Highly selective and sensitive DNA assay based on electrocatalytic oxidation of ferrocene bearing zinc(II)−cyclen complexes with diethylamine

Shiddiky, Muhammad J. A., Torriero, Angel A. J., Zeng, Zhanghua, Spiccia, Leone and Bond, Alan M. (2010) Highly selective and sensitive DNA assay based on electrocatalytic oxidation of ferrocene bearing zinc(II)−cyclen complexes with diethylamine. Journal of the American Chemical Society, 132 29: 10053-10063. doi:10.1021/ja1021365


Author Shiddiky, Muhammad J. A.
Torriero, Angel A. J.
Zeng, Zhanghua
Spiccia, Leone
Bond, Alan M.
Title Highly selective and sensitive DNA assay based on electrocatalytic oxidation of ferrocene bearing zinc(II)−cyclen complexes with diethylamine
Journal name Journal of the American Chemical Society   Check publisher's open access policy
ISSN 0002-7863
1943-2984
1520-5126
Publication date 2010-07-28
Sub-type Article (original research)
DOI 10.1021/ja1021365
Open Access Status
Volume 132
Issue 29
Start page 10053
End page 10063
Total pages 11
Editor Peter J. Stang
Place of publication Washington DC, United States
Publisher American Chemical Society
Language eng
Subject C1
Formatted abstract
A highly selective and sensitive electrochemical biosensor has been developed that detects DNA hybridization by employing the electrocatalytic activity of ferrocene (Fc) bearing cyclen complexes (cyclen = 1,4,7,10-tetraazacyclododecane, Fc[Zn(cyclen)H2O] 2(ClO4)4 (R1), Fc(cyclen)2 (R2), Fc[Zn(cyclen)H2O](ClO4)2 (R3), and Fc(cyclen) (R4)). A sandwich-type approach, which involves hybridization of a target probe hybridized with the preimmobilized thiolated capture probe attached to a gold electrode, is employed to fabricate a DNA duplex layer. Electrochemical signals are generated by voltammetric interrogation of a Fc bearing Zn-cyclen complexes that selectively and quantitatively binds to the duplex layers through strong chelation between the cyclen complexes and particular nucleobases within the DNA sequence. Chelate formation between R1 or R3 and thymine bases leads to the perturbation of base-pair (A-T) stacking in the duplex structure, which greatly diminishes the yield of DNA-mediated charge transport and displays a marked selectivity to the presence of the target DNA sequence. Coupling the redox chemistry of the surface-bound Fc bearing Zn-cyclen complex and dimethylamine provides an electrocatalytic pathway that increases sensitivity of the assay and allows the 100 fM target DNA sequence to be detected. Excellent selectivity against even single-base sequence mismatches is achieved, and the DNA sensor is stable and reusable.
© 2010 American Chemical Society.
Q-Index Code C1
Q-Index Status Confirmed Code
Institutional Status Non-UQ

Document type: Journal Article
Sub-type: Article (original research)
Collections: Non HERDC
Australian Institute for Bioengineering and Nanotechnology Publications
 
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Created: Tue, 02 Nov 2010, 20:47:59 EST by Dr Muhammad J. A. Shiddiky on behalf of Aust Institute for Bioengineering & Nanotechnology