Molecular design of an acid-base cooperative catalyst for RNA cleavage based on a dizinc complex

Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry
Morio Yashiro, Ryuto Kawahara

Abstract

The effects of donor groups of dizinc complexes, formed from a 2:1 mixture of Zn(II) and a dinucleating ligand, on adenylyl(3'-5')adenosine (ApA) cleavage have been studied. Two dinucleating ligands were used: one had two 2-pyridylmethyl and two 2-hydroxyethyl moieties on the 1,3-diamino-2-propanol linker moiety (2), and the other had two 2-pyridylmethyl and two carboxymethyl moieties on the 1,3-diamino-2-propanol linker moiety (3(2-)). The dizinc complex with2 [(Zn(2+))(2)-2] showed higher activities toward ApA cleavage than the dizinc complex using an analogous dinucleating ligand having four 2-pyridylmethyl donor moieties [(Zn(2+))(2)-1] at pH 5-8. The former showed a bell-shaped pH-rate constant profile, whereas the latter showed a sigmoidal pattern. The differences in the pH-rate constant profile are attributable to the various distributions of the monohydroxo-dizinc species, i.e. dideprotonated species, which are responsible for ApA cleavage. The monohydroxo species of (Zn(2+))(2)-2 has two acidic protons, which are not present in the corresponding monohydroxo species of (Zn(2+))(2)-1. The existence of both intracomplex acid (ROH or H(2)O) and base catalysts (RO(-) or OH(-)) in (Zn(2+))(2)-2 can explain its higher activit...Continue Reading

References

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Jul 15, 2004·Dalton Transactions : an International Journal of Inorganic Chemistry·Morio YashiroMakoto Komiyama

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