Advertisement

Microchimica Acta

, 185:461 | Cite as

Microwave-assisted synthesis of thymine-functionalized graphitic carbon nitride quantum dots as a fluorescent nanoprobe for mercury(II)

  • Ojodomo J. Achadu
  • Neerish Revaprasadu
Original Paper
  • 68 Downloads

Abstract

A microwave-assisted hydrothermal method was employed to prepare thymine-modified graphitic carbon nitride quantum dots (T-gCNQDs) which are shown to be a novel fluorescent nanoprobe for Hg(II). They exhibit excellent optical properties (blue emission with a fluorescence quantum yield of 46%) and water solubility. The incorporation of thymine into the gCNQDs results in an enhancement in photoluminescence properties. It is found that fluorescence, best measured at excitation/emission wavelengths of 350/445 nm, is much more strongly quenched by Hg(II) compared to the thymine-free nanoprobe. The quenching is highly selective even in the presence other metal ions. This is ascribed to the formation of T-Hg(II)-T base complexes. Fluorescence drops linearly in the 1.0 to 500 nM Hg(II) concentration range, and the limit of detection is 0.15 nM. The method was applied to the determination of Hg(II) in spiked samples of tap and pond water. Recoveries were found to be >95%, thus demonstrating the practical applicability of the assay.

Graphical abstract

A microwave-assisted hydrothermal route was employed to prepare thymine-functionalized graphitic carbon nitride QDs (T-gCNQDs). A selective fluorescence quenching mechanism occurred between T-gCNQDs and Hg(II) due to thymine functionalization. T-gCNQDs was utilized to detect Hg(II) in real samples.

Keywords

Thymine Thymine-modified graphitic carbon nitride quantum dots Fluorescence quenching Stern-Volmer plot Nanoprobe 

Notes

Acknowledgements

The authors acknowledge the National Research Foundation (NRF), South Africa through the South African Research Chair Initiative (SARChI). OJA thanks the National Research Foundation (NRF) for a postdoctoral fellowship and funding under SA Research Chair for Nanotechnology.

Compliance with ethical standards

The author(s) declare that they have no competing interests.

Supplementary material

604_2018_3004_MOESM1_ESM.docx (239 kb)
ESM 1 (DOCX 239 kb)

References

  1. 1.
    Kim KH, Kabir E, Jahan SA (2016) A review on the distribution of hg in the environment and its human health impacts. J Hazard Mater 306:376–385CrossRefGoogle Scholar
  2. 2.
    Oehme I, Wolfbeis OS (1997) Optical sensors for determination of heavy metal ions. Microchim Acta 126:177–192CrossRefGoogle Scholar
  3. 3.
    Ding Y, Wang S, Li J, Chen L (2016) Nanomaterial-based optical sensors for mercury ions. Trends Anal Chem 82:175–190CrossRefGoogle Scholar
  4. 4.
    Shah AQ, Kazi TG, Baig JA, Afridi HI, Arain MB (2012) Simultaneously determination of methyl and inorganic mercury in fish species by cold vapour generation atomic absorption spectrometry. Food Chem 134:2345–2349CrossRefGoogle Scholar
  5. 5.
    de Souza SS, Campiglia AD, Barbosa F (2013) A simple method for methylmercury, inorganic mercury and ethylmercury determination in plasma samples by high performance liquid chromatography–cold-vapor-inductively coupled plasma mass spectrometry. Anal Chim Acta 761:11–17CrossRefGoogle Scholar
  6. 6.
    Yan F, Kong D, Luo Y, Ye Q, He J, Guo X, Chen L (2016) Carbon dots serve as an effective nanosensor for the quantitative determination and for intracellular imaging of mercury(II). Microchim Acta 183:1611–1618CrossRefGoogle Scholar
  7. 7.
    Xu H, Zhang K, Liu Q, Liu Y, Xie M (2017) Visual and fluorescent detection of mercury ions by using a dually emissive ratiometric nanohybrid containing carbon dots and CdTe quantum dots. Microchim Acta 184:1199–1206CrossRefGoogle Scholar
  8. 8.
    Zarlaida F, Adlim M (2017) Gold and silver nanoparticles and indicator dyes as active agents in colorimetric spot and strip tests for mercury(II) ions: a review. Microchim Acta 184:45–58.  https://doi.org/10.1007/s00604-016-1967-4 CrossRefGoogle Scholar
  9. 9.
    Zaib M, Athar MM, Saeed A, Farooq U (2015) Electrochemical determination of inorganic mercury and arsenic – a review. Biosens Bioelectron 74:895–908CrossRefGoogle Scholar
  10. 10.
    Abdelhamid HN, Wu HF (2015) Reduced graphene oxide conjugate thymine as a new nanosensor for ultrasensitive and selective fluorometric determination of mercury (II) ions. Microchim Acta 182:1609–1617CrossRefGoogle Scholar
  11. 11.
    Wolfbeis OS (2005) Materials for fluorescence-based optical chemical sensors. J Mater Chem 15:2657–2669CrossRefGoogle Scholar
  12. 12.
    Gao M, Tang BZ (2017) Fluorescent sensors based on aggregation-induced emission: recent advances and perspectives. ACS Sens 2:1382–1399CrossRefGoogle Scholar
  13. 13.
    Benítez-Martínez S, Valcárcel M (2015) Graphene quantum dots in analytical science. Trends Anal Chem 72:93–113CrossRefGoogle Scholar
  14. 14.
    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 22:21832–21837CrossRefGoogle Scholar
  15. 15.
    Zhuang Q, Sun L, Ni Y (2017) One-step synthesis of graphitic carbon nitride nanosheets with the help of melamine and its application for fluorescence detection of mercuric ions. Talanta 164:458–462CrossRefGoogle Scholar
  16. 16.
    Li Y, Cai J, Liu F, Yu H, Lin F, Yang H, Lin Y, Li S (2018) Highly crystalline graphitic carbon nitride quantum dots as a fluorescent nanosensor for detection of Fe(III) via an innner filter effect. Microchim Acta 185:134–140CrossRefGoogle Scholar
  17. 17.
    Niu X, Zhang H, Xu L, Zhao S, Chen H, Chen X (2015) Switch-on fluorescence sensing of glutathione in food samples based on a graphitic carbon nitride quantum dot (gCNQDs-Hg2+) chemosensor. J Agric Food Chem 63:1747–1755CrossRefGoogle Scholar
  18. 18.
    Shiravanda G, Badiei A, Ziarani GM (2017) Carboxyl-rich g-C3N4 nanoparticles: synthesis, characterization and their application for selective fluorescence sensing of Hg2+ and Fe3+ in aqueous media. Sensors Actuators B Chem 242:244–252CrossRefGoogle Scholar
  19. 19.
    Zhang S, Li J, Zeng M, Xu J, Wang X, Hu W (2014) Polymer nanodots of graphitic carbon nitride as effective fluorescent nanosensors for the detection of Fe3+ and Cu2+ ions. Nanoscale 6:4157–4162CrossRefGoogle Scholar
  20. 20.
    Guo J, Lin Y, Huang H, Zhang S, Huang T, Weng W (2017) One-pot fabrication of fluorescent carbon nitride nanoparticles with high crystallinity as a highly selective and sensitive sensor for free chlorine. Sensors Actuators B Chem 244:965–971CrossRefGoogle Scholar
  21. 21.
    Rong M, Lin L, Song X, Wang Y, Zhong Y, Yan J, Feng Y, Zeng X, Chen X (2015) Fluorescence sensing of chromium (VI) and ascorbic acid using graphitic carbon nitride nanosheets as a fluorescent switch. Biosens Bioelectron 68:210–217CrossRefGoogle Scholar
  22. 22.
    Miyake Y, Togashi H, Tashiro M, Yamaguchi H, Oda S, Kudo M, Tanaka Y, Kondo Y, Sawa R, Fujimoto T, Machinami T, Ono A (2006) MercuryII-mediated formation of thymine – HgII – thymine base pairs in DNA duplexes. J Am Chem Soc 128:2172–2173CrossRefGoogle Scholar
  23. 23.
    Achadu OJ, Nyokong T (2017) In situ one-pot synthesis of graphitic carbon nitride quantum dots and its 2, 2, 6, 6-tetramethyl (piperidin-1-yl) oxyl derivatives as fluorescent nanosensors for ascorbic acid. Anal Chim Acta 991:113–126CrossRefGoogle Scholar
  24. 24.
    Zhu S, Song Y, Zhao X, Shao J, Zhang J, Yang B (2015) The photoluminescence mechanism in carbon dots (graphene quantum dots, carbon nanodots, and polymer dots): current state and future perspective. Nano Res 8:355–381CrossRefGoogle Scholar
  25. 25.
    Cayuela A, Soriano ML, Carrillo-Carrión C, Valcárcel M (2016) Semiconductor and carbon-based fluorescent nanodots: the need for consistency. Chem Commun 52:1311–1326CrossRefGoogle Scholar
  26. 26.
    Zhang J, Tang Y, Lv J, Fang SQ, Tang DP (2015) Glucometer-based quantitative determination of Hg(II) using gold particle encapsulated invertase and strong thymine-Hg(II)-thymine interaction for signal amplification. Microchim Acta 182:1153–1159CrossRefGoogle Scholar
  27. 27.
    Liu S, Leng X, Wang X, Pei Q, Cui X, Wang Y, Huang J (2017) Enzyme-free colorimetric assay for mercury(II) using DNA conjugated to gold nanoparticles and strand displacement amplification. Microchim Acta 184:1969–1976CrossRefGoogle Scholar
  28. 28.
    Li L, Zhang L, Zhao Y, Chen Z (2018) Colorimetric detection of Hg(II) by measurement the color alterations from the “before” and “after” RGB images of etched triangular silver nanoplates. Microchim Acta 185:235–241CrossRefGoogle Scholar
  29. 29.
    Li MK, Hu LY, Niu CG, Huang DW, Zeng GM (2018) A fluorescent DNA based nanosensor for Hg(II) based on thymine-Hg(II)-thymine interaction and enrichment via magnetized graphene oxide. Microchim Acta 185:207–213CrossRefGoogle Scholar
  30. 30.
    Chen Z, Zhang C, Tan Y, Zhou T, Ma H, Wan C, Lin Y, Li K (2014) Chitosan-functionalized gold nanoparticles for colorimetric detection of mercury ions based on chelation-induced aggregation. Microchim Acta 182:611–616CrossRefGoogle Scholar
  31. 31.
    Xu Y, Li H, Wang B, Liu H, Zhao L, Zhou T, Liu M, Huang N, Li Y, Ding L, Chen Y (2018) Microwave-assisted synthesis of carbon dots for "turn-on" fluorometric determination of Hg(II) via aggregation-induced emission. Microchim Acta 185:252–258CrossRefGoogle Scholar
  32. 32.
    Zangeneh Kamali K, Pandikumar A, Jayabal S, Ramaraj R, Lim HN, Ong BO, Bien CSD, Kee YY, Huang NM (2016) Amalgamation based optical and colorimetric sensing of mercury(II) ions with silver@graphene oxide nanocomposite materials. Microchim Acta 183:369–377CrossRefGoogle Scholar
  33. 33.
    Jiang Y, Tian J, Hu K, Zhao Y, Zhao S (2014) Sensitive aptamer-based fluorescence polarization assay for mercury(II) ions and cysteine using silver nanoparticles as a signal amplifier. Microchim Acta 181:1423–1430CrossRefGoogle Scholar
  34. 34.
    Lu Y, Chen J, Wang A, Bao N, Feng J, Wang W, Shao L (2015) Facile synthesis of oxygen and sulfur co-doped graphitic carbon nitride fluorescent quantum dots and their application for mercury(II) detection and bioimaging. J Mater Chem C 3:73–78CrossRefGoogle Scholar
  35. 35.
    Shamsipur M, Safavi A, Mohammadpour Z, Ahmadi R (2016) Highly selective aggregation assay for visual detection of mercury ion based on competitive binding of sulfur-doped carbon nanodots to gold nanoparticles and mercury ions. Microchim Acta 183:2327–2335CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Austria, part of Springer Nature 2018

Authors and Affiliations

  1. 1.Department of ChemistryUniversity of ZululandKwaDlangezwaSouth Africa

Personalised recommendations