A Turn-on Biosensor-Based Aptamer-Mediated Carbon Quantum Dots Nanoaggregate for Acetamiprid Detection in Complex Samples

  • Zhe JiaoEmail author
  • Hongfeng Zhang
  • Shaohe Jiao
  • Zongning Guo
  • Dan Zhu
  • Xiaofang Zhao


In this paper, we developed a new biosensor-based on aptamer-mediated carbon quantum dots (apt-CQDs) nanoaggregate for acetamiprid detection. The acetamiprid aptamer, 5′- and its complementary DNA were labeled on CQDs, respectively. The hybridization of aptamer and its complementary DNA triggered the formation of nanoaggregate of CQDs, leading to the fluorescence quenching of the CQDs. Upon addition of acetamiprid, specific recognition of acetamiprid caused the release of the cDNA-CQDs and the fluorescence intensity recovered which was linearly related to the concentration of acetamiprid. The sensor provided a linear range from 0.2 to 20 ng/L for acetamiprid with a detection limit of 0.04 ng/L in an aqueous buffer. The same linear range was obtained in spiked human serum samples and lettuce samples with similar detection limits (0.15 and 0.11 ng/L), demonstrating high robustness of the sensor in a complex sample matrix. The as-prepared biosensor was used to monitor acetamiprid level in real samples with recovery ranged from 86 to 107%, and RSDs ranged from 1.3–6.9% (n = 3). The proposed study not only provided a simple method through CQDs nanoaggregate and also provided a turn-on detection mode for acetamiprid in real samples with high signal-to-noise ratios.

Graphical abstract

Fabrication of CQDs and principle for detection of acetamiprid by CQDs nanoaggregates.


Carbon quantum dots Aptamer Biosensor Acetamiprid 


Author Contributions

Hongfeng Zhang contributed to the independent LC-MS/MS method for acetamiprid detection.

Funding Information

This work was supported by the National Natural Science Foundation of China (21305013) and the Guangdong Provincial Key Platform and Major Scientific Research Projects for Colleges and Universities (Nos. 2014KZDXM073, 2015KCXTD029).

Compliance with Ethical Standards

Ethical Approval

This article does not contain any studies with human participants or animals performed by any of the authors.

Informed Consent

Not applicable.

Conflict of Interest

Zhe Jiao declares that she/he has no conflict of interest. Hongfeng Zhang declares that she/he has no conflict of interest. Shaohe Jiao declares that she/he has no conflict of interest. Zongning Guo declares that she/he has no conflict of interest. Dan Zhu declares that she/he has no conflict of interest. Xiaofang Zhao declares that she/he has no conflict of interest.

Supplementary material

12161_2018_1393_MOESM1_ESM.doc (2.6 mb)
ESM 1 (DOC 2631 kb)


  1. Abnous K, Danesh NM, Ramezani M, Alibolandi M, Lavaee P, Taghdisi SM (2017) Aptamer based fluorometric acetamiprid assay using three kinds of nanoparticles for powerful signal amplification. Microchim Acta 184:81–90CrossRefGoogle Scholar
  2. Chen BB, Liu ZX, Deng WC, Zhan L, Liu ML, Huang CZ (2016) A large-scale synthesis of photoluminescent carbon quantum dots: a self-exothermic reaction driving the formation of the nanocrystalline core at room temperature. Green Chem 18:5127–5132CrossRefGoogle Scholar
  3. Choi JH, Chen KH, Strano MS (2006) Aptamer-capped nanocrystal quantum dots: a new method for label-free protein detection. J Am Chem Soc 128:15584–15585CrossRefGoogle Scholar
  4. Ellington AD, Szostak JW (1992) Selection in vitro of single-stranded DNA molecules that fold into specific ligand-binding structures. Nature 355(6363):850–852CrossRefGoogle Scholar
  5. He J, Liu Y, Fan M, Liu X (2011) Isolation and identification of the DNA aptamer target to acetamiprid. J Agric Food Chem 59(5):1582–1586CrossRefGoogle Scholar
  6. He X, Zeng T, Li Z, Wang G, Ma N (2016) Catalytic molecular imaging of microRNA in living cells by DNA-programmed nanoparticle disassembly. Angew Chem Int Ed 55(9):3073–3076CrossRefGoogle Scholar
  7. Hu J, Wang ZY, Li CC, Zhang CY (2017a) Advances in single quantum dot-based nanosensors. Chem Commun 53:13284–13295CrossRefGoogle Scholar
  8. Hu J, Li Y, Li Y, Tang B, Zhang CY (2017b) Single quantum dot-based nanosensor for sensitive detection of O-GlcNAc transferase activity. Anal Chem 89:12992–12999CrossRefGoogle Scholar
  9. Liu L, Li Y, Zhan L, Liu Y, Huang CZ (2011) One-step synthesis of fluorescent hydroxyls-coated carbon dots with hydrothermal reaction and its application to optical sensing of metal ions. Sci China Chem 54:1342–1347CrossRefGoogle Scholar
  10. Liu J, Liu Y, Yang X, Wang K, Wang Q, Shi H, Li L (2013) Exciton energy transfer-based fluorescent sensing through aptamer-programmed self-assembly of quantum dots. Anal Chem 85:1121–11128Google Scholar
  11. Ma Y, Zhang Z, Xu Y, Ma M, Chen B, Wei L, Xiao L (2016) A bright carbon-dot-based fluorescent probe for selective and sensitive detection of mercury ions. Talanta 161:476–481CrossRefGoogle Scholar
  12. Qiu ZL, Shu J, He Y, Lin ZZ, Zhang KY, Lv S, Tang DP (2017) CdTe/CdSe quantum dot-based fluorescent aptasensor with hemin/G-quadruplex DNzyme for sensitive detection of lysozyme using rolling circle amplification and strand hybridization. Biosens Bioelectron 87:18–24CrossRefGoogle Scholar
  13. Shi HJ, Zhao GH, Liu MC, Fan LF, Cao TC (2013) Aptamer-based colorimetric sensing of acetamiprid in soil samples: sensitivity, selectivity and mechanism. J Hazard Mater 260:754–761CrossRefGoogle Scholar
  14. Shi ZH, Zhang SL, Huai QR, Xu D, Zhang HY (2017) Methylamine-modified graphene-based solid phase extraction combined with UPLC-MS/MS for the analysis of neonicotinoid insecticides in sunflower seeds. Talanta 162:300–308CrossRefGoogle Scholar
  15. Taghdisi SM, Danesh NM, Ramezani M, Abnous K (2017) Electrochemical aptamer based assay for the neonicotinoid insecticide acetamiprid based on the use of an unmodified gold electrode. Microchim Acta 184:499–505CrossRefGoogle Scholar
  16. Wang H, Yang RH, Yang L, Tan WH (2009) Nucleic acid conjugated nanomaterials for enhanced molecular recognition. ACS Nano 3:2451–2460CrossRefGoogle Scholar
  17. Wang B, Chen YF, Wu YY, Weng B, Liu YS, Lu ZS, Li CM, Yu C (2016) Aptamer induced assembly of fluorescent nitrogen-doped carbon dots on gold nanoparticles for sensitive detection of AFB1. Biosens Bioelectron 78:23–30CrossRefGoogle Scholar
  18. Wang LJ, Luo ML, Zhang Q, Tang B, Zhang CY (2017) Single quantum dot-based nanosensor for rapid and sensitive detection of terminal deoxynucleotidyl transferase. Chem Commun 53:11016–11019CrossRefGoogle Scholar
  19. Wang ZY, Wang LJ, Zhang Q, Tang B, Zhang CY (2018) Single quantum dot-based nanosensor for sensitive detection of 5-methylcytosine at both CpG and non-CpG sites. Chem Sci 9:1330–1338CrossRefGoogle Scholar
  20. Watanabe E, Miyake S, Baba K, Eun H, Endo S (2006) Immunoassay for acetamiprid detection: application to residue analysis and comparison with liquid chromatography. Anal Bioanal Chem 386:1441–1448CrossRefGoogle Scholar
  21. Wu ZL, Zhang P, Gao MX, Liu CF, Wang W, Leng F, Huang CZ (2013) One-pot hydrothermal synthesis of highly luminescent nitrogen-doped amphoteric carbon dots for bioimaging from Bombyx mori silk–natural proteins. J Mater Chem B 1:2868–2873CrossRefGoogle Scholar
  22. Xiang L, Tang JS (2017) QD-aptamer as a donor for a FRET-based chemosensor and evaluation of affinity between acetamiprid and its aptamer. RSC Adv 7:8332–8337CrossRefGoogle Scholar
  23. Xiong LH, Cui R, Zhang ZL, Yu X, Xie Z, Shi YB, Pang DW (2014) Uniform fluorescent nanobioprobes for pathogen detection. ACS Nano 8(5):5116–5124CrossRefGoogle Scholar
  24. Xu Q, Du S, Jin GD, Li HB, Hu XY (2011) Determination of acetamiprid by a colorimetric method based on the aggregation of gold nanoparticles. Microchim Acta 173:323–329CrossRefGoogle Scholar
  25. Yang L, Zhang X, Ye M, Jiang J, Yang R, Fu T, Chen Y, Wang KM, Liu C, Tan WH (2011) Aptamer-conjugated nanomaterials and their applications. Adv Drug Deliv Rev 63:1361–1370CrossRefGoogle Scholar
  26. Yang Q, Wei L, Zheng X, Xiao L (2015) Single particle dynamic imaging and Fe3+ sensing with bright carbon dots derived from bovine serum albumin proteins. Sci Rep 5:17727CrossRefGoogle Scholar
  27. Yin J, He X, Wang K, Xu F, Shangguan J, He D, Shi H (2013) Label-free and turn-on aptamer strategy for cancer cells detection based on a DNA-silver nanocluster fluorescence upon recognition-induced hybridization. Anal Chem 85:12011–12019CrossRefGoogle Scholar
  28. Zhang L, Cui P, Zhang B, Gao F (2013) Aptamer-based turn-on detection of thrombin in biological fluids based on efficient phosphorescence energy transfer from Mn-doped ZnS quantum dots to carbon Nanodots. Chem Eur J 19(28):9242–9250CrossRefGoogle Scholar
  29. Zhang Y, Chang YQ, Han L, Zhang Y, Chen ML, Shu Y, Wang JH (2017) Aptamer-anchored di-polymer shell-capped mesoporous carbon as a drug carrier for bi-trigger targeted drug delivery. J Mater Chem B 5:6882–6889CrossRefGoogle Scholar
  30. Zhao HX, Liu LQ, Liu ZD, Wang Y, Zhao XJ, Huang CZ (2011) Highly selective detection of phosphate in very complicated matrixes with an off-on fluorescent probe of europium-adjusted carbon dots. Chem Commun 47:2604–2606CrossRefGoogle Scholar
  31. Zhou QX, Ding YJ, Xiao JP (2006) Sensitive determination of thiamethoxam, imidacloprid and acetamiprid in environmental water samples with solid-phase extraction packed with multiwalled carbon nanotubes prior to high-performance liquid chromatography. Anal Bioanal Chem 385:1520–1525CrossRefGoogle Scholar
  32. Zhou J, Yang Y, Zhang CY (2013) A low-temperature solid-phase method to synthesize highly fluorescent carbon nitride dots with tunable emission. Chem Commun 49:8605–8607CrossRefGoogle Scholar
  33. Zhu S, Meng Q, Wang L, Zhang J, Song Y, Jin H, Zhang K, Sun H, Wang H, Yang B (2013) Highly photoluminescent carbon dots for multicolor patterning, sensors, and bioimaging. Angew Chem 125:4045–4049CrossRefGoogle Scholar
  34. Zhu L, Xu G, Song Q, Tang T, Wang X, Wei F, Hu Q (2016) Highly sensitive determination of dopamine by a turn-on fluorescent biosensor based on aptamer labeled carbon dots and nano-graphite. Sensors Actuators B Chem 231:506–512CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media, LLC, part of Springer Nature 2018

Authors and Affiliations

  • Zhe Jiao
    • 1
    Email author
  • Hongfeng Zhang
    • 2
  • Shaohe Jiao
    • 3
  • Zongning Guo
    • 4
  • Dan Zhu
    • 1
  • Xiaofang Zhao
    • 5
  1. 1.School of Environment and Civil EngineeringDongguan University of TechnologyDongguanChina
  2. 2.Guangzhou Center for Disease Control and PreventionGuangzhouChina
  3. 3.Tobacco Science Institute of Jiangxi ProvinceNanchangChina
  4. 4.Integrated Technology Center of Dongguan Entry-Exit Inspection and Quarantine BureauDongguanChina
  5. 5.School of Electrical Engineering and IntelligentizationDongguan University of TechnologyDongguanChina

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