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001-es BibID:	BIBFORM016466
Első szerző:	Jarenmark, Martin
Cím:	Unsymmetrical dizinc complexes as models for the active sites of phosphohydrolases / Martin Jarenmark, Edit Csapó, Jyoti Singh, Simone Wöckel, Etelka Farkas, Franc Meyer, Matti Haukka, Ebbe Nordlander
Dátum:	2010
ISSN:	1477-9226
Megjegyzések:	The unsymmetrical dinucleating ligand 2-(N-isopropyl-N-((2-pyridyl) methyl) aminomethyl)-6-(N-( carboxylmethyl)-N-((2-pyridyl) methyl) aminomethyl)-4-methylphenol (IPCPMP or L) has been synthesized to model the active site environment of dinuclear metallohydrolases. It has been isolated as the hexafluorophosphate salt H4IPCPMP(PF6)(2)center dot 2H(2)O (H4L), which has been structurally characterized, and has been used to form two different Zn(II) complexes, [{Zn-2(IPCPMP)(OAc)}(2)]-[PF6](2) (2) and [{Zn-2(IPCPMP)(Piv)}(2)][PF6](2) (3) (OAc = acetate; Piv = pivalate). The crystal structures of 2 and 3 show that they consist of tetranuclear complexes with very similar structures. Infrared spectroscopy and mass spectrometry indicate that the tetranuclear complexes dissociate into dinuclear complexes in solution. Potentiometric studies of the Zn(II) : IPCPMP system in aqueous solution reveal that a mononuclear complex is surprisingly stable at low pH, even at a 2 : 1 Zn(II) : L ratio, but a dinuclear complex dominates at high pH and transforms into a dihydroxido complex by a cooperative deprotonation of two, probably terminally coordinated, water molecules. A kinetic investigation indicates that one of these hydroxides is the active nucleophile in the hydrolysis of bis(2,4-dinitrophenyl) phosphate (BDNPP) enhanced by complex 2, and mechanistic proposals are presented for this reaction as well as the previously reported transesterification of 2-hydroxypropyl p-nitrophenyl phosphate (HPNP) promoted by Zn(II) complexes of IPCPMP.
Tárgyszavak:	Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban purple acid-phosphatases dinuclear metal-complexes zinc(ii) complexes zn(ii) complex bis(2,4-dinitrophenyl) phosphate binuclear metallohydrolases diester transesterification phosphodiester cleavage (feznii)-zn-iii complex functional models
Megjelenés:	Dalton Transactions. - 39 (2010), p. 8183-8194. -
További szerzők:	Csapó Edit (1983-) (vegyész) Singh, Jyoti Wockel, Simone Farkas Etelka (1948-) (vegyész) Meyer, Franc Haukka, Matti Nordlander, Ebbe
Internet cím:	DOI Intézményi repozitóriumban (DEA) tárolt változat
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