Dinuclear Zn2+ complexes in the hydrolysis of the phosphodiester linkage in a diribonucleoside monophosphate diester

Dalton Transactions : an International Journal of Inorganic Chemistry
M YashiroM Komiyama

Abstract

Dizinc complexes that were formed from 2:1 mixtures of Zn(NO3)2 and dinucleating ligands TPHP (1), TPmX (2) or TPpX (3) in aqueous solutions efficiently hydrolyzed diribonucleoside monophosphate diesters (NpN) under mild conditions. The dinucleating ligand affected the structure of the aquo-hydroxo-dizinc core, resulting in different characteristics in the catalytic activities towards NpN cleavage. The pH-rate profile of ApA cleavage in the presence of (Zn2+)(2)-1 was sigmoidal, whereas those of (Zn2+)(2)-2 and (Zn2+)(2)-3 were bell-shaped. The pH titration study indicated that (Zn2+)(2)-1 dissociates only one aquo proton (up to pH 12), whereas (Zn2+)(2)-2 dissociates three aquo protons (up to pH 10.7). The observed differences in the pH-rate profile are attributable to the various distributions of the monohydroxo-dizinc species, which are responsible for NpN cleavage. As compared to that using (Zn2+)(2)-1, the NpN cleavage using (Zn2+)(2)-2 showed a greater rate constant, with a higher product ratio of 3'-NMP/2'-NMP. The saturation behaviors of the rate, with regard to the concentration of NpN, were analyzed by Michaelis-Menten type kinetics. Although the binding of (Zn2+)(2)-2 to ApA was weaker than that of (Zn2+)(2)-1, (Zn2+...Continue Reading

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Citations

Sep 17, 2004·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Morio Yashiro, Ryuto Kawahara
Dec 30, 2015·Analytical Chemistry·Tsukuru MinamikiShizuo Tokito
Aug 23, 2007·Dalton Transactions : an International Journal of Inorganic Chemistry·Ryan A MathewsJohn P Richard
Dec 17, 2008·Dalton Transactions : an International Journal of Inorganic Chemistry·Rebecca R BuchholzLawrence R Gahan
Aug 26, 2009·Journal of Biochemical and Molecular Toxicology·Pengfei ShiQin Jiang
Oct 6, 2005·Angewandte Chemie·Robert TrokowskiA Dean Sherry
Oct 19, 2013·Organic & Biomolecular Chemistry·Heidi KorhonenSatu Mikkola
Jan 25, 2011·Organic & Biomolecular Chemistry·Harri Lönnberg
Jul 22, 2006·Annali Di Chimica·Liberato CiavattaFrancesco Salvatore
Mar 29, 2013·Chemical Communications : Chem Comm·Javier Hernández-GilJuan C Mareque-Rivas
Dec 14, 2011·Chemistry : a European Journal·Heidi KorhonenNicholas H Williams
Oct 11, 2008·Journal of the American Chemical Society·Kido NweJanet R Morrow
Sep 14, 2006·Chemical Reviews·Michael Kruppa, Burkhard König

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