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Investigating the Uptake and Fate of Poly- and Perfluoroalkylated Substances (PFAS) in Sea Ice Using an Experimental Sea Ice Chamber.

ABSTRACT: Poly- and perfluoroalkyl substances (PFAS) are contaminants of emerging Arctic concern and are present in the marine environments of the polar regions. Their input to and fate within the marine cryosphere are poorly understood. We conducted a series of laboratory experiments to investigate the uptake, distribution, and release of 10 PFAS of varying carbon chain length (C₄-C₁₂) in young sea ice grown from artificial seawater (NaClsolution). We show that PFAS are incorporated into bulk sea ice during ice formation and regression analyses for individual PFAS concentrations in bulk sea ice were linearly related to salinity (r² = 0.30 to 0.88, n = 18, p < 0.05). This shows that their distribution is strongly governed by the presence and dynamics of brine (high salinity water) within the sea ice. Furthermore, long-chain PFAS (C₈-C₁₂), were enriched in bulk ice up to 3-fold more than short-chain PFAS (C₄-C₇) and NaCl. This suggests that chemical partitioning of PFAS between the different phases of sea ice also plays a role in their uptake during its formation. During sea ice melt, initial meltwater fractions were highly saline and predominantly contained short-chain PFAS, whereas the later, fresher meltwater fractions predominantly contained long-chain PFAS. Our results demonstrate that in highly saline parts of sea ice (near the upper and lower interfaces and in brine channels) significant chemical enrichment (ε) of PFAS can occur with concentrations in brine channels greatly exceeding those in seawater from which it forms (e.g., for PFOA, ε_brine = 10 ± 4). This observation has implications for biological exposure to PFAS present in brine channels, a common feature of first-year sea ice which is the dominant ice type in a warming Arctic.

SUBMITTER: Garnett J

PROVIDER: S-EPMC8296678 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Human ingestion of per- and polyfluoroalkyl substances (PFAS) from contaminated food and water is linked to the development of several cancers, birth defects and other illnesses. The complete mineralisation of aqueous PFAS by ultrasound (sonolysis) into harmless inorganics has been demonstrated in many studies. However, the range and interconnected nature of reaction parameters (frequency, power, temperature etc.), and variety of reaction metrics used, limits understanding of degradation mechanisms and parametric trends. This work summarises the state-of-the-art for PFAS sonolysis, considering reaction mechanisms, kinetics, intermediates, products, rate limiting steps, reactant and product measurement techniques, and effects of co-contaminants. The meta-analysis showed that mid-high frequency (100 - 1,000 kHz) sonolysis mechanisms are similar, regardless of reaction conditions, while the low frequency (20 - 100 kHz) mechanisms are specific to oxidative species added, less well understood, and generally slower than mid-high frequency mechanisms. Arguments suggest that PFAS degradation occurs via adsorption (not absorption) at the bubble interface, followed by headgroup cleavage. Further mechanistic steps toward mineralisation remain to be proven. For the first time, complete stoichiometric reaction equations are derived for perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) sonolysis, which add H2 as a reaction product and consider CO an intermediate. Fluorinated intermediate products are derived for common, and more novel PFAS, and a naming system proposed for novel perfluoroether carboxylates. The meta-analysis also revealed the transition between pseudo first and zero order PFOA/S kinetics commonly occurs at 15 - 40 µM. Optimum values of; ultrasonic frequency (300 - 500 kHz), concentration (>15 - 40 μM), temperature (≈20 °C), and pH range (3.2 - 4) for rapid PFOX degradation are derived by evaluation of prior works, while optimum values for the dilution factor applied to PFAS containing firefighting foams and applied power require further work. Rate limiting steps are debated and F- is shown to be rate enhancing, while SO42- and CO2 by products are theorised to be rate limiting. Sonolysis was compared to other PFAS destructive technologies and shown to be the only treatment which fully mineralises PFAS, degrades different PFAS in order of decreasing hydrophobicity, is parametrically well studied, and has low-moderate energy requirements (several kWh g-1 PFAS). It is concluded that sonolysis of PFAS in environmental samples would be well incorporated within a treatment train for improved efficiency.

Project description:BackgroundHuman exposure to per- and polyfluoroalkyl substances (PFAS) has been primarily attributed to contaminated food and drinking water. However, additional PFAS exposure pathways have been raised by a limited number of studies reporting correlations between commercial and industrial products and PFAS levels in human media and biomonitoring. Systematic review (SR) methodologies have been widely used to evaluate similar questions using an unbiased approach in the fields of clinical medicine, epidemiology, and toxicology, but the deployment in exposure science is ongoing. Here we present a systematic review protocol that adapts existing systematic review methodologies and study evaluation tools to exposure science studies in order to investigate evidence for important PFAS exposure pathways from indoor media including consumer products, household articles, cleaning products, personal care products, plus indoor air and dust.ObjectivesWe will systematically review exposure science studies that present both PFAS concentrations from indoor exposure media and PFAS concentrations in blood serum or plasma. Exposure estimates will be synthesized from the evidence to answer the question, "For the general population, what effect does exposure from PFAS chemicals via indoor media have on blood, serum or plasma concentrations of PFAS?" We adapt existing systematic review methodologies and study evaluation tools from the U.S. EPA's Systematic Review Protocol for the PFBA, PFHxA, PFHxS, PFNA, and PFDA IRIS Assessments and the Navigation Guide for exposure science studies, as well as present innovative developments of exposure pathway-specific search strings for use in artificial intelligence screening software.Data sourcesWe will search electronic databases for potentially relevant literature, including Web of Science, PubMed, and ProQuest. Literature search results will be stored in EPA's Health and Environmental Research Online (HERO) database.Study eligibility and criteriaIncluded studies will present exposure measures from indoor media including consumer products, household articles, cleaning products, personal care products, plus indoor air and dust, paired with PFAS concentrations in blood, serum or plasma from adults and/or children in the general population. We focus on a subset of PFAS chemicals including perfluorooctanoic acid (PFOA), perfluorooctanesulfonate (PFOS), perfluorobutanoic acid (PFBA), perfluorobutane sulfonate (PFBS), perfluorodecanoic acid (PFDA), perfluorohexanoic acid (PFHxA), perfluorohexanesulfonate (PFHxS), and perfluorononanoic acid (PFNA).Study appraisal and synthesis methodsStudies will be prefiltered at the title and abstract level using computationally intelligent search strings to expedite the screening process for reviewers. Two independent reviewers will screen the prefiltered studies against inclusion criteria at the title/abstract level and then full-text level, after which the reviewers will assess the studies' risk of bias using an approach modified from established systematic review tools for exposure studies. Exposure estimates will be calculated to investigate the proportion of blood, serum or plasma) PFAS concentrations that can be explained by exposure to PFAS in indoor media.

Dataset Information

Investigating the Uptake and Fate of Poly- and Perfluoroalkylated Substances (PFAS) in Sea Ice Using an Experimental Sea Ice Chamber.

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