Dans ce travail, nous nous sommes intéressés à l’imogolite-méthylée, un nanotube dispersé en phase aqueuse avec une nanocavité hydrophobe.Nous avons tout d’abord étudié ses mécanismes de formation. A court terme, les premiers précipités formés se réorganisent en nanoobjets ayant la même structure locale que l’imogolite et dont la taille dépend des conditions de synthèses (concentration, précurseur). Ils conduisent à la formation d’objets cylindriques (imogolite) ou sphériques (allophane).Sur le long terme, nous avons observé que l’imogolite-méthylée coexiste avec des sous-produits (hydroxyde d’aluminium, proto-imogolite et allophane). En choisissant judicieusement les paramètres de synthèse (rapport molaire entre les précurseurs, température de synthèse) il est possible de réduire la proportion de ces sous-produits mais pas de les éliminer complétement.Ensuite, nous avons étudié la fonctionnalisation de ces nanotubes par substitution d’une partie des groupes méthyles internes par des groupes dopants. L’encapsulation de Nile Red, un colorant solvatochromique, dans la cavité interne des nanotubes hybrides a mis en évidence la fonctionnalisation des imogolites avec les différents groupes utilisés. Enfin, nous avons exploré l’encapsulation de molécules organiques (polaires, apolaires, solubles et insolubles dans l’eau) dans la cavité des nanotubes. Les courbes de diffusion X montrent que l’imogolite-méthylée piège toutes les molécules testées. De plus, les quantités adsorbées calculées sont comparables à celles mesurées dans le cas où des charbons actifs ou des zéolithes sont employés comme adsorbants. / In this work, we studied methyl-imogolite, an inorganic nanotube dispersed in water with a hydrophobic cavity.First, we examined the formation mechanisms. On a short time scale, the initial precipitates reorganize to give nano-objects with the same local structure as imogolite. Their size depends on the synthesis conditions (concentration, precursor) and could lead to the formation of cylindrical (imogolite) or spherical (allophane) objects.On a long time scale, we observed that methyl-imogolite coexists with byproducts (aluminum hydroxide, proto-imogolite and allophane). It is possible to reduce their proportion by wisely selecting the synthesis parameter (molar ratio between precursors, synthesis temperature). However, they cannot be fully eliminated. Then, we studied the functionalisation of this nanotube by substituting part of the internal methyl groups by doping ones. Encapsulation of Nile Red, a solvatochromic dye, in the internal cavity of these hybrid nanotubes highlighted the functionalisation of the imogolite with the various groups used.Finally, we investigated the encapsulation of organic molecules (polar, apolar, soluble or insoluble in water) in the nanotubes cavity. SAXS curves evidenced the trapping of all the molecules tested by methyl-imogolite. Moreover, calculated adsorption capacities are similar to the ones obtained when activated carbon or zeolites are used as adsorbents.

Sulfonamides are antibiotics that are frequently used both in human and veterinary medicine. The combinations of abundant use of these antibiotics and their natural resistance to decay leads often to long term persistence in the environment. This accumulation, especially in living organisms, may lead to subsequent toxicosis. Also, presence of these antibiotic in nature poses problems with regard to the spread of genes for antibiotic resistance between potential pathogens. These facts led to an increase interest in studying the sulfonamide biodegradation and subsequent sulfonamide removal from the environment. In this work it was possible to isolate and characterize the microorganism Acinetobacter sp. strain 49. This microorganism was able to biodegrade under right conditions sulfamethoxazole with 80 % efficiency. Sulfamethoxazole is one of the most commonly found sulfonamide in the nature.

Lake Macquarie is the largest estuarine lake in New South Wales and is located on the eastern seaboard of Australia, approximately 85 km north of Sydney.The study of heavy metal concentrations in surficial sediments, sediment cores, seagrasses and fish conducted by the New South Wales Department of Mines in 1974 revealed that significant heavy metal contamination of Lake Macquarie has occurred. The metalloid selenium was found in elevated concentrations in 1987. Selenium has a complex chemistry and is both an important nutrient and in high concentrations toxic. This review describes briefly the Lake Macquarie environment and suggests some approaches of modelling the remobilisation and cycling of selenium in sediment. The biogeochemical cycling of selenium in an estuarine environment is exceedingly complex. Factors include Eh, pH, ligand complexing ability, solubility of selenium containing minerals, sediment/soil characteristics, microbially-mediated reactions and physical reworking by biota (bioturbation). The goal of the model will be to be able to estimate the transport rates from a calculated value of Se concentration in sediment pore water resulting in a Se flux value for the interface between sediment and overlaying water. / www.ima.kth.se

In the early years of the 20th century the first tailing dams were constructed, the upstream tailing dam being the first type. Before this the tailings were disposed in the nearest stream or river. This caused legal issues between farmers and the mining companies, which ended the random discharge of the tailings. During the 20th century many tailing dams collapsed raising questions whether the technology is sufficient and safe. The known failures are just a fraction of the actual number since not all failures are documented. If a tailing dam were to break the consequenses could be fatal not only on impact but longterm, affecting many generations to come. This paper analyses an active tailing dam in China using the software COMSOL 3.4. The main aspects are the seepage, stability and pollution transport of the unsaturated upstream tailing dam. The results indicate that the dam at this point in time is stable, based on the aspects studied, the inputdata and models that were created.

Die Schadstoffsituation der Böden der Siedlungsgebiete von Annaberg-Buchholz und Aue (Erzgebirge) wurde mit unterschiedlichen methodischen Ansätzen und Interpolationsverfahren flächenhaft dargestellt und evaluiert. Festgestellt wurde, dass sich Punktinformationen zu Schadstoffgehalten auch in Siedlungsbereichen des Erzgebirges zumeist mit ausreichender Aussagesicherheit in Karten darstellen lassen. Dabei erwies sich keine der bislang bekannten Methoden für die Übertragung von Punktinformationen auf die Fläche als grundsätzlich vorteilhaft; jede Methode zeigte gebietsspezifisch und für einzelne Metalle Stärken und Schwächen. Erstmals kam ein Verfahren der künstlichen Intelligenz (Software advangeo®) erfolgreich zum Einsatz. Die Vorteile dieses Verfahrens zeigten sich gerade in sehr klein strukturierten Siedlungsbereichen und der Vielzahl von Einflussgrößen auf die Stoffgehalte. Damit ließ sich der Einfluss der oberflächennahen Erzgänge auf die Arsen-Konzentration der Böden im Siedlungsgebiet Annaberg gesichert abbilden. Die Erfahrungen aus den Testgebieten münden in Empfehlungen zur optimalen Anwendung der methodischen Ansätze und untersuchten Verfahren.

Stormwater runoff may contain high levels of pollutants and is regulated by the Federal National Pollution Discharge Elimination System (NPDES). Stormwater bioretention (BR) systems are often used to satisfy these regulations. BR systems collect accumulated runoff that leaches into groundwater. A greenhouse study evaluated nutrient and metal removal among plant species that are typically found growing in BR systems. A field demonstration study assessed citric acid enhanced metal bioaccumulation potential under typical BR system conditions. The greenhouse experiment examined pollutant retention, and bioaccumulation potential for six plant species undergoing three hydraulic and pollutant loads. Results verified there was 98% recovery of total phosphorous over the study period. Biomass increased with higher hydraulic and pollutant loads for all species. Phragmites australis, Carex praegracilis, and Carex microptera took up significantly more total phosphorous and nitrogen mass into shoots than Typha latifolia, Scirpus valid us, and Scirpus acutus. This study also found that 89% of applied metals were removed within the top 27 em of soil in all treatments. Similar results were found regarding copper, lead, and zinc concentrations and bioaccumulation. Carex praegracilis, and Carex microptera exhibited higher metal distribution in plant tissue and exfiltrate, and lower distribution in the soil media than the other species. This indicated species differences in biological and chemical processes taking place within the simulated BRsystems. The field experiment investigated citric acid enhanced metal bioaccumulation potential among three different plant species under representative BR conditions. Citric acid significantly increased metal concentrations in the soil pore water for the planted treatments, but this did not result in increased metal uptake into plant tissue. However, notable differences were found among species, where Carex microptera accumulated more AI, Cr, Cu, and Fe in the above ground tissue than Helianthus maximiliani and Typha /atifolia (except for Cu in Helianthus). These results provide greater insight into the biological and chemical process that affect transport, uptake and translocation of nutrients and metals, and confirm the importance of species selection in BR systems to optimize nutrient and metal retention and recovery from stormwater runoff to minimize subsequent groundwater pollutant loading.

Air emissions from animal feeding operations have become a growing concern. Much work has been done to study occupational exposures and the exhaust concentrations associated with animal facilities; however little information has been provided about air quality around the houses. Ammonia (NH3 ), ethanol (EtOH), nitrous oxide (N2O), carbon dioxide (CO2), and particulate matter (PM 2.5 and PM10) emissions were monitored in two different buildings for laying hens in northern Utah. Over the six-month sampling period, the observed average temperatures for the west and east fan banks of the high-rise building were 21.2±4 and 19.4±1.3°C, respectively, and the average inside relative humidities during the same period were 43.7±7.2 and 48.4±7.9%, respectively. Furthermore, the observed average temperatures for the west and east fan banks of the manure-belt building were 20.6±4.4 and 17.9±2.7°C, respectively, and the average percent inside relative humidities during the same period were 44.4 ±7.6 and 49.3±7.4%, respectively. The ventilation rates ranged from 0.80 m3 h-1 bird-1 to 4.80 m3 h-1 bird -1 with an average of 2.02 m3 h -1 bird -1 for the high-rise barn and from 0.80 m3 h-1 bird -1 to 6.0 m3 h-1 bird-1 with an average of 2.20 m3 h-1 bird-1 for the manure-belt building over the sampling period of September, October, November, and December 2008 and January 2009. Average NH3 emission factors were 72±17 g d-1 AU-1 for the high-rise system and 9.1±7 g d-1 AU-1 for the manure-belt (1 AU is equal to 500 kg of animal live weight). The NH3 emission reduction factor for the manure-belt technique compared to the high-rise technique was 87%. Ammonia levels outside the house appeared to be less than 1 ppm. No significant emissions were registered for N2O, H2S, and EtOH, which were consistently close to zero for both techniques. The carbon dioxide (CO2) emission factor from the high-rise building was 104±11 g day-1 AU-1 and from the manure-belt building, 105±20 g day-1 AU-1. PM emissions were greater from the manure-belt system in comparison with the high-rise system, showing mean values of 165 vs. 114 g day-1 AU-1 for PM 2.5, 1,987 vs. 1,863 g day-1 AU-1for PM10 and 4,460 vs. 3,462 g day-1 AU-1 for TSP respectively. None of the 24-h PM 2.5 measurements collected from both management techniques exceeded the U.S. EPA 24-hr National Ambient Air Quality Standard (NAAQS) of 35 μg/m 3.

<p>Indoor air quality in office buildings can impact the health, well-being, and productivity of occupants. In most buildings, occupants exhaled breath is the primary source of carbon dioxide (CO₂). Concentrations of indoor CO₂ are also strongly associated with the operational mode of the mechanical ventilation system. While CO2 is routinely monitored in indoor environments, there are few spatially-resolved real-time measurements of CO₂ throughout mechanical ventilation systems. Such measurements can provide insight into indoor- and outdoor-generated CO₂ dispersion throughout a building and between the building and the outdoor atmosphere. This thesis aims to investigate spatiotemporal variations in CO₂ concentrations and mass fluxes throughout a mechanical ventilation system of a living laboratory office in a LEED-certified building. The impact of human occupancy patterns and ventilation conditions of CO₂ concentrations and fluxes was evaluated. </p> <p>A four-month measurement campaign was conducted in one of the four living laboratory offices at the Ray W. Herrick Laboratories. The living laboratory offices feature precise control and monitoring of the mechanical ventilation system via an advanced building automation system. Various mechanical ventilation modes were implemented, such as variable outdoor air exchange rates (AERs) and recirculation ratios. A novel multi-location sampling manifold was used to measure CO₂ at eight locations throughout the ventilation system, such as across the outdoor, supply, and return air ducts. Office occupancy was measured via a chair-based temperature sensor array. Volumetric airflow rate data and CO₂ concentration data were used to estimate CO₂ mass fluxes through the ventilation system. The CO₂ mass flux for the outdoor and exhaust air was used to evaluate the net CO₂ transport from the office to the outdoor atmosphere. </p> <p>The measurements demonstrate that there exist significant spatiotemporal variations in CO₂ concentrations across the outdoor, supply, and return air ducts. CO₂ concentrations varied with human occupancy in the office and the outdoor AER of the mechanical ventilation system. Due to human-associated CO₂ emissions, the net CO₂ mass flux from the office to the outdoor environment was approximately 700 kg of CO₂ per year. Thus, occupied offices may represent an important, yet unrecognized, source of CO₂ to the urban atmosphere.</p>

The expanding urbanisation, growing population, and industrial development are threatening global surface water quality. With increasing concern about surface-water quality, it is crucial to deeply understand the evolution of surface-water quality problems and comprehensively de-termine its fundamental driving forces. In this Dissertation, systematic work on the mechanisms of water pollution with trace elements has been carried out in three steps: i) to identify the sources contributing to surface water pollution by receptor-based models, ii) to determine the factors dominating the pollution risk transmission from sources to surface water by a source-based model, and iii) to capture the primary driving forces to the spatiotemporal variation in surface water pollution by Bayesian-based approaches. The following specific topics were ad-dressed based on five publications: a) The temporal trends of trace metal pollution in the surface water were characterised by the Mann-Kendall test and the Generalised Additive Model. b) The primary source contributors to the long-term trace metal pollution in a river system were determined by the Self-organised Map, Positive Matrix Factorization receptor model, and Bayesian multivariate receptor model. The distributions of the source contributions to trace metal pollution were estimated. c) The risk transmission of trace pollutants in the surface water was estimated by a source-based dynamic model. The sensitivities of the risk to human activities, characteristics of wastewater treatment plants, and river flow regimes were evaluated. d) The contributions of hydro-chemical factors, climate impact, and sampling methods to water pollution and data uncertainty were analysed by the Wavelet Analysis and Bayesian Net-work. Both the models’ accuracy and robustness were evaluated by statistical analysis. The methods and results provided herein could improve the standard of statistical rigour and support the authorities’ decision-making.

This thesis analyzes the characteristics of flow pattern and vehicle-emitted pollutant dispersion in roughness surface layer. In an urban environment, wind flow and transported-pollutant source interfere strongly with buildings and other roughness elements on the surface ground, which results in complex characteristics of flow pattern and pollutant dispersion in 3D circumstances. The present study intends to simplify the research domain and investigate the fundamental modeling problems that exist in the field. The current physical research topic is restricted to 2D street canyon in equilibrium conditions. The study is motivated by the fact that characteristics of flow pattern and pollutant distribution inside street canyons are important for public health. The research has applied the computational fluid dynamics (CFD) methodology. To date, insights have typically focused on idealized street canyons without strictly limited boundary conditions and turbulence models. Those approaches face challenges related to their applicability to real urban scenarios or the reliability of prediction results. The thesis examines the influence of grid density, turbulence models and turbulent Schmidt number on pollutant distribution at windward and leeward surfaces of street canyon. Since numerical results usually are validated with wind-tunnel measurement data, the results between full-size model and wind-tunnel model are compared in order to test the Reynolds number effect. The lack of measurement data means that the morphometric method is used to generate upcoming wind profile, including the mean vertical velocity and turbulence parameters. The thesis also analyzes the potential errors brought by the method (Scenario A). Based on the evaluated numerical model, the thesis continues to study the impacts of surrounding buildings and geometry of street canyon on flow and pollutant distribution inside street canyons. The effect of wind on pollutant distribution inside street canyons was also investigated (Scenario A). Furthermore, the influence of roof shape and configuration of street canyon on characteristics of flow and pollutant distribution is also systematically studied, with the results shown in scenario B. The main conclusions of the thesis are that the uncertainty of numerical results derives from different aspects. Wind profile in the inlet profile generated by morphometric method brings major error to the simulation results. Current turbulence models cannot compromise the simulation results between flow field and pollutant distribution field. Ignored small-scale obstacles also need to be handled carefully. Numerical results revealed that flow and pollutant distribution inside street canyons are mainly dominated by the geometry of the street canyon itself. Medium-spaced surrounding buildings are also better able to transport pollutant out of the street canyon. Through systematic analysis, roof shape is proven to have a significant effect on flow and pollutant distribution inside a street canyon. The major impact is altered turbulence intensity depth and strength of shear layer inside the street canyon, which is important for pollutant removal process out of the street canyon. In the future, advanced turbulence models accompanied by small-obstacle effect models need to be developed in order to reliably simulate flow and pollutant dispersion simultaneously. Based on the advanced turbulence model, simulation of flow and pollutant dispersion in a complex 3D environment is essential in the next steps for the purpose of engineering application. Accurate vertical wind profile provided for inlet profile is another interesting direction for further development. Keywords: Flow; Pollutant dispersion; CFD; Street canyon; Reliability / <p>QC 20130215</p>