ABSTRACT
In densely populated urban areas, the pressure on water resources is considerable and will tend to intensify over the next decades. Preserving water resources therefore seems fundamental, but many questions remain as to the transfer of contaminants to subsurface waters in these largely sealed areas. Because of their toxicity and persistence in the environment, this work focused on the study of polycyclic aromatic hydrocarbons (PAHs), ubiquitous pollutants mainly produced by human activities. To better understand the main factors leading to the retention or transport of these pollutants in urban environments, vertical transects, from the surface to several meters down, were established on three study sites in or near Paris (France), selected according to an urbanization gradient. Soil samples collected at the surface and urban secondary carbonate deposits (USCD), similar to cave speleothems, sampled underground in quarries and aqueducts were analyzed. As the hydrophobic properties of PAHs favor their sorption onto organic matter, the latter was also studied using organic carbon analysis and UV fluorescence spectroscopy. The USCD located closest to the urbanized surface contained high concentrations of PAHs (76.8 ± 5.3 ng g-1), while the USCD located at greater depth with organic soil on the surface contained the lowest amount of PAHs (2.9 ± 0.4 ng g-1), and no PAHs with log KOC > 5. The results highlight the predominant role played by the presence of organic topsoil at the surface in retaining and storing large amounts of PAHs (1914-2595 ng. gsoil-1), particularly the most hydrophobic ones (i.e. 60% of the 15 PAHs are characterized by a Log KOC >5), which are also the most toxic. The lithology and thickness of the bedrock (between the surface and the USCD) also play an important role in the retention of PAHs, particularly those adsorbed on the particulate phase.
ABSTRACT
Preserving water resources and limiting pollution are central environmental issues in the current context of intense anthropization. Among organic pollutants, polycyclic aromatic hydrocarbons (PAHs) are commonly analysed as part of water quality assessments. After being emitted into the atmosphere, these persistent organic pollutants are deposited on the continental surface, where they are transported to the aquatic environment by run-off and infiltration waters. Mainly due to anthropogenic emissions, PAHs can therefore be considered as a proxy for human activities. Urban secondary carbonate deposits (USCDs), similar to cave speleothems, have recently been studied for their potential as natural archives of water quality. However, USCDs have never been used to trace water organic pollution and only a few studies on PAHs in speleothems are available. This study focuses on a well-dated USCD covering the last 300 years from the Great Aqueduct of Belleville (north-east of Paris, France). The aim is to determine the nature and variation of trapped organic compounds over time and to discuss their origin, transport, and link with changes in soil occupation due to human activities. To do so, high-resolution solid-phase UV fluorescence imaging analyses were combined with chemical analyses of PAHs and organic carbon carried out on low-weight samples. The results show that PAHs have been present in urban surface water for 300 years. Over the last few decades, a 7-fold increase is observed, accompanied by a change in the pollution source, enriched in high-molecular-weight PAHs, probably linked to urban dust. This study also reveals modes of transport directly influenced by changes in the soil occupation that are very different from those usually encountered in natural environments. This work thus paves the way for a better long-term understanding of the impact of human activity on the transfer of pollutants to sub-surface waters.
