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    Calibration and performance of synchronous SIM/scan mode for simultaneous targeted and discovery (non-targeted) analysis of exhaled breath samples from firefighters
    (Elsevier Science Bv, 2017) Wallace, M. Ariel Geer; Pleil, Joachim D.; Mentese, Sibel; Oliver, Karen D.; Whitaker, Donald A.; Fent, Kenneth W.
    Traditionally, gas chromatography-mass spectrometry (GC/MS) analysis has used a targeted approach called selected ion monitoring (SIM) to quantify specific compounds that may have adverse health effects. Dueto method limitations and the constraints of preparing duplicate samples, the information that could be obtained from separately collecting the full scan chromatogram of the sample has often been sacrificed. However, the hybrid technique called synchronous SIM/scan mode alternates between the two acquisition modes, maintaining the accuracy and sensitivity of SIM for targeted analysis while also providing the full scan chromatogram for discovery of non-target compounds. This technology was assessed using calibration data and real-world breath samples from a joint EPA/NIOSH collaboration that investigated the safety of firefighters' protective gear during controlled structure burns. Collecting field samples is costly and must be performed strategically to ensure that time points and replicates are accurate and representative of the intended population. This is difficult to accomplish with firefighters who are working under volatile conditions. The synchronous SIM/scan method decreases the number of field samples that need to be collected by half and reduces error in trying to recreate time points since a breath sample from a single sorbent tube can be used to collect both the SIM and scan data simultaneously. As a practical demonstration of the method, we investigate thirty-six firefighter breath samples, document organic compounds of interest, and identify additional non-target compounds. Published by Elsevier B.V.
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    Non-targeted GC/MS analysis of exhaled breath samples: Exploring human biomarkers of exogenous exposure and endogenous response from professional firefighting activity
    (Taylor & Francis Inc, 2019) Wallace, M. Ariel Geer; Pleil, Joachim D.; Oliver, Karen D.; Whitaker, Donald A.; Mentese, Sibel; Fent, Kenneth W.; Horn, Gavin P.
    A non-targeted analysis workflow was applied to analyze exhaled breath samples collected from firefighters pre- and post-structural fire suppression. Breath samples from firefighters functioning in attack and search positions were examined for target and non-target compounds in automated thermal desorption-GC/MS (ATD-GC/MS) selected ion monitoring (SIM)/scan mode and reviewed for prominent chemicals. Targeted chemicals included products of combustion such as benzene, toluene, xylenes, and polycyclic aromatic hydrocarbons (PAH) that serve as a standard assessment of exposure. Sixty unique chemical features representative of exogenous chemicals and endogenous compounds, including single-ring aromatics, polynuclear aromatic hydrocarbons, volatile sulfur-containing compounds, aldehydes, alkanes, and alkenes were identified using the non-targeted analysis workflow. Fifty-seven out of 60 non-targeted features changed by at least 50% from pre- to post-fire suppression activity in at least one subject, and 7 non-targeted features were found to exhibit significantly increased or decreased concentrations for all subjects as a group. This study is important for (1) alerting the firefighter community to potential new exposures, (2) expanding the current targeted list of toxicants, and (3) finding biomarkers of response to firefighting activity as reflected by changes in endogenous compounds. Data demonstrate that there are non-targeted compounds in firefighters' breath that are indicative of environmental exposure despite the use of protective gear, and this information may be further utilized to improve the effectiveness of personal protective equipment.
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    Targeted GC-MS analysis of firefighters' exhaled breath: Exploring biomarker response at the individual level
    (Taylor & Francis Inc, 2019) Wallace, M. Ariel Geer; Pleil, Joachim D.; Oliver, Karen D.; Whitaker, Donald A.; Mentese, Sibel; Fent, Kenneth W.; Horn, Gavin P.
    Biomarker measurements can provide unambiguous evidence of environmental exposures as well as the resultant biological responses. Firefighters have a high rate of occupational cancer incidence, which has been proposed to be linked in part to their increased environmental exposure to byproducts of combustion and contaminants produced during fire responses. In this article, the uptake and elimination of targeted volatile organic compounds were investigated by collecting the exhaled breath of firefighters on sorbent tubes before and after controlled structure burns and analyzing samples using automated thermal desorption-gas chromatography (ATD-GC/MS). Volatile organic compounds exposure was assessed by grouping the data according to firefighting job positions as well as visualizing the data at the level of the individual firefighter to determine which individuals had expected exposure responses. When data were assessed at the group level, benzene concentrations were found to be elevated post-exposure in both fire attack, victim search, and outside ventilation firefighting positions. However, the results of the data analysis at the individual level indicate that certain firefighters may be more susceptible to post-exposure volatile organic compounds increases than others, and this should be considered when assessing the effectiveness of firefighting protective gear. Although this work focuses on firefighting activity, the results can be translated to potential human health and ecological effects from building and forest fires.