DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Utilizing ion mobility spectrometry and mass spectrometry for the analysis of polycyclic aromatic hydrocarbons, polychlorinated biphenyls, polybrominated diphenyl ethers and their metabolites

Abstract

Polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) are persistent environmental pollutants originating from incomplete combustion of organic materials and synthetic sources. PAHs, PCBs, and PBDEs have all been shown to have a significant effect on human health with correlations to cancer and other diseases. Therefore, measuring the presence of these xenobiotics in the environment and human body is imperative for assessing their health risks. To date, their analyses require both gas chromatography and liquid chromatography separations in conjunction with mass spectrometry measurements for detection of both the parent molecules and their hydroxylated metabolites, making their studies extremely time consuming. Here in this work, we characterized PAHs, PCBs, PBDEs and their hydroxylated metabolites using ion mobility spectrometry coupled with mass spectrometry (IMS-MS) and in combination with different ionization methods including electrospray ionization (ESI), atmospheric pressure chemical ionization (APCI) and atmospheric pressure photoionization (APPI). In conclusion, the collision cross section and m/z trend lines derived from the IMS-MS analyses displayed distinct trends for each molecule type. Additionally, the rapid isomeric and molecular separations possible with IMS-MS showed great promise for quickly distinguishing the parent and metabolized PAH, PCB, and PDBE molecules in complex environmental and biological samples.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Biological Sciences Division
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1437019
Alternate Identifier(s):
OSTI ID: 1703100
Report Number(s):
PNNL-SA-130591
Journal ID: ISSN 0003-2670; PII: S0003267018302824
Grant/Contract Number:  
AC05-76RL01830; AC05-76RL0 1830
Resource Type:
Accepted Manuscript
Journal Name:
Analytica Chimica Acta
Additional Journal Information:
Journal Volume: 1037; Journal ID: ISSN 0003-2670
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 59 BASIC BIOLOGICAL SCIENCES; Ion mobility spectrometry; Collision cross section; Xenobiotics; Polycyclic aromatic hydrocarbons; Polychlorinated biphenyls; Polybrominated diphenyl ethers; Electrospray ionization; Atmospheric pressure chemical ionization; Atmospheric pressure photoionization

Citation Formats

Zheng, Xueyun, Dupuis, Kevin T., Aly, Noor A., Zhou, Yuxuan, Smith, Francesca B., Tang, Keqi, Smith, Richard D., and Baker, Erin S. Utilizing ion mobility spectrometry and mass spectrometry for the analysis of polycyclic aromatic hydrocarbons, polychlorinated biphenyls, polybrominated diphenyl ethers and their metabolites. United States: N. p., 2018. Web. doi:10.1016/j.aca.2018.02.054.
Zheng, Xueyun, Dupuis, Kevin T., Aly, Noor A., Zhou, Yuxuan, Smith, Francesca B., Tang, Keqi, Smith, Richard D., & Baker, Erin S. Utilizing ion mobility spectrometry and mass spectrometry for the analysis of polycyclic aromatic hydrocarbons, polychlorinated biphenyls, polybrominated diphenyl ethers and their metabolites. United States. https://doi.org/10.1016/j.aca.2018.02.054
Zheng, Xueyun, Dupuis, Kevin T., Aly, Noor A., Zhou, Yuxuan, Smith, Francesca B., Tang, Keqi, Smith, Richard D., and Baker, Erin S. Fri . "Utilizing ion mobility spectrometry and mass spectrometry for the analysis of polycyclic aromatic hydrocarbons, polychlorinated biphenyls, polybrominated diphenyl ethers and their metabolites". United States. https://doi.org/10.1016/j.aca.2018.02.054. https://www.osti.gov/servlets/purl/1437019.
@article{osti_1437019,
title = {Utilizing ion mobility spectrometry and mass spectrometry for the analysis of polycyclic aromatic hydrocarbons, polychlorinated biphenyls, polybrominated diphenyl ethers and their metabolites},
author = {Zheng, Xueyun and Dupuis, Kevin T. and Aly, Noor A. and Zhou, Yuxuan and Smith, Francesca B. and Tang, Keqi and Smith, Richard D. and Baker, Erin S.},
abstractNote = {Polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) are persistent environmental pollutants originating from incomplete combustion of organic materials and synthetic sources. PAHs, PCBs, and PBDEs have all been shown to have a significant effect on human health with correlations to cancer and other diseases. Therefore, measuring the presence of these xenobiotics in the environment and human body is imperative for assessing their health risks. To date, their analyses require both gas chromatography and liquid chromatography separations in conjunction with mass spectrometry measurements for detection of both the parent molecules and their hydroxylated metabolites, making their studies extremely time consuming. Here in this work, we characterized PAHs, PCBs, PBDEs and their hydroxylated metabolites using ion mobility spectrometry coupled with mass spectrometry (IMS-MS) and in combination with different ionization methods including electrospray ionization (ESI), atmospheric pressure chemical ionization (APCI) and atmospheric pressure photoionization (APPI). In conclusion, the collision cross section and m/z trend lines derived from the IMS-MS analyses displayed distinct trends for each molecule type. Additionally, the rapid isomeric and molecular separations possible with IMS-MS showed great promise for quickly distinguishing the parent and metabolized PAH, PCB, and PDBE molecules in complex environmental and biological samples.},
doi = {10.1016/j.aca.2018.02.054},
journal = {Analytica Chimica Acta},
number = ,
volume = 1037,
place = {United States},
year = {2018},
month = {3}
}

Journal Article:

Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: a) Representative chemical structures of PAHs, PCBs and PDBEs. PAHs consist of fused benzene rings (i.e. naphthalene, anthracene and benzo(a)pyrene) as shown in the top panel, while the different phenyl linkages and nomenclature of PCBs and PBDEs are shown below. For the PCBs and PDBEs, chlorines and brominesmore » are substituted for hydrogens at the 10 possible positions on the two phenyl rings and they are numbered as 2 to 6 on the first ring and 2´ to 6´ on the second. The 2, 2´, 6 and 6´ positions closest to the diphenyl (or diphenyl ether) bond are described as ortho, while para corresponds to the 4 and 4´ positions and meta has the 3, 3´, 5 and 5´ positions. The number and location of chlorines and bromines determine both the physical and biological activities of each molecule. b) A schematic of ion mobility spectrometry separation principle. Briefly, in an IMS separation, the ions travel through a drift cell filled with buffer gas (i.e. N2) under the influence of a weak electric field. The separation depends on the mass, charge and the shape of the ions. For isomers with the same m/z, compact structures will travel faster than more extended structures.« less

Save / Share:

Works referenced in this record:

Cumulative exposure assessment for trace-level polycyclic aromatic hydrocarbons (PAHs) using human blood and plasma analysis
journal, July 2010


Developmental toxicity of polychlorinated biphenyls (PCBs): a systematic review of experimental data
journal, April 2004


Towards a global historical emission inventory for selected PCB congeners — A mass balance approach
journal, May 2007


Exposure to Polychlorinated Biphenyls (PCBs) and Male Reproduction
journal, January 2010


Health effects and exposure to polychlorinated biphenyls (PCBs) and metals in a contaminated community
journal, September 2012


Dietary exposure to polychlorinated biphenyls and risk of breast, endometrial and ovarian cancer in a prospective cohort
journal, September 2016

  • Donat-Vargas, Carolina; Åkesson, Agneta; Berglund, Marika
  • British Journal of Cancer, Vol. 115, Issue 9
  • DOI: 10.1038/bjc.2016.282

PCBs and OH-PCBs in Serum from Children and Mothers in Urban and Rural U.S. Communities
journal, March 2013

  • Marek, Rachel F.; Thorne, Peter S.; Wang, Kai
  • Environmental Science & Technology, Vol. 47, Issue 7
  • DOI: 10.1021/es304455k

Occurrence and Distribution of Two Hydroxylated Polychlorinated Biphenyl Congeners in Chicago Air
journal, December 2015

  • Awad, Andrew M.; Martinez, Andres; Marek, Rachel F.
  • Environmental Science & Technology Letters, Vol. 3, Issue 2
  • DOI: 10.1021/acs.estlett.5b00337

Enhancing bottom-up and top-down proteomic measurements with ion mobility separations
journal, July 2015

  • Baker, Erin Shammel; Burnum-Johnson, Kristin E.; Ibrahim, Yehia M.
  • PROTEOMICS, Vol. 15, Issue 16
  • DOI: 10.1002/pmic.201500048

Uncovering biologically significant lipid isomers with liquid chromatography, ion mobility spectrometry and mass spectrometry
journal, January 2016

  • Kyle, Jennifer E.; Zhang, Xing; Weitz, Karl K.
  • The Analyst, Vol. 141, Issue 5
  • DOI: 10.1039/C5AN02062J

Towards unsupervised polyaromatic hydrocarbons structural assignment from SA-TIMS –FTMS data
journal, June 2015

  • Benigni, Paolo; Marin, Rebecca; Fernandez-Lima, Francisco
  • International Journal for Ion Mobility Spectrometry, Vol. 18, Issue 3-4
  • DOI: 10.1007/s12127-015-0175-y

Conformational Ordering of Biomolecules in the Gas Phase: Nitrogen Collision Cross Sections Measured on a Prototype High Resolution Drift Tube Ion Mobility-Mass Spectrometer
journal, February 2014

  • May, Jody C.; Goodwin, Cody R.; Lareau, Nichole M.
  • Analytical Chemistry, Vol. 86, Issue 4, p. 2107-2116
  • DOI: 10.1021/ac4038448

Development of a new ion mobility time-of-flight mass spectrometer
journal, February 2015

  • Ibrahim, Yehia M.; Baker, Erin S.; Danielson, William F.
  • International Journal of Mass Spectrometry, Vol. 377
  • DOI: 10.1016/j.ijms.2014.07.034

An Interlaboratory Evaluation of Drift Tube Ion Mobility–Mass Spectrometry Collision Cross Section Measurements
journal, August 2017


Negative ion-atmospheric pressure photoionization-mass spectrometry
journal, February 2004

  • Kauppila, Tiina J.; Kotiaho, Tapio; Kostiainen, Risto
  • Journal of the American Society for Mass Spectrometry, Vol. 15, Issue 2
  • DOI: 10.1016/j.jasms.2003.10.012

Detection and Monitoring of PAH and Oxy-PAHs by High Resolution Mass Spectrometry: Comparison of ESI, APCI and APPI Source Detection
journal, January 2012

  • Ghislain, Thierry; Faure, Pierre; Michels, Raymond
  • Journal of The American Society for Mass Spectrometry, Vol. 23, Issue 3
  • DOI: 10.1007/s13361-011-0304-8

Charge Exchange Reaction in Dopant-Assisted Atmospheric Pressure Chemical Ionization and Atmospheric Pressure Photoionization
journal, April 2016

  • Vaikkinen, Anu; Kauppila, Tiina J.; Kostiainen, Risto
  • Journal of The American Society for Mass Spectrometry, Vol. 27, Issue 8
  • DOI: 10.1007/s13361-016-1399-8

Distinguishing d - and l -aspartic and isoaspartic acids in amyloid β peptides with ultrahigh resolution ion mobility spectrometry
journal, January 2017

  • Zheng, Xueyun; Deng, Liulin; Baker, Erin S.
  • Chemical Communications, Vol. 53, Issue 56
  • DOI: 10.1039/C7CC03321D

Structural Elucidation of cis / trans Dicaffeoylquinic Acid Photoisomerization Using Ion Mobility Spectrometry-Mass Spectrometry
journal, March 2017

  • Zheng, Xueyun; Renslow, Ryan S.; Makola, Mpho M.
  • The Journal of Physical Chemistry Letters, Vol. 8, Issue 7
  • DOI: 10.1021/acs.jpclett.6b03015

Lipid and Glycolipid Isomer Analyses Using Ultra-High Resolution Ion Mobility Spectrometry Separations
journal, January 2017

  • Wojcik, Roza; Webb, Ian; Deng, Liulin
  • International Journal of Molecular Sciences, Vol. 18, Issue 1
  • DOI: 10.3390/ijms18010183

Works referencing / citing this record:

Ion Mobility Spectrometry in Food Analysis: Principles, Current Applications and Future Trends
journal, July 2019

  • Hernández-Mesa, Maykel; Ropartz, David; García-Campaña, Ana M.
  • Molecules, Vol. 24, Issue 15
  • DOI: 10.3390/molecules24152706

Software Tools and Approaches for Compound Identification of LC-MS/MS Data in Metabolomics
journal, May 2018


Use of carbon quantum dots and fluorescein isothiocyanate in developing an improved competitive fluoroimmunoassay for detecting polybrominated diphenyl ether
journal, February 2019


Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.