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• W2038502014 abstract "[RhCl(COD)]2 (COD = 1,5-cyclooctadiene) reacts with PPh2(o-C6H4CHO) in the presence of 2-aminopyridine (apy) to give the diacyl [RhCl(PPh2(o-C6H4CO))2(apy)] (1) with evolution of hydrogen. 1 is a mixture of two isomers, 1a with trans P atoms and cis acyl groups and 1b with cis P atoms and trans acyl groups. In solution fast exchange between phosphorus atoms of the two isomers and also decreasing of the 1a:1b ratio occur on raising the temperature. This behavior can be due to intramolecular opening of the acyl-phosphine chelate. Complex 1 reacts with bidentate N-donor ligands to afford cationic diacyl derivatives [Rh(PPh2(o-C6H4CO))2(NN)]+ (NN = 2,2‘-bipyridine, 2; glyoxaldihydrazone, 3; 1,2-phenylenediamine, 4; ethylenediamine, 5; 2-(aminomethyl)pyridine (ampy), 6, 7; 8-aminoquinoline (aqui), 8) with high stereoselectivity depending on the N-donor ligand employed. Diimine ligands give only complexes with trans phosphorus atoms (2, 3), diamine ligands give only derivatives containing cis phosphorus atoms (4, 5), and ligands containing amino-imine functionalities afford both types of isomers. Ampy allows the isolation of both complexes 6 and 7. Complex 6, with trans phosphorus atoms, is the kinetic product of the reaction, and 7, with cis phosphorus atoms, is the most stable thermodynamic isomer. The rate of the isomerization reaction of 6 into 7 depends on the solvent and also on the counterion, suggesting that this reaction may be assisted by ion-pair formation via hydrogen bonding. The reaction of [RhCl(COD)]2 with PPh2(o-C6H4CHO) in the presence of ampy or the reaction of the phosphine-aldehyde complex [RhClH(PPh2(o-C6H4CO))(κ2-PPh2(o-C6H4CHO))] (10) with ampy leads to [RhH(PPh2(o-C6H4CO))(PNN)]Cl (9) (PNN = κ3-PPh2(o-C6H4CHOH-NH-CH2-C5H4N)), containing a hemiaminal group (>CH(OH)NH−) formed by the reaction of the aldehyde with the amino group. Complex 10 reacts with aqui to afford [RhH(PPh2(o-C6H4CO))(PPh2(o-C6H4CHN-C9H6N))]+ (11), containing a PNN ligand with an imine functionality. The hemiaminal stability seems to be favored by the presence of a single sp3 carbon atom in 9. All the complexes were fully characterized spectroscopically. Single-crystal X-ray diffraction analysis was performed on 1a and 7." @default.
• W2038502014 created "2016-06-24" @default.
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• W2038502014 creator A5076661893 @default.
• W2038502014 date "2007-09-28" @default.
• W2038502014 modified "2023-09-27" @default.
• W2038502014 title "Selective Formation of Rhodium Diacyl or Acyl Hydrido Hemiaminal Complexes in the Reaction of <i>o</i>-(Diphenylphosphino)benzaldehyde with Rhodium 2-Aminopyridine or 2-(Aminomethyl)pyridine Compounds" @default.
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• W2038502014 doi "https://doi.org/10.1021/om7005134" @default.
• W2038502014 hasPublicationYear "2007" @default.
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