京都大学 / 0048 / 新制・課程博士 / 博士(地球環境学) / 甲第17932号 / 地環博第111号 / 新制||地環||22(附属図書館) / 30752 / 京都大学大学院地球環境学舎環境マネジメント専攻 / (主査)教授 藤井 滋穂, 教授 伊藤 禎彦, 准教授 田中 周平 / 学位規則第4条第1項該当 / Doctor of Global Environmental Studies / Kyoto University / DFAM

PFCs are used in a wide variety of industrial and commercial applications for more than 50 years. Among variation of PFCs, Perfluorooctane sulfonate (PFOS) (CF3(CF2)7SO3-) and perfluorooctanoic acid (PFOA) (CF3(CF2)6COO-) are the most dominant PFCs. In May 2009, PFOS, its salts and perfluorooctane sulfonyl fluoride (PFOSF) are designated as new Persistent Organic Compounds (POPs) which are resistant, bio-accumulating, and having potential of causing adverse effects to humans and environment (IISD, 2009). However, products containing PFCs are still being manufactured and used, which could be the main reason why they are still observed in the environment and biota (Berger et al., 2004; Saito et al., 2003; Sinclair et al., 2004). The study is focused on the PFCs contamination in water and industrial wastewater around the Central and Eastern Thailand, where is one of the major industrialized areas in the country. The samplings were conducted in major rivers, Chao Phraya, Bangpakong and Tachin River. PFCs were contaminated in all rivers. The average total PFCs were 15.10 ng/L, 18.29 ng/L and 7.40 ng/L in Chao Phraya, Bangpakong and Tachin River, respectively. PFOS and PFOA were the predominant PFCs in all samples. The total of 118.6 g/d PFOS and 323.6 g/d PFOA were released from the three rivers to the Gulf of Thailand. The survey was also conducted in small rivers, reservoirs, and coastal water around Eastern Thailand, where many industrial zones (IZ) are located. The geometric mean (GM) concentration of each PFC was ranged from 2.3 to 107.7 ng/L in small rivers, 2.2 to 212.2 ng/L in reservoirs, and 0.8 to 41.1 ng/L in coastal water samples. The higher PFCs contaminations were detected in the surface water around the industrial zones, where might be the sources of these compounds. Field surveys were also conducted in ten industrial zones (IZ1 – IZ10) to identify the occurrences of PFCs from in industries. The recovery rates of PFCs in the samples indicated that the matrix interference or enhancement was an important problem in PFCs analysis. The elevated concentrations were detected in electronics, textile, chemicals and glass making industries. Total PFCs concentrations in the influent of WWTP were ranged from 39.6 to 3, 344.1 ng/L. Ten industrial zones released 188.41 g/d of PFCs. All of the treatment processes inside industrial zones were biological processes, which were reported that they were not effective to remove PFCs. The influence of industrial discharges was affected not only the rivers and reservoirs but also in the coastal water. The PFCs in rivers and reservoirs were discharged to the Gulf of Thailand, which is the important food source for Thai people and exports. Due to the problems in industrial wastewater analysis, several optimizing options were applied in PFCs analytical method especially in Solid Phase Extraction (SPE) procedure. The combination of PresepC-Agri and Oasis®HLB was the better option for analyzing PFCs in water samples. The optimum flow rate for loading the samples was 5 mL/min. Methanol (2 mL) plus Acetronitrile (2 mL) was the effective way to elute PFCs from the cartridges. The specific solvent percentages to elute each PFCs were identified for both water and industrial wastewater samples. The matrix removal methods by using Envi-Carb and Ultrafilter were effective for different types of industrial wastewater samples. PFCs were detected in surface waters, which are the sources of tap and drinking water for the people in Central and Eastern Thailand. The surveys were conducted in Bangkok city. Samples were collected from water treatment plants (WTPs), tap water, and drinking water. PFCs were detected in all tap water and drinking water samples. PFOS and PFOA concentrations in raw water of WTP were found 4.29 ng/L and 16.54 ng/L, respectively. The average PFOS and PFOA concentrations in tap water were detected 0.17 and 3.58 ng/L, respectively. The tap water results also showed that PFOS and PFOA concentrations were not similarly detected in all area in the city. PFOA were detected higher in the western area, while PFOS concentration was quite similar in all areas. Overall, it can be concluded that the current treatment processes were not completely remove PFCs. Nevertheless, PFCs in particulate phase were effectively removed by the primary sedimentation and rapid sand filtration. Elevated PFCs were found in the industrial zones (IZ2 and IZ5). To understand the distribution and fate of PFCs during industrial wastewater process, PFCs mass flows were studied. Higher PFCs in adsorbed phase were detected only in activated sludge and some influent samples. In IZ2, PFOA loading in the dissolved phase increased after activated sludge process by 5%. There was no degradation of PFOA inside the polishing pond. The highest loading to the treatment plant was PFOS with the loading of 2, 382 mg/d and 1, 529 mg/d in dissolved and adsorbed phase, respectively. Unlike PFCAs that showed no removal in the treatment process, PFOS were decreased during the treatment processes with 36% in the activated sludge process and 36% in the polishing pond. The predominant in this IZ5 was PFOS. The increasing of PFOS was also found in this treatment plant dissimilar to IZ2. PFOS was increasing by 45% in dissolved phase and 47% in adsorbed phase. All of PFCs in this industrial zone were detected higher in the effluent, indicated that PFCs’ precursors should be the major effects of this contamination. / Kyoto University (京都大学) / 0048 / 新制・課程博士 / 博士(工学) / 甲第14930号 / 工博第3157号 / 新制||工||1473(附属図書館) / 27368 / UT51-2009-M844 / 京都大学大学院工学研究科都市環境工学専攻 / (主査)教授 田中 宏明, 教授 清水 芳久, 教授 藤井 滋穂 / 学位規則第4条第1項該当

Kyoto University (京都大学) / 0048 / 新制・課程博士 / 博士(工学) / 甲第15659号 / 工博第3317号 / 新制||工||1501(附属図書館) / 28196 / 京都大学大学院工学研究科都市環境工学専攻 / (主査)教授 田中 宏明, 教授 清水 芳久, 教授 藤井 滋穂 / 学位規則第4条第1項該当

The presence of emerging contaminants (ECs) in water and wastewater systems has become a subject of significant concern worldwide. These emerging contaminants are complex organic molecules which potentially affect human health and environment. Conventional wastewater treatment plants are unable to completely remove these contaminants from water and therefore can discharge them into environment. The need to develop effective methods for ECs removal is essential. This study assess the potential of ozone based advanced oxidation processes (AOP) to oxidize number of emerging contaminants. Different combinations of ozone with hydrogen peroxide and sodium persulfate were tested. For this study 1-4, dioxane, perfluorinated compounds (PFCs), N,N-Diethyl-metatoluamide, and three pharmaceuticals sulfamethoxazole, trimethoprim and carbamazepine have been selected. The effect of different process parameters such as chemical dosages, ozone weight percent, ozone flow rates, etc. on destruction of ECs were examined. It was observed that 1, 4-dioxane were persistent to direct ozone reaction, however were easily oxidized by hydroxyl radical. However, ozonation was solely very effective (> 99 %) in removing pharmaceuticals such as sulfamethoxaole, trimethoprim and carbamazepine. It was not very efficient for the removal of perfluorinated compound and N,N-Diethylmeta-toluamide. The operational conditions were optimized for maximum removal of every compound and their influence on the degradation process is discussed. / Civil Engineering