1987
DOI: 10.1021/ja00258a061
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Metal-activated hydrolytic cleavage of DNA

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Cited by 155 publications
(81 citation statements)
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“…A number of metal ion complexes have been shown to hydrolyze phosphate esters (13,14) as well as RNA with various efficiencies (15)(16)(17)(18); however, these complexes are unable to hydrolyze the phosphate diester backbone of DNA. The only reported metal-catalyzed DNA hydrolysis thus far is effected by Cu2+, Zn2+, Cd2+, or Pb2+ complexed to a polyamine ligand tethered to a DNA-binding [Ru(phen)3]2+ derivative (19), which afforded nicked (single-stranded break) pBR322 at 37°C after 5-7 hr. Here we report a dinuclear iron complex, Fe2(HPTB)(OH)(NO3)4 (where HPTB is N,N,N',N'-tetrakis (2-benzimidazolylmethyl)-2-hydroxy-1,3-diaminopropane (20, 21), which in concert with H202 or 02 effects double-stranded cleavage of pBR322 via a "hydrolytic" mechanism.…”
mentioning
confidence: 99%
“…A number of metal ion complexes have been shown to hydrolyze phosphate esters (13,14) as well as RNA with various efficiencies (15)(16)(17)(18); however, these complexes are unable to hydrolyze the phosphate diester backbone of DNA. The only reported metal-catalyzed DNA hydrolysis thus far is effected by Cu2+, Zn2+, Cd2+, or Pb2+ complexed to a polyamine ligand tethered to a DNA-binding [Ru(phen)3]2+ derivative (19), which afforded nicked (single-stranded break) pBR322 at 37°C after 5-7 hr. Here we report a dinuclear iron complex, Fe2(HPTB)(OH)(NO3)4 (where HPTB is N,N,N',N'-tetrakis (2-benzimidazolylmethyl)-2-hydroxy-1,3-diaminopropane (20, 21), which in concert with H202 or 02 effects double-stranded cleavage of pBR322 via a "hydrolytic" mechanism.…”
mentioning
confidence: 99%
“…35 This strategy coupled to a DNA binding functionality has also been exploited, albeit inefficiently, in the hydrolytic cleavage of doublehelical DNA by Ru(DIPhMacro with Zn 2 +, Cd 2 +, or Pb 2 + added in situ. 36 In this complex (see Figure 8.6), the central portion of the molecule, held together by the ruthenium(II), is responsible for DNA binding. Tethered onto the coordinatively saturated ruthenium complex are two diethylenetriamine functionalities (in the Macro ligand), however, and these serve to coordinate hydrolytically active metal ions such as Zn(II) and Co(II) , which promote DNA hydrolysis once delivered to the sugar-phosphate backbone by the DNA-binding domain.…”
Section: Hydrolytic Chemistrymentioning
confidence: 99%
“…34 (B) Ru(DIPhMacro, a metal complex constructed to contain a central DNA-binding domain (Ru(DIP)32+) with two tethered amine arms to chelate additional metal ions (Zn 2 +) to deliver to the sugar-phosphate backbone and promote hydrolytic strand cleavage. 36 (C) RNA site-specificially hydrolyzed by lead ion. Diagram of the proposed mechanism of sugar-phosphate backbone cleavage between residue D 17 and G I8 in yeast RNA…”
Section: Hydrolytic Chemistrymentioning
confidence: 99%
“…Such agents can be used for a great variety of applications, e.g., for DNA footprinting [2], location of base mismatches and loop regions [3], identification of conformational variations in DNA [4], and as chemotherapeutic agents [5]. It has been reported that the DNA-cleaving ability of metal complexes varies not only from metal to metal [6], but is also influenced by the coordinating groups [7] [8]. Because DNA cleavage with metal complexes is a radical-based process [2] [9] that gives rise to products lacking 3'-or 5'-phosphate groups [10] (not being amenable to further enzymatic manipulation), their use has been limited.…”
mentioning
confidence: 99%