Date of Award

2019

Degree Type

Thesis

Degree Name

Master of Science in Oceanography

Specialization

Chemical Oceanography

Department

Oceanography

First Advisor

Rainer Lohmann

Abstract

Fluorotelomer alcohols (FTOHs) and other poly- and per-fluorinated alkyl substances (PFASs) are common and ubiquitous by-products of various industrial telomerization processes. This class of volatile and semi-volatile compounds has been shown to degrade into a wide variety of perfluorinated carboxylic acids (PFCAs) including perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS), persistent organic pollutants. Recent atmospheric studies have shown fluorotelomer alcohols and their degradation products present in high concentrations spreading out from point sources in North America, Europe, and Asia. This study developed a method for measuring fluorotelomer alcohols through the use of polyethylene (PE) passive samplers coupled to their analysis via gas chromatography-mass spectrometry (GC/MS). Polyethylene-water partitioning coefficients, log KPEW, were determined in a laboratory study and ranged from log KPEW 3.2 to 6.7. Field deployment of PE samplers in aqueous systems was conducted in the outflow of a local waste-water treatment plant. Target FTOH, perfluorosulfonamidoethanol (FOSE), and perfluorosulfonamide (FOSA) compounds were detected in all PE samplers above background concentrations. Maximum accumulated amounts from aqueous exposure ranged from 1860 ng per sheet for 6:2 FTOH down to 3.5 ng per sheet for EtFOSE. Polyethylene-air partitioning coefficients, log KPEA, were estimated using a field deployment of PEs directly compared to active sampling. Atmospheric concentrations of targeted PFASs in Providence (RI, USA) varied daily, with the FTOHs found to be most prevalent (average 10.1 – 14.5 pg/m3). Measured concentrations fall within accepted range of literature values for urban environments and indicate the effectiveness of PE passive samplers in detecting FTOHs, FOSAs, and FOSEs in atmospheric deployments. This thesis demonstrated PE samplers are effective in ambient aqueous environments for detecting and quantifying FTOHs, FOSAs, and FOSEs above their blank levels. Additional laboratory experiments are necessary to verify estimated PE-water partitioning constants.

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