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Ultrasensitive zero-background photoelectrochemical biosensor for analysis of organophosphorus pesticide based on in situ formation of DNA-templated Ag2S photoactive materials

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Abstract

Herein, a novel signal-on photoelectrochemical (PEC) biosensor with nearly zero background noise (ZBN) was first fabricated to determine the presence of organophosphorus pesticide based on in situ formation of DNA-templated Ag2S photoactive materials, accompanied by hybridization chain reaction (HCR) signal amplification. The capture probe (S1) on the gold nanoparticle-modified electrode can hybridize with the aptamer molecule to generate a simple PEC biosensor. In the presence of a target molecule, the aptamer molecule is released on the double-stranded DNA (dsDNA)-modified PEC biosensor. Meanwhile, the capture probe remains on the electrode and can open the DNA hairpins (H1, H2) which are rich in cytosine, to trigger the HCR reaction. The rich “C” strands are uncovered after formation of a long dsDNA polymer strand, which can assemble multiple silver ions (Ag+) by means of by C–Ag+–C chelation. Then, a large number of Ag2S can be generated by challenging with S2− solution, producing a satisfactory photocurrent signal. The photoactive material is formed in situ, which eliminates the laborious operation. Moreover, the signal can be highly amplified with nearly zero background noise and HCR signal amplification. Under optimal conditions, the ZBN aptasensor exhibited high sensitivity and selectivity, with a low detection limit of 2 pg mL−1 for malathion. Importantly, the sensing platform can also be applied to determine the presence of malathion in real samples.

Graphical abstract

In this assay, a novel signal-on photoelectrochemical biosensor with nearly zero background noise was first fabricated to determine the presence of organophosphorus pesticide based on in situ formation of DNA-templated Ag2S photoactive materials, accompanied by hybridization chain reaction signal amplification.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (21864013), the Science Foundation for Excellent Young Scholars of Jiangxi Province (20202ZDB01003), the Natural Science Foundation of Jiangxi Province (20202BAB203008), and the Postdoctoral Science Foundation of Jiangxi Province (2019KY40).

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Authors and Affiliations

  1. Key Laboratory for Green Chemistry of Jiangxi Province, Key Laboratory of Functional Small Molecules for Ministry of Education, Jiangxi Normal University, 99 Ziyang Avenue, Nanchang, 330022, Jiangxi, People’s Republic of China

    Zhiyao Zeng, Juan Tang & Ming Zhang

  2. Jiangxi Key Laboratory of Organic Chemistry, Nanchang, 330013, Jiangxi, People’s Republic of China

    Juan Tang & Shouzhi Pu

  3. Key Laboratory of Analysis and Detection for Food Safety (Ministry of Education of China and Fujian Province), Department of Chemistry, Fuzhou University, Fuzhou, 350108, Fujian, People’s Republic of China

    Dianping Tang

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  1. Zhiyao Zeng
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Zeng, Z., Tang, J., Zhang, M. et al. Ultrasensitive zero-background photoelectrochemical biosensor for analysis of organophosphorus pesticide based on in situ formation of DNA-templated Ag2S photoactive materials. Anal Bioanal Chem 413, 6279–6288 (2021). https://doi.org/10.1007/s00216-021-03582-3

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