Kyoto University (京都大学) / 0048 / 新制・課程博士 / 博士(工学) / 甲第16887号 / 工博第3608号 / 新制||工||1545(附属図書館) / 29562 / 京都大学大学院工学研究科化学工学専攻 / (主査)教授 松坂 修二, 教授 宮原 稔, 教授 大嶋 正裕 / 学位規則第4条第1項該当

Leachate from landfills is contaminated in many ways and per- and polyfluoroalkyl substances (PFAS)-contamination is one of them. Recent studies have demonstrated the environmental and human concerns of PFAS. Therefore, the treatment of leachate is important. One technique to reduce the PFAS concentration is by using aeration and foam fractionation. Hovgården is a landfill northeast of Uppsala, where previous measurements have shown high levels of PFAS in the leachate. Earlier small-scale experiments using aeration foam fractionation as a treatment technique for PFAS removal have been done successfully, but with upcoming requirements of PFAS concentrations there is a need to investigate whether an upscaling is possible or not. In this study, this has been investigated by pumping PFAS contaminated leachate from the landfill in to a 0.046 square metre plastic cylinder and aerated the leachate with an airflow of ten L min-1. A total of six experiments were conducted were the contact time and fraction of extracted foam was parameters that was varying. Four experiments were done with a contact time of ten min and foam fraction of five, ten, twenty and thirty percent and two experiments were made with a foam fraction of five percent and a contact time of twenty respectively thirty min. The average ΣPFAS removal, i.e., the percentage difference in ΣPFAS concentrations between the influent and effluent water in the different runs varied between 31 % and 66 %. The removal of long chained PFAS (≥C6) was higher than the removal of short chained PFAS(≤C5) even if all experiments did reduce the PFAS concentration. Carbon chains with a functional group containing a carboxylic acid is called perfluorocarboxylic acids (PFCA) and with a functional group containing a sulfonic acid is called perfluoroalkane sulfonic acids (PFSA). Precursors are PFAS that after a reaction degrades into PFCA and PFSA. The average removal efficiency of PFCA were 48 %, of PFSA 59 % and of precursors 78 %. The highest removal efficiency was discovered in the experiment with a 30-min contact time and five percent foam fraction with an average ΣPFAS removal of 58 % and an average Σlong chained PFAS removal of 92 %. The lowest removal efficiency was discovered in the experiment with a 10-min contact time and 20 percent foam fraction with an average ΣPFAS removal of 41 % and an average Σlong chained PFAS removal of 67 %. In conclusion a connection between increased contact time and increased removal efficiency was discovered but no clear connections between foam fraction and removal efficiency were found. However, it cannot be stated beyond reasonable doubt that the contact time is the decisive factor. Another conclusion is that the enrichment of short chained PFAS are higher in the water and a higher enrichment of long chained PFAS in the foam. In general, a higher inlet concentration of PFAS in the influent water resulted in a higher removal efficiency.

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Wastewater treatment plants (WWTPs) are originally not constructed to remove pharmaceuticals from the wastewater. Biological treatment technologies used in many WWTPs today, e.g., activated sludge, MBBR and trickling filters, can, however, remove some pharmaceuticals well. Advanced treatment technologies, like ozonation, can be used as a complement to biological treatment for an even better removal. Käppala WWTP is not required to remove pharmaceuticals today, but is obligated to follow the development of advanced treatment technologies and prepare to implement one in the future. Additionally, a new wastewater treatment directive is under development with stronger regulations of pharmaceutical removal. Because of this, it is important to gather information about removal efficiencies for different treatment technologies in Käppala and other WWTPs. In this project, direct injection-UHPLC-Orbitrap-MS/MS was used to analyze wastewater from seven different WWTPs, including Käppala, with the aim to detect as many pharmaceuticals as possible. The removal efficiencies for 59 identified compounds, most of them pharmaceuticals, were used to evaluate the WWTPs and their treatment technologies. 55 of these compounds were detected in Käppala WWTP while 48 were detected in all seven WWTPs. In Käppala WWTP, around half of all compounds were removed with less than 20 %, including most of the compounds that is proposed to be regulated in the new wastewater treatment directive. This highlights the need for Käppala WWTP to introduce new treatment technologies. Two Swiss plants with ozonation had a removal efficiency > 80 % across the whole plant for 79 % and 67 % of the compounds respectively. In the WWTPs that lacked advanced treatment technologies only 12-33 % of the compounds had a removal > 80 %. One compound, chlorothiazide, did however increase 30 times across the plants with ozonation treatment. The trickling filter in one WWTP barely removed any compound with more than 20 % and was thereby the biological treatment technology with lowest removal efficiency. Activated sludge without N-removal also had a slightly lower removal of pharmaceuticals compared to activated sludge with N-removal and MBBR, possibly due to a shorter hydraulic retention time (HRT) and sludge retention time (SRT).

No description available.

No description available.

Roads, buildings, vehicles, and human activities cause spreading of pollutants, which partly end up in stormwater. The pollutant load contains solid particles of various size, hydrocarbons, organics, metals, nutrients, and microorganisms, which can have negative effects on water quality of surface-, coastal- and ground waters. Furthermore, urban development causes hardening of ground and reduced soil permeability that promotes rapid runoff during precipitation. The conversion from permeable to impermeable surfaces therefore lead to increased volumes stormwater but also decrease in stormwater water quality.  Stormwater runoff metals are bound to various particles or occur in the dissolved fraction which is more toxic to aquatic life. Infiltration to soil, sand or other media is common practice to reduce runoff and filtrate metals and many treatment facilities and filter media have therefore been assessed for their metal removal efficiencies. High metal removal is often achieved for total metals, but removal of dissolved fraction remains elusive in many studies. Hence the importance of evaluate removal of dissolved metals before application to stormwater treatment facilities.  The experimental column study of metal removal using commercially available reactive filter media showed that all filter media removal efficiencies in the order of zinc > copper > nickel. Removal efficiencies of chromium and lead were not considerably higher in tested filter media compared to the reference filter sand. Two filter media also leached chromium during the initial part of the experiment. / Vägar, byggnader, fordon och mänskliga aktiviteter orsakar spridning av föroreningar av vilka en del förekommer i dagvatten. Urban bebyggelse orsakar också hårdgörande av ytor och reducerar jordens permeabilitet vilket skapar snabb avrinning vid nederbörd. Avrinningen innehåller bland annat partiklar, kolväten och andra organiska ämnen, metaller, näringsämnen och mikroorganismer vilka kan ha negativa effekter på yt-, kust- och grundvatten. Omvandlingen till hårdgjorda ytor orsakar därför både ökade volymer avrinning och sämre vattenkvalité.  Metaller i dagvatten är ofta bundna till olika partiklar eller förekommer i löst form där den lösta formen anses vara mest miljöfarlig. Infiltration i jord, sand eller annan media är vanliga sätt att reducera avrinning och filtrera metaller. Hög förmåga att avskilja metaller kan ofta hittas för totala koncentrationen av metall men avskiljning av den lösta formen är ofta oklar. Utvärdering av olika filtermaterials förmåga att reducera lösta metaller är därför av särskilt intresse.  Kolonnförsöken gjorda för att utvärdera metallavskiljningskapacitet med kommersiellt tillgängliga reaktiva filtermaterial har i denna uppsats visat att filtermaterialen har högst procentuell avskiljning för zink följt av koppar och därefter nickel. Krom och bly avskiljs inte mer i dessa filtermaterial än vad de gör i sandfilter. Två av filtermaterial läckte dessutom initialt höga koncentrationer krom.

Les rejets de station d'épuration (STEP) sont considérés comme un vecteur majeur d'entrée des micropolluants dans les milieux aquatiques. Certains micropolluants, fortement présents dans les eaux à traiter ou trop faiblement éliminés par les filières de traitement, sont ainsi retrouvés dans les eaux usées traitées à des concentrations pouvant atteindre plusieurs centaines de ng/L. Ce travail de recherche vise à identifier et simuler les processus d'élimination de micropolluants au sein du procédé à boues activées en aération prolongée, procédé le plus couramment utilisé en France. Nous nous sommes intéressés à 53 micropolluants, dont l'élimination de la file eau par le procédé à boues activées n'est que partielle (rendement compris entre 30 et 70 % selon AMPERES). Cinq familles de substances aux propriétés physico-chimiques différentes ont ainsi été étudiées : 11 métaux, 14 composés pharmaceutiques, 19 hydrocarbures aromatiques polycycliques, 5 alkylphénols, 4 pesticides. L'objectif de la démarche expérimentale proposée a consisté à identifier et caractériser les principaux mécanismes d'élimination. Ces mécanismes ont été étudiés à deux échelles d'observation, échelle industrielle (STEP vraie grandeur) et une échelle pilote. Le suivi d'un procédé boues à activées au sein d'une STEP (2900 EH) a permis de réaliser 8 bilans matières (file eau et file globale) répartis sur une année. Nous avons ainsi mesuré les variations de concentrations des micropolluants ciblés dans les eaux usées brutes, les eaux usées traitées et les boues, ainsi que les variations de performances d'élimination suivant les conditions de fonctionnement de la STEP (température, durée de présence d'oxygène, taux de MES). Les essais à l'échelle pilote en réacteur fermé ont permis de déterminer les coefficients de sorption et les constantes cinétiques de biodégradation de ces micropolluants en conditions contrôlées. La biodégradation de ces micropolluants a été évaluée pour différentes conditions opératoires relatives aux conditions rédox (aérobie et anoxie) et à différentes conditions de substrat (absence de substrat biodégradable, présence de substrat biodégradable carboné et azoté, présence de substrat azoté seulement). Un modèle dynamique calé est proposé, décrivant le comportement des micropolluants dans les phases dissoute et particulaire. Le paramétrage est obtenu à partir des données expérimentales, à savoir les coefficients de sorption et de biodégradation déterminés en réacteur fermé et des performances d'élimination mesurées pour la STEP. / Discharges from wastewater treatment plants (WWTP) are considered as a major input of micropollutants in the aquatic environment. Some micropollutants are found in treated wastewater at concentrations of several hundred ng/L, due to their high concentration in the raw wastewater or to their low removal by WWTP. This work proposes to model the fate of micropollutants in the activated sludge with extended aeration process, most commonly used in France. We investigated 53 micropollutants, particularly those partially removed from the water line by activated sludge process (between 30 and 70% according to the AMPERES project). Five families of substances with different physicochemical properties were studied: 11 metals, 14 pharmaceutical compounds, 19 polycyclic aromatic hydrocarbons, 5 alkylphenols and 4 pesticides. The objective of the experimental strategy is to characterize the two main removal mechanisms: sorption and biodegradation. It combines a study of a process at WWTP scale and tests at laboratory scale. We have monitored an activated sludge process to achieve eight mass balances (water line and global line) for a year. We have characterized variations of concentration in raw wastewater, treated wastewater and sludge as well as variations in removal efficiency depending on operating conditions. Laboratory scale tests were used to determine sorption coefficients and kinetic biodegradation constants of micropollutants in monitored conditions. We evaluated biodegradation kinetics in different redox conditions (aerobic and anoxic) and different substrate conditions (absence of biodegradable substrate, presence of biodegradable substrate carbon and nitrogen, presence of substrate nitrogen only). The model describing the fate of dissolved and particulate phases is calibrated from sorption and biodegradation constants and removal efficiencies observed for the activated sludge process at WWTP scale.

Utsläpp av läkemedelsrester till miljön är ett växande problem och negativa effekter på fiskar och vattenlevande djur har observerats vid mycket låga halter. I detta examensarbete studerades fem svenska spillvattenvåtmarkers förmåga att avskilja aktiva läkemedelssubstanser som passerat genom avloppsreningsverket. Halter av 24 läkemedelssubstanser bestämdes i inkommande och utgående vatten till och från spillvattenvåtmarkerna i Eskilstuna, Hässleholm, Nynäshamn, Trosa och Oxelösund. De substanser som generellt sett återfanns i de högsta halterna i inkommande avloppsvatten till våtmarkerna var några vanliga antiinflammatoriska ämnen: naproxen, ibuprofen och diklofenak; några blodtryckssänkande ämnen: atenolol, hydroklortiazid, furosemid och metoprolol; och det lugnande ämnet oxazepam. Dessa ämnen förekom i koncentrationer mellan 0,7 μg/l och 10 μg/l. Resultaten visade att 47 % av de påträffade substanserna reducerades mellan 20 och 80 % och 47 % reducerades 80 % eller mer. Alla våtmarker visade en hög avskiljning av diklofenak, furosemid, hydroklortiazid och naproxen. Avskiljningsgraden för dessa ämnen var 74–100 %. Generellt sett uppvisade alla fem våtmarker en hög reningseffekt på aktiva läkemedelssubstanser men en något högre reningsgrad observerades i Oxelösund, Nynäshamn och Trosa våtmark. En möjlig förklaring till den höga reningseffekten kan vara våtmarkernas karakteristiska hydraulik, där spillvattendammar växelvis fylls och töms, i jämförelse med våtmarkerna i Eskilstuna och Hässleholm som har ett kontinuerligt flöde av spillvatten. En jämförelse gjordes också med tidigare reningsresultat under vinterförhållanden. Resultaten visade att avskiljningen av samtliga substanser var betydligt högre under de nu studerade sommarförhållandena. / The release of pharmaceutical residues to the environment is a growing problem of global concern. Many studies have reported the negative effects of pharmaceutical residues on fish and other aquatic organisms. This master thesis has assessed five constructed wetlands on their removal efficiency of active pharmaceutical substances. Influent and effluent wastewaters were analyzed for 24 common pharmaceutical substances in constructed wetlands in Eskilstuna, Hässleholm, Nynäshamn, Trosa and Oxelösund. The pharmaceuticals found in highest concentration in the influent were some common anti-inflammatory substances: naproxen, ibuprofen and diclofenac; a few antihypertensive substances: atenolol, hydrochlorothiazide, furosemide and metoprolol and the sedative substance, oxazepam. The concentrations varied between 0.7 μg/l and 10 μg/l. For 47% of the substances there was an observed removal efficiency of greater than 80% and for 47% of the substances a removal efficiency of 20–80 % was observed. Diclofenac, furosemide, hydrochlorothiazide and naproxen showed the greatest removal efficiencies, 74–100 %. In general, all five constructed wetlands showed high removal efficiencies for most pharmaceutical compounds, with greater removal efficiencies observed in Oxelösund, Nynäshamn and Trosa. The higher removal efficiency in these wetlands is believed to be due to their characteristic hydraulics, where wastewater basins are filled and emptied, whereas the basins in Eskilstuna and Hässleholm have continuous flow of wastewater. A comparison of removal efficiencies was also assessed for summer and winter conditions in Eskilstuna, Nynäshamn, Trosa and Oxelösund wetlands. The observed removal efficiencies were significantly greater during summer conditions.

<p>The purpose of this diploma work was to investigate the problem of insufficient fibre recovery in the dissolved air flotation-cell at the new thermomechanical pulping-line at Braviken Paper Mill. An investigation of the effect of process parameters on the removal efficiency in the micro-flotation process was undertaken.</p><p>The experiments were carried out for two setups at the Noss pilot plant with a small-scale flotation unit. Factorial design helped plan the experiments and four factors were controlled; temperature, fibre-size distribution, water quality and feed concentration. Three samples, feed, overflow and filtrate, were taken from each experiment and concentration measurements were made. The results were analyzed using the software MODDE.</p><p>The results from showed an influence from the fibre-size distribution. To see if the fibre-size distribution really had an effect on the results, follow-up experiments were carried out. These experiments showed no influence from temperature, fibre-size distribution or water quality. This concludes that none of those three factors influenced the results significantly.</p><p>Additional experiments were done to examine the influence from concentration and fibre-size distribution on the flotation efficiency and these showed an influence from the feed concentration. When increasing the feed concentration the efficiency of the flotation process decreased.</p>