Humans are exposed to persistent organic pollutants (POPs) such as brominated flame retardants (BFRs, specifically polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD)) and perfluoroalkyl acids (PFAAs, specifically perfluoroalkane sulfonate (PFOS) and perfluorooctanoic acid (PFOA)). They are used in consumer products found in cars, offices, homes and day care centers. Diet was earlier thought to be a major human exposure route for legacy POPs, but does not account for body burdens found for many new POPs and indoor exposure from air and dust has been hypothesized as also important. In this thesis, BFRs in air and dust, and PFAAs in dust from different indoor microenvironments in Sweden were analysed, and the results used to estimate human exposure. BFRs and PFAAs were detected in dust from all microenvironments and PBDEs in all air samples. BFR and PFAA exposure occurs mostly in peoples’ homes with toddlers having higher intakes from dust ingestion than adults. Inhalation and dust ingestion play minor roles compared to diet for humans with median exposures, but in worst case scenarios, dust ingestion may be significant for a small part of the Swedish population. Sampling using home vacuum cleaner bag dust and researcher-collected above floor dust was compared. Correlations were seen for ∑OctaBDE and ∑DecaBDE but not for ∑PentaBDE and HBCD. Higher PBDE concentrations were found in above floor dust but higher HBCD concentrations were found in vacuum cleaner bag dust. BDE-47 concentrations were correlated between vacuum cleaner bag dust and breast milk, indicating exposure through dust ingestion. Similar concentrations of PBDEs were measured in indoor and outgoing air from day care centers, apartment and office buildings. Indoor air explained 54-92% of ∑PentaBDE and 24-86% of BDE-209 total emissions to outdoor air in Sweden, supporting the hypothesis that the indoor environment is polluting ambient air via ventilation systems. / <p>At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 2: Accepted. Paper 3: Accepted. Paper 4: Manuscript.</p>

abstract: Monitoring human exposure to chemicals posing public health threats is critically important for risk management and for informing regulatory actions. Chemical threats result from both environmental pollutants and elected substance use (e.g., consumption of drugs, alcohol and tobacco). Measuring chemical occurrence and concentrations in environmental matrices can help to pinpoint human exposure routes. For instance, indoor dust, a sink of indoor environmental contaminants, can serve to assess indoor air contamination and associated human exposures. Urban wastewater arriving at treatment plants contains urine and stool from the general population, the analysis of which can provide information on chemical threats in the community and ongoing harmful exposures. Analysis of sewage sludge can serve to reveal the identity and quantity of persistent organic pollutants in cities and inform estimates of toxic body burdens in local populations. The objective of this dissertation was to investigate the occurrence and quantity of select, potentially harmful, anthropogenic chemicals in various environmental matrices and to explore the diagnostic value of analytical assays for informing public health decision-making. This dissertation (i) is the first to report spatio-temporal variations and estrogenic burdens of five parabens in sewage sludge from at the U.S. nationwide scale; (ii) represents the first China-wide survey to assess the occurrence and toxic emissions of parabens, triclosan, triclocarban, as well as triclocarban metabolites and transformation products contained in Chinese sewage sludge; (iii) documents the first use of a dispersive solid phase extraction method for indoor dust to measure dust-borne parabens, triclosan and triclocarban and estimating associated human exposures from dust ingestion; and (iv) is the first U.S. study to assess population-level alcohol and nicotine consumption in three U.S. communities using wastewater-based epidemiology (WBE). Obtained data on baseline levels of selected emerging contaminants in sewage sludge and indoor dust can serve to inform the future monitoring needs, risk assessment, and policy making. This work showcases the utility of WBE and urban metabolism metrology via dust and sewage sludge analysis to assess human behavior (e.g., drinking and smoking) and exposure risks more rapidly, efficiently and anonymously than traditional approaches can. / Dissertation/Thesis / Doctoral Dissertation Biological Design 2018

Per-and polyfluoroalkyl substances (PFAS) are anthropogenic compounds that have been spread all over the world. The use of fluorotelomer compounds, short-chained homologues, and other PFASs with perfluorinated moieties has emerged recent years. One of these emerging compound classes is polyfluoroalkyl phosphate esters (PAPs), which have the ability to degrade into persistent PFCAs. The aim of this thesis was to assess the contribution of PAPs and other precursors to the exposure of PFCAs to humans and the environment. The main objective was to analyze a wide range of PFAS in human serum, wild bird eggs, indoor dust, waste water, and sludge. There was a significant contribution from selected precursors to the total amount of PFASs in the abiotic compartments indoor dust, waste water, and sludge. Levels of PAPs found in house dust exceeded those of PFCAs and perfluorosulfonic acids (PFSAs), revealing PAPs as a world-wide important exposure source. A net increase was during waste water treatment was observed for several PFASs in Swedish waste water treatment plants. Together with presence of precursor compounds and intermediates in the influent water and the sludge, this suggest that degradation of PFCA precursors contributed to the increase of PFCAs. Detection of precursors in human serum, together with slow declining trends of PFCAs, revealed an ongoing exposure of PFCAs to the general population of Australia. The diPAPs and the FTSAs were also detected in raptor bird eggs from Sweden from both the terrestrial and the freshwater environment. The precursors concentrations and patterns observed reveal that current regulatory measures are insufficient for the purpose of protecting humans and the environment from PFASs exposure.

京都大学 / 新制・論文博士 / 博士(工学) / 乙第13495号 / 論工博第4202号 / 新制||工||1786(附属図書館) / (主査)教授 米田 稔, 教授 高野 裕久, 教授 松井 康人 / 学位規則第4条第2項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DGAM