Investigation of perfluorooctanoic acid induced DNA damage using electrogenerated chemiluminescence associated with charge transfer in DNA.
An electrogenerated chemiluminescence (ECL)-DNA sensor was designed and fabricated for the investigation of DNA damage by a potential environmental pollutant, perfluorooctanoic acid (PFOA). The ECL-DNA sensor consisted of a Au electrode that had a self-assembled monolayer of 15 base-pair double-stranded (ds) DNA oligonucleotides with covalently attached semiconductor CdSe quantum dots (QDs) at the distal end of the DNA. Characterization of the ECL-DNA sensor was conducted with X-ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), ECL, and cyclic voltammetry before and after the exposure of the sensor to PFOA. Consistent data revealed that the dsDNA on Au was severely damaged upon the incubation of the electrode in PFOA, causing significant increase in charge (or electron) transfer (CT) resistance within DNA strands. Consequently, the cathodic coreactant ECL responses of the Au/dsDNA-QDs electrode in the presence of K2S2O8 were markedly decreased. The strong interaction between DNA and PFOA via the hydrophobic interaction, especially the formation of F···H hydrogen bonds by insertion of the difluoro-methylene group of PFOA into the DNA base pairs, was believed to be responsible for the dissociation or loosening of dsDNA structure, which inhibited the CT through DNA. A linear relationship between the ECL signal of the sensor and the logarithmical concentration of PFOA displayed a dynamic range of 1.00 × 10(-14)-1.00 × 10(-4) M, with a limit of detection of 1.00 × 10(-15) M at a signal-to-noise ratio of 3. Graphical Abstract Illustration of ECL detection of PFOA on a Au/dsDNA-QDs ECL-DNA sensor.
Key Laboratory of Beijing on Regional Air Pollution Control, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing, 100124, China. lipinglu@bjut.edu.cn.
Liping
L
Lu
Key Laboratory of Beijing on Regional Air Pollution Control, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing, 100124, China.
Linqing
L
Guo
Key Laboratory of Beijing on Regional Air Pollution Control, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing, 100124, China.
Meng
M
Li
Key Laboratory of Beijing on Regional Air Pollution Control, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing, 100124, China.
Tianfang
T
Kang
Key Laboratory of Beijing on Regional Air Pollution Control, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing, 100124, China.
Shuiyuan
S
Cheng
Key Laboratory of Beijing on Regional Air Pollution Control, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing, 100124, China. wujian.miao@usm.edu.|Department of Chemistry and Biochemistry, The University of Southern Mississippi, 118 College Drive, Hattiesburg, MS, 39406, USA. wujian.miao@usm.edu.
Wujian
W
Miao
D015374:Biosensing Techniques / Q000379:methods; D019187:Cadmium Compounds / Q000737:chemistry; D002210:Caprylates / Q000633:toxicity*; D004249:DNA Damage / Q000187:drug effects*; D058266:Dielectric Spectroscopy / Q000379:methods; D055664:Electrochemical Techniques / Q000379:methods*; D004566:Electrodes; D004583:Electrons; D004785:Environmental Pollutants / Q000633:toxicity*; D005466:Fluorocarbons / Q000633:toxicity*; D006046:Gold / Q000737:chemistry; D049449:Luminescence; D008163:Luminescent Measurements / Q000379:methods*; D045663:Quantum Dots / Q000737:chemistry; D018036:Selenium Compounds / Q000737:chemistry
D019187:Cadmium Compounds; D002210:Caprylates; D004785:Environmental Pollutants; D005466:Fluorocarbons; D018036:Selenium Compounds; D006046:Gold; C023036:perfluorooctanoic acid; C058667:cadmium selenide
Biosensors; DNA charge transfer; DNA damage; Electrogenerated chemiluminescence (ECL); Perfluorooctanoic acid (PFOA); Quantum dots