Ultrasensitive Electrogenerated Chemiluminescence Biosensor for the Determination of Mercury Ion Incorporating G4 PAMAM Dendrimer and Hg(II)-Specific Oligonucleotide
Document Type
Article
Publication Date
2-1-2012
Department
Chemistry and Biochemistry
School
Mathematics and Natural Sciences
Abstract
A novel electrogenerated chemiluminescence (ECL) biosensor for highly sensitive and selective detection of mercury ion was developed on the basis of mercury-specific oligonucleotide (MSO) served as a molecular recognition element and the ruthenium(II) complex (Ru1) as an ECL emitting species. The biosensor was fabricated on a glassy carbon electrode coated with a thin layer of single wall carbon nanotubes, where the ECL probe, NH2-(CH2)6-oligo(ethylene oxide)6-MSO ↔ Dend-Ru1, was covalently attached. The Dend-Ru1 pendant was prepared by covalent coupling Ru1 with the 4th generation polyamidoamine dendrimer (Dend), in which each dendrimer contained 35 Ru1 units so that a large amplification of ECL signal was obtained. Upon binding of Hg2+ to thymine (T) bases of the MSO, the T–Hg–T structure was formed, and the MSO changed from its linear shape to a “hairpin” configuration. Consequently, the Dend-Ru1 approached the electrode surface resulting in the increase of anodic ECL signal in the presence of the ECL coreactant tri-n-propylamine. The reported biosensor showed a high reproducibility and possessed long-term storage stability (92.3% initial ECL recovery over 30 day's storage). An extremely low detection limit of 2.4 pM and a large dynamic range of 7.0 pM to 50 nM Hg2+ were obtained. An apparent binding constant of 1.6 × 109 M−1 between Hg2+ and the MSO was estimated using an ECL based extended Langmuir isotherm approach involving multilayer adsorption. Determination of Hg2+ contents in real water samples was conducted and the data were consistent with the results from cold vapor atomic fluorescence spectroscopy.
Publication Title
Biosensors and Bioelectronics
Volume
32
Issue
1
First Page
37
Last Page
42
Recommended Citation
Ma, F.,
Zhang, Y.,
Qi, H.,
Gao, Q.,
Zhang, C.,
Miao, W.
(2012). Ultrasensitive Electrogenerated Chemiluminescence Biosensor for the Determination of Mercury Ion Incorporating G4 PAMAM Dendrimer and Hg(II)-Specific Oligonucleotide. Biosensors and Bioelectronics, 32(1), 37-42.
Available at: https://aquila.usm.edu/fac_pubs/8874