[Truncated abstract] To date, many subsurface contaminant modelling studies have focused on increasing model complexity and measurement requirements to improve model accuracy and widen model application. However, due to the highly complex and heterogeneous nature of flow in the subsurface, the greater benefit in model development may lie in decreasing complexity by identifying key processes and parameters, simplifying the relationships that exist between them, and incorporating these relationships into simple models that recognise or quantify the inherent complexity and uncertainty. To address this need, this study aims to identify and isolate the key processes and parameters that control dense nonaqueous phase liquid (DNAPL) and aqueous phase migration through single, onedimensional fractures. This is a theoretical representation which allows the study of processes through conceptual and mathematical models. Fracture systems typically consist of multiple two-dimensional fractures in a three-dimensional network; however, these systems are computationally and conceptually demanding to investigate and were outside of the scope of this study. This work initially focuses on DNAPL migration in single, one-dimensional fractures. The similitude techniques of dimensional and inspectional analysis are performed to simplify the system and to develop breakthrough time scale factors. This approach relies heavily on the limitations of the equation used for the analysis and on the difficulty in representing variable aperture scenarios. The complexity of the conceptual model is then increased by embedding the fracture in a two-dimensional, porous matrix. ... These tools can be readily applied by the field investigator or computer modeller to make order-of-magnitude estimates of breakthrough times, reduce or target measurement requirements, and lessen the need to employ numerical multiphase flow models. To determine the implications of the results found in the one-dimensional studies to applications at the field scale, the complexity of the conceptual model was increased to a single, two-dimensional, planar fracture embedded in a three-dimensional porous matrix. The focus of this study was not DNAPL breakthrough times but the relative importance and interaction of different mass transport processes and parameters on plume migration and evolution. Observations clearly show that estimates of the size, location and concentration of the plume is highly dependent on the geologic media, the temporal and spatial location and resolution of measurements, and on the history, mass and location of the DNAPL source. In addition, the processes controlling mass transport (especially matrix diffusion and back diffusion) act in combination at the field scale in ways not always expected from an analysis of processes acting individually at smaller spatial and temporal scales. Serious concerns over the application of the common '1% Rule of Thumb' to predict DNAPL presence and the use of remediation efforts that rely largely on natural attenuation are raised. These findings have major implications for the field worker and computer modeller, and any characterisation, monitoring or remediation program development needs to be sensitive to these findings.

Submitted by Marco Antonio Oliveira da Silva (maosilva@ipen.br) on 2016-08-26T11:02:10Z No. of bitstreams: 0 / Made available in DSpace on 2016-08-26T11:02:10Z (GMT). No. of bitstreams: 0 / As áreas contaminadas por NAPL (Non-Aqueous Phase-Liquids ou fase líquida não aquosa ou ainda fase livre) podem causar riscos à saúde humana e aos ecossistemas, restrições para o desenvolvimento urbano e diminuição do valor imobiliário das propriedades. Este trabalho utilizou o gás radônio como um indicador para a análise de gás subsuperficial do solo, uma vez que este gás nobre apresenta boa solubilidade em uma ampla gama de NAPL, sendo parcialmente retido na contaminação NAPL. Portanto, uma diminuição da atividade de gás radônio no solo contaminado pode ser esperada, devido à elevada capacidade de particionamento do radônio em NAPL, o que permite que o NAPL retenha uma parte do radônio anteriormente disponível nos poros do solo. O levantamento foi realizado em uma indústria abandonada, contaminada por NAPL pouco volátil, localizada na zona sudeste da cidade de São Paulo, entre junho de 2014 e maio de 2015. A concentração de radônio foi avaliada pela metodologia de detecção passiva com detectores sólidos de traços nucleares (SSNTD) tipo CR-39 em dez estações de monitoramento instaladas na área contaminada investigada e nomeadas de A até J. A média das concentrações de atividade de radônio para as oito estações de monitoramento em locais supostamente não contaminados variou de (22 ± 4) kBq.m-3 a (39 ± 4) kBq.m-3. Para as duas estações de monitoramento supostas como locais contaminados, as concentrações de radônio foram (1,4 ± 0,4) kBq.m-3 e (13 ± 9) kBq.m-3. Os resultados demonstraram que o método utilizado foi consistente com as técnicas convencionais de investigação ambiental para a maioria das estações de monitoramento em diferentes estações do ano. Resultados obtidos com CR-39 variam ao longo dos períodos de exposição, devido à sazonalidade. Não foi observada relação entre as oscilações das concentrações de atividade de radônio e o volume de chuva acumulada nos diferentes períodos de exposição dos detectores CR-39. As menores concentrações de atividade do 222Rn ocorreram nas estações de monitoramento G e H e verificou-se por espectrometria gama, que a baixa atividade não está relacionada à concentração de atividade de seu pai 226Ra na série do decaimento radioativo do 238U, reforçando a teoria de retenção do gás radônio nos locais contaminados por NAPL. Resultados da etapa de remediação comprovaram que a técnica utilizada neste trabalho foi mais eficiente que as técnicas convencionais de investigação ambiental, especialmente para as estações de monitoramento D e G na área contaminada investigada. / Dissertação (Mestrado em Tecnologia Nuclear) / IPEN/D / Instituto de Pesquisas Energéticas e Nucleares - IPEN-CNEN/SP

The method of using stimulated reductive dechlorination when remediating sites contaminated with chlorinated solvents is not unusual, but not many studies have been done on the overall process outside of a controlled environment. In order to investigate the process, principal component analysis (PCA) and partial least square (PLS) regression was used to identify the most important parameters for the degradation of the chlorinated solvents. The most important parameter for all chlorinated compounds turned out to be oxygen, with levels of degradation products increasing with decreasing levels of dissolved oxygen. Dissolved oxygen was deemed the most important variable to measure during a control program on the site. The degradation dynamics of the process were investigated to examine the behaviour of the chlorinated solvents and their degradation products. The degradation products of the main contaminant TCE were found in all observation points, which indicates an ongoing reductive dechlorination all over the site. A large amount of the mother product, TCE, was found in two observation points, which were believed to be situated close to the sources of the TCE contamination. Over the observation period of 2,5 years the levels of TCE in the source areas decreased significantly to below the remediation goal. However, the levels of TCE increased in another observation point further downstream, with concentrations still increasing at the end of this study. The levels in this point were lower than those measured initially in the source area, but still much higher than the accepted values. Possible reasons for this appearance of TCE could be an isolated sheet of contaminants being pushed into the observation point from a nearby location or transport of the contaminants from the source area in units of higher conductivity such as sand lenses or fractures in the clayey soil. / Att använda stimulerad reduktiv deklorering som metod för att sanera fastigheter förorenade med klorerade lösningsmedel är inte ovanligt, men få studier har undersökt det övergripande saneringsförloppet utanför de kontrollerade förhållanden i en labbmiljö. För att undersöka nedbrytningsprocessen användes principalkomponentsanalys (PCA) och partial least square (PLS) regression i syfte att identifiera de parametrar som hade störst påverkan på nedbrytningen av de klorerade föroreningarna. Den enskilt viktigaste parametern visade sig vara halten löst syre i grundvattnet, då halterna av nedbrytningsprodukter ökade med minskande syrehalt. Därför ses syre som den viktigaste parametern för att följa förloppet och är den parameter som bör mätas i kontrollprogram över nedbrytningsprocessen.   Nedbrytningsdynamiken analyserades under en observationsperiod på 2,5 år för att studera hur de klorerade föroreningarna betedde sig under nedbrytningsförloppet. Nedbrytningsprodukter hittades i provtagningspunkter över hela fastigheten vilket visar på en pågående reduktiv deklorering. En stor mängd av moderprodukten TCE hittades i två punkter som bedömdes vara källor till TCE-spridningen. Under observationsperioden sjönk halterna av TCE i dessa två punkter till under gränsen för åtgärdsmålet, dock ökade koncentrationen av TCE i en annan provpunkt längre nedströms källområdet. Halterna i provpunkten var inte lika höga som de initiala halterna i källområdet, men de var långt högre än det fastställda åtgärdsmålen och ökade fortfarande när undersökningen avslutades. Möjliga förklaringar till varför halterna ökade i denna provpunkt är att ett sjok av TCE från omkringliggande sediment har transporterats till provpunkten, eller att en föroreningstransport har skett från källområdet via områden med högre konduktivitet i till exempel sandlinser eller sprickor.

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