Screening of lake sediments for emerging contaminants by liquid chromatography atmospheric pressure photoionization and electrospray ionization coupled to high resolution mass spectrometry.

We developed a multiresidue method for the target and suspect screening of more than 180 pharmaceuticals, personal care products, pesticides, biocides, additives, corrosion inhibitors, musk fragrances, UV light stabilizers, and industrial chemicals in sediments. Sediment samples were freeze-dried, extracted by pressurized liquid extraction, and cleaned up by liquid-liquid partitioning. The quantification and identification of target compounds with a broad range of physicochemical properties (log K(ow) 0-12) was carried out by liquid chromatography followed by electrospray ionization (ESI) and atmospheric pressure photoionization (APPI) coupled to high resolution Orbitrap mass spectrometry (HRMS/MS). The overall method average recoveries and precision are 103% and 9% (RSD), respectively. The method detection limits range from 0.010 to 4 ng/g(dw), while limits of quantification range from 0.030 to 14 ng/g(dw). The use of APPI as an alternative ionization source helped to distinguish two isomeric musk fragrances by means of different ionization behavior. The method was demonstrated on sediment cores from Lake Greifensee located in northeastern Switzerland. The results show that biocides, musk fragrances, and other personal care products were the most frequently detected compounds with concentrations ranging from pg/g(dw) to ng/g(dw), whereas none of the targeted pharmaceuticals were found. The concentrations of many urban contaminants originating from wastewater correlate with the highest phosphorus input into the lake as a proxy for treatment efficiency. HRMS enabled a retrospective analysis of the full-scan data acquisition allowing the detection of suspected compounds like quaternary ammonium surfactants, the biocide triclocarban, and the tentative identification of further compounds without reference standards, among others transformation products of triclosan and triclocarban.

[1]  L. D. de Alencastro,et al.  Irgarol 1051, an Antifouling Compound in Freshwater, Sediment, and Biota of Lake Geneva , 1996, Bulletin of environmental contamination and toxicology.

[2]  René P Schwarzenbach,et al.  Identification of transformation products of organic contaminants in natural waters by computer-aided prediction and high-resolution mass spectrometry. , 2009, Environmental science & technology.

[3]  T. Poiger,et al.  Azole fungicides: occurrence and fate in wastewater and surface waters. , 2008, Environmental science & technology.

[4]  M. Blades,et al.  Effects of solvent flow, dopant flow, and lamp current on dopant-assisted atmospheric pressure photoionization (DA-APPI) for LC-MS. Ionizationvia proton transfer , 2005 .

[5]  H Fromme,et al.  Polycyclic musk fragrances in different environmental compartments in Berlin (Germany). , 2001, Water research.

[6]  V. Andreu,et al.  Determination of pharmaceuticals in soils and sediments by pressurized liquid extraction and liquid chromatography tandem mass spectrometry. , 2010, Journal of chromatography. A.

[7]  K. Bester.  Analysis of musk fragrances in environmental samples. , 2009, Journal of chromatography. A.

[8]  Martin Krauss,et al.  LC–high resolution MS in environmental analysis: from target screening to the identification of unknowns , 2010, Analytical and bioanalytical chemistry.

[9]  C. Reddy,et al.  Free and bound benzotriazoles in marine and freshwater sediments , 2000 .

[10]  M. Blades,et al.  State-of-the-art in atmospheric pressure photoionization for LC/MS. , 2008, Analytica chimica acta.

[11]  C. Stamm,et al.  Significance of urban and agricultural land use for biocide and pesticide dynamics in surface waters. , 2010, Water research.

[12]  W. Giger,et al.  The historical record of PCB and PCDD/F deposition at Greifensee, a lake of the Swiss plateau, between 1848 and 1999. , 2007, Chemosphere.

[13]  T. Nakahara,et al.  Determination of perfluorooctane sulfonate in river water by liquid chromatography/atmospheric pressure photoionization mass spectrometry by automated on-line extraction using turbulent flow chromatography. , 2003, Rapid communications in mass spectrometry : RCM.

[14]  U. Ceglarek,et al.  Rapid quantification of steroid patterns in human serum by on-line solid phase extraction combined with liquid chromatography-triple quadrupole linear ion trap mass spectrometry. , 2009, Clinica chimica acta; international journal of clinical chemistry.

[15]  Amber D. Wellman,et al.  Electron capture atmospheric pressure photoionization mass spectrometry: analysis of fullerenes, perfluorinated compounds, and pentafluorobenzyl derivatives. , 2007 .

[16]  Jörg Römbke,et al.  Environmental fate of pharmaceuticals in water/sediment systems. , 2005, Environmental science & technology.

[17]  T. Poiger,et al.  Combined sewer overflows to surface waters detected by the anthropogenic marker caffeine. , 2006, Environmental science & technology.

[18]  Kohji Yamamoto,et al.  Steroid hormone profiles of urban and tidal rivers using LC/MS/MS equipped with electrospray ionization and atmospheric pressure photoionization sources. , 2006, Environmental science & technology.

[19]  R. Schwarzenbach,et al.  The Challenge of Micropollutants in Aquatic Systems , 2006, Science.

[20]  H. Nakata,et al.  Occurrence and concentrations of benzotriazole UV stabilizers in marine organisms and sediments from the Ariake Sea, Japan. , 2009, Environmental science & technology.

[21]  Steven J Lehotay,et al.  Fast and easy multiresidue method employing acetonitrile extraction/partitioning and "dispersive solid-phase extraction" for the determination of pesticide residues in produce. , 2003, Journal of AOAC International.

[22]  Robert Baudot,et al.  Development of a multi-residue method using acetonitrile-based extraction followed by liquid chromatography-tandem mass spectrometry for the analysis of steroids and veterinary and human drugs at trace levels in soil. , 2012, Journal of chromatography. A.

[23]  O. Cheshnovsky,et al.  Proton transfer reactions in neutral gas-phase clusters: 1-Naphthol with H2O, D2O, CH3OH, NH3 and piperidine , 1988 .

[24]  Xiaolin Li,et al.  Analysis of quaternary ammonium compounds in estuarine sediments by LC-ToF-MS: very high positive mass defects of alkylamine ions as powerful diagnostic tools for identification and structural elucidation. , 2009, Analytical chemistry.

[25]  F. Hernández,et al.  Current use of high-resolution mass spectrometry in the environmental sciences , 2012, Analytical and Bioanalytical Chemistry.

[26]  C. Cren-olivé,et al.  Multiresidue method for the determination of 13 pesticides in three environmental matrices: water, sediments and fish muscle. , 2011, Talanta.

[27]  D. Barceló,et al.  Presence of surfactants and their degradation intermediates in sediment cores and grabs from the Cadiz Bay area. , 2006, Environmental pollution.

[28]  N. Itoh,et al.  Optimization of the dopant for the trace determination of polycyclic aromatic hydrocarbons by liquid chromatography/dopant-assisted atmospheric-pressure photoionization/mass spectrometry. , 2006, Journal of chromatography. A.

[29]  Xiaojun Luo,et al.  Distribution of polycyclic musks in surface sediments from the Pearl River Delta and Macao coastal region, South China , 2008, Environmental toxicology and chemistry.

[30]  A. Sapkota,et al.  Detection of triclocarban and two co-contaminating chlorocarbanilides in US aquatic environments using isotope dilution liquid chromatography tandem mass spectrometry. , 2007, Environmental research.

[31]  Watze de Wolf,et al.  Removal of fragrance materials during U.S. and European wastewater treatment. , 2002, Environmental science & technology.

[32]  D. Barceló,et al.  Immunosorbents Coupled On-Line with Liquid Chromatography/Atmospheric Pressure Chemical Ionization/Mass Spectrometry for the Part per Trillion Level Determination of Pesticides in Sediments and Natural Waters Using Low Preconcentration Volumes , 1997 .

[33]  Aaron M. Peck,et al.  Synthetic musk fragrances in Lake Michigan. , 2004, Environmental science & technology.

[34]  O. Mcconnell,et al.  Advantages of atmospheric pressure photoionization mass spectrometry in support of drug discovery. , 2005, Rapid communications in mass spectrometry : RCM.

[35]  S. Tanabe,et al.  Bioaccumulation, temporal trend, and geographical distribution of synthetic musks in the marine environment. , 2007, Environmental science & technology.

[36]  Christopher M. Reddy,et al.  Environmental Chemistry of Benzothiazoles Derived from Rubber , 1997 .

[37]  H. Singer,et al.  Triclosan: occurrence and fate of a widely used biocide in the aquatic environment: field measurements in wastewater treatment plants, surface waters, and lake sediments. , 2002, Environmental science & technology.

[38]  J. Ritchie,et al.  Fate of triclosan and evidence for reductive dechlorination of triclocarban in estuarine sediments. , 2008, Environmental science & technology.

[39]  J. Henion,et al.  Atmospheric pressure photoionization liquid chromatographic-mass spectrometric determination of idoxifene and its metabolites in human plasma. , 2002, Journal of chromatography. A.

[40]  Aaron M. Peck,et al.  Synthetic musk fragrances in Lake Erie and Lake Ontario sediment cores. , 2006, Environmental science & technology.

[41]  Walter Giger,et al.  Benzotriazole and tolyltriazole as aquatic contaminants. 1. Input and occurrence in rivers and lakes. , 2006, Environmental science & technology.

[42]  Jun-ichi Ebina,et al.  Simultaneous determination of total nitrogen and total phosphorus in water using peroxodisulfate oxidation , 1983 .

[43]  R. Kostiainen,et al.  Gas chromatography/mass spectrometry of polychlorinated biphenyls using atmospheric pressure chemical ionization and atmospheric pressure photoionization microchips. , 2008, Rapid communications in mass spectrometry : RCM.

[44]  E. P. Hunter,et al.  Evaluated Gas Phase Basicities and Proton Affinities of Molecules: An Update , 1998 .

[45]  J. Knezovich,et al.  The bioavailability of sediment-sorbed organic chemicals: A review , 1987 .

[46]  D. Grandjean,et al.  Toxic effects of Irgarol 1051 on phytoplankton and macrophytes in Lake Geneva. , 2002, Water research.

[47]  R. Kostiainen,et al.  Effect of eluent on the ionization process in liquid chromatography-mass spectrometry. , 2009, Journal of chromatography. A.

[48]  M. Balogh,et al.  Ultra performance liquid chromatography-atmospheric pressure photoionization-tandem mass spectrometry for high-sensitivity and high-throughput analysis of U.S. Environmental Protection Agency 16 priority pollutants polynuclear aromatic hydrocarbons. , 2009, Analytical chemistry.

[49]  Anton Lindström,et al.  Occurrence and environmental behavior of the bactericide triclosan and its methyl derivative in surface waters and in wastewater. , 2002, Environmental science & technology.

[50]  T. Ternes,et al.  Determination of acidic pharmaceuticals, antibiotics and ivermectin in river sediment using liquid chromatography-tandem mass spectrometry. , 2003, Journal of chromatography. A.

[51]  W. Giger,et al.  Temporal trends, congener patterns, and sources of octa-, nona-, and decabromodiphenyl ethers (PBDE) and hexabromocyclododecanes (HBCD) in Swiss lake sediments. , 2008, Environmental science & technology.

[52]  W. Eckhoff,et al.  Trace Analysis of Fragrance Materials in Wastewater and Treated Wastewater , 2000 .

[53]  K. Carlson,et al.  Temporal and spatial trends in the occurrence of human and veterinary antibiotics in aqueous and river sediment matrices. , 2007, Environmental science & technology.