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Perfluorinated acids (PFAs) are widespread global and human blood organohalogen contaminants. These monomer decomposition products used in surface treatment products and in fluoropolymer manufacturing and fire fighting may disrupt maternal thyroid hormone homeostasis given that animal studies demonstrate an apparent hypothyroxinemic condition upon PFA exposure. Firstly, we developed a method for properly quantifying perfluorohexane sulfonate (PFHxS), a PFA suspected of overreporting in past literature. We then investigated whether perfluorooctanoate (PFOA), PFHxS and perfluorooctane sulfonate (PFOS) were determinants of maternal hypothyroxinemia in a pregnant women population from Edmonton using a case-control design. Free thyroxine (fT4) and thyroid stimulating hormone (TSH) were screened in 974 women collected during 15-20 weeks of pregnancy. Cases (n=96, hypothyroxinemic: normal TSH and fT4: lowest 10th percentile) and controls (n=175, fT4: 50th and 90th percentile) were matched based on age and physician. Conditional logistic regression indicated that these PFAs are not associated with maternal hypothyroxinemia. / Environmental Health Sciences

The overall aim of this thesis was to investigate the fate of perfluorinated alkyl compounds (PFCs) in biological systems. During the past several years, it has been shown that wildlife are ubiquitously contaminated with two classes of PFCs, the perfluoroalkyl carboxylates (CxF2x+1C(O)OH, PFCAs) and sulfonates (CxF2x+1SO3H, PFSAs). However, there is still considerable uncertainty regarding how wildlife are accumulating these PFCs, particularly in remote areas such as the Canadian arctic. The potential for fluorotelomer acrylate monomers (CxF2x+1CH2CH2OC(O)CH=CH2, FTAcs) to act as precursors to PFCAs through atmospheric oxidation was investigated using smog chamber experiments. FTAc atmospheric fate is determined by OH radical reaction with a lifetime of approximately 1 day. The sole primary product of this reaction was the 4:2 fluorotelomer glyoxylate which is expected to undergo further atmospheric oxidation or photolysis to ultimately yield PFCAs. Temporal and spatial trends of PFCs in arctic ringed seals and seabirds were investigated to assist in understanding PFC transport mechanisms to remote regions. In ringed seals, perfluorooctane sulfonate (PFOS) levels decreased rapidly, coinciding with the phase out by the major manufacturer. These findings are consistent with volatile precursors as the dominant source of PFCs to arctic wildlife. The bioaccumulation and biotransformation of the 8:2 FTAc was investigated in two complimentary studies with rainbow trout. During the in vivo dietary exposure study, fish rapidly accumulated and biotransformed the 8:2 FTAc, with intermediate metabolites observed within 1 hour of dosing. Perfluorooctanoate (PFOA), perfluorononanoate (PFNA) and perfluoroheptanoate (PFHpA) were formed and accumulated in low yields. The carboxylesterase activity in the trout liver and stomach was investigated using in vivo sub-cellular (S9) incubations. Very high esterase activities were shown with approximately equal efficiency in the stomach and liver. The metabolic pathway of the 8:2 fluorotelomer alcohol (8:2 FTOH) was investigated by separately dosing whole rainbow trout with three intermediate metabolites that represented important branching points. The 7:3 fluorotelomer saturated carboxylate (FTCA) did not form PFOA, but formed PFHpA and the 7:3 fluorotelomer unsaturated carboxylate (FTUCA). The 8:2 FTCA and 8:2 FTUCA did form PFOA, confirming a “beta-like-oxidation” mechanism.

The overall aim of this thesis was to investigate the fate of perfluorinated alkyl compounds (PFCs) in biological systems. During the past several years, it has been shown that wildlife are ubiquitously contaminated with two classes of PFCs, the perfluoroalkyl carboxylates (CxF2x+1C(O)OH, PFCAs) and sulfonates (CxF2x+1SO3H, PFSAs). However, there is still considerable uncertainty regarding how wildlife are accumulating these PFCs, particularly in remote areas such as the Canadian arctic. The potential for fluorotelomer acrylate monomers (CxF2x+1CH2CH2OC(O)CH=CH2, FTAcs) to act as precursors to PFCAs through atmospheric oxidation was investigated using smog chamber experiments. FTAc atmospheric fate is determined by OH radical reaction with a lifetime of approximately 1 day. The sole primary product of this reaction was the 4:2 fluorotelomer glyoxylate which is expected to undergo further atmospheric oxidation or photolysis to ultimately yield PFCAs. Temporal and spatial trends of PFCs in arctic ringed seals and seabirds were investigated to assist in understanding PFC transport mechanisms to remote regions. In ringed seals, perfluorooctane sulfonate (PFOS) levels decreased rapidly, coinciding with the phase out by the major manufacturer. These findings are consistent with volatile precursors as the dominant source of PFCs to arctic wildlife. The bioaccumulation and biotransformation of the 8:2 FTAc was investigated in two complimentary studies with rainbow trout. During the in vivo dietary exposure study, fish rapidly accumulated and biotransformed the 8:2 FTAc, with intermediate metabolites observed within 1 hour of dosing. Perfluorooctanoate (PFOA), perfluorononanoate (PFNA) and perfluoroheptanoate (PFHpA) were formed and accumulated in low yields. The carboxylesterase activity in the trout liver and stomach was investigated using in vivo sub-cellular (S9) incubations. Very high esterase activities were shown with approximately equal efficiency in the stomach and liver. The metabolic pathway of the 8:2 fluorotelomer alcohol (8:2 FTOH) was investigated by separately dosing whole rainbow trout with three intermediate metabolites that represented important branching points. The 7:3 fluorotelomer saturated carboxylate (FTCA) did not form PFOA, but formed PFHpA and the 7:3 fluorotelomer unsaturated carboxylate (FTUCA). The 8:2 FTCA and 8:2 FTUCA did form PFOA, confirming a “beta-like-oxidation” mechanism.

The overall aim of this thesis was to investigate the fate of perfluorinated alkyl compounds (PFCs) in biological systems. During the past several years, it has been shown that wildlife are ubiquitously contaminated with two classes of PFCs, the perfluoroalkyl carboxylates (CxF2x+1C(O)OH, PFCAs) and sulfonates (CxF2x+1SO3H, PFSAs). However, there is still considerable uncertainty regarding how wildlife are accumulating these PFCs, particularly in remote areas such as the Canadian arctic. The potential for fluorotelomer acrylate monomers (CxF2x+1CH2CH2OC(O)CH=CH2, FTAcs) to act as precursors to PFCAs through atmospheric oxidation was investigated using smog chamber experiments. FTAc atmospheric fate is determined by OH radical reaction with a lifetime of approximately 1 day. The sole primary product of this reaction was the 4:2 fluorotelomer glyoxylate which is expected to undergo further atmospheric oxidation or photolysis to ultimately yield PFCAs. Temporal and spatial trends of PFCs in arctic ringed seals and seabirds were investigated to assist in understanding PFC transport mechanisms to remote regions. In ringed seals, perfluorooctane sulfonate (PFOS) levels decreased rapidly, coinciding with the phase out by the major manufacturer. These findings are consistent with volatile precursors as the dominant source of PFCs to arctic wildlife. The bioaccumulation and biotransformation of the 8:2 FTAc was investigated in two complimentary studies with rainbow trout. During the in vivo dietary exposure study, fish rapidly accumulated and biotransformed the 8:2 FTAc, with intermediate metabolites observed within 1 hour of dosing. Perfluorooctanoate (PFOA), perfluorononanoate (PFNA) and perfluoroheptanoate (PFHpA) were formed and accumulated in low yields. The carboxylesterase activity in the trout liver and stomach was investigated using in vivo sub-cellular (S9) incubations. Very high esterase activities were shown with approximately equal efficiency in the stomach and liver. The metabolic pathway of the 8:2 fluorotelomer alcohol (8:2 FTOH) was investigated by separately dosing whole rainbow trout with three intermediate metabolites that represented important branching points. The 7:3 fluorotelomer saturated carboxylate (FTCA) did not form PFOA, but formed PFHpA and the 7:3 fluorotelomer unsaturated carboxylate (FTUCA). The 8:2 FTCA and 8:2 FTUCA did form PFOA, confirming a “beta-like-oxidation” mechanism.

The overall aim of this thesis was to investigate the fate of perfluorinated alkyl compounds (PFCs) in biological systems. During the past several years, it has been shown that wildlife are ubiquitously contaminated with two classes of PFCs, the perfluoroalkyl carboxylates (CxF2x+1C(O)OH, PFCAs) and sulfonates (CxF2x+1SO3H, PFSAs). However, there is still considerable uncertainty regarding how wildlife are accumulating these PFCs, particularly in remote areas such as the Canadian arctic. The potential for fluorotelomer acrylate monomers (CxF2x+1CH2CH2OC(O)CH=CH2, FTAcs) to act as precursors to PFCAs through atmospheric oxidation was investigated using smog chamber experiments. FTAc atmospheric fate is determined by OH radical reaction with a lifetime of approximately 1 day. The sole primary product of this reaction was the 4:2 fluorotelomer glyoxylate which is expected to undergo further atmospheric oxidation or photolysis to ultimately yield PFCAs. Temporal and spatial trends of PFCs in arctic ringed seals and seabirds were investigated to assist in understanding PFC transport mechanisms to remote regions. In ringed seals, perfluorooctane sulfonate (PFOS) levels decreased rapidly, coinciding with the phase out by the major manufacturer. These findings are consistent with volatile precursors as the dominant source of PFCs to arctic wildlife. The bioaccumulation and biotransformation of the 8:2 FTAc was investigated in two complimentary studies with rainbow trout. During the in vivo dietary exposure study, fish rapidly accumulated and biotransformed the 8:2 FTAc, with intermediate metabolites observed within 1 hour of dosing. Perfluorooctanoate (PFOA), perfluorononanoate (PFNA) and perfluoroheptanoate (PFHpA) were formed and accumulated in low yields. The carboxylesterase activity in the trout liver and stomach was investigated using in vivo sub-cellular (S9) incubations. Very high esterase activities were shown with approximately equal efficiency in the stomach and liver. The metabolic pathway of the 8:2 fluorotelomer alcohol (8:2 FTOH) was investigated by separately dosing whole rainbow trout with three intermediate metabolites that represented important branching points. The 7:3 fluorotelomer saturated carboxylate (FTCA) did not form PFOA, but formed PFHpA and the 7:3 fluorotelomer unsaturated carboxylate (FTUCA). The 8:2 FTCA and 8:2 FTUCA did form PFOA, confirming a “beta-like-oxidation” mechanism.

Perfluorinated compounds are organic compounds in which all hydrogen atoms in a carbon chain are substituted with fluorine atoms. These compounds are highly stable, persistent and bioaccumulative. They are purely anthropogenic compounds contained in biota and abiota. Partition coefficient between n-octanol and water is the essential toxicological parameter of a compound. This parameter helps us to assess behaviour of compound in the environment as well as in the living organisms. The shake flask method and the RP-HPLC method were employed to measure the Kow of nine perfluorinated acids. Using the shake flask method, the surface activity of compounds and the acid dissociation caused false results of the measurement. But behaviour of these compounds in the environment can be assess. Accurate and precise results were measured by the RP-HPLC method using an acetate buffer. Log Kow of perfluoro- carboxylic acids, with the carbon chain length of 5-14, were found out, their final value ranging between 1.66 and 5.10. Log Kow of acid with 12 carbons was estimated based on the linear regression of dependence of log Kow on the number of carbons. There were significant differences in the results obtained by various software. Thus, the results cannot be considered relevant. These software are not suitable for...