Skip to main content
SpringerLink
Log in

Facile synthesis of highly efficient fluorescent carbon dots for tetracycline detection

  • Short Research and Discussion Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Rampant use of tetracycline in animal feed is a threat to food security, the environment, and human health because of the risk of drug residues. Therefore, it is necessary to establish a sensitive, efficient, and reliable method for qualitative and quantitative detection of tetracycline. In this paper, we synthesized fluorescent carbon dots (FCDs) by thermal cracking of crab shell waste, and obtained a fluorescence quantum yield of 30%. Characterization of the FCDs by transmission electron microscopy, Fourier-transform infrared spectroscopy, ultraviolet visible absorption spectroscopy, and photoluminescence spectroscopy showed that they were fluorescent and evenly distributed with an average size of approximately 10 nm. We designed a sensitive probe for detecting tetracycline using the fluorescence intensity change of the FCDs. This method is sensitive, inexpensive, and environmentally friendly. The concentration of tetracycline was examined by comparing the fluorescence intensities of the FCDs before and after tetracycline addition. The limit of detection for tetracycline was 0.005 mg/L (signal-to-noise ratio = 3), which is promising for method development.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8

Similar content being viewed by others

References

  • Ahn HJ, Lee JH, Jeong Y, Lee JH, Chi CS, Oh HJ (2007) Nanostructured carbon cloth electrode for desalination from aqueous solutions. Mater Sci Eng A 449:841–845

    Article  CAS  Google Scholar 

  • Baker SN, Baker GA (2011) ChemInform abstract: luminescent carbon nanodots: emergent nanolights. cheminform 42

  • Blasco C, Corcia AD, Picó Y (2009) Determination of tetracyclines in multi-specie animal tissues by pressurized liquid extraction and liquid chromatography–tandem mass spectrometry. Food Chem 116:1005–1012

    Article  CAS  Google Scholar 

  • Breton MHL, Savoy-Perroud MC, Diserens JM (2007) Validation and comparison of the Copan Milk Test and Delvotest SP-NT for the detection of antimicrobials in milk. Anal Chim Acta 586:280–283

    Article  CAS  Google Scholar 

  • Cai W, Huang H, Li C, Zhang J, Zeng H (2018) Effects of humus on heavy metals absorption of maize in heavy metal contaminated soil. IOP Conference Series Materials Science and Engineering 394

  • Chee-Sanford JC, Mackie RI, Koike S, Krapac IG, Lin YF, Yannarell AC, Maxwell S, Aminov RI (2009) Fate and transport of antibiotic residues and antibiotic resistance genes following land application of manure waste. J Environ Qual 38:1086–1108

    Article  CAS  Google Scholar 

  • Chen J (2018) Analysis of adverse effects of penicillin combined with chloramphenicol and tetracycline. China Continuing Medical Education

  • Conzuelo F, Campuzano S, Gamella M, Pinacho DG, Reviejo AJ, Marco MP, Pingarrón JM (2013) Integrated disposable electrochemical immunosensors for the simultaneous determination of sulfonamide and tetracycline antibiotics residues in milk. Biosens Bioelectron 50:100–105

    Article  CAS  Google Scholar 

  • Cui X, Chemistry DO, University QN (2014) SWCNTs quenching CdTe quantum dots fluorescence nanosensing system for determination of thrombin. Journal of Qinghai Normal University 4:38–40

  • Ganiga M, Cyriac J (2017) Direct one pot synthesis of blue luminescent polymeric carbon dots gel and their application for selective detection of Ag+ Ions. Soft Materials

  • Garg D, Mehta A, Mishra A, Basu S (2018) A sensitive turn on fluorescent probe for detection of biothiols using MnO2@carbon dots nanocomposites. Spectrochim Acta A Mol Biomol Spectrosc 192:411–419

    Article  CAS  Google Scholar 

  • Huang S, Shi HE, Wei X, Xue G, Gao P (2015) Pollution characteristics of tetracycline residues and tetracycline resistance genes in sewage treatment plants:A review. Chem Ind Eng Prog 43:232–239

    Google Scholar 

  • Ibarra IS, Rodriguez JA, Miranda JM, Marisol V, Enrique B (2011) Magnetic solid phase extraction based on phenyl silica adsorbent for the determination of tetracyclines in milk samples by capillary electrophoresis. J Chromatogr A 1218:2196–2202

    Article  CAS  Google Scholar 

  • Jeon M, Kim J, Paeng KJ, Park SW, Paeng IR (2008) Biotin–avidin mediated competitive enzyme-linked immunosorbent assay to detect residues of tetracyclines in milk. Microchem J 88:26–31

    Article  CAS  Google Scholar 

  • Ji H, Zhou F, Gu J, Shu C, Xi K, Jia X (2016) Nitrogen-doped carbon dots as a new substrate for sensitive glucose determination. Sensors 16:630

    Article  CAS  Google Scholar 

  • Kim YJ, Kim YS, Niazi JH, Gu MB (2010) Electrochemical aptasensor for tetracycline detection. Bioprocess Biosyst Eng 33:31–37. https://doi.org/10.1007/s00449-009-0371-4

    Article  CAS  Google Scholar 

  • Li Y, Gao F, Gao F, Shan F, Bian J, Zhao C (2009) Study on the interaction between 3 flavonoid compounds and alpha-amylase by fluorescence spectroscopy and enzymatic kinetics. J Food Sci 74:C199–C203

    Article  CAS  Google Scholar 

  • Li H, He X, Liu Y, Huang H, Lian S, Lee ST, Kang Z (2011) One-step ultrasonic synthesis of water-soluble carbon nanoparticles with excellent photoluminescent properties. Carbon 49:605–609

    Article  CAS  Google Scholar 

  • Li F, Cao X, Zhao L, Wang J, Ding Z (2014) Effects of mineral additives on biochar formation: carbon retention, stability, and properties. Environ Sci Technol 48:11211–11217

    Article  CAS  Google Scholar 

  • Li J, Cai F, Dong Y, Zhu Z, Sun X, Zhang H, He S (2017a) A portable confocal hyperspectral microscope without any scan or tube lens and its application in fluorescence and Raman spectral imaging. Opt Commun 392:1–6

    Article  CAS  Google Scholar 

  • Li J, Zuo G, Pan X, Wei W, Qi X, Su T, Dong W (2017b) Nitrogen-doped carbon dots as a fluorescent probe for the highly sensitive detection of Ag+ and cell imaging. Luminescence 33:243–248

    Article  CAS  Google Scholar 

  • Linage B, Gonzalo C, Carriedo JA, Asensio JA, Blanco MA, De La Fuente LF, San Primitivo F (2007) Performance of blue-yellow screening test for antimicrobial detection in ovine milk. J Dairy Sci 90:5374–5379

    Article  CAS  Google Scholar 

  • Liu JM, Lin LP, Wang XX, Lin SQ, Cai WL, Zhang LH, Zheng ZY (2012a) Highly selective and sensitive detection of Cu2+ with lysine enhancing bovine serum albumin modified-carbon dots fluorescent probe. Analyst 137:2637–2642

    Article  CAS  Google Scholar 

  • Liu Y, Liu C, Zhang Z (2012b) Synthesis of highly luminescent graphitized carbon dots and the application in the Hg2+ detection. Appl Surf Sci 263:481–485

    Article  CAS  Google Scholar 

  • Liu R, Li H, Kong W, Liu J, Liu Y, Tong C, Zhang X, Kang Z (2013) Ultra-sensitive and selective Hg2+ detection based on fluorescent carbon dots. Mater Res Bull 48:2529–2534

    Article  CAS  Google Scholar 

  • Loo AH, Sofer Z, Bouša D, Ulbrich P, Bonanni A, Pumera M (2016) Carboxylic carbon quantum dots as a fluorescent sensing platform for DNA detection. ACS Appl Mater Interfaces 8:1951–1957

    Article  CAS  Google Scholar 

  • Ma H, Liu X, Wang X, Li X, Yang C, Iqbal A, Liu W, Li J, Qin W (2016) Sensitive fluorescent light-up probe for enzymatic determination of glucose using carbon dots modified with MnO2 nanosheets. Microchim Acta 184:1–9

    Google Scholar 

  • Min Z, Shaobo R, Shi L, Tingting S, Dan Q, Haifeng Z, Zhigang X, Huile G, Xiabin J, Zaicheng S (2015) Self-targeting fluorescent carbon dots for diagnosis of brain cancer cells. ACS Nano 9:11455

    Article  CAS  Google Scholar 

  • Moussout H, Ahlafi H, Aazza M, Bourakhouadar M (2016) Kinetics and mechanism of the thermal degradation of biopolymers chitin and chitosan using thermogravimetric analysis. Polym Degrad Stab 130:1–9

    Article  CAS  Google Scholar 

  • Qin J, Xie L, Ying Y (2016) Rapid determination of tetracyclines hydrochloride using ATR FT-MIR spectroscopy. Food Anal Methods 9:2880–2886

    Article  Google Scholar 

  • Qiu T, Gao M, Han M (2015) Decreases of Tetracyclines and antibiotics-resistant bacteria during composting of chicken manure. Journal of Agro-Environment Science 34:795–800

  • Qu K, Wang J, Ren J, Qu X (2013) Carbon dots prepared by hydrothermal treatment of dopamine as an effective fluorescent sensing platform for the label-free detection of iron(III) ions and dopamine. Chemistry 19:7243–7249

    Article  CAS  Google Scholar 

  • Sarmah AK, Meyer MT, Boxall ABA (2006) A global perspective on the use, sales, exposure pathways, occurrence, fate and effects of veterinary antibiotics (VAs) in the environment. Chemosphere 65:725–759

    Article  CAS  Google Scholar 

  • Shalaby AR, Salama NA, Abou-Raya SH, Emam WH, Mehaya FM (2011) Validation of HPLC method for determination of tetracycline residues in chicken meat and liver. Food Chem 124:1660–1666

    Article  CAS  Google Scholar 

  • Shan X, Chai L, Ma J, Qian Z, Chen J, Feng H (2014) B-doped carbon quantum dots as a sensitive fluorescence probe for hydrogen peroxide and glucose detection. Analyst 139:2322–2325

    Article  CAS  Google Scholar 

  • Shen F, Fu J, Zhang X, Qi X (2019) Crab shell-derived lotus rootlike porous carbon for high efficiency isomerization of glucose to fructose under mild conditions. ACS Sustain Chem Eng 7:4466–4472. https://doi.org/10.1021/acssuschemeng.8b06512

    Article  CAS  Google Scholar 

  • Sun Q, Long Y, Pan S, Liu H, Yang J, Hu X (2018) Carbon dot-based fluorescent probes for sensitive and selective detection of luteolin through the inner filter effect. Luminescence 33:1401–1407. https://doi.org/10.1002/bio.3562

    Article  CAS  Google Scholar 

  • Wang YP, Ma Y (2008) Potential public hazard of using antibiotics in livestock industry. Chin J Antibiot 33:519–523

    Google Scholar 

  • Wang ZF, Zeng S, Li Y, Wang W, Zhang Z, Zeng H, Wang W, Sun L (2017) Luminescence mechanism of carbon-incorporated silica nanoparticles derived from rice husk biomass. Ind Eng Chem Res 56:5906–5912

    Article  CAS  Google Scholar 

  • Wang Y, Jie X, Li L, Wang F, Xu Z, Wen Z (2018) Multi-functional carbon dots-based nanoprobe for ratiometric enzyme reaction monitoring and biothiol analysis. Sensors Actuators B Chem 264:296–303

    Article  CAS  Google Scholar 

  • Wenjun B, Huzhi Z, Yijuan L, Xiaojiao M, Mei G, Lingyan Z (2011) A carbon dots-based fluorescence turn-on method for DNA determination. Anal Sci 27:243

    Article  Google Scholar 

  • Yan Y, Liu JH, Li RS, Li YF, Huang CZ, Zhen SJ (2019) Carbon dots synthesized at room temperature for detection of tetracycline hydrochloride. Anal Chim Acta 1063:144–151

    Article  CAS  Google Scholar 

  • Yu J, Song N, Zhang YK, Zhong SX, Wang AJ, Chen J (2015) Green preparation of carbon dots by Jinhua bergamot for sensitive and selective fluorescent detection of Hg2+ and Fe3+. Sensors Actuators B Chem 214:29–35

    Article  CAS  Google Scholar 

  • Yu S, Chen K, Wang F, Zhu Y, Zhang X (2017) Polymer composite fluorescent hydrogel film based on nitrogen-doped carbon dots and their application in the detection of Hg2+ ions. Luminescence 32:970–977

    Article  CAS  Google Scholar 

  • Yu J, Liu C, Yuan K, Lu Z, Cheng Y, Li L, Zhang X, Jin P, Meng F, Liu H (2018) Luminescence mechanism of carbon dots by tailoring functional groups for sensing Fe3+ ions. Nanomaterials 8:233

    Article  CAS  Google Scholar 

  • Zhang HM, Zhang MK, Guo-Ping GU (2008) Residues of Tetracyclines in livestock and poultry manures and agricultural soils from north Zhejiang province. J Ecol Rural Environ 24:69–73

    Google Scholar 

  • Zhang W, Ren G, Xu H, Zhang J, Liu H, Mu S, Cai X, Wu T (2016) Genipin cross-linked chitosan hydrogel for the controlled release of tetracycline with controlled release property, lower cytotoxicity, and long-term bioactivity. J Polym Res 23:156

    Article  CAS  Google Scholar 

  • Zhang S, Lin B, Yu Y, Cao Y, Guo M, Shui L (2018) A ratiometric nanoprobe based on silver nanoclusters and carbon dots for the fluorescent detection of biothiols. Spectrochim Acta A Mol Biomol Spectrosc 195:230–235

    Article  CAS  Google Scholar 

  • Zhu W, Jian Z, Jiang Z, Wang W, Liu X (2014) High-quality carbon dots: synthesis, peroxidase-like activity and their application in the detection of H2O2, Ag+ and Fe3+. RSC Adv 4:17387–17392

    Article  CAS  Google Scholar 

  • Zong J, Yang X, Trinchi A, Hardin S, Cole I, Zhu Y, Li C, Muster T, Wei G (2014) Carbon dots as fluorescent probes for "off-on" detection of Cu2+ and L-cysteine in aqueous solution. Biosens Bioelectron 51:330–335

    Article  CAS  Google Scholar 

  • Zu F, Yan F, Bai Z, Xu J, Wang Y, Huang Y, Zhou X (2017) The quenching of the fluorescence of carbon dots: a review on mechanisms and applications. Microchim Acta 184:1899–1914

    Article  CAS  Google Scholar 

Download references

Acknowledgments

We thank Gabrielle David, PhD, for editing the English text of a draft of this manuscript.

Funding

The authors received financial support from China National Natural Science Foundation (no: 31270620) and Dalian Scientific and Technological Innovation Foundation (no: 2018J12SN072).

Author information

Authors and Affiliations

  1. School of Ocean Science and Technology, Dalian University of Technology, Panjin Campus, Liaoning, China

    Feng Guo, Zihan Zhu, Zhangqin Zheng, Ying Jin, Xiaoxuan Di, Zhonghao Xu & Hongwei Guan

Authors
  1. Feng Guo
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Zihan Zhu
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Zhangqin Zheng
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Ying Jin
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Xiaoxuan Di
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Zhonghao Xu
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Hongwei Guan
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

Author Feng Guo, Zihan Zhu, Zhangqin Zheng, Ying Jin, Xiaoxuan Di, Zhonghao Xu, and Hongwei Guan aided in preparing/carrying out all the experiments and in drafting the manuscript. Feng Guo and Zihan Zhu designed and led all the experiments and the construction of the final version of the submitted manuscript.

Corresponding author

Correspondence to Feng Guo.

Additional information

Responsible editor: Philippe Garrigues

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Electronic supplementary material

ESM 1

(PPTX 259 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Guo, F., Zhu, Z., Zheng, Z. et al. Facile synthesis of highly efficient fluorescent carbon dots for tetracycline detection. Environ Sci Pollut Res 27, 4520–4527 (2020). https://doi.org/10.1007/s11356-019-06779-3

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-019-06779-3

Keywords

Search

Navigation