protons in Heterolytic Activation of H2O2 over Nb(V): Insights from Model Studies on Nb-Substituted Polyoxometalates // ACS Catalysis. 2018. Vol. 8. No. 10. pp. 9722-9737.
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Maksimchuk N. V., Maksimov G. M., Evtushok V. Yu., Ivanchikova I. D., Chesalov Y. A., Maksimovskaya R. I., Kholdeeva O., Solé Daura A., Poblet J. M., Carbo J. Relevance of Protons in Heterolytic Activation of H2O2 over Nb(V): Insights from Model Studies on Nb-Substituted Polyoxometalates // ACS Catalysis. 2018. Vol. 8. No. 10. pp. 9722-9737.
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TY - JOUR
DO - 10.1021/acscatal.8b02761
UR - https://doi.org/10.1021/acscatal.8b02761
TI - Relevance of Protons in Heterolytic Activation of H2O2 over Nb(V): Insights from Model Studies on Nb-Substituted Polyoxometalates
T2 - ACS Catalysis
AU - Maksimchuk, Nataliya V.
AU - Maksimov, Gennadii M.
AU - Evtushok, Vasilii Yu
AU - Ivanchikova, Irina D
AU - Chesalov, Yuriy A
AU - Maksimovskaya, Raisa I
AU - Kholdeeva, O.A.
AU - Solé Daura, Albert
AU - Poblet, Josep M.
AU - Carbo, Jorge
PY - 2018
DA - 2018/09/10
PB - American Chemical Society (ACS)
SP - 9722-9737
IS - 10
VL - 8
SN - 2155-5435
ER -
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@article{2018_Maksimchuk,
author = {Nataliya V. Maksimchuk and Gennadii M. Maksimov and Vasilii Yu Evtushok and Irina D Ivanchikova and Yuriy A Chesalov and Raisa I Maksimovskaya and O.A. Kholdeeva and Albert Solé Daura and Josep M. Poblet and Jorge Carbo},
title = {Relevance of Protons in Heterolytic Activation of H2O2 over Nb(V): Insights from Model Studies on Nb-Substituted Polyoxometalates},
journal = {ACS Catalysis},
year = {2018},
volume = {8},
publisher = {American Chemical Society (ACS)},
month = {sep},
url = {https://doi.org/10.1021/acscatal.8b02761},
number = {10},
pages = {9722--9737},
doi = {10.1021/acscatal.8b02761}
}
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MLA
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Maksimchuk, Nataliya V., et al. “Relevance of Protons in Heterolytic Activation of H2O2 over Nb(V): Insights from Model Studies on Nb-Substituted Polyoxometalates.” ACS Catalysis, vol. 8, no. 10, Sep. 2018, pp. 9722-9737. https://doi.org/10.1021/acscatal.8b02761.
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