Structural, kinetic, and theoretical studies on models of the zinc-containing phosphodiesterase active center: medium-dependent reaction mechanisms.

Structural, kinetic, and theoretical studies on models of the zinc-containing phosphodiesterase active center: medium-dependent reaction mechanisms. Research Abstract Details 

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Structural, kinetic, and theoretical studies on models of the zinc-containing phosphodiesterase active center: medium-dependent reaction mechanisms. Abstract Text:

Katalin Selmeczi,Carine Michel,Anne Milet,Isabelle Gautier-Luneau,Christian Philouze,Jean-Louis Pierre,David Schnieders,Annette Rompel,Catherine Belle,Katalin Selmeczi,Carine Michel,Anne Milet,Isabelle Gautier-Luneau,Christian Philouze,Jean-Louis Pierre,David Schnieders,Annette Rompel,Catherine Belle,

Dinuclear zinc(II) complexes [Zn(2)(bpmp)(mu-OH)](ClO(4))(2) (1) and [Zn(2)(bpmp)(H(2)O)(2)](ClO(4))(3) (2) (H-BPMP=2,6-bis[bis(2-pyridylmethyl)aminomethyl]-4-methylphenol) have been synthesized, structurally characterized, and pH-driven changes in metal coordination observed. The transesterification reaction of 2-hydroxypropyl p-nitrophenyl phosphate (HPNP) in the presence of the two complexes was studied both in a water/DMSO (70:30) mixture and in DMSO. Complex 2 was not reactive whereas for 1 considerable rate enhancement of the spontaneous hydrolysis reaction was observed. A detailed mechanistic investigation by kinetic studies, spectroscopic measurements ((1)H, (31)P NMR spectroscopy), and ESI-MS analysis in conjunction with ab initio calculations was performed on 1. Based on these results, two medium-dependent mechanisms are presented and an unusual bridging phosphate intermediate is proposed for the process in DMSO.

Structural, kinetic, and theoretical studies on models of the zinc-containing phosphodiesterase active center: medium-dependent reaction mechanisms. Publishing Authors By Initials

K Selmeczi,C Michel,A Milet,I Gautier-Luneau,C Philouze,JL Pierre,D Schnieders,A Rompel,C Belle,K Selmeczi,C Michel,A Milet,I Gautier-Luneau,C Philouze,JL Pierre,D Schnieders,A Rompel,C Belle,

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Structural, kinetic, and theoretical studies on models of the zinc-containing phosphodiesterase active center: medium-dependent reaction mechanisms. Journal Published:

PUBLICATION TYPE: Research Support, Non-U.S. Gov

Journal: Chemistry (Weinheim an der Bergstrasse, Germany)

VOLUME: 13

Page Numbers: 9093-106

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ISSN: 0947-6539

DAY: 30

MONTH: 10

YEAR: 2007

Structural, kinetic, and theoretical studies on models of the zinc-containing phosphodiesterase active center: medium-dependent reaction mechanisms. Information

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LANGUAGE: eng

NlmUniqueID: 9513783

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Grant and Affiliation Information for Structural, kinetic, and theoretical studies on models of the zinc-containing phosphodiesterase active center: medium-dependent reaction mechanisms.

AFFILIATION: Département de Chimie Moléculaire, Université J. Fourier, Grenoble I, UMR-5250, ICMG FR-2607, CNRS BP-53, 38041 Grenoble, France.

Country: Germany

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MEDLINETA: Chemistry

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