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Use and Development of Diffusive Samplers to Analyse the Fate of Polycyclic Aromatic Compounds, Polychlorinated Biphenyls and Pharmaceuticals in Wastewater Treatment Processes
Umeå University, Faculty of Science and Technology, Chemistry.
2008 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The efficiency of wastewater treatment systems is commonly measured by the reductions of parameters such as biological oxygen demand (BOD), chemical oxygen demand (COD) and total suspended solids (TSS) and/or reductions in levels of selected macro compounds (e.g. long-chained hydrocarbons and inorganic compounds). Less attention has generally been paid to micropollutants with high potential toxic effects, such as polycyclic aromatic compounds (PACs), including unsubstituted and alkylated polycyclic aromatic hydrocarbons (PAHs) and dibenzothiophenes, polychlorinated biphenyls (PCBs), human pharmaceuticals and by-products formed during the treatment process. These organic micropollutants occur in wastewaters at trace and ultra-trace levels, therefore their detection requires advanced, costly analyses and large sample volumes. Furthermore, concentrations of micropollutants can fluctuate widely both diurnally and between days. Thus, in order to understand the fate of micropollutants in wastewaters there is a need to develop sampling techniques that allow representative samples to be readily collected.

In the work underlying this thesis two types of diffusive passive samplers, semipermeable membrane devices (SPMDs) and polar organic chemical integrative samplers (POCISs), were used to monitor non-polar and polar organic micropollutants in wastewaters subjected to various treatment processes. The pollutants sequestered in these samplers represent micropollutants in the dissolved phase that are available for aquatic organisms. Further, since they collect pollutants in an integrative manner, i.e. they sample continuously during the selected exposure time (usually approx. one to ca. three weeks), the results provide time-weighted average (TWA) concentrations. In addition, the effects of various environmental factors on the uptake of analyzed micropollutants in POCISs and SPMDs were investigated using laboratory calibration and in situ calibration with performance reference compounds (PRCs).

The results confirm that SPMDs are good sampling tools for investigating the efficacy of wastewater treatment processes for removing non-polar PACs and PCBs, and the effects of varying the process settings. In addition, analyses of process streams in municipal sewage treatment plants demonstrated that conventional sewage treatment processes are not optimized for removing dissolved four-ringed PAHs, some of the five-ringed PAHs, and tri- to hexa-chlorinated biphenyls. The removal of bioavailable PACs was enhanced by adding sorbents with high sorption capacities to the sludge used in the activated sludge treatment step, and a biologically activated carbon system was designed that robustly removed bioavailable PACs, with removal efficiencies of 96.9-99.7 percent across the tested ranges of five varied process parameters.

In situ SPMD calibration data acquired show that uptake of PACs, described by SPMD sampling rates (Rs), were four to eight times higher than published laboratory calibrated Rs values, mainly due to strong (bio)fouling and turbulence effects. In addition, the laboratory calibration study demonstrated that temperature affects the POCIS uptake of pharmaceuticals. The uptake of four pharmaceuticals was higher, by 10-56 percent, at 18 °C compared to 5 °C. For two of the pharmaceuticals our data indicate that the uptake was lower by 18-25 percent at 18 °C. Our results also indicate that uptake of the studied pharmaceuticals was in the linear phase throughout the 35 day exposure period at both temperatures. Finally, calibration studies enabled aqueous concentrations of micropollutants to be more accurately estimated from amounts collected in the passive samplers.

Place, publisher, year, edition, pages
Umeå: Kemi , 2008. , 49 p.
Keyword [en]
bioavailable, biologically activated carbon, PRCs, sampling rate, SPMD, sorption, wastewater treatment, diffusive passive samplers, human pharmaceuticals, municipal sewage treatment plant, organic micropollutants, polycyclic aromatic compounds, PAHs, PCBs, POCIS
National Category
Environmental Sciences
Identifiers
URN: urn:nbn:se:umu:diva-1912ISBN: 978-91-7264-688-9 (print)OAI: oai:DiVA.org:umu-1912DiVA: diva2:142405
Public defence
2008-12-05, KB3A9, KBC, Umeå, 10:00 (English)
Opponent
Supervisors
Available from: 2008-11-10 Created: 2008-11-10 Last updated: 2009-06-18Bibliographically approved
List of papers
1. PAH and PCB removal efficiencies in Umeå (Sweden) and Šiauliai (Lithuania) municipal wastewater treatment plants
Open this publication in new window or tab >>PAH and PCB removal efficiencies in Umeå (Sweden) and Šiauliai (Lithuania) municipal wastewater treatment plants
2006 (English)In: Water, Air and Soil Pollution, ISSN 0049-6979, Vol. 175, no 1-4, 291-303 p.Article in journal (Refereed) Published
Abstract [en]

Dissolved concentrations of polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) in the influents and effluents of two municipal sewage treatment plants (STPs) were monitored over 16- (Umeå, Sweden) and 22- (Šiauliai, Lithuania) day sampling periods. Sampling was performed using a passive sampling technique (semipermeable membrane devices; SPMDs) for sequestration of the dissolved (readily bioavailable) fraction of persistent organic pollutants (POPs). Removal efficiencies for individual low molecular weight (LMW) PAH compounds varied from 84% to levels at which the compounds were not detected in effluents from Umeå. The corresponding efficiencies of the Šiauliai plant were 33–95%. Measurements revealed that dissolved concentrations of most of the PCBs and some of the high molecular weight (HMW) PAHs increased during the conventional wastewater treatment at both plants. The release of dissolved PAHs and PCBs in the effluents from municipal wastewater treatment plants might increase the environmental contamination by readily bioavailable pollutants in the recipient waters; the rivers Umeälven and Kulpè. SPMDs were found to be suitable sampling tools for long-term (weeks-month) integrative monitoring of trace concentrations of the dissolved fraction of hydrophobic pollutants in the wastewater process, since the sampling and clean-up steps were easy to perform.

Place, publisher, year, edition, pages
Netherlands: Springer , 2006
Keyword
Analysis, Bioavailable fraction, Diffusive sampling, Effluent, PAHs, PCBs, SPMDs, Wastewater treatment efficiency
Identifiers
urn:nbn:se:umu:diva-3616 (URN)
Available from: 2008-11-10 Created: 2008-11-10Bibliographically approved
2. Estimation of Water Sampling Rates and Concentrations of PAHs in a Municipal Sewage Treatment Plant Using SPMDs with Performance Reference Compounds
Open this publication in new window or tab >>Estimation of Water Sampling Rates and Concentrations of PAHs in a Municipal Sewage Treatment Plant Using SPMDs with Performance Reference Compounds
2007 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 41, no 14, 5044-5049 p.Article in journal (Refereed) Published
Abstract [en]

Semipermeable membrane devices (SPMDs) were exposed at ten sampling points, each representing a different stage in the treatment process, in a municipal sewage treatment plant. Differences in SPMD uptake kinetics of polycyclic aromatic hydrocarbons (PAHs) due to variations in conditions at the sampling sites were evaluated by using five performance reference compounds (PRCs) with log Kow values of 4.20 to 6.34. PRC release rate constants (ke,PRC values) were calculated for PRCs for which 50-98% of the initial amounts were lost during the sampling period. The ke,PRC values were high, ranging from 0.08 to 0.11 day-1 for the studied PRCs, at sampling site W1 (raw sewage), the only sampling site where significant amounts of the PRCs with log Kow values >5 were released from the SPMDs. At the other sampling sites, only PRCs with log Kow values between 4.20 and 4.50 were released in significant amounts. The release rates at these sites were lowest (0.04 day-1) at sampling site W9 (the secondary clarifier) and highest (0.18 day-1) at W8 (the active sludge aeration basin). Differences between sampling rates (Rs) obtained using published laboratory-calibrated data and PRC-corrected Rs values were visualized by principal component analysis (PCA). The water concentrations of 24 studied PAHs fell substantially during the course of the sewage treatment process. However, low molecular weight PAHs were more effectively removed than high molecular weight PAHs. Significant deviations between actual and estimated water concentrations may arise unless PRC-corrected Rs values are applied.

Identifiers
urn:nbn:se:umu:diva-16041 (URN)doi:10.1021/es070054+ (DOI)
Available from: 2007-08-16 Created: 2007-08-16 Last updated: 2017-12-14Bibliographically approved
3. Chemical and Ecotoxicological Assessment of Selected Biologically Activated Sorbents for Treating Wastewater Polluted with Petroleum Products with Special Emphasis on Polycyclic Aromatic Hydrocarbons
Open this publication in new window or tab >>Chemical and Ecotoxicological Assessment of Selected Biologically Activated Sorbents for Treating Wastewater Polluted with Petroleum Products with Special Emphasis on Polycyclic Aromatic Hydrocarbons
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2008 (English)In: Water, Air, & Soil Pollution, ISSN 0049-6979 (Print) 1573-2932 (Online), Vol. 195, no 1-4, 243-56 p.Article in journal (Refereed) Published
Abstract [en]

A chemical and ecotoxicological assessment of treatment of wastewater that had been polluted with petroleum products using only Activated Sludge (AS) and four biologically activated sorbents (BASs), consisting of activated sludge plus: coal-based activated carbon (-C1), coconut shell-based activated carbon (-C2), zeolite (-Z), and anthracite (-A) were conducted. The efficiency and robustness of the four wastewater treatment systems were evaluated by calculating the reduced total petroleum hydrocarbon (TPH) and polycyclic aromatic hydrocarbon (PAH) contents and the acute ecotoxicity of the effluents. The chemical analysis showed that the combined treatment systems were very effective for reducing the total petroleum hydrocarbon and readily bioavailable PAH contents. The most efficient systems were the BAS-C1 and -C2, which removed 60–88% and 99.5–99.6% of TPH and PAH, respectively. The activated sludge-only treatment was the least effective for purifying the wastewater. Chemical oxygen demand was reduced by >90% by all carbon-based BASs (BAS-C1, BAS-C2 and BAS-A). Shifts in the relative composition of the individual PAHs were identified in samples taken before and after treatment. Algal and bacterial bioassays showed that the toxicities of effluents following treatment by all four systems (except AS for algae) were reduced by more than 80% and 90%, respectively. However, crustacean tests indicated that the carbon-based BASs reduced the toxicity [V tox(50)] only by 19–67%. Our results indicated that the combination of sorption and biodegradation processes have great potential in the treatment of petroleum products polluted wastewater and is less sensitive for inhibitors of the biological process than treatments in which activated sludge alone is used. The assessment of chemical and ecotoxicological endpoints provided valuable information, but contrasting results for one of the assays indicates that further analysis on the capacity of the different treatment systems is warranted.

Keyword
Biodegradation, Biologically activated sorbents (BASs), Ecotoxicity, Petroleum products, Polycyclic aromatic hydrocarbons (PAHs), Semipermeable membrane devices (SPMDs), Sorption, Wastewater treatment
Identifiers
urn:nbn:se:umu:diva-10194 (URN)doi:10.1007/s11270-008-9743-7 (DOI)
Available from: 2008-10-10 Created: 2008-10-10 Last updated: 2011-01-10Bibliographically approved
4. Multivariate analysis of a biologically activated carbon (BAC) system and its efficiency for removing PAHs and aliphatic hydrocarbons from wastewater polluted with petroleum products
Open this publication in new window or tab >>Multivariate analysis of a biologically activated carbon (BAC) system and its efficiency for removing PAHs and aliphatic hydrocarbons from wastewater polluted with petroleum products
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2009 (English)In: Journal of Hazardous Materials, ISSN 0304-3894, E-ISSN 1873-3336, Vol. 170, no 1, 103-110 p.Article in journal (Refereed) Published
Abstract [en]

The efficiency of a biologically activated carbon system for treating wastewater polluted with petroleum products was examined and the effects of process parameters on its efficacy were evaluated. In each experiment 17 alkylated and 19 non-alkylated polycyclic aromatic hydrocarbons (PAHs) and total petroleum hydrocarbons (TPHs, C10-C40) were extracted using semipermeable membrane devices from wastewater before and after treatment. The acquired data during experiments were analyzed using principal component analysis (PCA). The treatment system robustly removed dissolved PAHs across the studied ranges of the process parameters, providing overall removal efficiencies of 96.9-99.7% for the sum of 36 PAHs. However, the major contributor to their removal was sorption rather than biodegradation, and despite the general efficiency of the process there was up to a 9-fold range in the sums of quantified PAHs in the effluents between experiments. Combinations of long process contact time (24 h) with high temperature (24 degrees C) and moderate oxygen concentration (6-7mg O2 L-1) resulted in good removal of bioavailable PAHs. The removal of TPHs was more dependent on biological activities during the wastewater treatment, and consequently more dependent on the process parameters. In addition, small but significant proportions of PAHs were volatilized and released during the wastewater treatment.

Place, publisher, year, edition, pages
Elsevier, 2009
Keyword
Biodegradation, Polycyclic aromatic hydrocarbons (PAHs), Sorption, Semipermeable membrane devices (SPMDs), Total petroleum hydrocarbons (TPHs)
National Category
Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-23177 (URN)10.1016/j.jhazmat.2009.04.129 (DOI)19482425 (PubMedID)
Available from: 2009-06-02 Created: 2009-06-02 Last updated: 2017-12-13Bibliographically approved
5. Laboratory evaluation of the temperature effect on the uptake of selected pharmaceuticals by the polar organic chemical integrative sampler (POCIS)
Open this publication in new window or tab >>Laboratory evaluation of the temperature effect on the uptake of selected pharmaceuticals by the polar organic chemical integrative sampler (POCIS)
(English)Manuscript (Other academic)
Identifiers
urn:nbn:se:umu:diva-3620 (URN)
Available from: 2008-11-10 Created: 2008-11-10 Last updated: 2010-01-13Bibliographically approved

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