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Contamination of groundwater supplies by gasoline and other petroleum-derived hydrocarbons released from underground or aboveground storage tanks is a serious and widespread environmental problem. Corrosion, ground movement, and poor sealing can cause leaks in tanks and associated piping. Petroleum hydrocarbons contain methyl tertiary-butyl ether (MTBE) (a fuel oxygenate), benzene, toluene, ethylbenzene, and xylene isomers (BTEX), the major components of gasoline, which are hazardous substances regulated by many nations. MTBE possesses all the characteristics of a persistent compound in the subsurface: high solubility, low volatility, low sediment sorption, and resistance to biodegradation. The objectives of this study were to (1) evaluate the biodegradibility of MTBE under aerobic conditions, and (2) assess the potential of using the aerobic bioremediation technique to clean up aquifers contaminated by MTBE. In this study, microcosms were constructed to determine the feasibility of biodegrading MTBE by intrinsic microbial consortia (aquifer sediments) under aerobic and aerobic cometabolic conditions. In the cometabolic microcosms, propane, ethanol, and BTEX were applied as the primary substracts to enhance the biodegradation of MTBE. The inocula used in this microcosm study were aquifer sediments collected from the contaminated-zones of a petroleum-hydrocarbon (including MTBE) contaminated site. Microcosms were constructed with nutrient medium (or site groundwater), sediments, and MTBE solution in 70-mL serum bottles sealed with Teflon-lined rubber septa. MTBE was analyzed using purge-and-trap instrument following gas chromatography (GC)/flame ionization detector (FID). Results show that the indigenous microorganisms were able to biodegrade MTBE under aerobic conditions using MTBE as the sole primary substrate. Microcosms with site groundwater as the medium solution show higher MTBE biodegradation rate. This indicates that site groundwater might contain some trace minerals or organics, which could enhance the MTBE biodegradation rate. Results show that the addition of BTEX would also enhance the MTBE removal. However, no significant MTBE biodegradation was observed in microcosms with propane and ethanol as the primary substrates. This reveals that the supplement of the second carbon source might inhibit the degradation of MTBE due to the preferential removal of some organics over MTBE. Results from the microcosm study suggest that aerobic biodegradation plays an important role on the MTBE removal. Intrinsic bioremediation is a feasible technology to remediate the studied MTBE-contaminated site.

Groundwater contamination by petroleum hydrocarbons has become one of the serious environmental problems in many countries. The sources of petroleum-hydrocarbon contaminants may be released from above ground and underground storage tanks, and pipelines. Petroleum hydrocarbons are mainly composed of benzene, toluene, ethyl- benzene, and xylems (BTEX), and other constituents such as methyl-tert-butyl ether (MTBE), naphthalene, 1,3,5-trimethylbenzene (1,3,5-TMB), and 1,2,4-trimethylbenzene (1,2,4-TMB). It is generally recognized that petroleum hydrocarbons have high risks to environmental receptors when hydrocarbon releases occur. Various biological, physical, and chemical remediation technologies (e.g. pump and treat, air sparging, enhanced bioremediation, and chemical oxidation) can be used to remediate petroleum-hydrocarbon contaminated groundwater. However, many of these techniques are typically costly or have limited applications. Permeable reactive barriers (PRBs) are a promising technology for the passive and in situ treatment of contaminated groundwater. A PRB can be defined as ¡§an emplacement of reactive materials in the subsurface designed to intercept a contaminant plume, provide a preferential flow path through the reactive media, and transform the contaminant(s) into environmentally acceptable forms to attain remediation concentration goals at points of compliance.¡¨ The oxygen release materials can be emplaced in the PRBs to passive increase dissolved oxygen (DO) in the subsurface to enhance the intrinsic biodegradation of dissolved hydrocarbons. In the first part of this study, guidelines for PRBs installation have been developed for the remediation of petroleum hydrocarbons, heavy metals, and organic solvents contaminated groundwater. PRB is a cost-effective approach for the remediation of contaminated aquifers. As contaminated groundwater moves through a permeable reactive barrier, the contaminants are scavenged or degraded, and uncontaminated groundwater emerges from the downgradient side of the reactive zone. The permeable reactive barrier concept has several advantages over other remediation technologies currently in use (e.g., pump and treat, air sparging), including absence of mechanical facilities and the electric power, no groundwater extraction and reinjection, treatment in situ, and cost-effective. The first part of this study presents the designs, applications, and case studies of PRB systems on groundwater remediation. In the second part of this study, oxygen release materials have been constructed and evaluated for the appropriate components in batch experiments. Microbial degradation of petroleum hydrocarbons in groundwater can occur naturally. Since the petroleum-hydrocarbons are generally degraded faster under aerobic conditions, aerobic bioremediation can be applied to enhance the biodegradation of petroleum-hydrocarbons within of the plume if oxygen can be provided to the subsurface economically. Batch experiments were conducted to design and identify the components of the oxygen-releasing materials. Cement and gypsum were used as a binder in this mixtures experments. (1) using cement as the binding material The mixtures of the oxygen release material were prepared by blending cement, peat, sand, ethylene-vinyl acetate copolymer(EVA), calcium peroxide (CaO2), and water together at a ratio of 1.0¡G0.18¡G0.20¡G0.10¡G1.12¡G1.74 by weight. Cement was used as a binder and regular medium filter sand was used to increase the permeability of the mixture. Calcium peroxide releases oxygen upon contact water. The designed material with a density of 1.9 g/cm3 was made of 3.5 cm cube for the batch experiment. Results show that the oxygen release rate of the material is 0.046 mg O2/day/g rock. The oxygen release material was able to remain active in oxygen release for more than three months. (2) using gypsum as the binding material The mixtures of the oxygen release material were prepared by blending gypsum, CaO2, sand, and water together at a ratio of 1¡G0.5¡G0.14¡G0.75 by weight. Gypsum was used as a binder and regular medium filter sand was used to increase the permeability of the mixture. Calcium peroxide releases oxygen upon contact water. The designed material with a density of 1.1 g/cm3 was made of 3.5 cm cube for the batch experiment. Results show that the oxygen release rate of the material is 0.031 mg/day/g. The oxygen release material was able to remain active in oxygen release for more than three months. In the third part of this study, immobilization technology was applied to produce the low permeability wrapping film for the construction of oxygen-releasing granular materials. The mixtures of the oxygen release material were prepared by blending alginate, CaO2, and sand together at a ratio of 8.3¡G1.0¡G1 by weight. The low permeability wrapping film of the oxygen release material was able to remain active in oxygen release for two months. In the fourth part of this study, a laboratory-scale column experiment was conducted to evaluate the feasibility of this proposed system on the bioremediation of petroleum-hydrocarbon contaminated groundwater. This system was performed using a series of continuous-flow glass columns including four consecutive soil columns. Simulated petroleum-hydrocarbons contaminated groundwater with a flow rate of 0.263 m/day was pumped into this system. In the column experiment, the samples of column influent and specified sampling ports were collected and analyzed for pH, DO, BTEX, MTBE, and microbial populations. Results show that up to 99% of BTEX removal was observed in this passive system. Results from this study would be useful in designing an efficient and cost-effective passive oxygen-releasing and bioremediation system to remediate petroleum- hydrocarbon contaminated aquifer.

Evolution of strategies for biodegradation of synthetic organic pollutants relies on recruitment of genes from catabolic pathways for natural compounds. Investigation of metabolic diversity in nature can provide insight into biochemical strategies that could be recruited for bioremediation of pollutants. As part of a search for novel metabolic diversity we isolated soil bacteria able to degrade 2-nitroimidazole (2NI) and 5-nitroanthranilic acid (5NAA), and determined the biochemistry and molecular biology of their biodegradation pathways. 2NI and its analogs are increasingly used as prodrugs for the treatment of both tuberculosis and cancer. The biodegradation of 2NI by a soil Mycobacterium sp. is initiated by an unusual hydrolytic denitration. The reaction is catalyzed by a novel nitrohydrolase with a divergent sequence and represents the discovery of a previously unreported drug resistance mechanism in soil prior to its identification in clinical situations. 5NAA is the starting material for various nitroaromatic compounds and dyes. The biodegradation pathway of 5NAA is initiated by an unusual hydrolytic deamination. The corresponding gene is very distantly related to biochemically characterized genes in the NCBI database. The nitro group of 5NAA is eliminated as nitrite during the spontaneous formation of lactones from a ring fission product, a previously unreported mechanism. Degradation pathways of 5NAA and 2NI serve as precedents for those of nitroaniline and nitroimidazole pollutants. The work supports the hypothesis that the study of the metabolism of natural organic compounds selected on the basis of unusual structural features and ecological roles can reveal new metabolic diversity.

<p>Analytical analyses conducted at the Himmerfjärden WWTP (285.000 PE connected) identified 70 pharmaceutical compounds belonging to different therapeutic classes. Such organic micropollutants at low detected concentration range of µg - ng l^-1 did not affect the treatment processes at WWTP. Results from analytical studies indicated continuous discharge of organic micropollutants to the surface water with a calculated load amounting to 1.51 kg day-1. Metoprolol, carbamazepine and naproxen were chosen for testing different removal methods. Oxygen Uptake Rate (OUR) tests were conducted to assess the bacterial activity of an activated sludge taken from a full scale aeration plant with the presence of selected target compounds.</p><p>A semi-technical scale membrane bioreactor ZeeWeed10™, treating final effluent from the Himmerfjärden WWTP (Sweden) was seeded with activated sludge from full scale biological stage. The membrane bioreactor (MBR) system placed after the final treatment appeared to be an insufficient technology for removal of residual amounts of organic micropollutants from WWTP effluents. Batch test studies with activated sludge taken from the membrane bioreactor and with application of granular activated carbon (GAC) filtration resulted in giving an overall assessment of removal efficiency. Metoprolol and carbamazepine tend to be resistant to the biodegradation process and in the dosed high concentration lead to bacterial cell decomposition in the activated sludge. Apparently, removal efficiency for naproxen exceeded the value of 46% with the spiked initial amount of 3.3 mg NAP g^-1MLSS. Application of the GAC filtration proved to be an efficient technique for removal of pharmaceutical compounds from treated wastewater.</p><p>Application of the statistical programme Modde7 was a time saving tool in studies of fouling occurrence. The effect of fouling phenomenon, which is a highly limiting factor for MBR performance, was minimised by adjusting the operational parameters as predicted by the Modde7 programme.</p>

published_or_final_version / Environmental Management / Master / Master of Science in Environmental Management

Waste management in the leather industry worldwide is an issue of major importance for both solid and liquid wastes. It has been recognised that there are major environmental impacts from the poorly managed disposal of such wastes and these have a clear health impact upon human society. Within Europe, under EU driven legislation, the costs of wastes management are increasing rapidly and there is a clear need to research improved methods to cost effectively deal with leather industry wastes. Biodegradation (anaerobic), as a management option, of solid wastes from the leather industry is an area that is attracting increased interest in recent years as being a technique that has wide public acceptability as well as process efficiency. However, tanning agents that prolong the lifetime of leather goods have a negative impact on biodegradation and this needs to be addressed before efficient treatment can occur. To drive the agenda this research has the aims of • Highlighting the effects of tanning agent on anaerobic digestion. • Understanding the mechanism(s) by which different leather tannages can biodegraded. • Developing a process to reverse the action of tannage. Leather solid wastes were anaerobically digested using Serum Bottle Assays (SBA). The effect of a range of vegetable, mineral and aldehyde tanning agents of leather on the rate of anaerobic digestion was assessed. Common tanning agents used included; myrica, valonea, glutaraldehyde and chrome. To further identify key factors for cost effective anaerobic digestion, tanned hide powders and tanned leathers were also pre-treated using autoclaving, liming, enzymes etc, in an attempt to determine whether tannage may be reversed. Major techniques used in the research include: anaerobic digestion, Biochemical Methane Potential (BMP), Total Solids contents (TS), Gas Chromatography (GC) and Gas Chromatography Mass Spectrometry (GC-MS). Hydrolysable tannins are less resistant to anaerobic digestion than condensed tannins. However, enzymatic pre-treatment reduces the resistance and this offers a new effective pre-treatment route. Thermal pre-treatment also decreased resistance to anaerobic digression especially for chrome, glutaraldehyde, myrica and tannic acid tanned leathers. Chemical pre-treatment also generally lowered the resistance to anaerobic digestion. Selective pre-treatment offers a means of improving the cost effectiveness of anaerobic digestion of leather and therefore enabling a new waste management method to be adopted by the industry. A relationship emerges, in some cases, between chemical structure of tanning agent and inhibition of anaerobic digestion. This offers the possibility of producing new, designed organic tanning agents with, suitable properties, to be adopted by the industiy, The research agenda within the leather industry is still ongoing and recommendations for future research are addressed

published_or_final_version / Botany / Master / Master of Philosophy