Abstract
A fluorometric and electrochemical dual-mode method is described for sensitive and specific detection of tetracycline (Tc). A novel nanoprobe was designed that is making use of a Tc-specific aptamer (apta), carbon nitride quantum dots (CNQDs) and silver nanoparticles (AgNPs). The aptamer was linked to the CNQDs which then were used as templates to synthesize the apta-CNQD@AgNP nanocomposites. The blue fluorescence of the nanocomposites (with excitation/emission maxima at 365/440 nm) is quenched. The addition of Tc leads to fluorescence recovery and a decrease in the electroconductivity of a gold electrode modified with apta-CNQD@AgNPs. The fluorometric method has a linear response in the 0.1 μM - 10 mM Tc concentration range and a 15 nM detection limit. The amperometric method (best performed at a working voltage of 0.21 V vs. Ag/AgCl) has a linear response in the 1 nM to 0.1 mM Tc concentration range and a 0.26 nM detection limit. Recoveries of Tc from spiked milk samples were comparable to data obtained by HPLC.
Similar content being viewed by others
References
Lan L, Yao Y, ** J, Ying Y (2017) Recent advances in nanomaterial-based biosensors for antibiotics detection. Biosens Bioelectron 91:504–514
Jalalian SH, Karimabadi N, Ramezani M, Abnous K, Taghdisi SM (2018) Electrochemical and optical aptamer-based sensors for detection of tetracyclines. Trends Food Sci Technol 73:45–57
Ramezani M, Danesh NM, Lavaee P, Abnous K, Taghdisi SM (2015) A novel colorimetric triple-helix molecular switch aptasensor for ultrasensitive detection of tetracycline. Biosens Bioelectron 70:181–187
Fritz JW, Zuo Y (2007) Simultaneous determination of tetracycline, oxytetracycline, and 4-epitetracycline in milk by high-performance liquid chromatography. Food Chem 105(3):1297–1301
Wang W, Yu JC, Shen Z, Chan DK, Gu T (2014) G-C3N4 quantum dots: direct synthesis, upconversion properties and photocatalytic application. Chem Commun 50(70):10148–10150
Li H, Shao F-Q, Huang H, Feng J-J, Wang A-J (2016) Eco-friendly and rapid microwave synthesis of green fluorescent graphitic carbon nitride quantum dots for vitro bioimaging. Sensors Actuators B Chem 226:506–511. https://doi.org/10.1016/j.snb.2015.12.018
Cheng Q, He Y, Ge Y, Zhou J, Song G (2018) Ultrasensitive detection of heparin by exploiting the silver nanoparticle-enhanced fluorescence of graphitic carbon nitride (g-C 3 N 4 ) quantum dots. Microchim Acta 185(7):332
Chan MH, Liu RS (2016) Carbon nitride quantum dots and their applications. Springer, Singapore
Liu T, Li N, Dong JX, Zhang Y, Fan YZ, Lin SM, Luo HQ, Li NB (2017) A colorimetric and fluorometric dual-signal sensor for arginine detection by inhibiting the growth of gold nanoparticles/carbon quantum dots composite. Biosens Bioelectron 87:772–778
Jia X, Ji X (2015) Electrochemical probing of carbon quantum dots: not suitable for a single electrode material. RSC Adv 5(130):107270–107275
Wang H, Lu Q, Li M, Li H, Liu Y, Li H, Zhang Y, Yao S (2018) Electrochemically prepared oxygen and sulfur co-doped graphitic carbon nitride quantum dots for fluorescence determination of copper and silver ions and biothiols. Anal Chim Acta 1027:121–129. https://doi.org/10.1016/j.aca.2018.03.063
Seok Kim Y, Ahmad Raston NH, Bock Gu M (2016) Aptamer-based nanobiosensors. Biosens Bioelectron 76:2–19. https://doi.org/10.1016/j.bios.2015.06.040
Hu X, Shi J, Shi Y, Zou X, Arslan M, Zhang W, Huang X, Li Z, Xu Y (2019) Use of a smartphone for visual detection of melamine in milk based on au@carbon quantum dots nanocomposites. Food Chem 272:58–65. https://doi.org/10.1016/j.foodchem.2018.08.021
Hu X, Shi J, Shi Y, Zou X, Tahir HE, Holmes M, Zhang W, Huang X, Li Z, Xu Y (2019) A dual-mode sensor for colorimetric and fluorescent detection of nitrite in hams based on carbon dots-neutral red system. Meat Sci 147:127–134. https://doi.org/10.1016/j.meatsci.2018.09.006
Paramelle D, Sadovoy A, Gorelik S, Free P, Hobley J, Fernig DG (2014) A rapid method to estimate the concentration of citrate capped silver nanoparticles from UV-visible light spectra. Analyst 139(19):4855–4861
Dong J, Zhao Y, Chen HY, Liu L, Zhang W, Sun B, Yang M, Wang Y, Dong L (2018) Fabrication of PEGylated graphitic carbon nitride quantum dots as traceable, pH-sensitive drug delivery systems. New J Chem 42(17):14263–14270
Barman S, Sadhukhan M (2012) Facile bulk production of highly blue fluorescent graphitic carbon nitride quantum dots and their application as highly selective and sensitive sensors for the detection of mercuric and iodide ions in aqueous media. J Mater Chem 22(41):21832–21837
Mandani S, Sharma B, Dey D, Sarma TK (2015) Carbon nanodots as ligand exchange probes in au@C-dot nanobeacons for fluorescent turn-on detection of biothiols. Nanoscale 7(5):1802–1808. https://doi.org/10.1039/C4NR05424E
Zhan Y, Liu Z, Liu Q, Huang D, Wei Y, Hu Y, Lian X, Hu C (2017) A facile and one-pot synthesis of fluorescent graphitic carbon nitride quantum dots for bio-imaging application. New J Chem 41(10):3930–3938
Cao X, Ma J, Lin Y, Yao B, Li F, Wen W, Lin X (2015) A facile microwave-assisted fabrication of fluorescent carbon nitride quantum dots and their application in the detection of mercury ions. Spectrochim Acta A Mol Biomol Spectrosc 151(1):875–880
Song Y, Xu G, Wei F, Cen Y, Sohail M, Shi M, Xu X, Ma Y, Ma Y, Hu Q (2018) Aptamer-based fluorescent platform for ultrasensitive adenosine detection utilizing Fe 3 O 4 magnetic nanoparticles and silver nanoparticles. Microchim Acta 185(2):139
Yu M, Wang H, Fu F, Li L, Li J, Li G, Song Y, Swihart MT, Song E (2017) Dual-recognition Förster resonance energy transfer based platform for one-step sensitive detection of pathogenic Bacteria using fluorescent vancomycin-gold nanoclusters and aptamer-gold nanoparticles. Anal Chem 89(7)
Yiwei X, Wen Z, ** C, Tahir HE, Zhihua L (2018) A self-assembled L-cysteine and electrodeposited gold nanoparticles-reduced graphene oxide modified electrode for adsorptive strip** determination of copper. Electroanalysis 30(1):194–203. https://doi.org/10.1002/elan.201700637
Kashefi-Kheyrabadi L, Mehrgardi MA (2012) Aptamer-conjugated silver nanoparticles for electrochemical detection of adenosine triphosphate. Biosens Bioelectron 37(1):94–98
Liu X, Zheng S, Hu Y, Li Z, Luo F, He Z (2016) Electrochemical Immunosensor based on the chitosan-magnetic nanoparticles for detection of tetracycline. Food Anal Methods 9(10):2972–2978
Wang Y, Hu A (2015) Carbon quantum dots: synthesis, properties and applications. J Funct Mater 2(34):6921–6939
Liu ZH, Ye N, Guo WL, Huang YL, Zhang CP, Guo XH, Huang QY (2009) Development of an ELISA method for multi-residue detecting of tetracyclines. Sci Agric Sin 42(1):318–323
Qi M, Tu C, Dai Y, Wang W, Wang AJ, Chen J (2018) A simple colorimetric analytical assay using gold nanoparticles for specific detection of tetracycline in environmental water sample. Anal Methods 10(27):3402–3407
Shen Z, Zhang C, Yu X, Li J, Wang Z, Zhang Z, Liu B (2018) Microwave synthesis of cyclen functional carbon dots to construct ratiometric fluorescent probe for tetracycline detection. J Mater Chem C 6:9636–9641
Zhang L, Chen L (2016) Fluorescence probe based on hybrid mesoporous silica/quantum dot/molecularly imprinted polymer for detection of tetracycline. ACS Appl Mater Interfaces 8(25):16248–16256. https://doi.org/10.1021/acsami.6b04381
Li X, Hong M, Min D, Iqbal A, Liu X, Bo L, Liu WS, Li J, Qin W (2017) Europium functionalized Ratiometric fluorescent transducer silicon nanoparticles based on FRET for highly sensitive detection of tetracycline. J Mater Chem C 5(1–8):2149–2152
Le T, Phuc Pham V, La H, Binh Phan T, Huan Le Q (2016) Electrochemical aptasensor for detecting tetracycline in milk. Adv Nat Sci 7(1):015008. https://doi.org/10.1088/2043-6262/7/1/015008
Tang Y, Liu P, Xu J, Li L, Yang L, Liu X, Liu S, Zhou Y (2018) Electrochemical aptasensor based on a novel flower-like TiO2 nanocomposite for the detection of tetracycline. Sensors Actuators B Chem 258:906–912. https://doi.org/10.1016/j.snb.2017.11.071
Cui R, Pan H-C, Zhu J-J, Chen H-Y (2007) Versatile immunosensor using CdTe quantum dots as electrochemical and fluorescent labels. Anal Chem 79(22):8494–8501
Acknowledgments
The authors gratefully acknowledge the financial support provided by the National Natural Science Foundation of China (31671844, 31601543), National Key Technology Research and Development Program of China (2018YFD040080, 2017YFC1600805, 2017YFC1600806) and Six Talent Peaks Project in Jiangsu Province (GDZB-016).
Author information
Authors and Affiliations
Corresponding authors
Ethics declarations
Conflict of interest
The authors declare that they have no conflict of interest.
Informed consent
Informed consent is not applicable for the nature of this study.
Additional information
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Electronic supplementary material
ESM 1
(DOC 5513 kb)
Rights and permissions
About this article
Cite this article
Hu, X., Xu, Y., Cui, X. et al. Fluorometric and electrochemical dual-mode nanoprobe for tetracycline by using a nanocomposite prepared from carbon nitride quantum dots and silver nanoparticles. Microchim Acta 187, 83 (2020). https://doi.org/10.1007/s00604-019-3828-4
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s00604-019-3828-4