Toward Comprehensive Per- and Polyfluoroalkyl Substances Annotation Using FluoroMatch Software and Intelligent High-Resolution Tandem Mass Spectrometry Acquisition

Koelmel, Jeremy P.; Paige, Matthew K.; Aristizabal‐Henao, Juan J.; Robey, Nicole M.; Nason, Sara L.; Stelben, Paul; Li, Yang; Kroeger, Nicholas; Napolitano, Michael P.; Savvaides, Tina; Vasiliou, Vasilis; Rostkowski, Paweł; Garrett, Timothy J.; Lin, Elizabeth Z.; Deigl, Chris; Jobst, Karl J.; Townsend, Timothy G.; Pollitt, Krystal J. Godri; Bowden, John A.

doi:10.1021/acs.analchem.0c01591

Cited by 69 publications

(60 citation statements)

References 44 publications

(83 reference statements)

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“…Calibration points, blanks, and daily, weekly, and 5-week composite samples were analyzed using an alternating full MS and all ion fragmentation (AIF) method. Additionally, the 5-week composite samples were analyzed using data dependent MS2 (ddMS2) analysis with an iterative inclusion approach, which has similar advantages to previously reported intelligent acquisition methods (57,58). Briefly, we used the full scan data to generate inclusion lists including all features after blank filtering to ensure ddMS2 spectra were collected for each peak in the three 5-week composite samples.…”

Section: Methodsmentioning

confidence: 99%

Traffic, Drugs, Mental Health, and Disinfectants: Changes in Sewage Sludge Chemical Signatures During a COVID-19 Community Lockdown

Nason

Lin²,

Eitzer³

et al. 2021

Preprint

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<p>The COVID-19 pandemic and related shutdowns have caused changes in everyday activities for many people, and signs of those changes are present in the chemical signatures of sewage sludge produced during the pandemic. We analyzed primary sewage sludge samples from a wastewater treatment plant in New Haven, CT USA collected between March 19 and June 30, 2020. This time period encompassed the first wave of the COVID-19 pandemic, the initial statewide stay at home order, and the first phase of reopening. We used liquid chromatography coupled with high resolution mass spectrometry and targeted and suspect screening strategies to identify contaminants in the sludge. We and found evidence of increasing opioid, cocaine, and antidepressant use, as well as upward trends in chemicals used in disinfectants and sunscreens during the study period. Benzotriazole, an anti-corrosion chemical associated with traffic pollution, decreased through the stay-at-home period, and increased during reopening. Hydroxychloroquine, a drug that received significant attention for its potential to treat COVID-19, had elevated concentrations in the week following the implementation of the United States Emergency Use Authorization. Our results directly relate to nationwide reports of increased demand for fentanyl, antidepressants, and other medications, as well as reports of increased drug overdose deaths during the pandemic. Though wastewater surveillance during the pandemic has largely focused on measuring SARS-CoV-2 RNA concentrations, chemical analysis can also show trends that are important for revealing the public and environmental health effects of the pandemic. </p>

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Section: Methodsmentioning

confidence: 99%

Traffic, Drugs, Mental Health, and Disinfectants: Changes in Sewage Sludge Chemical Signatures During a COVID-19 Community Lockdown

Nason

Lin²,

Eitzer³

et al. 2021

Preprint

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“…I met several other scientists via the taskforce, who I now have active collaborations with. So far, we have four publications related to PFAS (Koelmel et al, 2020, Koelmel et al, 2021Nason et al, 2020;Hagstrom et al, 2021) and two funded grant proposals, with more in progress! My work on this collaborative community project kick started all these additional activities.…”

Section: An Ongoing Storymentioning

confidence: 99%

A community based PFAS phytoremediation project at the former Loring Airforce Base

Nason

Stanley

PeterPaul³

et al. 2021

iScience

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The Loring Airforce Base (AFB) in Aroostook County, Maine, USA was active from 1947 through 1994. Like many military sites, it has a substantial history of pollution from a wide variety of toxins. Currently, some of the AFB land belongs to the Micmac Nation, an Indigenous tribe, who are very concerned about the contamination on the land. Starting in 2019, a group of community activists, research scientists, and tribal members came together to test methods for cleaning the land. This backstory features perspectives from six project participants. BEGINNINGSWhat are the goals of this project? How did you decide what to investigate?Dr. Sara L. Nason (Connecticut Agricultural Experiment Station): The overall goal of our work is to improve the quality of the land on the former Loring AFB, which now belongs to the Aroostook band of the Micmac Nation. Specifically, we are testing the use of fiber hemp plants for phytoremediation of per-and polyfluoroalkyl substances (PFAS). PFAS are a class of emerging contaminants that are highly toxic at low concentrations and are frequently found on former military bases owing to their use in firefighting foams (Hagstrom et al., 2021). They are often called ''forever chemicals,'' as they are highly resistant to degradation. Part of the land acquired by the Micmac people was formerly used as a firefighting testing area. The US Airforce has detected concerning levels of PFAS in groundwater at this site, but did not conduct any remediation (Baker, 2018). There are limited technologies available for removing PFAS Currently, some of the Loring Airforce Base (AFB) land belongs to the Micmac Nation, an Indigenous tribe, who are very concerned about the contamination on the land. Starting in 2019, a group of community activists, research scientists, and tribal members came together to test methods for cleaning the land. This backstory features perspectives from six project participants.

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“…As of November 2020, the United States Environmental Protection Agency (EPA) has compiled a list of over 8000 PFAS structures [28] made available via their CompTox Chemicals Dashboard [29]. This list is not exhaustive and previous studies have found compounds that are not contained on the list [30]. At the time of writing, the dashboard has less than one million chemicals (~883,000) and other databases such as CAS SciFinder, ChemSpider, and PubChem each contain tens of millions of substances with additional tens of thousands of PFAS.…”

Section: Introductionmentioning

confidence: 99%

“…Whereas the original release of FluoroMatch [30] used a suspect screening approach that targeted compounds based on available MS/MS spectra acquired from standards and information available in literature, FluoroMatch 2.0 uses truly nontargeted methods which can be used to enhance the identification and discovery of known, uncommon, and unknown PFAS. FluoroMatch 2.0 introduces an automated workflow which includes blank filtering, mass defect filtering, Kendrick mass defect plots (normalized to CF 2 ) [33], retention time pattern analysis, and exact mass matching to take full advantage of retention time and exact mass data.…”

Section: Introductionmentioning

confidence: 99%

FluoroMatch 2.0—making automated and comprehensive non-targeted PFAS annotation a reality

et al. 2021

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Because of the pervasiveness, persistence, and toxicity of per-and polyfluoroalkyl substances (PFAS), there is growing concern over PFAS contamination, exposures, and health effects. The diversity of potential PFAS is astounding, with nearly 10,000 PFAS catalogued in databases to date (and growing). The ability to detect the thousands of known PFAS, and discover previously uncatalogued PFAS, is necessary to understand the scope of PFAS contamination and to identify appropriate remediation and regulatory solutions. Current non-targeted methods for PFAS analysis require manual curation and are time-consuming, prone to error, and not comprehensive. FluoroMatch Flow 2.0 is the first software to cover all steps of data processing for PFAS discovery in liquid chromatography-high-resolution tandem mass spectrometry samples. These steps include feature detection, feature blank filtering, exact mass matching to catalogued PFAS, mass defect filtering, homologous series detection, retention time pattern analysis, class-based MS/MS screening, fragment screening, and predicted MS/MS from SMILES structures. In addition, a comprehensive confidence level criterion is implemented to help users understand annotation certainty and integrate various layers of evidence to reduce overreporting. Applying the software to aqueous film forming foam analysis, we discovered over one thousand likely PFAS including previously unreported species. Furthermore, we were able to filter out 96% of features which were likely not PFAS. FluoroMatch Flow 2 increased coverage of likely PFAS by over tenfold compared to the previous release. This software will enable researchers to better characterize PFAS in the environment and in biological systems.

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Toward Comprehensive Per- and Polyfluoroalkyl Substances Annotation Using FluoroMatch Software and Intelligent High-Resolution Tandem Mass Spectrometry Acquisition

Cited by 69 publications

References 44 publications

Traffic, Drugs, Mental Health, and Disinfectants: Changes in Sewage Sludge Chemical Signatures During a COVID-19 Community Lockdown

Traffic, Drugs, Mental Health, and Disinfectants: Changes in Sewage Sludge Chemical Signatures During a COVID-19 Community Lockdown

A community based PFAS phytoremediation project at the former Loring Airforce Base

FluoroMatch 2.0—making automated and comprehensive non-targeted PFAS annotation a reality

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