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Highly reproducible solid-phase extraction membrane for removal and surface-enhanced Raman scattering detection of antibiotics

  • Biomaterials
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Abstract

A disposable solid-phase extraction (SPE) membrane was developed for rapid removal and sensitive surface-enhanced Raman scattering (SERS) detection of antibiotics in water samples. The membrane was fabricated on commercially available SPE column by filtration of the activated carbon modified with silver nanoparticles (Ag NPs/AC). The prepared SPE membrane exhibited outstanding preconcentration ability due to the high adsorption properties of AC, and excellent ability to enhance Raman signal resulting from “hot spots” between the embedded Ag NPs, improving the sensitivity of SERS detection. A detection limit (LOD) of 5.0 × 10−11 and 1.6 × 10−10 M was achieved for rhodamine 6G and p-aminothiophenol. In addition, the membrane exhibited high reproducibility with spot-to-spot variation in SERS spectral intensity less than 15%. Based on the membrane, the qualitative and quantitative analysis of the antibiotics in aqueous solution was accomplished with the LOD at nM level, demonstrating the feasibility of the disposable SPE membrane for in situ rapid preconcentration and detection.

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References

  1. Martens E, Demain AL (2011) Platensimycin and platencin: promising antibiotics for future application in human medicine. J Antibiot 43(11):705–710

    Article  Google Scholar 

  2. Yang JH, Bhargava P, McCloskey D, Mao N, Palsson BO, Collins JJ (2017) Antibiotic-Induced Changes to the Host Metabolic Environment Inhibit Drug Efficacy and Alter Immune Function. Cell Host Microbe 22(6):757-765.e3

  3. Faten F, Azzazy HME, Niessen WMA (2015) Challenges in the determination of aminoglycoside antibiotics: a review. Anal Chim Acta 890(26):21–43

    Google Scholar 

  4. Thorsten C, Schneider RJ, Färber HA, Dirk S, Meyer MT, Goldbach HE (2010) Determination of antibiotic residues in manure, soil, and surface waters. CLEAN Soil Air Water 31(1):36–44

    Google Scholar 

  5. Zhou JL, Kang Y (2013) Matrix effect in high-performance liquid chromatography-tandem mass spectrometry analysis of antibiotics in environmental water samples. J Sep Sci 36(3):564–571

    Article  Google Scholar 

  6. Cazorlareyes R, Romerogonzález R, Frenich AG, Rodríguez Maresca MA, Martínez Vidal JL (2014) Simultaneous analysis of antibiotics in biological samples by ultra high performance liquid chromatography-tandem mass spectrometry. J Pharm Biomed Anal 89(4):203–212

    Article  Google Scholar 

  7. Moreno-González D, Hamed AM, Gilbert-López B, Gámiz-Gracia L, García-Campaña AM (2017) Evaluation of a multiresidue capillary electrophoresis-quadrupole-time-of-flight mass spectrometry method for the determination of antibiotics in milk samples. J Chromatogr A 1510:100–107

    Article  Google Scholar 

  8. Preu M, Guyot D, Petz M (1998) Development of a gas chromatography-mass spectrometry method for the analysis of aminoglycoside antibiotics using experimental design for the optimisation of the derivatisation reactions. J Chromatogr A 818(1):95–108

    Article  Google Scholar 

  9. Lan L, Yao Y, Ping J, Ying Y (2017) Recent advances in nanomaterial-based biosensors for antibiotics detection. Biosens Bioelectron 91:504–514

    Article  Google Scholar 

  10. Adrian J, Pinacho DG, Granier B, Diserens JM, Sãn BF, Marco MP (2008) A multianalyte ELISA for immunochemical screening of sulfonamide, fluoroquinolone and ss-lactam antibiotics in milk samples using class-selective bioreceptors. Anal Bioanal Chem 391(5):1703–1712

    Article  Google Scholar 

  11. Li YT, Qu LL, Li DW, Song QX, Fathi F, Long YT (2013) Rapid and sensitive in situ detection of polar antibiotics in water using a disposable Ag–graphene sensor based on electrophoretic preconcentration and surface-enhanced Raman spectroscopy. Biosens Bioelectron 43(10):94–100

    Article  Google Scholar 

  12. Cacciatore G, Petz M, Rachid S, Hakenbeck R, Bergwerff AA (2004) Development of an optical biosensor assay for detection of B-lactam antibiotics in milk using the penicillin-binding protein 2x*. Anal Chim Acta 520(1):105–115

    Article  Google Scholar 

  13. Xu KC, Yan HP, Tan CF, Lu YY, Li Y, Ho GW, Ji R, Hong M (2018) Hedgehog inspired CuO nanowires/Cu2O composites for broadband visible-light-driven recyclable surface enhanced Raman scattering. Adv Opt Mater 6(7):1701167

    Article  Google Scholar 

  14. Qu LL, Li DW, Xue JQ, Zhai WL, Fossey JS, Long YT (2012) Batch fabrication of disposable screen printed SERS arrays. Lab Chip 12(5):876–881

    Article  Google Scholar 

  15. Cherukulappurath S, Si HL, Campos A, Haynes CL, Oh SH (2014) Rapid and sensitive in situ SERS detection using dielectrophoresis. Chem Mater 26(7):2445–2452

    Article  Google Scholar 

  16. Carrasco S, Benitopena E, Navarrovilloslada F, Langer J, Sanzortiz MN, Reguera J, Lizmarzan LM, Morenobondi MC (2016) Multi-branched gold-mesoporous silica nanoparticles coated with molecularly imprinted polymer for label-free antibiotic SERS analysis. Chem Mater 28(21):7947–7954

    Article  Google Scholar 

  17. Holthoff EL, Stratis-Cullum DN, Hankus ME (2011) A nanosensor for TNT detection based on molecularly imprinted polymers and surface enhanced Raman scattering. Sensors 11(3):2700–2714

    Article  Google Scholar 

  18. Li D, Duan HZ, Wang YH, Zhang QM, Cao HR, Deng W, Li DW (2018) On-site preconcentration of pesticide residues in a drop of seawater by using electrokinetic trapping, and their determination by surface-enhanced Raman scattering. Microchim Acta 185(1):10

    Article  Google Scholar 

  19. Torul H, Çiftçi H, Çetin D, Suludere Z, Boyacı IH, Tamer U (2015) Paper membrane-based SERS platform for the determination of glucose in blood samples. Anal Bioanal Chem 407(27):8243–8251

    Article  Google Scholar 

  20. Balakrishnan VK, Terry KA, Toito J (2006) Determination of sulfonamide antibiotics in wastewater: a comparison of solid phase microextraction and solid phase extraction methods. J Chromatogr A 1131(1–2):1–10

    Article  Google Scholar 

  21. Lai Y, Cui J, Jiang X, Zhu S, Zhan J (2013) Combination of solid phase extraction and surface-enhanced Raman spectroscopy for rapid analysis. Analyst 138(9):2598–2603

    Article  Google Scholar 

  22. Y-e Shi, Li L, Yang M, Jiang X, Zhao Q, Zhan J (2014) A disordered silver nanowires membrane for extraction and surface-enhanced Raman spectroscopy detection. Analyst 139(10):2525–2530

    Article  Google Scholar 

  23. Markina NE, Markin AV, Zakharevich AM, Goryacheva IY (2017) Calcium carbonate microparticles with embedded silver and magnetite nanoparticles as new SERS-active sorbent for solid phase extraction. Microchim Acta 184(10):3937–3944

    Article  Google Scholar 

  24. Markina NE, Markin AV, Zakharevich AM, Gorin DA, Rusanova TY, Goryacheva IY (2016) Multifunctional silver nanoparticle-doped silica for solid-phase extraction and surface-enhanced Raman scattering detection. J Nanopart Res 18(12):353

    Article  Google Scholar 

  25. Lee PC, Meisel D (1982) Adsorption and surface-enhanced Raman of dyes on silver and gold sols. J Phys Chem 86(17):3391–3395

    Article  Google Scholar 

  26. Leopold N, Lendl B (2003) A new method for fast preparation of highly surface-enhanced Raman scattering (SERS) active silver colloids at room temperature by reduction of silver nitrate with hydroxylamine hydrochloride. J Phys Chem B 107(24):5723–5727

    Article  Google Scholar 

  27. Zhang C, Jiang SZ, Huo YY, Liu AH, Xu SC, Liu XY, Sun ZC, Xu YY, Man BY (2015) SERS detection of R6G based on a novel graphene oxide/silver nanoparticles/silicon pyramid arrays structure. Opt Expresss 23(19):24811–24821

    Article  Google Scholar 

  28. Zhao XM, Zhang BH, Ai KL, Zhang G, Cao LY, Liu XJ, Sun HM, Wang HS, Lu LH (2009) Monitoring catalytic degradation of dye molecules on silver-coated ZnO nanowire arrays by surface-enhanced Raman spectroscopy. J Mater Chem 19(31):5547–5553

    Article  Google Scholar 

  29. SungpyoKim AgaD (2007) Potential ecological and human health impacts of antibiotics and antibiotic-resistant bacteria from wastewater treatment plants. J Toxicol Environ Health B 10(8):559–573

    Article  Google Scholar 

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Acknowledgements

This research was supported by the National Natural Science Foundations of China (21505057, 61575087 and 21605062), the Natural Science Foundation of Jiangsu Province (BK20150227, BK20151164), the Priority Academic Program Development of Jiangsu Higher Education Institutions, the Brand Major of Universities in Jiangsu Province, and the Top-notch Academic Programs Project of Jiangsu Higher Education Institution (TAPP).

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  1. Qin Jia and Zhi-Qin Geng have contributed equally to this work.

Authors and Affiliations

  1. School of Chemistry and Materials Science, Jiangsu Normal University, Xuzhou, 221116, Jiangsu, China

    Qin Jia, Zhi-Qin Geng, Yang Liu, Guo-Hai Yang, Haitao Li & Lu-Lu Qu

  2. Jiangsu Key Laboratory of Advanced Laser Materials and Devices, School of Physics and Electronic Engineering, Jiangsu Normal University, Xuzhou, 221116, Jiangsu, China

    Wen Wang & Cai-Qin Han

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  1. Qin Jia
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Correspondence to Cai-Qin Han, Haitao Li or Lu-Lu Qu.

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Jia, Q., Geng, ZQ., Liu, Y. et al. Highly reproducible solid-phase extraction membrane for removal and surface-enhanced Raman scattering detection of antibiotics. J Mater Sci 53, 14989–14997 (2018). https://doi.org/10.1007/s10853-018-2745-y

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  • DOI: https://doi.org/10.1007/s10853-018-2745-y

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