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Development of a comprehensive screening method for more than 300 organic chemicals in water samples using a combination of solid-phase extraction and liquid chromatography-time-of-flight-mass spectrometry

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Abstract

A comprehensive screening method for 311 organic compounds with a wide range of physicochemical properties (log Pow −2.2–8.53) in water samples was developed by combining solid-phase extraction with liquid chromatography–high-resolution time-of-flight mass spectrometry. Method optimization using 128 pesticides revealed that tandem extraction with styrene-divinylbenzene polymer and activated carbon solid-phase extraction cartridges at pH 7.0 was optimal. The developed screening method was able to extract 190 model compounds with average recovery of 80.8% and average relative standard deviations (RSD) of 13.5% from spiked reagent water at 0.20 μg L−1, and 87.1% recovery and 10.8% RSD at 0.05 μg L−1. Spike-recovery testing (0.20 μg L−1) using real sewage treatment plant effluents resulted in an average recovery and average RSD of 190 model compounds of 77.4 and 13.1%, respectively. The method was applied to the influent and effluent of five sewage treatment plants in Kitakyushu, Japan, with 29 out of 311 analytes being observed at least once. The results showed that this method can screen for a large number of chemicals with a wide range of physicochemical properties quickly and at low operational cost, something that is difficult to achieve using conventional analytical methods. This method will find utility in target screening of hazardous chemicals with a high risk in environmental waters, and for confirming the safety of water after environmental incidents.

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References

  • Bester K (2007) Personal care compounds in the environment. Weinheim, Wiley VCH

    Google Scholar 

  • Brack W, Altenburger R, Schuurmann G et al (2015) The SOLUTIONS project: challenges and responses for present and future emerging pollutants in land and water resources management. Sci Total Environ 503-504:22–31

    Article  CAS  Google Scholar 

  • Duong TH, Kadomami K, Matsuura N, Nguyen QT (2014a) Screening analysis of a thousand micro-pollutants in Vietnamese rivers. In: Yamamoto K, Furumai H, Katayama H, Chiemchaisri C, Puetpaiboon U, Visvanathan C, Satoh H (eds) Southeast Asian Water Environment 5. IWA, London, pp 195–202

    Google Scholar 

  • Duong TH, Kadomami K, Pan S, Matsuura N, Nguyen QT (2014b) Screening and analysis of 940 organic micro-pollutants in river sediments in Vietnam using an automated identification and quantification database system for GC–MS. Chemosphere 107:462–472

    Article  CAS  Google Scholar 

  • EMA (2006) Guideline on the environmental risk assessment of medicinal products for human use, EMEA CHMP/SWP/4447/00. Committee for Medicinal Products for Human Use, European Medicines Agency, London

  • EPA (2007) Method 1694: pharmaceuticals and personal care products in water, soil, sediment, and biosolids by HPLC/MS/MS. United States Environmental Protection Agency EPA-821-R-08-002

  • Ferrer I, Thurman EM (2007) Multi-residue method for the analysis of 101 pesticides and their degradates in food and water samples by liquid chromatography/time-of-flight mass spectrometry. J Chromatogr A 1175:24–37

    Article  CAS  Google Scholar 

  • Ferrer I, Thurman EM (2012) Analysis of 100 pharmaceuticals and their degradates in water samples by liquid chromatography/quadrupole time-of-flight mass spectrometry. J Chromatogr A 1259:148–157

    Article  CAS  Google Scholar 

  • Gómez MJ, Gómez-Ramos MM, Malato O, Mezcua M, Férnandez-Alba AR (2010) Rapid automated screening, identification and quantification of organic micro-contaminants and their main transformation products in wastewater and river waters using liquid chromatography-quadrupole-time-of-flight mass spectrometry with an accurate-mass database. J Chromatogr A 1217:7038–7054

    Article  CAS  Google Scholar 

  • Gracia-Lor E, Sancho JV, Hernández F (2011) Multi-class determination of around 50 pharmaceuticals, including 26 antibiotics, in environmental and wastewater samples by ultra-high performance liquid chromatography-tandem mass spectrometry. J Chromatogr A 1218:2264–2275

    Article  CAS  Google Scholar 

  • Hernández F, Portolés T, Ibáñez M, Bustos-López MC, Díaz R, Botero-Coy AM, Fuentes CL, Peñuela G (2012) Use of time-of-flight mass spectrometry for large screening of organic pollutants in surface waters and soils from a rice production area in Colombia. Sci Total Environ 439:246–259

    Article  CAS  Google Scholar 

  • Jinya D, Iwamura T, Kadokami K, Kusuda T (2011) Development of a comprehensive analytical method for semi-volatile organic compounds an water samples by a combination of solid-phase extraction and gas chromatography-mass spectrometry database system. J Environ Chem 21:35–48 (in Japanese)

    Article  CAS  Google Scholar 

  • Jinya D, Iwamura T, Kadokami K (2013) Comprehensive analytical method for semi-volatile organic compounds in water samples by combination of disk-type solid-phase extraction and gas chromatography-mass spectrometry database system. Anal Sci 29:483–486

    Article  CAS  Google Scholar 

  • Kadokami K, Tanada K, Taneda K, Nakagawa K (2004) Development of a novel GC-MS database for simultaneous determination of hazardous chemicals. J Environ Chem 53:581–588 (in Japanese)

    CAS  Google Scholar 

  • Kadokami K, Tanada K, Taneda K, Nakagawa K (2005) Novel gas chromatography-mass spectrometry database for automatic identification and quantification of micropollutants. Chromatogr A 1089:219–226

    Article  CAS  Google Scholar 

  • Kadokami K, Pan S, Duong TH, Li X, Miyazaki T (2012) Development of a comprehensive analytical method for semi-volatile organic compounds in sediments by using an automated identification and quantification system with a GC-MS database. Anal Sci 28:1183–1189

    Article  CAS  Google Scholar 

  • Kolpin DW, Furlong ET, Meyer MT, Thurman EM, Zaugg SD, Barber LB, Buxton HT (2002) Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999-2000: a national reconnaissance. Environ Sci Technol 36:1202–1211

    Article  CAS  Google Scholar 

  • Kong L, Kadokami K, Wang S, Duong TH, Chau TCH (2015) Monitoring of 1300 organic micro-pollutants in surface waters from Tianjin, North China. Chemosphere 122:125–130

    Article  CAS  Google Scholar 

  • Kümmerer K (2009) Antibiotics in the aquatic environment—a review—part I. Chemosphere 75:417–434

    Article  CAS  Google Scholar 

  • Luo Y, Guo W, Ngo HH, Nghiem LD, Hai FI, Zhang J, Liang S, Wang XC (2014) A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment. Sci Total Environ 473-474:619–641

    Article  CAS  Google Scholar 

  • Martínez Bueno MJ, Ulaszewska MM, Gomez MJ, Hernando MD, Fernández-Alba AR (2012) Simultaneous measurement in mass and mass/mass mode for accurate qualitative and quantitative screening analysis of pharmaceuticals in river water. J Chromatogr A 1256:80–88

    Article  CAS  Google Scholar 

  • Masiá A, Ibáñez M, Blasco C, Sancho JV, Picó Y, Hernández F (2013) Combined use of liquid chromatography triple quadrupole mass spectrometry and liquid chromatography quadrupole time-of-flight mass spectrometry in systematic screening of pesticides and other contaminants in water samples. Anal Chim Acta 761:117–127

    Article  CAS  Google Scholar 

  • MOE (n.d.) Environmental quality standards for water pollution. Ministry of the Environment Japan. https://www.env.go.jp/en/water/wq/wp.pdf. Accessed 17 Jan 2017

  • Nakada N, Komori K, Suzuki Y, Konishi C, Houwa I, Tanaka H (2007) Occurrence of 70 pharmaceutical and personal care products in Tone River basin in Japan. Water Sci Technol 56:133–140

    Article  CAS  Google Scholar 

  • Narimiya M, Okuda T, Nakada N, Yamashita N, Tanaka H, Sato K, Sueoka M, Ohiwa T (2009) Occurrence and fate of pharmaceuticals and personal care products during wastewater treatments. Environ Eng Res 46:175–186 (in Japanese)

    Google Scholar 

  • Okuda T, Yamashita N, Tanaka H, Matsukawa H, Tanabe K (2009) Development of extraction method of pharmaceuticals and their occurrences found in Japanese wastewater treatment plants. Environ Int 35:815–820

    Article  CAS  Google Scholar 

  • Pan S, Kadokami K, Li X, Duong TH, Horiguchi T (2014) Target and screening analysis of 940 micro-pollutants in sediments inTokyo Bay, Japan. Chemosphere 99:109–116

    Article  CAS  Google Scholar 

  • Petrovic M, Farré M, de Alda ML, Perez S, Postigo C, Köck M, Radjenovic J, Gros M, Barcelo D (2010) Recent trends in the liquid chromatography-mass spectrometry analysis of organic contaminants in environmental samples. J Chromatogr A 1217:4004–4017

    Article  CAS  Google Scholar 

  • PFSB (2005) Analytical methods for residual compositional substances of agricultural chemicals, feed additives, and veterinary drugs in food (notice no.0124001). Ministry of Health, Labour and Welfare Japan Web. http://www.mhlw.go.jp/stf/seisakunitsuite/bunya/kenkou_iryou/shokuhin/zanryu/zanryu3/siken.html. Accessed 17 Jan 2017 (in Japanese)

  • Robles-Molina J, Lara-Ortega FJ, Gilbert-López B, García-Reyes JF, Molina-Díaz A (2014) Multi-residue method for the determination of over 400 priority and emerging pollutants in water and wastewater by solid-phase extraction and liquid chromatography-time-of-flight mass spectrometry. J Chromatogr A 1350:30–43

    Article  CAS  Google Scholar 

  • Rodil R, Quintana JB, López-Mahía P, Muniategui-Lorenzo S, Prada-Rodríguez D (2009) Multi-residue analytical method for the determination of emerging pollutants in water by solid-phase extraction and liquid chromatography-tandem mass spectrometry. J Chromatogr A 1216:2958–2969

    Article  CAS  Google Scholar 

  • Saito S, Nemoto S, Matsuda R (2012) Multi-residue analysis of pesticides in agricultural products by liquid chromatography time-of-flight mass spectrometry. Food Hyg Saf Sci 53:255–263

    Article  CAS  Google Scholar 

  • Scheurer M, Michel A, Brauch HJ, Ruck W, Sacher F (2012) Occurrence and fate of the antidiabetic drug metformin and its metabolite guanylurea in the environment and during drinking water treatment. Water Res 46:4790–4802

    Article  CAS  Google Scholar 

  • Shao B, Chen D, Zhang J, Wu Y, Sun C (2009) Determination of 76 pharmaceutical drugs by liquid chromatography-tandem mass spectrometry in slaughterhouse wastewater. J Chromatogr A 1216:8312–8318

    Article  CAS  Google Scholar 

  • Stahnke H, Reemtsma T, Alder L (2009) Compensation of matrix effects by postcolumn infusion of a monitor substance in multiresidue analysis with LC-MS/MS. Anal Chem 81:2185–2192

    Article  CAS  Google Scholar 

  • Tanabe S, Subramanian A (2011) Great Eastern Japan Earthquake—possible marine environmental contamination by toxic pollutants. Mar Pollut Bull 62:883–884

    Article  CAS  Google Scholar 

  • Trautwein C, Berset JD, Wolschke H, Kümmerer K (2012) Occurrence of the antidiabetic drug metformin and its ultimate transformation product Guanylurea in several compartments of the aquatic cycle. Water Res 70:203–212

    Google Scholar 

  • UNEP (2006) 9th special session of the governing council of the United Nations Environment Programme/Global Ministerial Environment Forum. UNEP Web. http://www.unep.org/documents.multilingual/default.asp?DocumentID=469&ArticleID=5138&l=en. Accessed 17 Jan 2017

  • Weinmann W, Gergov M, Goerner M (2000) MS/MS-libraries with triple quadrupole-tandem mass spectrometers for drug identification and drug screening. Analusis 28:934–941

    Article  CAS  Google Scholar 

Download references

Acknowledgements

A part of this study was carried out by the support of Agilent Technologies Foundation Research Project Gift: 08564-JPNUR; the Health and Labor Sciences Research Grant (H25-Kenki-Ippan-007) from the Ministry of Health, Labor, and Welfare, Japan; and Research Grant of Kitakyushu Foundation for the Advancement of Industry Science and Technology. We thank our laboratory members for their enthusiastic support of this work. We are grateful to Associate Professor Graeme Allinson (RMIT University, Melbourne, Australia) and Dr. Mayumi Allinson (University of Melbourne, Melbourne, Australia) for their kind proofreading, useful comments, and constructive suggestions on this manuscript.

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Authors and Affiliations

  1. The University of Kitakyushu, Kitakyushu, Japan

    Hong Thi Cam Chau & Kiwao Kadokami

  2. Kitakyushu Life Science Center, Kitakyushu, Japan

    Tomomi Ifuku

  3. Saito-consultant, Tottori, Japan

    Yusuke Yoshida

Authors
  1. Hong Thi Cam Chau
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  2. Kiwao Kadokami
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  3. Tomomi Ifuku
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  4. Yusuke Yoshida
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Correspondence to Kiwao Kadokami.

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Responsible editor: Ester Heath

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Chau, H.T.C., Kadokami, K., Ifuku, T. et al. Development of a comprehensive screening method for more than 300 organic chemicals in water samples using a combination of solid-phase extraction and liquid chromatography-time-of-flight-mass spectrometry. Environ Sci Pollut Res 24, 26396–26409 (2017). https://doi.org/10.1007/s11356-017-9929-x

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  • DOI: https://doi.org/10.1007/s11356-017-9929-x

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