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Feifei CAO Approche Interdisciplinaire Pour La Caractérisation Hydrogéologique Du Milieu Crayeux : Application Au Transfert De

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Feifei CAO Approche Interdisciplinaire Pour La Caractérisation Hydrogéologique Du Milieu Crayeux : Application Au Transfert De Ecole doctorale ABIES GEGENAA Université de Reims Champagne-Ardenne Thèse présentée et soutenue publiquement par Feifei CAO Le 5 Mars 2020 En vue de l’obtention du grade de Docteur de l’Université de Reims Champagne-Ardenne Discipline : Géochimie de l'Environnement Approche interdisciplinaire pour la caractérisation hydrogéologique du milieu crayeux : application au transfert de perchlorates dans la craie de Champagne Composition du jury Patrick Höhener, Professeur, Aix-Marseille Université, Président Alain Dassargues, Professeur, Université de Liège (Belgique), Rapporteur Laurent Charlet, Professeur, Université Grenoble Alpes, Rapporteur Danièle Valdes, Maître de Conférences, Sorbonne Université, Examinatrice Neil Sturchio, Professeur, University of Delaware (United States), Invité Vincent Barbin, Professeur, Université de Reims Champagne-Ardenne, Directeur Jessy Jaunat, Maître de Conférences, Université de Reims Champagne-Ardenne, Co-encadrant Patrick Ollivier, PhD, chercheur, BRGM Orléans, Co-encadrant Résumé - Des analyses ont mis en évidence la présence de perchlorate (ClO4 , suspecté d’être un perturbateur endocrinien) dans des captages d’eau potable de Champagne-Ardenne. Deux sources sont suspectées : une source militaire liée à la Grande Guerre et une source agricole liée à l’utilisation passée de nitrates - chiliens. Les objectifs de l’étude sont de déterminer l’origine et le comportement des ClO4 dans les eaux souterraines de la craie de Champagne et d’expliquer les hétérogénéités observées en précisant le fonctionnement de la nappe. La zone d'étude se trouve à l'est de Reims, où une étude historique, hydrologique, géochimique et isotopique est réalisée. Une forte hétérogénéité géochimique des eaux de la nappe est observée. Un modèle conceptuel du fonctionnement de la nappe est proposé, mettant en évidence les facteurs - -1 contrôlant la géochimie des eaux souterraines. Les teneurs élevées en ClO4 (> 4 µgL ) sont détectées principalement en aval des Monts de Champagnes, où de grandes quantités de munitions ont été utilisées, stockées et détruites pendant et après la Grande Guerre. Une origine militaire post-conflit est mise en - évidence par l’analyse isotopique des ClO4 et la détermination de l’âge des eaux. L’évolution spatio- - temporelle des concentrations est discutée sur la base des teneurs en ClO4 , du fonctionnement de la nappe et des informations historiques, permettant de préciser les sources (e.g. munitions non explosés - et sites de destruction des munitions) et les mécanismes de transfert des ClO4 . La contamination en - ClO4 de l’aquifère de la craie de Champagne ne semble pas diminuer à court et moyen termes en raison - de la forte persistance des sources de ClO4 . Mots clés : Perchlorate, Nappe de la Craie, Isotopes, Temps de séjour, Grand Guerre 1 2 Ecole doctorale ABIES GEGENAA Université de Reims Champagne-Ardenne Thesis presented and defensed by Feifei CAO Mars 5, 2020 For the degree of Doctor in University of Reims Champagne-Ardenne Discipline: Environmental Geochemistry Interdisciplinary approach for the hydrogeological characterization of the Chalk aquifer: application on perchlorate transfer in the Champagne Chalk Composition of the Commitee Patrick Höhener, Professor, Aix-Marseille Université, President Alain Dassargues, Professor, Université de Liège (Belgique), Reviewer Laurent Charlet, Professor, Université Grenoble Alpes, Reviewer Danièle Valdes, Assistant professor, Sorbonne Université, Examiner Neil Sturchio, Professor, University of Delaware (United States), Invited Vincent Barbin, Professor, Université de Reims Champagne-Ardenne, Thesis director Jessy Jaunat, Assistant professor, Université de Reims Champagne-Ardenne, Supervisor Patrick Ollivier, PhD, Research scientist, BRGM Orléans, Supervisor 3 4 Abstract - Perchlorate (ClO4 ) has frequently been detected in groundwater at concentrations relevant to human - health. Analyzes in Champagne-Ardenne have highlighted the presence of ClO4 in groundwater for - drinking water supply. The ClO4 has two suspected sources: a military source related to World War I (WWI) and an agricultural source related to past use of Chilean nitrate fertilizers. The objectives of the - study are to determine the sources and behavior of ClO4 in the Champagne Chalk aquifer and to explain the heterogeneities observed by specifying the aquifer functioning. The study area is located east of Reims. A methodology involving historical, hydrodynamic, geochemistry, groundwater dating and isotope analysis has been developed. High spatio-temporal heterogeneities are observed in the Chalk aquifer. A conceptual model of aquifer functioning is proposed, - highlighting main factors governing the Chalk groundwater geochemistry. ClO4 is detected throughout the area with high concentrations (> 4 µg L-1) detected mainly downgradient the Champagne Mounts, where large quantities of ammunition were used, stored and destroyed during and after WWI. A post- - WWI military origin of ClO4 is inferred from isotopic analysis and groundwater ages. Different - - tendencies of ClO4 variation are observed and interpreted by a combination of ClO4 concentrations, - aquifer functioning and historical investigations, revealing major sources of ClO4 (e.g., unexploded - ammunitions, ammunition destruction sites) and its transfer mechanisms in the aquifer. ClO4 contamination in the Champagne Chalk seems unlikely to decrease in the short- to medium-term due to the long persistence time of major sources. Key words: Perchlorate, Chalk aquifer, Isotope analysis, Groundwater dating, World War I 5 6 Remerciements Le temps est venu de remercier toutes les personnes qui ont contribué de près ou de loin à la réalisation de ce travail tout au long de ces trois années extrêmement enrichissantes. Cette thèse a été menée au sein du laboratoire GEGENAA, et n’aurait pu aboutir sans les supports financiers du BRGM, de l’Agence de l’Eau Seine-Normandie, du Grand Reims, de la Région Grand- Est, et de l’ARS Grand-Est. Je tiens tout d’abord à faire part de ma plus profonde reconnaissance à Jessy Jaunat et Patrick Ollivier, les deux encadrants de cette thèse, pour leur implication dans cette étude, leur grande disponibilité, leur gentillesse et leurs nombreux conseils. Merci de m’avoir fait partager vos connaissances et vos expériences, et surtout de m’avoir donné le courage et la motivation d’aller au bout de cette aventure ! Je remercie Vincent Barbin, directeur de thèse, pour m’avoir donné la possibilité et les moyens de réaliser les travaux de cette thèse. Merci pour l’ensemble de vos supports et remarques. Je tiens également à exprimer toutes mes gratitudes envers les membres du jury pour l’intérêt qu’ils ont porté à mon travail en acceptant d’évaluer cette thèse : Patrick Höhener, professeur au sein du Laboratoire Chimie Environnement de Aix-Marseille Université, en tant que président de ce jury en plus de sa qualité d’examinateur ; Alain Dassargues, professeur au département d’Hydrogéologie & Géologie de l'environnement de l’Université de Liège, et Laurent Charlet, professeur à l'Institut des sciences de la Terre (Isterre) de l’Université Grenoble Alpes , en tant que rapporteurs ; et Daniele Valdes, Maître de Conférence de Sorbonne Université en tant que examinatrice de ces travaux. J’adresse un grand merci à Neil Sturchio, professeur au département de Géologie de l’Université du Delaware aux Etats-Unis, qui m’a accueilli durant un mois au sein de son laboratoire et formé sur l’extraction et la purification des perchlorates et l’analyse isotopique des ions perchlorate. Merci de m’avoir donné de nombreux conseils sur l’interprétation des résultats d’analyses, et surtout de m’avoir fait l’honneur de se déplacer depuis l’autre bout du monde à Reims en tant qu’invité de la soutenance de ces travaux. Merci à Luc Aquilina et Virginie Vergnaud de l’OSUR, Géoscience Rennes de l’Université Rennes 1, pour les analyses permettant la datation des eaux souterraines et pour les nombreux conseils et les précieuses discussions autour de l’interprétation des résultats d’analyses. Merci à Luc Aquilina d’avoir accepté de devenir membre de mon comité de thèse et pour les nombreux commentaires ayant permis l’aboutissement de ces travaux de recherche. Merci à Virginie Vergnaud pour sa gentillesse et sa disponibilité lors de nos échanges par mail et téléphone pour répondre à mes nombreuses questions concernant l’âge des eaux souterraines. 7 Je remercie également Emilie Garel du Laboratoire des Sciences Pour l’Environnement de l’Université de Corse Pascal Paoli d’avoir accepté d’être membre de mon comité de thèse, et de m’avoir donné de nombreux conseils et propositions sur les aspects de ma thèse portant sur l’hydrogéologie. Les résultats acquis au cours de cette étude étant en une grande partie issue de prélèvements et mesures sur le terrain, ces travaux n’auraient pas été réalisable sans la collaboration des propriétaires des piézomètres et des stations de pompages. Je tiens à remercie en particulier l’Aérodrome de Reims- Prunay, Veolia et Cristal Union Sillery pour leurs autorisations d’accès aux forages et leur support sur le terrain lors des prélèvements. Merci également à Monsieur et Madame Baudart et Monsieur Rannou de m’avoir donné l’accès à leurs forages privés. Les campagnes de prélèvement mensuelles pendant plus de 2 ans n’auraient pas été réalisées sans l’aide précieuses et la participation active d’Alexandra, Julien et bien sûr Jessy. Je les remercie de m’avoir accompagné sur site, sous la pluie, sous le soleil et
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