Le sol est une ressource non renouvelable à conserver en raison de son importance socio-économique et environnementale. Mais, les activités (bio)industrielles peuvent le dégrader et entraîner l'apparition de friches à pollutions persistantes. La capacité de Miscanthus x giganteus à s'adapter aux sols de friches pollués en éléments traces métalliques (ETM), tout en favorisant la consolidation des processus de bioremédiation des polluants, sans entraîner d'impact négatif sur l'environnement, est étudiée. Des terrains lorrains, très impactés par l'activité industrielle passée, sont utilisés. Considérant la complexité des relations sol-plante-microorganismes, différents outils d'évaluation complémentaires (i.e. in vitro, en mésocosme et sur le terrain) sont employés afin de déterminer la réponse de chaque composante et de leurs interactions et ainsi déduire la durabilité de la méthode. La culture de M. x giganteus a un potentiel pour la réhabilitation des sols de friche à pollutions multimétalliques ou mixtes (+HAP), avec un double bénéfice : la phytostabilisation des ETM au niveau racinaire et la production d'une biomasse aérienne revalorisable (transfert limité des ETM). La plante n'altère pas les caractéristiques du sol qui participent à la mobilité des ETM (pH, CEC) ; les variations de celles liées à la fertilité du sol, de la toxicité (fraction liquide) et de l'accumulation des ETM par d'autres organismes, attestent de l'interaction avec le milieu qui rendrait les éléments plus disponibles. L'activité végétale est à l'origine des associations avec les bactéries du sol, où les phylotypes potentiellement métallorésistants (Zn, Cr) semblent communs aux sols utilisés / Soil is a nonrenewable resource to maintain because of its socio-economic and environmental importance. However, (bio)industrial activities can degrade soil and cause the appearance of persistent pollution brownfields. The ability of Miscanthus x giganteus to adapt to brownfield soils polluted with heavy metals (HM), while promoting the consolidation process of bioremediation of polluants, without causing a negative impact on the environment, is studied. Soils from Lorraine region (France), very affected by past industrial activity, are used. Considering the complexity of soil-plant-microorganisms relationships, various complementary assessment tools (i.e. in vitro,mesocosm and field) are used to determine the response of each component and their interactions, and thus deduce the sustainability of the method. The culture of M. x giganteus has great potential for rehabilitation of brownfield soils having a multimetallic pollution or mixed (+PAH) with a double benefit: phytostabilisation of HM at the root level and the production of biomass reclaimable (limited transfer of HM). The plant does not alter the characteristics of the soil involved in the mobility of HM (pH, CEC) ; but changes from those related to soil fertility, toxicity (liquid fraction) and the accumulation of HM by other organisms attest to the interaction of the plant with the elements that would make them more available. Plant's activity is causing associations with soil bacteria, for which the phylopes potentially métalloresistants (Zn, Cr) seem common in soils used

Local weather data (wind direction, wind speed and temperature) from meteorological stations and daily synoptic data have been examined in relation to airborne particulate material (PM10) concentrations recorded at 17 pollution monitoring sites throughout Kent for the period 2000 to 2008, as an aid to understanding dispersal patterns in relation to topography. In general, local and synoptic wind direction patterns followed the same trends: the yearly distribution is dominated by southwesterly winds, followed by winds from the west and the northwest. Detailed analysis of local wind patterns at four sites (two coastal and two inland) strongly suggested the presence of seas breezes, reaching maximum frequency between March and August and fewest occurrences between November and February. Transport of PM10 over 30 km inland was also inferred. In addition to local wind transport, the location of the pollution monitoring sites and their environment are key to explaining the differences in PM10 concentrations recorded between the sites. The 10 sites located on roadsides registered the highest number of particle counts, followed by the five sites located within urban areas. The lowest amount of particles was found at the two rural sites. The five roadside sites closest to London (two in Gravesham and three in Dartford) exceeded the daily recommended amount of 50 μg/m3 several times each month, probably reflecting the increased road traffic in those areas. Aside from the variation in PM10 amount between sites, seasonal differences were also observed, with the lowest amount of PM10 recorded in the autumn and the highest in spring. Episodes of pollution affecting the whole of Kent were also observed. These were more clearly related to the synoptic situation rather than any local wind variations and appear to indicate regional or trans-boundary pollution transport. The latter is also supported by preliminary evidence from a PM10 trap sampling at a site on the south coast.

A methodology for the thermodynamic-kinetic evaluation of circulating systems as TSA carbon capture processes is developed and used in the assessment of a novel CFB configuration against a benchmark (co-current riser). The novel CFB features a counter-current adsorber, a counter-current regenerator and a riser, the latter element playing a double role of solids conveyer and co-current adsorber. The advantages sought by using a counter-current adsorber are not only the more efficient gas-solid contact mode with respect co-current, but also a low pressure drop derived from operation at lower gas velocities and hydrostatic head partially supported on the contactor internals. Knowledge of the adsorption equilibrium alone is sufficient to realise the much higher sorbent circulation rates required by co-current configurations –compared to counter-current– to meet the stringent carbon capture specifications of 90% recovery and 95% purity. Higher solids circulation rates imply higher energy requirements for regeneration, and therefore research and development of co-current gas-solid contactors cannot be justified in terms of searching for energy-efficient post-combustion carbon capture processes. Parallel experimental investigation in the operation and fluid dynamics of cold model CFB rigs is carried out with the purposes of: 1) providing information that may impact the process performance and can be fed into the mathematical model used in the theoretical assessment for more realistic evaluation, and 2) determine gas and solids residence time distributions (RTDs), which are used for the estimation of axial dispersion and comparison with published results in similar systems. Gas RTD data is generated using a tracer pulse injection-detection technique, whereas RTD for the solid phase is studied using positron emission particle tracking (PEPT). The PEPT technique proved to be adequate for the identification of flow regimes in the novel design of the counter-current adsorber, featuring inclined orifice trays. At low gas velocities the particles flow straight down through the tray holes, whereas at higher velocities the particles flow down in zig-zag, increasing the residence time of the particles and reducing the particle axial dispersion, both beneficial in terms of separation efficiency.

Polycyclic aromatic hydrocarbons (PAH) are ubiquitous compounds produced through incomplete combustion processes from various sources in different proportions. They are of concern because of their recognized mutagenic and carcinogenic properties. There are a number of receptor modelling (RM) studies that identify sources of urban atmospheric PAH, despite concerns over the application of RM to the relatively reactive PAH. This thesis utilizes Positive Matrix Factorization (PMF) with extensive PAH datasets, and compares the results with local and national emission inventories. An atmospheric chemical reactivity study for PAH is also investigated; highlighting the importance of taking reactivity into consideration when applying source apportionment models. The results demonstrate that traffic sources are significantly responsible for the PAH mass (∑PAH) at UK urban sites throughout the year. A substantial fraction of benzo[a]pyrene emissions was apportioned to solid fossil fuel combustion sources, showing significant seasonal variations. A conceptual simulation of PAH ratios has been investigated using urban and rural data. Results were in good agreement between simulated ratios and empirically obtained values. The results provide a better understanding of PAH reactivity and their atmospheric fate, indicating the potential for long-range transport of high molecular weight PAH.

BNFL Sellafield has been authorised to discharge radionuclides to the Irish Sea since 1952. In the aquatic environment the radionuclides are adsorbed by sediments and are thus redistributed by sediment transport mechanisms. This sediment is known to accumulate in the estuaries of the Irish Sea. BNFL Springfields is also licensed to discharge isotopically different radionuclides directly to the Ribble estuary. Thus there is a need to understand the sediment dynamics of the Ribble estuary in order to understand the fate of these radionuclides within the Ribble estuary. Estuaries are highly dynamic environments that are difficult to monitor using the conventional sampling techniques. However, remote sensing provides a potentially powerful tool for monitoring the hydrodynamics of the estuarine environment by providing data that are both spatially and temporally representative. This research develops a methodology for mapping suspended sediment concentration (SSC) in the Ribble estuary using airborne remote sensing. The first hypothesis, that there is a relationship between SSC and l37Cs concentration is proven in-situ (R2=O.94), thus remotely sensed SSC can act as a surrogate for \37Cs concentration. Initial in-situ characterisation of the suspended sediments was investigated to identify spatial and temporal variability in grain size distributions and reflectance characteristics for the Ribble estuary. Laboratory experiments were then perfonned to clearly define the SSC reflectance relationship, identify the optimum CASI wavelengths for quantifying SSC and to demonstrate the effects on reflectance of the environmental variables of salinity and clay content. Images were corrected for variation in solar elevation and angle to give a ground truth calibration for SSC, with an R2=O.76. The remaining scatter in this relationship was attributed to the differences in spatial and temporal representation between sampling techniques and remote sensing. The second hypothesis assumes that a series of images over a flood tide can be animated to provide infonnation on the hydrodynamic regime, erosion, and deposition. Spatial and temporal data demonstrated the complex controls on sediment transport. The data also showed the importance of microphytobenthos in the stabilisation of intertidal sediments, highlighting their importance in defining sources and sinks of radionuclides in intertidal areas. Water volume data from the VERSE model were combined with SSC from the imagery to calculate the total sediment in suspension for each flight line. This provided the figures used to detennine total erosion and deposition, which were then used to derive net suspended sediment and l37Cs influxes of 2.01xl06kg and 604MBq per flood tide.

No description available.

The estimated global production of red mud, a by-product of alumina production, is ~120 million t per year. Little is known about the long-term chemical, physical and ecological responses in aquatic ecosystems following pollution with red mud. To date, no whole-lake assessment of the impact of red mud and recovery trajectories has been conducted. Kinghorn Loch, Fife, Scotland, is an important example of a red mud polluted aquatic ecosystem. This is due mainly to the availability of long-term data documenting changes in the lake during the pollution and recovery following diversion of red mud leachate in 1983 to date. Long-term data were assessed to determine the time scale of recovery for a range of specific pollutants in the surface waters of Kinghorn Loch, and field surveys and a laboratory controlled experiment were conducted to investigate lake sediment-pollutant interactions and arsenic (As) species bioaccumulation in aquatic plants. Results showed recovery of the lake water column, with a significant decrease of pH and the concentrations of all red mud constituents in surface water since the cessation of pollution. Using generalised additive models the chemical recovery period was 5 years for pH and from 22 to 26 years for As, vanadium (V) and phosphorus (P), with aluminium (Al) still not reaching the end-point recovery following this period. A 12- month field survey showed that concentrations of phosphate (PO4-P), total phosphorus (TP), dissolved and total As and V in lake water varied significantly throughout the year, with depth of overlying water contributing to variation in P concentrations in water above sediment. A range of physico-chemical factors, including dissolved oxygen (DO), pH and concentrations of pollutant binding element controlled seasonal and spatial variations in water column contaminant concentrations. The behaviour of V differed from As and P concentrations in water, with maximum V concentrations occurring in spring and the highest concentrations of As and P in surface water and dissolved As and PO4-P in water above sediment observed in summer. With the exception of V in deeper layers of the water column in spring and winter, observed total As and V concentrations met standards for Protection of Aquatic Life in the UK (50 and 20 μg L-1, respectively). Sediment in Kinghorn Loch is still contaminated 30 years into the lake recovery period. The highest seasonal mean concentrations in the upper (0-4 cm) sediment layer were 231 mg kg-1 for V and 185 mg kg-1 for As, the latter considerably exceeding Canadian Sediment Quality Guidelines for the Protection of Aquatic Life for As (17 mg kg-1). Evidence from the laboratory experiment and the field observations suggests that the lake still processes red mud contaminants, with seasonal mobilisation of As and P from lake sediment under reducing conditions. In contrast, release of V from sediment into overlying water appeared not to be driven predominantly by redox conditions, but instead by interactions between pH, competitive ion concentrations and DO. Higher pollutant concentrations observed throughout the year in deeper layers of the water column compared to surface water indicated that the impact of sediment on the water column is generally confined to the bottom waters of the lake. Macrophytes in Kinghorn Loch contained relatively high concentrations of As, predominantly in the inorganic form which is most toxic to organisms. The highest As content measured in roots of Persicaria amphibia (L.) Gray (40.4 – 218 mg kg-1) greatly exceeded the 3 – 10 mg kg-1 range suggested as a potential phytotoxic level. Accumulation of toxic As species by plants suggested toxicological risk to higher organisms in the food web and indicated that ecological recovery of the lake is still in progress. The results of this research at Kinghorn Loch will help water resource managers to understand not only the environmental and human health effects of multiple pressures related to red mud pollution, but also the likely recovery time scales in relation to water quality targets.

Low level nuclear waste arising from UK nuclear sites, research establishments, hospitals and industry is currently disposed of at the Drigg Disposal Facility in Cumbria. Waste is packed into steel canisters before being compacted and grouted into larger steel storage containers. The aqueous chemistry of wastes, especially radionuclides, in the presence of grout material is of major interest. The gout used at the Drigg site is a mixture of Ordinary Portland Cement and Pulverised Fly Ash additive, from which ingressing water will leach high levels of calcium, sodium and potassium and produce waters of a high pH. Aerobic environments are expected to dominate over the early period of the vault life, after which the combined effect of canister corrosion and microbial activity will lead to anaerobic conditions. After a much longer period (100,000 years) anaerobic conditions may cease and yield once again an aerobic environment where migration of radionuclides may be sorption-controlled rather than on hydroxide precipitation at high pH. Work has been performed under both aerobic and anaerobic conditions to study uranium solubility in the presence of complexing ligands that may be present in the waters of the nearfield of a low-level waste disposal vault. Eleven ligands have been investigated: carbonate, phosphate, chloride, sulphate, acetate, citrate, EDTA, NTA and organic matter- humic acid, fulvic acid and iso-sacchannic acid. Anaerobic conditions were achieved by two different procedures; the first used ferrous ions in hydroxide solution and the second used dithionite in hydroxide solution. Both methods produce reducing electrode potentials and high pH. Computer software has been used to model experimental results, thereby predicting uranium solubilities and speciation, and to propose new formation constants to fit the experimental results more closely. Studies have also been perforined to measure uranium sorption by grout material at high pH in the presence of the above ligands. This work makes a significant contribution to the understanding of uranium solubility and speciation in waters. at high pH and under conditions relevant to low level nuclear waste disposal.

Of the various dissolved species contained in the effluents from the mining and milling of uranium ores, the one which is of particular concern for environmental protection is Radium-226. The literature shows that, in recent years, considerable efforts have been made to develop treatment systems that can achieve the stricter effluent discharge standards imposed by the regulatory bodies. There has also been a concern to treat the already existent sludges from previous treatments. The main priority is to limit, as much as possible, the arising of sludge from future treatment systems. The most common treatment used is the addition of lime and limestone to raise the pH followed by barium chloride to form a very finely divided Ba(Ra)S04 precipitate which is then settled in large ponds or basins. In spite of the high decontamination factors obtained with this technique, these may not be satisfactory in terms of environmental protection. In addition, the industry is increasingly aware of the economical benefits resulting from treatment processes that allow water reuse to the process.

Adsorption in porous materials is a promising technology for CO2 capture and storage. Particularly important applications are adsorption separation of streams associated with the fossil fuel power plants operation, as well as natural gas sweetening. High surface area activated carbons are a promising family of materials for these applications, especially in the high pressure regimes. As the streams under consideration are generally multi-component mixtures, development and optimization of adsorption processes for their separation would substantially benefit from predictive simulation models. In this project we combine experimental data and molecular simulations to systematically develop a model for a high surface area carbon material, taking activated carbon Maxsorb MSC-30 as a reference. Our study starts from the application of the well-established slit pore model, and then evolves through the development of a more realistic model, based on a random packing of small graphitic fragments. In the construction of the model, we introduce a number of constraints, such as the value of the accessible surface area, concentration of the surface groups and pore volume, to bring the properties of the model structure close to the reference porous material. Once a plausible model is developed, its properties are further tuned through comparison between simulated and experimental results for carbon dioxide and methane. The model is then validated by predictions for the same species at different conditions and by prediction of other species involved in the carbon capture processes. The model is applied to simulate the separations involved in pre and post combustion capture processes and sweetening of sour natural gas, using realistic conditions and compositions for the multicomponent mixtures. Finally, it is used to explore the effect of water in pre and post combustion separations.