Pre-Concentration and Determination of Tetracyclines Antibiotics Residues in Water Samples Using RGO/Fe3O4 Nanocomposite as Extraction Sorbent

https://doi.org/10.22146/ijc.64414

Ungku Amirul Arif Ungku Abdullah(1), Nor Suhaila Mohamad Hanapi(2*), Wan Nazihah Wan Ibrahim(3), Nursyamsyila Mat Hadzir(4), Nurzaimah Zaini(5), Ahmad Lutfi Anis(6), Noorfatimah Yahaya(7)

(1) School of Chemistry and Environment, Faculty of Applied Sciences, Universiti Teknologi MARA, 40450 Shah Alam, Selangor, Malaysia
(2) School of Chemistry and Environment, Faculty of Applied Sciences, Universiti Teknologi MARA, 40450 Shah Alam, Selangor, Malaysia
(3) School of Chemistry and Environment, Faculty of Applied Sciences, Universiti Teknologi MARA, 40450 Shah Alam, Selangor, Malaysia
(4) School of Chemistry and Environment, Faculty of Applied Sciences, Universiti Teknologi MARA, 40450 Shah Alam, Selangor, Malaysia
(5) School of Chemistry and Environment, Faculty of Applied Sciences, Universiti Teknologi MARA, 40450 Shah Alam, Selangor, Malaysia
(6) Faculty of Applied Sciences, Universiti Teknologi MARA, 94300 Kota Samarahan, Sarawak, Malaysia
(7) Integrative Medicine Cluster, Advanced Medical and Dental Institute (AMDI), Universiti Sains Malaysia, 13200 Bertam Kepala Batas, Penang, Malaysia
(*) Corresponding Author

Abstract


Existing methods used in tracing Tetracyclines' antibiotics (TCAs) residues which pose serious environmental problems, consume high amounts of organic solvents, are time-consuming, and are relatively expensive. A simple and effective magnetic solid-phase extraction (MSPE) based on reduced graphene oxide/magnetite (RGO/Fe3O4) nanocomposite sorbent was successfully developed for preconcentration and extraction of TCAs residues from water samples. The analytes were determined by high-performance liquid chromatography with a diode-array detector (HPLC-DAD). The synthesized nanocomposite was characterized using Fourier-transform infrared spectroscopy (FTIR), X-ray diffractometry (XRD), and field emission scanning electron microscopy (FESEM). Sample pH, amount of adsorbent, sample volume, extraction time, desorption time, and desorption solvent were evaluated and optimized. Under optimized conditions, the method demonstrated good linearity over the concentration range of 0.05–1.0 mg L–1 with the coefficient of determination (R2) ≥ 0.9978. Limit of detection (LOD) and limit of quantification (LOQ) were 0.006–0.011 mg L–1 and 0.019–0.036 mg L–1, respectively. The accuracy and precision of the developed method were proven by good analyte recovery (89.77–106.33%) and acceptable precision with relative standard deviation, RSD ≤ 5.54%. The results showed that magnetic solid RGO/Fe3O4 could be a suitable adsorbent in the preconcentration and extraction of TCAs in water samples.


Keywords


magnetic solid-phase extraction; reduced graphene oxide/magnetite; tetracycline antibiotics; water samples

Full Text:

Full Text PDF


References

[1] Hernández, M., Borrull, F., and Calull, M., 2003, Analysis of antibiotics in biological samples by capillary electrophoresis, TrAC, Trends Anal. Chem., 22 (7), 416–427.

[2] Borghi, A.A., and Palma, M.S.A., 2014, Tetracycline: Production, waste treatment and environmental impact assessment, Braz. J. Pharm. Sci., 50 (1), 25–40.

[3] Grenni, P., Ancona, V., and Caracciolo, A.B., 2018, Ecological effects of antibiotics on natural ecosystems: A review, Microchem. J., 136, 25–39.

[4] Chee‐Sanford, J.C., Mackie, R.I., Koike, S., Krapac, I.G., Lin, Y.F., Yannarell, A.C., Maxwell, S., and Aminov, R.I., 2009, Fate and transport of antibiotic residues and antibiotic resistance genes following land application of manure waste, J. Environ. Qual., 38 (3), 1086–1108.

[5] Daghrir, R., and Drogui, P., 2013, Tetracycline antibiotics in the environment: A review, Environ. Chem. Lett., 11 (3), 209–227.

[6] Khatibi, S.A., Hamidi, S., and Siahi-Shadbad, M.R., 2020, Application of liquid-liquid extraction for the determination of antibiotics in the foodstuff: Recent trends and developments, Crit. Rev. Anal. Chem., 0 (0), 1–16.

[7] Barbera, G.L., Capriotti, A.L., Cavaliere, C., Foglia, P., Montone, C.M., Chiozzi, R.Z., and Laganà, A., 2017, A rapid magnetic solid phase extraction method followed by liquid chromatography-tandem mass spectrometry analysis for the determination of mycotoxins in cereals, Toxins, 9 (4), 147.

[8] Kabir, A., Locatelli, M., and Ulusoy, H.I., 2017, Recent trends in microextraction techniques employed in analytical and bioanalytical sample preparation, Separations, 4 (4), 36.

[9] Gaudin, V., 2017, Advances in biosensor development for the screening of antibiotic residues in food products of animal origin–A comprehensive review, Biosens. Bioelectron., 90, 363–377.

[10] Herrero-Latorre, C., Barciela-García, J., García-Martín, S., Peña-Crecente, R.M., and Otárola-Jiménez, J., 2015, Magnetic solid-phase extraction using carbon nanotubes as sorbents: A review, Anal. Chim. Acta, 892, 10–26.

[11] Zhao, G., Song, S., Wang, C., Wu, Q., and Wang, Z., 2011, Determination of triazine herbicides in environmental water samples by high-performance liquid chromatography using graphene-coated magnetic nanoparticles as adsorbent, Anal. Chim. Acta, 708 (1-2), 155–159.

[12] Liu, S., Yu, B., Wang, S., Shen, Y., and Cong, H., 2020, Preparation, surface functionalization and application of Fe3O4 magnetic nanoparticles, Adv. Colloid Interface Sci., 281, 102165.

[13] Shen, Y.F., Tang, J., Nie, Z.H., Wang, Y.D., Ren, Y., and Zuo, L., 2009, Preparation and application of magnetic Fe3O4 nanoparticles for wastewater purification, Sep. Purif. Technol., 68 (3), 312–319.

[14] Zhang, Y., Chen, B., Zhang, L., Huang, J., Chen, F., Yang, Z., Yao, J., and Zhang, Z., 2011, Controlled assembly of Fe3O4 magnetic nanoparticles on graphene oxide, Nanoscale, 3 (4), 1446–1450.

[15] Liu, W.W., Chai, S.P., Mohamed, A.R., and Hashim, U., 2014, Synthesis and characterization of graphene and carbon nanotubes: A review on the past and recent developments, J. Ind. Eng. Chem., 20 (4), 1171–1185.

[16] Mohanadas, D., Ravoof, T.B.S.A., and Sulaiman, Y., 2020, A fast switching electrochromic performance based on poly(3,4-ethylenedioxythiophene)-reduced graphene oxide/metal-organic framework HKUST-1, Sol. Energy Mater. Sol. Cells, 214, 110596.

[17] Hidayah, N.M.S., Liu, W.W., Lai, C.W., Noriman, N.Z., Khe, C.S., Hashim, U., and Lee, H.C., 2017, Comparison on graphite, graphene oxide and reduced graphene oxide: Synthesis and characterization, AIP Conf. Proc., 1892 (1), 150002.

[18] Zong, M., Huang, Y., Zhao, Y., Wang, L., Liu, P., Wang, Y., and Wang, Q., 2013, One-pot simplified co-precipitation synthesis of reduced graphene oxide/Fe3O4 composite and its microwave electromagnetic properties, Mater. Lett., 106, 22–25.

[19] Vinodhkumar, G., Wilson, J., Inbanathan, S.S.R., Potheher, I.V., Ashokkumar, M., and Peter, A.C., 2020, Solvothermal synthesis of magnetically separable reduced graphene oxide/Fe3O4 hybrid nanocomposites with enhanced photocatalytic properties, Phys. B, 580, 411752.

[20] Saha, S., Jana, M., Samanta, P., Chandra Murmu, N., Kim, N.H., Kuila, T., and Lee, J.H., 2014, Hydrothermal synthesis of Fe₃O₄/RGO composites and investigation of electrochemical performances for energy storage applications, RSC Adv., 4 (84), 44777–44785.

[21] Liu, X., Huang, Y., Ding, L., Zhao, X., Liu, P., and Li, T., 2021, Synthesis of covalently bonded reduced graphene oxide-Fe3O4 nanocomposites for efficient electromagnetic wave absorption, J. Mater. Sci. Technol., 72, 93–103.

[22] Rezapour, M., 2018, One-step electrochemical synthesis and characterization of high performance magnetite/reduced graphene oxide nanocomposite, Anal. Bioanal. Electrochem., 10 (4), 450–464.

[23] Peik-See, T., 2015, Feasibility of Fe3O4 nanoparticles decorated reduced graphene oxide heterostructure as photocatalyst and chemical sensors, Dissertation, Department of Physics, University of Malaya, Kuala Lumpur.

[24] Peik-See, T., Pandikumar, A., Ngee, L.H., Ming, H.N., and Hua, C.C., 2014, Magnetically separable reduced graphene oxide/iron oxide nanocomposite materials for environmental remediation, Catal. Sci. Technol., 4 (12), 4396–4405.

[25] Shalaby, A.R., Salama, N.A., Abou-Raya, S.H., Emam, W.H., and Mehaya, F.M., 2011, Validation of HPLC method for determination of tetracycline residues in chicken meat and liver, Food Chem., 124 (4), 1660–1666.

[26] Ungku Abdullah, U.A.A., Mohamad Hanapi, N.S., Ibrahim, W.N.W., Saiful Azhar, S., Ishak, N.S., and Hamid, R.D., 2019, Rapid magnetic solid-phase extraction based on graphene oxide/magnetite nanoparticles for the determination of non-steroidal anti-inflammatory drugs and bisphenol-A in tap water, Asian J. Chem., 31 (6), 1294–1300.

[27] Ma, C., Yang, K., Wang, L., and Wang, X., 2017, Facile synthesis of reduced graphene oxide/Fe3O4 nanocomposite film, J. Appl. Biomater. Funct. Mater., 15 (Suppl. 1), 1–6.

[28] Boruah, P.K., Borah, D.J., Handique, J., Sharma, P., Sengupta, P., and Das, M.R., 2015, Facile synthesis and characterization of Fe3O4 nanopowder and Fe3O4/reduced graphene oxide nanocomposite for methyl blue adsorption: A comparative study, J. Environ. Chem. Eng., 3 (3), 1974–1985.

[29] Joint FAO/WHO Codex Alimentarius Commission, 2017, Codex Alimentarius: Guidelines on Performance Criteria for Methods of Analysis for The Determination of Pesticide Residues in Food and Feed, Food and Agriculture Organization of the United Nations, Rome.

[30] Karnes, H.T., and March, C., 1993, Precision, accuracy, and data acceptance criteria in biopharmaceutical analysis, Pharm. Res., 10 (10), 1420–1426.

[31] Lin, Y., Xu, S., and Li, J., 2013, Fast and highly efficient tetracyclines removal from environmental waters by graphene oxide functionalized magnetic particles, Chem. Eng. J., 225, 679–685.

[32] Hu, X., Zhao, Y., Wang, H., Tan, X., Yang, Y., and Liu, Y., 2017, Efficient removal of tetracycline from aqueous media with a Fe3O4 nanoparticles@ graphene oxide nanosheets assembly, Int. J. Environ. Res. Public Health, 14 (12), 1495.

[33] Yu, B., Bai, Y., Ming, Z., Yang, H., Chen, L., Hu, X., Feng, S., and Yang, S.T., 2017, Adsorption behaviors of tetracycline on magnetic graphene oxide sponge, Mater. Chem. Phys., 198, 283–290.

[34] Nodeh, H.R., Ibrahim, W.A.W., Ali, I., and Sanagi, M.M., 2016, Development of magnetic graphene oxide adsorbent for the removal and preconcentration of As(III) and As(V) species from environmental water samples, Environ. Sci. Pollut. Res., 23 (10), 9759–9773.

[35] Abadi, M.J., Nouri, S.M.M., Zhiani, R., Heydarzadeh, H.D., and Motavalizadehkakhky, A., 2019, Removal of tetracycline from aqueous solution using Fe-doped zeolite, Int. J. Ind. Chem., 10 (4), 291–300.

[36] Arabsorkhi, B., and Sereshti, H., 2018, Determination of tetracycline and cefotaxime residues in honey by micro-solid phase extraction based on electrospun nanofibers coupled with HPLC, Microchem. J., 140, 241–247.

[37] Al-Afy, N., Sereshti, H., Hijazi, A., and Nodeh, H.R., 2018, Determination of three tetracyclines in bovine milk using magnetic solid phase extraction in tandem with dispersive liquid-liquid microextraction coupled with HPLC, J. Chromatogr. B, 1092, 480–488.

[38] Abd Wahib, S.M., Ibrahim, W.A.W., Sanagi, M.M., Kamboh, M.A., and Keyon, A.S.A., 2018, Magnetic sporopollenin-cyanopropyltriethoxysilane-dispersive micro-solid phase extraction coupled with high performance liquid chromatography for the determination of selected non-steroidal anti-inflammatory drugs in water samples, J. Chromatogr. A, 1532, 50–57

[39] Han, X., Chen, J., Li, Z., and Qiu, H., 2019, Combustion fabrication of magnetic porous carbon as a novel magnetic solid-phase extraction adsorbent for the determination of non-steroidal anti-inflammatory drugs, Anal. Chim. Acta, 1078, 78–89.

[40] Saad, S.M., Aling, N.A., Miskam, M., Saaid, M., Mohamad Zain, N.N., Kamaruzaman, S., Raoov, M., Mohamad Hanapi, N.S., Ibrahim, W.N.W., and Yahaya, N., 2020, Magnetic nanoparticles assisted dispersive liquid–liquid microextraction of chloramphenicol in water samples, Royal Society Open Science, 7 (4), 200143.

[41] Ma, J., Jiang, L., Wu, G., Xia, Y., Lu, W., Li, J., and Chen, L., 2016, Determination of six sulfonylurea herbicides in environmental water samples by magnetic solid-phase extraction using multi-walled carbon nanotubes as adsorbents coupled with high-performance liquid chromatography, J. Chromatogr. A, 1466, 12–20.

[42] Abdullah, U.A.A.U., Hanapi, N.S.M., Ibrahim, W.N.W., Saim, N.A., and Yahaya, N., 2018, Micro-solid phase extraction (µ-SPE) based on alginate/multi-walled carbon nanotubes sorbent for the determination of bisphenol A in canned fruits, Chiang Mai J. Sci., 45 (6), 2348–2360.

[43] Kireeti, K.V.M.K., Chandrakanth, G., Kadam, M.M., and Jha, N., 2016, A sodium modified reduced graphene oxide–Fe3O4 nanocomposite for efficient lead(II) adsorption, RSC Adv., 6 (88), 84825–84836.

[44] Kaewsuwan, W., Kanatharana, P., and Bunkoed, O., 2017, Dispersive magnetic solid phase extraction using octadecyl coated silica magnetite nanoparticles for the extraction of tetracyclines in water samples, J. Anal. Chem., 72 (9), 957–965.

[45] Dettmer, K., and Engewald, W., 2002, Adsorbent materials commonly used in air analysis for adsorptive enrichment and thermal desorption of volatile organic compounds, Anal. Bioanal. Chem., 373 (6), 490–500.

[46] Nasrollahzadeh, M., Maham, M., Rostami-Vartooni, A., Bagherzadeh, M., and Sajadi, S.M., 2015, Barberry fruit extract assisted in situ green synthesis of Cu nanoparticles supported on a reduced graphene oxide–Fe3O4 nanocomposite as a magnetically separable and reusable catalyst for the O-arylation of phenols with aryl halides under ligand-free conditions, RSC Adv., 5 (79), 64769–64780.

[47] Samanidou, V.F., Nikolaidou, K.I., and Papadoyannis, I.N., 2007, Development and validation of an HPLC confirmatory method for the determination of seven tetracycline antibiotics residues in milk according to the European Union Decision 2002/657/EC, J. Sep. Sci., 30 (15), 2430–2439.

[48] Islas, G., Rodriguez, J.A., Perez-Silva, I., Miranda, J.M., and Ibarra, I.S., 2018, Solid-phase extraction and large-volume sample stacking-capillary electrophoresis for determination of tetracycline residues in milk, J. Anal. Methods Chem., 2018, 5394527.

[49] Lian, L., Lv, J., Wang, X., and Lou, D., 2018, Magnetic solid–phase extraction of tetracyclines using ferrous oxide coated magnetic silica microspheres from water samples, J. Chromatogr. A, 1534, 1–9.

[50] Cherkashina, K., Vakh, C., Lebedinets, S., Pochivalov, A., Moskvin, L., Lezov, A., and Bulatov, A., 2018, An automated salting-out assisted liquid-liquid microextraction approach using 1-octylamine: On-line separation of tetracycline in urine samples followed by HPLC-UV determination, Talanta, 184, 122–127.

[51] Jin, H., Kumar, A.P., Paik, D.H., Ha, K.C., Yoo, Y.J., and Lee, Y.I., 2010, Trace analysis of tetracycline antibiotics in human urine using UPLC–QToF mass spectrometry, Microchem. J, 94 (2), 139–147.

[52] Marinou, E., Samanidou, V.F., and Papadoyannis, I.N., 2019, Development of a high pressure liquid chromatography with diode array detection method for the determination of four tetracycline residues in milk by using QuEChERS dispersive extraction, Separations, 6 (2), 21.



DOI: https://doi.org/10.22146/ijc.64414

Article Metrics

Abstract views : 2255 | views : 2002


Copyright (c) 2021 Indonesian Journal of Chemistry

Creative Commons License
This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.

 

Indonesian Journal of Chemistry (ISSN 1411-9420 /e-ISSN 2460-1578) - Chemistry Department, Universitas Gadjah Mada, Indonesia.

Web Analytics View The Statistics of Indones. J. Chem.