Open Access
Bifunctional activation of amine-boranes by the W/Pd bimetallic analogs of “frustrated Lewis pairs”†
Elena S Osipova
1, 2, 3, 4, 5
,
Ekaterina S Gulyaeva
1, 2, 3, 4, 5
,
Evgenii I Gutsul
1, 2, 3, 4, 5
,
Vladislava A Kirkina
1, 2, 3, 4, 5
,
Alexander A Pavlov
1, 2, 3, 4, 5
,
Andrea Rossin
6, 7, 8, 9
,
Maurizio Peruzzini
6, 7, 8, 9
,
Lina M. epstein
1, 2, 3, 4, 5
,
Natalia V Belkova
1, 2, 3, 4, 5
,
Oleg A. Filippov
1, 2, 3, 4, 5
,
Elena S. Shubina
1, 2, 3, 4, 5
4
119991 Moscow
5
Russia
|
7
8
Sesto Fiorentino
|
9
ITALY
|
Publication type: Journal Article
Publication date: 2021-01-15
scimago Q1
wos Q1
SJR: 2.138
CiteScore: 12.6
Impact factor: 7.4
ISSN: 20416520, 20416539
PubMed ID:
34163642
General Chemistry
Abstract
The reaction between basic [(PCP)Pd(H)] (PCP = 2,6-(CH2P(t-C4H9)2)2C6H4) and acidic [LWH(CO)3] (L = Cp (1a), Tp (1b); Cp = η5-cyclopentadienyl, Tp = κ3-hydridotris(pyrazolyl)borate) leads to the formation of bimolecular complexes [LW(CO)2(μ-CO)⋯Pd(PCP)] (4a, 4b), which catalyze amine-borane (Me2NHBH3, tBuNH2BH3) dehydrogenation. The combination of variable-temperature (1H, 31P{1H}, 11B NMR and IR) spectroscopies and computational (ωB97XD/def2-TZVP) studies reveal the formation of an η1-borane complex [(PCP)Pd(Me2NHBH3)]+[LW(CO3)]− (5) in the first step, where a BH bond strongly binds palladium and an amine group is hydrogen-bonded to tungsten. The subsequent intracomplex proton transfer is the rate-determining step, followed by an almost barrierless hydride transfer. Bimetallic species 4 are easily regenerated through hydrogen evolution in the reaction between two hydrides.
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Osipova E. S. et al. Bifunctional activation of amine-boranes by the W/Pd bimetallic analogs of “frustrated Lewis pairs”† // Chemical Science. 2021. Vol. 12. No. 10. pp. 3682-3692.
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Osipova E. S. et al. Bifunctional activation of amine-boranes by the W/Pd bimetallic analogs of “frustrated Lewis pairs”† // Chemical Science. 2021. Vol. 12. No. 10. pp. 3682-3692.
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TY - JOUR
DO - 10.1039/d0sc06114j
UR - https://xlink.rsc.org/?DOI=D0SC06114J
TI - Bifunctional activation of amine-boranes by the W/Pd bimetallic analogs of “frustrated Lewis pairs”†
T2 - Chemical Science
AU - Osipova, Elena S
AU - Gulyaeva, Ekaterina S
AU - Gutsul, Evgenii I
AU - Kirkina, Vladislava A
AU - Pavlov, Alexander A
AU - Nelyubina, Yulia V.
AU - Rossin, Andrea
AU - Peruzzini, Maurizio
AU - epstein, Lina M.
AU - Belkova, Natalia V
AU - Filippov, Oleg A.
AU - Shubina, Elena S.
PY - 2021
DA - 2021/01/15
PB - Royal Society of Chemistry (RSC)
SP - 3682-3692
IS - 10
VL - 12
PMID - 34163642
SN - 2041-6520
SN - 2041-6539
ER -
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@article{2021_Osipova,
author = {Elena S Osipova and Ekaterina S Gulyaeva and Evgenii I Gutsul and Vladislava A Kirkina and Alexander A Pavlov and Yulia V. Nelyubina and Andrea Rossin and Maurizio Peruzzini and Lina M. epstein and Natalia V Belkova and Oleg A. Filippov and Elena S. Shubina and others},
title = {Bifunctional activation of amine-boranes by the W/Pd bimetallic analogs of “frustrated Lewis pairs”†},
journal = {Chemical Science},
year = {2021},
volume = {12},
publisher = {Royal Society of Chemistry (RSC)},
month = {jan},
url = {https://xlink.rsc.org/?DOI=D0SC06114J},
number = {10},
pages = {3682--3692},
doi = {10.1039/d0sc06114j}
}
Cite this
MLA
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Osipova, Elena S., et al. “Bifunctional activation of amine-boranes by the W/Pd bimetallic analogs of “frustrated Lewis pairs”†.” Chemical Science, vol. 12, no. 10, Jan. 2021, pp. 3682-3692. https://xlink.rsc.org/?DOI=D0SC06114J.