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Dynamic Behaviour of the [(Triphos)Rh(·1:·2-P4RR')]n+ Complexes [Triphos = MeC(CH2PPh2)3; R = H, Alkyl, Aryl; R' = Lone Pair, H, Me; n = 0, 1]: NMR and Computational Studies (Articolo in rivista)
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- Dynamic Behaviour of the [(Triphos)Rh(·1:·2-P4RR')]n+ Complexes [Triphos = MeC(CH2PPh2)3; R = H, Alkyl, Aryl; R' = Lone Pair, H, Me; n = 0, 1]: NMR and Computational Studies (Articolo in rivista) (literal)
- Anno
- 2008-01-01T00:00:00+01:00 (literal)
- Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#doi
- 10.1002/ejic.200701070 (literal)
- Alternative label
Barbaro, Pierluigi; Caporali, Maria; Ienco, Andrea; Mealli, Carlo; Peruzzini, Maurizio; Vizza, Francesco (2008)
Dynamic Behaviour of the [(Triphos)Rh(·1:·2-P4RR')]n+ Complexes [Triphos = MeC(CH2PPh2)3; R = H, Alkyl, Aryl; R' = Lone Pair, H, Me; n = 0, 1]: NMR and Computational Studies
in European journal of inorganic chemistry (Print)
(literal)
- Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#autori
- Barbaro, Pierluigi; Caporali, Maria; Ienco, Andrea; Mealli, Carlo; Peruzzini, Maurizio; Vizza, Francesco (literal)
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- Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#affiliazioni
- Consiglio Nazionale delle Ricerche, Istituto di Chimica dei Composti OrganoMetallici, Via Madonna del Piano 10, 50019 Sesto Fiorentino, Firenze, Italy (literal)
- Titolo
- Dynamic Behaviour of the [(Triphos)Rh(·1:·2-P4RR')]n+ Complexes [Triphos = MeC(CH2PPh2)3; R = H, Alkyl, Aryl; R' = Lone Pair, H, Me; n = 0, 1]: NMR and Computational Studies (literal)
- Abstract
- Solution multinuclear and multidimensional NMR analyses
of the [(triphos)Rh(?1:?2-P4RR?)]n+ complex cations [triphos =
MeC(CH2PPh2)3; R = H, Me, Ph; R? = lone pair, H, Me; n = 0,
1] confirm the same primary structure determined by X-rays
in the solid state. In addition, 2D 1H NOESY and 31P{1H} exchange
NMR spectroscopy show that these complexes are
nonrigid on the NMR time-scale over the 253-318 K temperature
range. A dynamic process that involves the terminal
phosphane groups of the triphos ligand is displayed by each
compound. The NMR spectroscopic data indicate a slow
Introduction
White phosphorus is a cheap chemical largely used in the
manufacturing of organophosphorus compounds.[1] These
industrially important derivatives are generally produced by
the reaction of PCl3 or PCl5 with suitable organic reagents.
The industrial process is not very environmentally sustainable
as the reaction involves gaseous chlorine and releases
huge amounts of hydrochloric acid into the atmosphere.
Therefore, the discovery of new and efficient methods for
the preparation of organophosphorus derivatives from P4
through non-chlorine routes remains a challenging task for
the industry.[2] Moreover, the underpinnings of the formation
of P-C and P-H bonds need to be understood in more
detail.[2,3] Advances in this area entail the use of transition
metal systems that are suitable for the activation of both
the P4 tetrahedron and the organic substrate. On the other
hand, a recent breakthrough in the area has been presented
by Bertrand et al. who have reported on the reactivity of
alkyl amino carbenes with P4. This process does not lead
to the formation of any metal intermediate and leads to very
reactive P-C bonds.[4]
Another important advancement in P4 activation/functionalization
was our previous finding that some rhodium
[a] Consiglio Nazionale delle Ricerche, Istituto di Chimica dei
Composti OrganoMetallici,
Via Madonna del Piano 10, 50019 Sesto Fiorentino, Firenze,
Italy
E-mail: maurizio.peruzzini@iccom.cnr.it
© 2008 Wiley-VCH Verlag 1392 GmbH & Co. KGaA, Weinheim Eur. J. Inorg. Chem. 2008, 1392-1399
scrambling motion in which the P4R unit tumbles with respect
to the (triphos)Rh moiety. DFT calculations outline a
possible turnstile mechanism involving the threefold and
twofold rotors into which the complex is subdivided. The process
goes through a transition state in which the axial and
equatorial dispositions of the PRR? and P=P donating groups
of the P4RR? ligand are inverted with respect to the ground
state. (literal)
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