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International audience; Centre de Congrès de Lyon 99ème congrès de l'Astee-2020 La modélisation géochimique comme outil d'aide à la décision pour les gestionnaires.

In water treatment systems described as "nature-based solutions" the retention of suspended solids can lead to the formation of a surface deposit layer. Both from the point of view of its capacity to interact with the pollutants during its presence on the treatment unit, and during its reuse, notably in land application after curing, pollutants speciation within the deposits and their prossess of remobilization are questioned. The objectives of this work was to better describe the organo-mineral assemblage of these deposits and to provide a better understanding of the influence of colloidal phases on the remobilization of major and trace elements in order to be able to provide predictive models on the remobilization of pollutants from deposits subjected to pH variations. A vertical flow constructed wetland sludge deposit was subjected to different pH conditions and the colloidal phases were studied. Remobilization of organic colloidal phases was found to be particularly sensitive to pH changes. In the acidic pH range, small organic molecules (< 3 kDa) are predominantly remobilized from the deposits. For near-neutral and alkaline pH, large organic colloids (>30 kDa) prevail in solution. This release of organic matter seems to favor the remobilization of iron and aluminum oxides within organo-mineral colloids. The nature and quantity of the remobilized colloidal phases have a large influence on the release of major and trace elements from the constructed wetland’s sludge deposits. However, the affinity of the elements for these colloidal phases is also controlled by the chemical class of the element considered, its oxidation state and the pH of the solution. The use of these experimental data allowed the development and calibration of a multi-surface geochemical model able to reproduce the release and speciation of a wide range of elements (Fe, Al, P, Ca, Mg, Cu, Cd, Cr, Zn, Pb, As) retained within a reed filter sludge. Due to the high concentration of organic matter measured in the sludge and their importance in the release and speciation of elements, the modeling of metal complexation on organic matter by WHAM-ModelVII has been the subject of numerous experiments. The modeling tests combined with the ultrafiltration results allowed to obtain a ratio of active organic matter allowing to improve the prediction of the elemental concentrations. In order to evaluate the robustness of the methodology used on this first sludge, the modeling strategy was applied to other samples. The multisurface models developed in this thesis have all shown their efficiency in calculating the release of many elements whatever the pH conditions and despite very variable initial constitutions. The information provided by this thesis have been fundamental in understanding the risks associated with the emission of trace metals in particular. In time these models could therefore be part of the decision supporting tools available to managers of these solid deposits., Dans les systèmes de traitement des eaux qualifiés de « solutions fondées sur la nature » la rétention des particules en suspensions peut conduire à la formation d’une couche de dépôts de surface. Tant du point de vue de sa capacité à interagir avec les polluants lors de sa présence sur l’unité de traitement, que lors de sa réutilisation notamment en épandage après curage, la spéciation des éléments au sein de ces dépôts et les mécanismes de remobilisation des polluants interrogent. Ce travail avait pour objectifs de mieux décrire l’assemblage organo-minéral de ces matrices et de fournir une meilleure compréhension de l’influence des phases colloïdales sur la remobilisation d’éléments majeurs et traces afin de pouvoir fournir des modèles de prédictions sur la remobilisation de polluants des dépôts soumis à des variations de pH. Un dépôt de surface de filtre planté de roseaux à écoulement vertical a été soumis à différentes conditions de pH et les phases colloïdales ont été étudiées. La remobilisation de phases colloïdales organiques s’est montrée particulièrement sensible aux variations de pH. Dans la gamme de pH acide, de petites molécules organiques (< 3 kDa) sont majoritairement remobilisées des dépôts. Pour des pH proches de la neutralité et alcalins, les gros colloïdes organiques (> 30 kDa) prévalent en solutions. Ce relargage de matière organique semble favoriser la remobilisation d’oxydes de fer et d’aluminium au sein de colloïdes organo-minéraux. La nature et la quantité des phases colloïdales remobilisées exercent une large influence sur le relargage d’éléments majeurs et traces depuis les dépôts de filtre planté de roseaux. Cependant, l’affinité des éléments pour ces phases colloïdales est aussi contrôlée par la classe chimique de l’élément considéré, son état d’oxydation ainsi que le pH de la solution. L’utilisation de ces données expérimentales a permis le développement et la calibration d’un modèle géochimique multi-surfacique capable de reproduire la spéciation d’une large gamme d’éléments (Fe, Al, P, Ca, Mg, Cu, Cd, Cr, Zn, Pb, As) contenue au sein d’une boue de filtre planté et ainsi de reproduire le relargage de ces éléments. De par la concentration importante en matière organique mesurée dans la boue et leur importance dans le relargage et la spéciation des éléments, la modélisation de la complexation des métaux sur la matière organique par WHAM-ModelVII a fait l’objet d’un développement particulier. Afin d’évaluer la robustesse de la méthodologie employée sur cette première boue, la stratégie de modélisation a été appliquée à d’autres échantillons. Les modèles multisurfaciques développés dans cette thèse ont tous montré leur efficacité à calculer le relargage de nombreux éléments quel que soit les conditions de pH et malgré des concentrations initiales en élément majeurs et traces très variables.

International audience; Vertical flow constructed wetlands (VFCW) are worldwideused ecological technologiesdesigned to treat wastewaters. During theiroperating time, asludge layer is formed at the surface of the first-stage filters by the retention of wastewater’s suspended solids. The depositconstituting this layer is now known to accumulate and degrade a large variety of contaminants during regular conditions of operation. The resilience and potential release of thesecontaminantsduring varying operational conditionsis therefore ofmajor concern.When the sludge deposit is subject to water flows, elements can be released underdissolved form or associated to colloidal carrier phases.This study investigated the influence of pH variations on the speciation andtransport of toxic metals and major elements bound to VFCW surface sludge deposits. The acid/base neutralisation capacity (environmental assessment procedure ANC/BNC) (according to CEN/TS 14429) was carried out to assess the release at different pHvalues. Samples of sludge deposits were put in contactwith solutions in a wide pH range;the suspensions were filtered through 0.45 μm acetate cellulose filters an were subsequently analyzed. In addition, the suspensions were also treated by ultrafiltration using successively membranes of decreasing pore size (30 kDa, 10 kDa and 3 kDa). The permeates were analyzed for major and trace elements and organic molecules. Depending on their affinity with the organic and/or mineral colloidal carrier phasesand the different pH conditions,three groups of elements were defined:(i) As, P, B, V, Na, Kweremostly present in solutions as free species, (ii) Co, Cu, Ni, Cd, Znwerepartially affected by colloidal transport and (iii)Cr, Ba, Mn, Ca, Li, Mg, Srwerestrongly affected by colloidal co-transport. Accompanied by geochemical modelling tools, these results provide important informationon the speciation of released pollutants. The quantity of released pollutants, their mobility and potential toxicity help to define critical pH ranges that shouldnot be exceeded in order to limit the impact of pollutant releaseon the environment

International audience

International audience

International audience

International audience

Online conference due to the COVID-19 pandemic; International audience

International audience