Active species for Ce(IV)-induced hydrolysis of phosphodiester linkage in cAMP and DNA

Jun Sumaoka; Kenichiro Furuki; Yuki Kojima; Masahiko Shibata; Kimihiko Hirao; Naoya Takeda; Makoto Komiyama

doi:10.1080/15257770600684209

Active species for Ce(IV)-induced hydrolysis of phosphodiester linkage in cAMP and DNA

Jun Sumaoka, Kenichiro Furuki, Yuki Kojima, Masahiko Shibata, Kimihiko Hirao, Naoya Takeda, Makoto Komiyama

Research output: Contribution to journal › Article › peer-review

10 Citations (Scopus)

Abstract

The hydrolysis of cyclic adenosine 3′,5′-monophosphate and 2′-deoxythymidylyl(3′-5′)2′-deoxythymidine by Ce(NH ₄)₂(NO₃)₆ was kinetically studied. The rate of hydrolysis was fairly proportional to the concentration of [Ce ₂^IV (OH)₄]⁴⁺, showing that this is the catalytically active species. According to quantum-chemical calculation, the two Ce(IV) ions in this [Ce₂^IV (OH)₄] ⁴⁺ cluster are bridged by two OH residues. Upon the complex formation with H₂PO₄^- (a model compound for the phosphodiesters), these two Ce(IV) ions bind the two oxygen atoms of the substrate and enhance the electrophilicity of the phosphorus atom. The catalytic mechanism of Ce(IV)-induced hydrolysis of phosphodiesters has been proposed on the basis these results.

Original language	English
Pages (from-to)	523-538
Number of pages	16
Journal	Nucleosides, Nucleotides and Nucleic Acids
Volume	25
Issue number	4-6
DOIs	https://doi.org/10.1080/15257770600684209
Publication status	Published - 2006 Jun 1
Externally published	Yes

Keywords

Artificial nuclease
Cerium
DNA cleavage
Enzyme models
Phosphodiester hydrolysis

ASJC Scopus subject areas

Biochemistry
Molecular Medicine
Genetics

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title = "Active species for Ce(IV)-induced hydrolysis of phosphodiester linkage in cAMP and DNA",

abstract = "The hydrolysis of cyclic adenosine 3′,5′-monophosphate and 2′-deoxythymidylyl(3′-5′)2′-deoxythymidine by Ce(NH 4)2(NO3)6 was kinetically studied. The rate of hydrolysis was fairly proportional to the concentration of [Ce 2IV (OH)4]4+, showing that this is the catalytically active species. According to quantum-chemical calculation, the two Ce(IV) ions in this [Ce2IV (OH)4] 4+ cluster are bridged by two OH residues. Upon the complex formation with H2PO4- (a model compound for the phosphodiesters), these two Ce(IV) ions bind the two oxygen atoms of the substrate and enhance the electrophilicity of the phosphorus atom. The catalytic mechanism of Ce(IV)-induced hydrolysis of phosphodiesters has been proposed on the basis these results.",

keywords = "Artificial nuclease, Cerium, DNA cleavage, Enzyme models, Phosphodiester hydrolysis",

author = "Jun Sumaoka and Kenichiro Furuki and Yuki Kojima and Masahiko Shibata and Kimihiko Hirao and Naoya Takeda and Makoto Komiyama",

year = "2006",

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T1 - Active species for Ce(IV)-induced hydrolysis of phosphodiester linkage in cAMP and DNA

AU - Sumaoka, Jun

AU - Furuki, Kenichiro

AU - Kojima, Yuki

AU - Shibata, Masahiko

AU - Hirao, Kimihiko

AU - Takeda, Naoya

AU - Komiyama, Makoto

PY - 2006/6/1

Y1 - 2006/6/1

N2 - The hydrolysis of cyclic adenosine 3′,5′-monophosphate and 2′-deoxythymidylyl(3′-5′)2′-deoxythymidine by Ce(NH 4)2(NO3)6 was kinetically studied. The rate of hydrolysis was fairly proportional to the concentration of [Ce 2IV (OH)4]4+, showing that this is the catalytically active species. According to quantum-chemical calculation, the two Ce(IV) ions in this [Ce2IV (OH)4] 4+ cluster are bridged by two OH residues. Upon the complex formation with H2PO4- (a model compound for the phosphodiesters), these two Ce(IV) ions bind the two oxygen atoms of the substrate and enhance the electrophilicity of the phosphorus atom. The catalytic mechanism of Ce(IV)-induced hydrolysis of phosphodiesters has been proposed on the basis these results.

AB - The hydrolysis of cyclic adenosine 3′,5′-monophosphate and 2′-deoxythymidylyl(3′-5′)2′-deoxythymidine by Ce(NH 4)2(NO3)6 was kinetically studied. The rate of hydrolysis was fairly proportional to the concentration of [Ce 2IV (OH)4]4+, showing that this is the catalytically active species. According to quantum-chemical calculation, the two Ce(IV) ions in this [Ce2IV (OH)4] 4+ cluster are bridged by two OH residues. Upon the complex formation with H2PO4- (a model compound for the phosphodiesters), these two Ce(IV) ions bind the two oxygen atoms of the substrate and enhance the electrophilicity of the phosphorus atom. The catalytic mechanism of Ce(IV)-induced hydrolysis of phosphodiesters has been proposed on the basis these results.

KW - Artificial nuclease

KW - Cerium

KW - DNA cleavage

KW - Enzyme models

KW - Phosphodiester hydrolysis

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JO - Nucleosides, Nucleotides and Nucleic Acids

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