An isotope dilution high-resolution mass spectrometry method for quantitative measurement of isomeric benzo[a]pyrene tetrol metabolites derived from albumin-bapde adducts as indicators of human exposure to polycyclic aromatic hydrocarbons

Angela D. Ragin, Kenroy E. Crawford, Christopher Davies, Miranda Hallett, Alisha A. Etheredge, James Grainger, Donald George Jr Patterson

Research output: Contribution to journalArticle

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Abstract

We evaluated in a pilot study a newly developed method of gas chromatography isotope dilution high-resolution mass spectrometry selected ion monitoring (GC-ID-HRMS-SIM). This method measures benzo[a]pyrene (B[a]P) tetrol metabolites released after albumin-BaPDE adduct hydrolysis. We isolated albumin adducts from the blood of a cohort of adult male and female smokers and nonsmokers randomly selected as exposed and nonexposed groups. Isomeric B[a]P tetrols released after adduct hydrolysis and silyl derivatization were quantified by GC-ID-HRMS-SIM using 13C6-isotopically labeled BaP tetrol isomer standards (+/-)-BaP-r-7,t-8,t-9,c-10-tetrol (BPTI-1), (+/-)-BaP-r-7,t-8,t-9,t-10-tetrol (BPTI-2), (+/-)-BaP-r-7,t-8,c-9,t-10-tetrol (BPTII-1) and (+/-)-BaP-r-7,t-8,c-9,c-10-tetrol (BPTII-2). In all donor samples analyzed the method was sensitive enough to detect BPTII-1 and BPTI-1 in the low fmol range. In both smokers and nonsmokers BPTI-1 levels were higher than BPTII-1 levels. The mean levels of BPTII-1 and BPTI-1 in smokers were 0.16 ± 0.04 fmol/mg albumin (ranging from 0.09 to 0.28 fmol/mg albumin) and 0.40 ± 0.06 fmol/mg albumin (ranging from 0.25 to 0.75 fmol/mg albumin), respectively. The mean levels of BPTII-1 and BPTI-1 in nonsmokers were 0.22 ± 0.07 fmol/mg albumin (ranging from 0.09 to 0.41 fmol/mg albumin) and 0.47 ± 0.06 fmol/mg albumin (ranging from 0.30 to 0.75 fmol/mg albumin), respectively. The results from this study are the first reported quantitative levels of specific benzo[a]pyrene tetrol isomers detected by isotope dilution high-resolution mass spectrometry measurements of BaPDE-albumin adducts using 13C6-isotopically labeled BaP tetrol isomer standards.

Original languageEnglish (US)
Pages (from-to)434-450
Number of pages17
JournalPolycyclic Aromatic Compounds
Volume28
Issue number4-5
DOIs
StatePublished - Aug 1 2008

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Polycyclic Aromatic Hydrocarbons
Pyrene
Polycyclic aromatic hydrocarbons
Metabolites
Isotopes
Isomers
Dilution
Mass spectrometry
Albumins
Hydrolysis
Gas chromatography
Blood
Monitoring
Ions
benzo(a)pyrene tetrol

All Science Journal Classification (ASJC) codes

  • Polymers and Plastics
  • Organic Chemistry
  • Materials Chemistry

Cite this

Ragin, Angela D. ; Crawford, Kenroy E. ; Davies, Christopher ; Hallett, Miranda ; Etheredge, Alisha A. ; Grainger, James ; Patterson, Donald George Jr. / An isotope dilution high-resolution mass spectrometry method for quantitative measurement of isomeric benzo[a]pyrene tetrol metabolites derived from albumin-bapde adducts as indicators of human exposure to polycyclic aromatic hydrocarbons. In: Polycyclic Aromatic Compounds. 2008 ; Vol. 28, No. 4-5. pp. 434-450.
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abstract = "We evaluated in a pilot study a newly developed method of gas chromatography isotope dilution high-resolution mass spectrometry selected ion monitoring (GC-ID-HRMS-SIM). This method measures benzo[a]pyrene (B[a]P) tetrol metabolites released after albumin-BaPDE adduct hydrolysis. We isolated albumin adducts from the blood of a cohort of adult male and female smokers and nonsmokers randomly selected as exposed and nonexposed groups. Isomeric B[a]P tetrols released after adduct hydrolysis and silyl derivatization were quantified by GC-ID-HRMS-SIM using 13C6-isotopically labeled BaP tetrol isomer standards (+/-)-BaP-r-7,t-8,t-9,c-10-tetrol (BPTI-1), (+/-)-BaP-r-7,t-8,t-9,t-10-tetrol (BPTI-2), (+/-)-BaP-r-7,t-8,c-9,t-10-tetrol (BPTII-1) and (+/-)-BaP-r-7,t-8,c-9,c-10-tetrol (BPTII-2). In all donor samples analyzed the method was sensitive enough to detect BPTII-1 and BPTI-1 in the low fmol range. In both smokers and nonsmokers BPTI-1 levels were higher than BPTII-1 levels. The mean levels of BPTII-1 and BPTI-1 in smokers were 0.16 ± 0.04 fmol/mg albumin (ranging from 0.09 to 0.28 fmol/mg albumin) and 0.40 ± 0.06 fmol/mg albumin (ranging from 0.25 to 0.75 fmol/mg albumin), respectively. The mean levels of BPTII-1 and BPTI-1 in nonsmokers were 0.22 ± 0.07 fmol/mg albumin (ranging from 0.09 to 0.41 fmol/mg albumin) and 0.47 ± 0.06 fmol/mg albumin (ranging from 0.30 to 0.75 fmol/mg albumin), respectively. The results from this study are the first reported quantitative levels of specific benzo[a]pyrene tetrol isomers detected by isotope dilution high-resolution mass spectrometry measurements of BaPDE-albumin adducts using 13C6-isotopically labeled BaP tetrol isomer standards.",
author = "Ragin, {Angela D.} and Crawford, {Kenroy E.} and Christopher Davies and Miranda Hallett and Etheredge, {Alisha A.} and James Grainger and Patterson, {Donald George Jr}",
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An isotope dilution high-resolution mass spectrometry method for quantitative measurement of isomeric benzo[a]pyrene tetrol metabolites derived from albumin-bapde adducts as indicators of human exposure to polycyclic aromatic hydrocarbons. / Ragin, Angela D.; Crawford, Kenroy E.; Davies, Christopher; Hallett, Miranda; Etheredge, Alisha A.; Grainger, James; Patterson, Donald George Jr.

In: Polycyclic Aromatic Compounds, Vol. 28, No. 4-5, 01.08.2008, p. 434-450.

Research output: Contribution to journalArticle

TY - JOUR

T1 - An isotope dilution high-resolution mass spectrometry method for quantitative measurement of isomeric benzo[a]pyrene tetrol metabolites derived from albumin-bapde adducts as indicators of human exposure to polycyclic aromatic hydrocarbons

AU - Ragin, Angela D.

AU - Crawford, Kenroy E.

AU - Davies, Christopher

AU - Hallett, Miranda

AU - Etheredge, Alisha A.

AU - Grainger, James

AU - Patterson, Donald George Jr

PY - 2008/8/1

Y1 - 2008/8/1

N2 - We evaluated in a pilot study a newly developed method of gas chromatography isotope dilution high-resolution mass spectrometry selected ion monitoring (GC-ID-HRMS-SIM). This method measures benzo[a]pyrene (B[a]P) tetrol metabolites released after albumin-BaPDE adduct hydrolysis. We isolated albumin adducts from the blood of a cohort of adult male and female smokers and nonsmokers randomly selected as exposed and nonexposed groups. Isomeric B[a]P tetrols released after adduct hydrolysis and silyl derivatization were quantified by GC-ID-HRMS-SIM using 13C6-isotopically labeled BaP tetrol isomer standards (+/-)-BaP-r-7,t-8,t-9,c-10-tetrol (BPTI-1), (+/-)-BaP-r-7,t-8,t-9,t-10-tetrol (BPTI-2), (+/-)-BaP-r-7,t-8,c-9,t-10-tetrol (BPTII-1) and (+/-)-BaP-r-7,t-8,c-9,c-10-tetrol (BPTII-2). In all donor samples analyzed the method was sensitive enough to detect BPTII-1 and BPTI-1 in the low fmol range. In both smokers and nonsmokers BPTI-1 levels were higher than BPTII-1 levels. The mean levels of BPTII-1 and BPTI-1 in smokers were 0.16 ± 0.04 fmol/mg albumin (ranging from 0.09 to 0.28 fmol/mg albumin) and 0.40 ± 0.06 fmol/mg albumin (ranging from 0.25 to 0.75 fmol/mg albumin), respectively. The mean levels of BPTII-1 and BPTI-1 in nonsmokers were 0.22 ± 0.07 fmol/mg albumin (ranging from 0.09 to 0.41 fmol/mg albumin) and 0.47 ± 0.06 fmol/mg albumin (ranging from 0.30 to 0.75 fmol/mg albumin), respectively. The results from this study are the first reported quantitative levels of specific benzo[a]pyrene tetrol isomers detected by isotope dilution high-resolution mass spectrometry measurements of BaPDE-albumin adducts using 13C6-isotopically labeled BaP tetrol isomer standards.

AB - We evaluated in a pilot study a newly developed method of gas chromatography isotope dilution high-resolution mass spectrometry selected ion monitoring (GC-ID-HRMS-SIM). This method measures benzo[a]pyrene (B[a]P) tetrol metabolites released after albumin-BaPDE adduct hydrolysis. We isolated albumin adducts from the blood of a cohort of adult male and female smokers and nonsmokers randomly selected as exposed and nonexposed groups. Isomeric B[a]P tetrols released after adduct hydrolysis and silyl derivatization were quantified by GC-ID-HRMS-SIM using 13C6-isotopically labeled BaP tetrol isomer standards (+/-)-BaP-r-7,t-8,t-9,c-10-tetrol (BPTI-1), (+/-)-BaP-r-7,t-8,t-9,t-10-tetrol (BPTI-2), (+/-)-BaP-r-7,t-8,c-9,t-10-tetrol (BPTII-1) and (+/-)-BaP-r-7,t-8,c-9,c-10-tetrol (BPTII-2). In all donor samples analyzed the method was sensitive enough to detect BPTII-1 and BPTI-1 in the low fmol range. In both smokers and nonsmokers BPTI-1 levels were higher than BPTII-1 levels. The mean levels of BPTII-1 and BPTI-1 in smokers were 0.16 ± 0.04 fmol/mg albumin (ranging from 0.09 to 0.28 fmol/mg albumin) and 0.40 ± 0.06 fmol/mg albumin (ranging from 0.25 to 0.75 fmol/mg albumin), respectively. The mean levels of BPTII-1 and BPTI-1 in nonsmokers were 0.22 ± 0.07 fmol/mg albumin (ranging from 0.09 to 0.41 fmol/mg albumin) and 0.47 ± 0.06 fmol/mg albumin (ranging from 0.30 to 0.75 fmol/mg albumin), respectively. The results from this study are the first reported quantitative levels of specific benzo[a]pyrene tetrol isomers detected by isotope dilution high-resolution mass spectrometry measurements of BaPDE-albumin adducts using 13C6-isotopically labeled BaP tetrol isomer standards.

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