Searching for anthropogenic contaminants in human breast adipose tissues using gas chromatography-time-of-flight mass spectrometry.

The potential of gas chromatography-time-of-flight mass spectrometry (GC-TOF MS) for screening anthropogenic organic contaminants in human breast adipose tissues has been investigated. Initially a target screening was performed for a list of 125 compounds which included persistent halogen pollutants [organochlorine (OC) pesticides, polychlorinated biphenylss (PCBs), polybrominated diphenyl ethers (PBDEs)], polyaromatic hydrocarbons (PAHs), alkylphenols, and a notable number of pesticides from the different fungicide, herbicide and insecticide families. Searching for target pollutants was done by evaluating the presence of up to five representative ions for every analyte, all measured at accurate mass (20-mDa mass window). The experimental ion abundance ratios were then compared to those of reference standards for confirmation. Sample treatment consisted of an extraction with hexane and subsequent normal-phase (NP) High performance liquid chromatography (HPLC) or SPE cleanup. The fat-free LC fractions were then investigated by GC-TOF MS.Full-spectral acquisition and accurate mass data generated by GC-TOF MS also allowed the investigation of nontarget compounds using appropriate processing software to manage MS data. Identification was initially based on library fit using commercial nominal mass libraries. This was followed by comparing the experimental accurate masses of the most relevant ions with the theoretical exact masses with calculations made using the elemental composition calculator included in the software.The application of both target and nontarget approaches to around 40 real samples allowed the detection and confirmation of several target pollutants including p,p'-DDE, hexachlorobenzene (HCB), and some polychlorinated biphenyls (PCBs) and polyaromatic hydrocarbons (PAHs). Several nontarget compounds that could be considered anthropogenic pollutants were also detected. These included 3,5-di-tert-butyl-4-hydroxy-toluene (BHT) and its metabolite 3,5-di-tert-butyl-4-hydroxybenzaldehyde (BHT-CHO), dibenzylamine, N-butyl benzenesulfonamide (N-BBSA), some naphthalene-related compounds and several PCBs isomers not included in the target list. As some of the compounds detected are xenoestrogens, the methodology developed in this paper could be useful in human breast cancer research.

[1]  J. M. Cruz,et al.  Determination of butylated hydroxytoluene in food samples by high-performance liquid chromatography with ultraviolet detection and gas chromatography/mass spectrometry. , 2007, Journal of AOAC International.

[2]  Joel A Pedersen,et al.  Xenobiotic organic compounds in runoff from fields irrigated with treated wastewater. , 2003, Journal of agricultural and food chemistry.

[3]  I. Meerts,et al.  In vitro estrogenicity of polybrominated diphenyl ethers, hydroxylated PDBEs, and polybrominated bisphenol A compounds. , 2001, Environmental health perspectives.

[4]  W. Jarman,et al.  Surveillance for previously unmonitored organic contaminants in the San Francisco Estuary. , 2003, Marine pollution bulletin.

[5]  Min-hua Yang,et al.  A rapid gas chromatographic method for direct determination of BHA, BHT and TBHQ in edible oils and fats , 2002 .

[6]  Olivier Humblet,et al.  Environmental pollutants and breast cancer: epidemiologic studies. , 2007, Cancer.

[7]  Wen-hua Wang,et al.  PM10-bound Polycyclic Aromatic Hydrocarbons (PAHs) and Cancer Risk Estimation in the Atmosphere Surrounding an Industrial Area of Shanghai, China , 2007 .

[8]  Tania Portolés,et al.  Potential of gas chromatography coupled to triple quadrupole mass spectrometry for quantification and confirmation of organohalogen xenoestrogen compounds in human breast tissues. , 2005, Analytical chemistry.

[9]  Norma B Tombesi,et al.  Application of solid-phase microextraction combined with gas chromatography-mass spectrometry to the determination of butylated hydroxytoluene in bottled drinking water. , 2002, Journal of chromatography. A.

[10]  J. Pedraz,et al.  Determination of low concentrations of dibenzylamine in human plasma and urine by gas chromatography with a nitrogen-phosphorus detector. , 1989, Journal of chromatography.

[11]  Tania Portolés,et al.  Target and nontarget screening of organic micropollutants in water by solid-phase microextraction combined with gas chromatography/high-resolution time-of-flight mass spectrometry. , 2007, Analytical chemistry.

[12]  J. V. Sancho,et al.  Critical review of the application of liquid chromatography/mass spectrometry to the determination of pesticide residues in biological samples , 2005, Analytical and bioanalytical chemistry.

[13]  M. Galceran,et al.  Modern developments in gas chromatography-mass spectrometry-based environmental analysis. , 2003, Journal of chromatography. A.

[14]  M. Stenstrom,et al.  Human Pharmaceuticals, Antioxidants, and Plasticizers in Wastewater Treatment Plant and Water Reclamation Plant Effluents , 2007, Water environment research : a research publication of the Water Environment Federation.

[15]  L. Herrero,et al.  Quantitative analysis of polybrominated diphenyl ethers in adipose tissue, human serum and foodstuff samples by gas chromatography with ion trap tandem mass spectrometry and isotope dilution. , 2006, Rapid communications in mass spectrometry : RCM.

[16]  A. Grange,et al.  Utility of three types of mass spectrometers for determining elemental compositions of ions formed from chromatographically separated compounds. , 2002, Rapid communications in mass spectrometry : RCM.

[17]  F. Hernández,et al.  Determination of PBDEs in human breast adipose tissues by gas chromatography coupled with triple quadrupole mass spectrometry , 2008, Analytical and bioanalytical chemistry.

[18]  Dana B Barr,et al.  Analytical methods for biological monitoring of exposure to pesticides: a review. , 2002, Journal of chromatography. B, Analytical technologies in the biomedical and life sciences.

[19]  Félix Hernández,et al.  Potential of liquid chromatography/time-of-flight mass spectrometry for the determination of pesticides and transformation products in water , 2006, Analytical and bioanalytical chemistry.

[20]  Damià Barceló,et al.  Characterisation of organic pollutants in textile wastewaters and landfill leachate by using toxicity-based fractionation methods followed by liquid and gas chromatography coupled to mass spectrometric detection , 2001 .

[21]  Ruthann A Rudel,et al.  Environmental pollutants and breast cancer , 2007, Cancer.

[22]  Félix Hernández,et al.  Strategies for quantification and confirmation of multi-class polar pesticides and transformation products in water by LC–MS2 using triple quadrupole and hybrid quadrupole time-of-flight analyzers , 2005 .

[23]  J. V. Sancho,et al.  Methodical approach for the use of GC-TOF MS for screening and confirmation of organic pollutants in environmental water. , 2007, Journal of mass spectrometry : JMS.

[24]  U. Brinkman,et al.  Evaluation of a high-resolution time-of-flight mass spectrometer for the gas chromatographic determination of selected environmental contaminants. , 2002, Journal of chromatography. A.

[25]  L. Fay,et al.  Potential of gas chromatography-orthogonal acceleration time-of-flight mass spectrometry (GC-oaTOFMS) in flavor research. , 2003, Journal of agricultural and food chemistry.

[26]  W. Püttmann,et al.  Analysis of the antioxidant butylated hydroxytoluene (BHT) in water by means of solid phase extraction combined with GC/MS. , 2002, Water research.

[27]  F. Hernández,et al.  Determination of priority organic micro-pollutants in water by gas chromatography coupled to triple quadrupole mass spectrometry. , 2007, Analytica chimica acta.

[28]  T. Cajka,et al.  Challenges of gas chromatography-high-resolution time-of-flight mass spectrometry for simultaneous analysis of polybrominated diphenyl ethers and other halogenated persistent organic pollutants in environmental samples. , 2005, Journal of separation science.

[29]  J. Hajšlová Gas Chromatography – Time-of-Flight Mass Spectrometry in Food Analysis , 2022 .

[30]  M. Nielen,et al.  Screening and confirmation criteria for hormone residue analysis using liquid chromatography accurate mass time-of-flight, Fourier transform ion cyclotron resonance and orbitrap mass spectrometry techniques. , 2007, Analytica chimica acta.

[31]  P. Verger,et al.  Dietary exposure of children and teenagers to benzoates, sulphites, butylhydroxyanisol (BHA) and butylhydroxytoluen (BHT) in Beirut (Lebanon). , 2007, Regulatory toxicology and pharmacology : RTP.

[32]  F. Iverson,et al.  Levels of BHA and BHT in human and animal adipose tissue: interspecies extrapolation. , 1986, Food and chemical toxicology : an international journal published for the British Industrial Biological Research Association.

[33]  M. Ibáñez,et al.  Comparison of different mass spectrometric techniques combined with liquid chromatography for confirmation of pesticides in environmental water based on the use of identification points. , 2004, Analytical chemistry.

[34]  Félix Hernández,et al.  Rapid non-target screening of organic pollutants in water by ultraperformance liquid chromatography coupled to time-of-light mass spectrometry , 2008 .

[35]  Evaluation of PAH bioaccumulation and DNA damage in mussels (Mytilus galloprovincialis) exposed to spilled Prestige crude oil. , 2004, Comparative biochemistry and physiology. Toxicology & pharmacology : CBP.

[36]  A. Sasco,et al.  Breast Cancer Risk and the Combined Effect of Environmental Estrogens , 2004, Cancer Causes & Control.

[37]  C. V. Van Peteghem,et al.  Monitoring of polychlorinated biphenyls in Belgian human adipose tissue samples. , 2005, Chemosphere.

[38]  Jana Hajslova,et al.  Determination of polybrominated diphenyl ethers in human milk samples in the Czech Republic: Comparative study of negative chemical ionisation mass spectrometry and time-of-flight high-resolution mass spectrometry , 2004 .

[39]  R. Fussell,et al.  Quantification and screening of pesticide residues in food by gas chromatography-exact mass time-of-flight mass spectrometry. , 2007, Journal of chromatography. A.