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001-es BibID:	BIBFORM084830
Első szerző:	Csajbók Éva (vegyész, kémikus)
Cím:	Dynamic NMR properties of DOTA ligand: variable pH and temperature 1H NMR study on [K(HxDOTA)](3-x)- species / Éva Csajbók, István Bányai, Ernő Brücher
Dátum:	2004
ISSN:	1477-9226
Megjegyzések:	The (1)H NMR spectra of [H(x)DOTA]((4-x)-) species are reported as a function of pH and temperature in aqueous solution. The spectra show line broadening both in ligand proton signals and also in the water proton signal by titration with KOH solution. The formation of different [K(H(x)DOTA)]((3-x)-) complexes is found to be responsible for this behaviour. At high pH the usual fluxional motions, i.e. the ring inversion and the change in the acetate arms' helicity, which are also characteristic for other but inert metal-DOTA complexes, have been detected. However, because of the kinetic lability of K(+)-O and K(+)-N coordinative bonds a new type of rearrangement appears. This new motion requires breaking of coordinative bonds in the complex and can be described as a certain type of "ring slewing" around the ring C-C bonds. At low temperature (about 270 K) the ring slewing slows down and becomes negligible compared with the ring inversion and the change in the arms' helicity. These two latter processes have the same rate. When the temperature is higher (about 320 K) the ring slewing accelerates and its rate exceeds the rate of ring inversion. At this temperature the change in the acetate arms' helicity has the same rate as the ring slewing. Additionally, in the pH range 4-5 a slow intermolecular proton exchange process has been observed between the water and the dissociable protons of [K(H(x)DOTA)]((3-x)-). A water-assisted proton exchange mechanism is proposed on the basis of the activation parameters. This finding supports the previously suggested slow proton motion hypothesis for the formation of DOTA complexes.
Tárgyszavak:	Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban folyóiratcikk
Megjelenés:	Dalton Transactions. - 2004 : 14 (2004), p. 2152-2156. -
További szerzők:	Bányai István (1953-) (vegyész) Brücher Ernő (1935-) (vegyész)
Pályázati támogatás:	OTKA T035127 OTKA
Internet cím:	Szerző által megadott URL DOI Intézményi repozitóriumban (DEA) tárolt változat
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