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Sols Pollués Par Les Métaux Lourds Résultant De L Université du Québec INRS Eau-Terre-Environnement Sols pollués par les métaux lourds résultant de l'enfouissement de déchets industriels (Montréal, Canada): Géochimie, spéciation des métaux, et décontamination par flottation Par Gérald Dermont Thèse présentée pour l'obtention du grade de Philosophiae Doctor (Ph. D.) en Sciences de la Terre et Environnement Jury d'évaluation Examinateur externe : Dr. Robert Hausler, Département du génie de la construction, École de Technologie Supérieure (Montréal) Examinateur externe : Dr. Catherine Mulligan, Département de génie du bâtiment et des génies civil et de l’environnement, Université Concordia (Montréal) Examinateur interne : Dr. Jean-François Blais, INRS-ETE Directeur de recherche : Dr. Mario Bergeron, INRS-ETE Codirecteur de recherche : Dr. Marc Richer Laflèche, INRS-ETE Codirecteur de recherche : Dr. Guy Mercier, INRS-ETE © droits réservés de Gérald Dermont, 2008 Résumé Les friches industrielles (brownfields) polluées par les métaux lourds sont des lieux potentiellement toxiques pour l’environnement. De plus, la présence de ces terrains contaminés en milieu urbain handicape largement l’aménagement du territoire. Dans la ville de Montréal, plus de 200 sites présentent une forte contamination métallique des sols. Dans le cadre de cette thèse, les travaux se focalisent sur un terrain situé à proximité du centre-ville de Montréal et affecté par des déchets minéralurgiques riches en métaux lourds. Le défi actuel est de promouvoir des solutions technologiques pour traiter les sols pollués plutôt que d’avoir recours à des techniques d’enfouissement. Une revue exhaustive de littérature permet de faire un état des lieux de la problématique des sols contaminés par les métaux et fournit l’éventail des techniques conventionnelles et innovatrices pour immobiliser ou extraire les métaux des sols. Le premier objectif de cette thèse est de déterminer la répartition spatiale des métaux dans plusieurs profils du sol afin d’évaluer leur potentiel de mobilisation dans l’environnement. Le second objectif est d’établir la spéciation et la répartition des métaux dans la phase solide du sol dans une perspective de lavage de sol. Enfin, le troisième objectif est de déterminer l’efficacité de l’enlèvement des métaux par flottation et d’évaluer les principaux paramètres (physiques et chimiques) influençant le processus de séparation. Le profil du sol est composé d’un horizon superficiel de remblais riches en déchets minéralurgiques reposant sur le sol naturel initial, lequel est composé d’un horizon organique (tourbe) et minéral calcaire (marne et sédiments lacustres). Dans l’horizon anthropique, les teneurs en As, Cd, Cu, Pb et Zn dépassent largement les critères génériques des sols établis par le Ministère du Développement durable, de l'Environnement et des Parcs du Québec (MDDEP, 1999). Les concentrations totales des métaux dans les horizons du sol naturel sont très souvent iii inférieures au niveau de fond géologique (critère A) établi par le MDDEP. Cependant, le calcul du facteur d’enrichissement des métaux révèle une forte « contamination » de l’horizon organique par rapport à l’horizon minéral. Cela suggère que la tourbe est contaminée par les métaux provenant d’une lixiviation potentielle des fragments de scories minéralurgiques. La distribution spatiale des contaminants dans l’horizon anthropique est très hétérogène. La concentration des métaux s’avère indépendante d’une composition géochimique particulière des échantillons de sol. Toute les fractions granulométriques étudiées sont affectées, et ce, même si les particules fines contiennent les plus hautes teneurs. L’étude micro-spectroscopique (microscope électronique à balayage couplé à un analyseur de rayons X par spectrométrie en énergie dispersive) d’environ 150 particules riches en métaux reflète une grande diversité de la spéciation des métaux en phase solide. La forme prédominante du Zn est la sphalérite (ZnS), tandis que le Cu et le Pb sont distribués dans un large panel de formes minéralogiques, particulièrement des oxydes/carbonates. La distribution du Cu, Pb et Zn est aussi évaluée selon la localisation de la phase métallique au sein de la particule (libérée, associée, incluse ou localisée à la surface). En outre, l’étude micro-spectroscopique montre que certaines particules auraient subi des altérations chimiques (weathering) importantes et que certaines phases riches en métaux seraient issues d’un processus de re-précipitation (par exemple des phases oxydes/hydroxydes riches en Cu, Pb et Zn sur la surface d’un grain de quartz). Ces observations consolident l’hypothèse de la contamination de l’horizon organique par une mobilisation des métaux dans le profil de sol provenant de l’altération lente des fragments des scories métallurgiques. Parmi les technologies éprouvées dans le traitement des minerais, la flottation est une alternative intéressante à explorer afin d’extraire les métaux des matrices environnementales. Le rôle de la flottation est de concentrer les particules riches en métal dans un plus petit volume de sol. Les expériences à l’échelle laboratoire ont permis de déterminer l’efficacité et les limites de iv cette technologie en intégrant les problématiques spécifiques aux sols à traiter. Le taux d’enlèvement des métaux, ainsi que la sélectivité de la séparation ont été évalués en fonction des paramètres opératoires liés à la technologie de flottation et de la distribution des métaux dans le sol (minéralogie et granulométrie). Le sol subit un prétraitement par broyage afin de traiter toutes les fractions fortement contaminées <10 mm et d’obtenir une granulométrie appropriée (<250 µm). L’influence des conditions chimiques (type et concentration d’agent collecteur, pH, prétraitement chimique, minéralogie) et des paramètres physiques (vitesse d’agitation, taille des particules, mode d’addition du collecteur, ultrasonication) a été évaluée dans le but de mieux comprendre les mécanismes de séparation des particules riches en métal. En général, la flottation a permis d’enlever suffisamment de métaux pour abaisser la concentration dans le sol résiduel du critère D au critère C. L’utilisation d’un agent tensioactif (collecteur) anionique, le KAX, a permis d’obtenir un bon compromis entre le taux d’enlèvement des métaux (42–52%) et la réduction de volume (>80%). L’utilisation d’un collecteur non ionique (le kérosène) a donné de meilleurs taux d’enlèvement, cependant la séparation est moins sélective. Deux mécanismes contribuent à l’enlèvement des particules riches en métaux : (1) le vrai mécanisme de flottation, basé sur la séparation sélective des particules hydrophobes; (2) l’entraînement mécanique des particules fines qui se fait indépendamment des propriétés des surfaces des particules. L’effet d’entraînement est responsable d’une grande part de l’enlèvement des métaux puisque les particules fines (<20 µm) contiennent une part importante de la contamination et que l’effet d’entraînement est significatif dans les cellules de flottation agitée. La sélectivité de la flottation est améliorée avec un temps de processus inférieur à 5 min et une addition en plusieurs étapes du collecteur. La sélectivité de la flottation est optimale pour la fraction particulaire intermédiaire (20–125 µm). v Remerciements Je désire remercier mon directeur de thèse, monsieur Mario Bergeron, qui a bien su me guider dans mes travaux, tout en me laissant la liberté d’explorer les voies qui me passionnent. Tous mes remerciements vont également à mes deux co-directeurs, messieurs Marc Richer- Laflèche et Guy Mercier, qui, par leurs précieux conseils et leur enthousiasme à partager leur savoir, m’ont supporté tout au long de mes recherches. Je souhaite également remercier les examinateurs qui ont gentiment accepté de participer à l’évaluation de cette thèse, madame Catherine Mulligan et messieurs Robert Hausler et Jean- François Blais. Au fil des ans, j’ai pu m’inspirer de leurs nombreux travaux afin d’approfondir mes recherches et d’élargir mes horizons. Je les remercie grandement pour l’intérêt porté à mes recherches. De plus, cette thèse aurait été impossible à réaliser sans le soutien financier de l’Institut national de recherche scientifique Eau Terre et Environnement (INRS-ETE), ainsi que le support technique, administratif et matériel des techniciens qui y travaillent. Je les remercie sincèrement. Je remercie également monsieur Bruno Boussicault pour son expertise en géophysique. Je tiens à remercier chaleureusement mes collègues doctorants: Belkacem, Loubna, Edgar, Satinder, Kokou, Amélie, Vladimir, Jorge, Mathieu…Je tiens finalement à offrir mes derniers remerciements à monsieur Angus Calderhead pour ses commentaires pertinents et ses suggestions fort enrichissantes, ainsi qu’à ma famille, mes amis, et ma compagne, Kathrine, pour leur affection et leurs encouragements constants. vii Avant-propos L’ensemble de cette thèse se focalise sur la décontamination des sols pollués par les métaux. Le document suivant s’articule en deux parties distinctes. La première partie (Chapitre 1) permet de faire le point sur la contribution des travaux et des publications dans le domaine du traitement des sols contaminés par les métaux. Elle comprend également des informations complémentaires aux écrits de la partie suivante. La deuxième partie (Chapitres 2 à 7) présente six articles publiés, acceptés ou sur le point d’être soumis à des revues scientifiques avec comité de lecture. Plus précisément, les trois premiers articles offrent un état des lieux de la problématique
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