Chitin belongs to the most abundant biopolymers on earth where it has an important role as a structural element in crustaceans, insects, fungi and some phytoplankton. Missing evidence for long-term accumulation of chitin in nature implies fast turnover and as chitin is composed of aminosugar subunits it holds central roles in both carbon and nitrogen cycles. The aim of this thesis was to contribute to a better understanding of organic matter cycling by learning more about the diversity, function and ecology of bacteria that degrade chitin. A metagenome-enabled study of the spatial distribution of chitinolytic bacteria in aquatic ecosystems identified salinity as the major environmental factor for shaping their community composition. To address the role of alternative environmental variables controlling chitinolytic communities, a temporally resolved study was completed in a dimictic freshwater lake. Pronounced seasonal change in the indigenous chitinolytic community was observed and parallel measured environmental parameters pointed to the availability and crystalline form of chitin as significant controlling factors.  The different ecological niches occupied by microbes that utilize chitin for growth were studied in an experimental study. Single-cell quantification of chitinolytic cells and cells incorporating chitin hydrolysis products suggested that commensal use of chitin hydrolysis products without simultaneous chitinase activity could be an important ecological strategy in freshwater bacterioplankton communities. Members of the ubiquitous and often quantitatively dominant group of freshwater Actinobacteria Ac1 were identified as particularly active in this “cheater” lifestyle. Further experiments based on artificially created gradients in bacterial diversity demonstrated the importance of specific bacterial populations and community composition rather than overall community richness in controlling more specific functions such as chitin and cellulose degradation. To conclude, results of this thesis provide insight into the biogeography, niche-separation and species interactions of the functional community of chitin degraders and the influence of general bacterial diversity to the respective system functioning. / Felaktigt tryckt som Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology 700

Pharmaceuticals, personal care products and dissolved organic matter (OM) are introduced to soil via irrigation with reclaimed wastewater. This thesis examines the basic factors that influence sorption of these components in soil. Sorption of dissolved OM samples of varying composition to clay surfaces was examined. Results indicate that preferential sorption is dependent on clay type but not necessarily OM composition. Analysis of soils revealed aliphatic components, carbohydrates and amino acids are prevalent at the soil-water interface whereas aromatics are inaccessible at the soil-water interface. No clear relationship between sorption affinity of 17β-estradiol, sulfamethoxazole, carbamazepine and phenanthrene and soil OM aromaticity or aliphaticity was observed. A negative relationship between sorption and O-alkyl content may be due to these components blocking contaminant access to high affinity sorption sites. Therefore, application of reclaimed wastewater to soils with O-alkyl-rich OM may result in higher mobility of contaminants.

Pharmaceuticals, personal care products and dissolved organic matter (OM) are introduced to soil via irrigation with reclaimed wastewater. This thesis examines the basic factors that influence sorption of these components in soil. Sorption of dissolved OM samples of varying composition to clay surfaces was examined. Results indicate that preferential sorption is dependent on clay type but not necessarily OM composition. Analysis of soils revealed aliphatic components, carbohydrates and amino acids are prevalent at the soil-water interface whereas aromatics are inaccessible at the soil-water interface. No clear relationship between sorption affinity of 17β-estradiol, sulfamethoxazole, carbamazepine and phenanthrene and soil OM aromaticity or aliphaticity was observed. A negative relationship between sorption and O-alkyl content may be due to these components blocking contaminant access to high affinity sorption sites. Therefore, application of reclaimed wastewater to soils with O-alkyl-rich OM may result in higher mobility of contaminants.

Monitoring data for potable water in the R.M. of Macdonald regional water system indicates elevated levels of chlorine disinfection by-products (DBPs), trihalomethanes (THMs). Dissolved Organic Carbon (DOC) and chlorine dose are the key precursors for the formation of THMs. Currently, the DOC is not removed efficiently at the Sanford water treatment plant, which supplies the R.M.’s potable water distribution system. The raw water DOC concentration incoming to the plant varied from 8.9mg/L to 31.8mg/L during this study. Sanford treated water effluent contained an average DOC of 6.5mg/L and the THM levels ranged from 86.6ppb to 175.7ppb. One of the objectives of this study was to conduct jar tests to optimize Sanford’s water treatment process to improve removal of DOC. Optimization of the coagulation process successfully reduced the DOC level in the plant effluent by 51% during the summer and 34% in the winter. The DOC reduction resulted in a THM reduction of 73.5ppb in the summer and 59.9ppb during the winter. Results showed that removal of 1mg/L of DOC eliminates 26.8ppb of THMs in summer and 11.9ppb during the winter. Another goal of this project was to investigate the relationship between THMs and their precursors, which includes: water DOC, free chlorine residual, and the chlorine contact time. Water samples were strategically collected throughout the Sanford regional water distribution system; the samples were tested for DOC, UV254, SUVA, chlorine residual, and contact time. A linear relationship between THM formation and chlorine contact time (R2 of 0.92) was found. This indicates that the content of THMs can be decreased by reducing the amount of time the water stays in the distribution system.

Mercury (Hg) is a known neurotoxin that is often found in concentrations exceeding safe consumption guidelines in aquatic biota. This is evident in northern Canada, where northerners consume significant amounts of animals such as beluga, seals and burbot. In the Mackenzie River Basin, recent increases in Hg concentration in many of these animals over the past 25 years have been observed. The warming climate, and with it, the changing carbon cycle, are hypothesised in this thesis to play a role in the increases. Within the context of the two major zones (mountainous and peatland), with distinct geomorphology, hydrology and geology, traditional fossil fuel exploration methods (Rock-Eval pyrolysis, organic petrography) have been employed in a novel manner on recent sediments to qualify and quantify the OM and several geochemical analyses have been used to determine the geochemical sources of Hg. The mountainous zone is composed mostly of refractory OM, from forest fire char and heavily reworked OM. It also contains, and fluxes, most of the Hg, which derives from oxidative weathering and erosion of widespread sulfide minerals. However, Hg from this zone is in chemical forms of limited bioavailability. The peatland zone has a greater proportion of labile OM, with higher concentrations of DOC and algal-derived OM. Lake-fed tributaries in this zone contain even higher proportions of labile OM. At one of these sites, the sediment core record shows that Hg has been increasingly associated with labile OM over time, due to increasing primary productivity accelerated by climate change, and is resulting in an increase in scavenged Hg. The temporal trend in algal-bound Hg in the sediment record matches very well with the temporal trend of Hg in burbot sampled from the area, providing one of the first and strongest lines of evidence for the climatic impact on Hg bioaccumulation in Arctic ecosystems.

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Monitoring data for potable water in the R.M. of Macdonald regional water system indicates elevated levels of chlorine disinfection by-products (DBPs), trihalomethanes (THMs). Dissolved Organic Carbon (DOC) and chlorine dose are the key precursors for the formation of THMs. Currently, the DOC is not removed efficiently at the Sanford water treatment plant, which supplies the R.M.’s potable water distribution system. The raw water DOC concentration incoming to the plant varied from 8.9mg/L to 31.8mg/L during this study. Sanford treated water effluent contained an average DOC of 6.5mg/L and the THM levels ranged from 86.6ppb to 175.7ppb. One of the objectives of this study was to conduct jar tests to optimize Sanford’s water treatment process to improve removal of DOC. Optimization of the coagulation process successfully reduced the DOC level in the plant effluent by 51% during the summer and 34% in the winter. The DOC reduction resulted in a THM reduction of 73.5ppb in the summer and 59.9ppb during the winter. Results showed that removal of 1mg/L of DOC eliminates 26.8ppb of THMs in summer and 11.9ppb during the winter. Another goal of this project was to investigate the relationship between THMs and their precursors, which includes: water DOC, free chlorine residual, and the chlorine contact time. Water samples were strategically collected throughout the Sanford regional water distribution system; the samples were tested for DOC, UV254, SUVA, chlorine residual, and contact time. A linear relationship between THM formation and chlorine contact time (R2 of 0.92) was found. This indicates that the content of THMs can be decreased by reducing the amount of time the water stays in the distribution system.

The purpose of this study was to determinate what requirements there should be on refilling material used as soil remediation based on the soil environment, i.e. soil processes and factors important to soil-dwelling organisms. The study was conducted by investigating which parameters that is important for the soil environment and by comparing them with each other. To exemplify how the parameters may change in different locations, data for total organic carbon, dry matter (i.e. water content), and pH were analyzed from different locations before and after soil remediation. Dry matter, organic matter, pH, compaction, grain size, porosity and soil composition were found to have a significant impact on various soil processes and soil organisms. Field investigations were made to examine dry- and organic matter and pH. The results were indicating that dry matter increased and that the organic matter decreased when the area was refilled with a coarse material. This study showed that there should be requirements on the characteristics of refilling material such as; organic matter content, good water holding capacity, a pH that is as neutral as possible and that the soil should not be too compact. A conclusion from this study was that crushed rock may not be the optimal refilling material after soil remediation.

Mercury (Hg) is a known neurotoxin that is often found in concentrations exceeding safe consumption guidelines in aquatic biota. This is evident in northern Canada, where northerners consume significant amounts of animals such as beluga, seals and burbot. In the Mackenzie River Basin, recent increases in Hg concentration in many of these animals over the past 25 years have been observed. The warming climate, and with it, the changing carbon cycle, are hypothesised in this thesis to play a role in the increases. Within the context of the two major zones (mountainous and peatland), with distinct geomorphology, hydrology and geology, traditional fossil fuel exploration methods (Rock-Eval pyrolysis, organic petrography) have been employed in a novel manner on recent sediments to qualify and quantify the OM and several geochemical analyses have been used to determine the geochemical sources of Hg. The mountainous zone is composed mostly of refractory OM, from forest fire char and heavily reworked OM. It also contains, and fluxes, most of the Hg, which derives from oxidative weathering and erosion of widespread sulfide minerals. However, Hg from this zone is in chemical forms of limited bioavailability. The peatland zone has a greater proportion of labile OM, with higher concentrations of DOC and algal-derived OM. Lake-fed tributaries in this zone contain even higher proportions of labile OM. At one of these sites, the sediment core record shows that Hg has been increasingly associated with labile OM over time, due to increasing primary productivity accelerated by climate change, and is resulting in an increase in scavenged Hg. The temporal trend in algal-bound Hg in the sediment record matches very well with the temporal trend of Hg in burbot sampled from the area, providing one of the first and strongest lines of evidence for the climatic impact on Hg bioaccumulation in Arctic ecosystems.

The objective of drinking water treatment is to provide water which is free of pathogens, is chemically and biologically stable, and is of good aesthetic quality. Natural organic matter (NOM) is present in all natural waters and can make meeting these goals more challenging. Not only does it undergo adverse reactions with disinfectants such as chlorine, it also impacts the biological stability of water within the distribution system and contributes to undesirable aesthetic qualities such as taste and odour. NOM has also been implicated in membrane fouling, which continues to be a significant operational problem preventing wider implementation of this process. Due to its highly variable heterogeneous nature, NOM can be difficult to characterize in terms of its specific composition, however recent analytical advancements are allowing for a better understanding of its behaviour in water treatment. Two promising tools for NOM characterization include Liquid Chromatography Organic Carbon Detection (LC-OCD) and Fluorescence Excitation Emission Matrix (FEEM) analyses. In this research both techniques were applied to samples taken from five full scale facilities in Ontario, Canada over all four seasons. The source waters for these treatment locations consisted of both river (Grand River, Ottawa River) and Great Lake waters (Lake Huron, Lake Erie, Lake Ontario), and an additional raw source (Saugeen River) was also monitored. The plants all employed granular media filtration, but had differences including enhanced coagulation, ozonation, biofiltration and sand ballasted flocculation. Other relevant water quality parameters were also monitored (TOC, DOC, UV254, pH, conductivity etc.) as well as plant operating conditions (dosages, flows, filter run times etc.) to investigate their impact on removal of specific NOM fractions. Four of the waters (Grand River, Ottawa River, Lake Erie and Lake Ontario) were selected based on the initial survey due to their NOM composition, for bench scale ultrafiltration (UF) membrane fouling experiments. The experiments were run at constant flux for a period of five days, with an automated permeation cycle and backwash. The impact of biopolymers on hydraulically reversible and irreversible fouling was of specific interest. Important seasonal trends were identified for all waters, with biopolymer content increasing at higher temperatures. Useful comparisons could also be made between different treatment processes including conventional and enhanced coagulation. The enhanced process while significantly improving the removal of humic substances, was not beneficial in terms of biopolymer removal, suggesting a different removal mechanism for these two fractions. The removal of low molecular weight ozonation by-products during full scale biofiltration was well demonstrated, and other fractions (building blocks, biopolymers) had varying degrees of removal, which was more dependent on temperature. Principle component analysis (PCA), an advanced multivariate statistical method, was successfully applied to a FEEM data set containing five different waters at varying degrees of treatment. Three principle components related to humic-like, protein-like and particulate/colloidal material were identified, and served as useful complementary information to the LC-OCD results. The humic-like component was found to have relatively good correlation to the humic fraction from LC-OCD analysis, with some deviation in the post-ozonation samples (which underwent greater structural changes not captured by LC-OCD). The biopolymer fraction was shown to have good correlation to hydraulically reversible membrane fouling across all four waters. The same could not be said for hydraulically irreversible fouling for which a combined fouling layer (with particulate and colloidal material) is hypothesized. This research provides those working in the water treatment sector with greater insight into NOM behaviour during various levels of treatment. As biopolymers were demonstrated to impact hydraulically reversible fouling (relatively independent of water quality), their removal prior to membrane filtration could significantly extend operational cycles by extending time between backwashes, thereby reducing energy requirements. As biopolymers are also suspected in forming a combined fouling layer, their removal can potentially minimize chemical cleaning requirements (and extend the life cycle of the membranes). The removal of biopolymers through coagulation was well demonstrated. Biofiltration is also expected to perform well as a membrane pre-treatment due its ability to remove biopolymers and particulate/colloidal matter. The ability of biofiltration to control biological re-growth in the distribution system (by removing low molecular weight biodegradable products) was also shown using LC-OCD and FEEM analysis.