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Thermodynamic and Structural Investigations on the Interactions Between Actinides and Phosphonate-Based Ligands Gaoyang Ye

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Thermodynamic and Structural Investigations on the Interactions Between Actinides and Phosphonate-Based Ligands Gaoyang Ye Thermodynamic and structural investigations on the interactions between actinides and phosphonate-based ligands Gaoyang Ye To cite this version: Gaoyang Ye. Thermodynamic and structural investigations on the interactions between actinides and phosphonate-based ligands. Radiochemistry. Université Paris-Saclay, 2018. English. NNT : 2018SACLS286. tel-02169209 HAL Id: tel-02169209 https://tel.archives-ouvertes.fr/tel-02169209 Submitted on 1 Jul 2019 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. Thermodynamic and structural investigations on the interactions between actinides and phosphonate- 2018SACLS286 2018SACLS286 : based ligands 2018SACLS286 NNT Thèse de doctorat de l'Université Paris-Saclay Préparée à l’Université Paris-Sud École doctorale n°576 Particules Hadrons Energie et Noyau : Instrumentation, Image, Cosmos et Simulation (PHENIICS) Spécialité de doctorat: Aval du cycle nucléaire, Radioprotection et Radiochimie Thèse présentée et soutenue à Orsay, le 19 septembre, par Gaoyang YE Composition du Jury : M. David Aitken Professeur, Université Paris-Sud Président M. Jean Aupiais Professeur, CEA/DAM bruyère le Chatel Rapporteur M. Gilles Montavon Professeur, SUBATECH - MINES Nantes Rapporteur M. Loic Charbonniere Professeur, CNRS Strasbourg Examinateur M. Christophe Den Auwer Professeur, Université de NICE Examinateur M. Wangsuo Wu Professeur, University of Lanzhou Examinateur M. Eric Simoni Professeur, Université Paris-Sud Directeur de thèse Acknowledgement This thesis work was done at l'institut de physique nucléaire d'orsay in the group of Radiochemistry, Université Paris-Sud. This work was funded by Chinese Science council. I want to thank in the first place my thesis director Eric Simoni for the trust he has given me throughout these three years, for enlightened advice whether at the lab or for the project. Thank you for your patience and your availability. I would like to thank Gilles Montavon and Jean Aupiais who accepted to be rapporteurs of my work, Loic Charbonniere, Christophe Den Auwer, Wangsuo Wu and David Aitken for having accepted to participate in my thesis jury. I would also like to thank the groupe of Synthèse Pour l’Analyse (SynPA) and more particularly Câline Christine and Alexandre Lecointre for the advice on organic synthesize, Raphael Gillet, Soumaya Khalfallah and Mohamadou Sy for the French language training, Anne Boos and Jérémy Brandel for your kindles help for the ligand characterization. I would like to thank l’équipe de Radiochimie Humaine et Environnementale (RHE). Special mention for Gaëlle, thank you for your support and your advice that often allowed me to avoid the traps of the IR, Many thanks for the help on EXAFS study of Jérome Roques (Groupe Radiochime), Christophe Den Auwer (RHE) and Pier-Lorenzo Solari as well as to the members of the MARS line. I also thank my ‘greater groupe radiochime family’: Florian Brulfert, Davide Rodrigues, Thi- Kim-Khanh Le, Gabriela Duran-Klie, Quentin Le Moëne, Céline Cannes, Sylvie Delpech, Romuald Drot, Elisabeth Seibert, Vladimir Sladkov and Véronika Zinovyeva, as well as Mingjian He, Thanks to you, these three years are filled with good memories. I would also like to express my thanks to Nicole Barre-Boscher, who help me fixed the instrument problem. Finally, I thank my family and friends for supporting me during these three years. First of all, my sincere gratitude to my parents who encouraged and advised me throughout my studies. I also thank to my friends to eat and drink together sometimes to pass the hard time. 2 3 Content General introduction............................................................................................... 4 Chapter 1: Bibliographic study 1 Conception of actinides decorporation ........................................................................ 8 2 General introduction of actinides ................................................................................ 8 2.1 Generality ............................................................................................................. 8 2.2 Uranium ................................................................................................................ 9 2.2.1 Uranium in the industry and environment .................................................... 9 2.2.2 Physic-chemical properties of uranium ...................................................... 11 2.3 Americium/curium ............................................................................................. 12 2.3.1 Americium/curium in the industry and environment .................................. 13 2.3.2 Physic-chemical properties of americium and curium, europium use as the chemical analogue ............................................................................................................ 13 3 Toxicology ................................................................................................................. 16 3.1 The contamination mode .................................................................................... 16 3.1.1 Main entry routes ........................................................................................ 17 3.1.2 Main excretion routes ................................................................................. 18 3.2 The factor which influences the toxicity ............................................................ 19 3.3 The bio-distribution of actinides ........................................................................ 19 3.3.1 Uranium ...................................................................................................... 21 3.3.2 Americium/curium ...................................................................................... 22 3.4 Human Health Effects ........................................................................................ 23 3.4.1 Uranium ...................................................................................................... 23 3.4.2 Americium/curium ...................................................................................... 24 3.5 Conclusion .......................................................................................................... 24 4 Chelation therapy ....................................................................................................... 24 4.1 Actinides chelating agents under studies............................................................ 26 4.1.1 The poly-amino-carboxylic ligands ............................................................ 27 4.1.2 Siderophores analogues: CAM & HOPO ................................................... 28 4.1.3 Phosphonate ligands .................................................................................... 31 4.2 Methods for in vitro study .................................................................................. 34 4.3 Conclusion .......................................................................................................... 34 5 Chelation study for biology simulation with calmodulin .......................................... 35 5.1 Description of the protein ................................................................................... 35 5.2 Interaction between calmodulin and calcium ..................................................... 36 1 5.3 Interactions between calmodulin and actinides .................................................. 37 Chapiter 2: synthesis of polyaminophosphonates ligands 1 General strategy ......................................................................................................... 42 2 Synthesis of precursor ............................................................................................... 42 2.1 Synthesis of pyridinic platform .......................................................................... 43 2.2 Synthesis of amine monophosphonate ............................................................... 43 3 Synthesis of bisphosphonate ligand L1 ...................................................................... 44 4 Synthesis of bisphosphonate ligand L2 ...................................................................... 44 5 Synthesis of bisphosphonate ligand L3 ...................................................................... 45 6 Conclusion ................................................................................................................. 47 7 Experimental part ...................................................................................................... 48 Chapiter 3: structural and thermodynamic study of uranyl with polyaminophosphonates ligands 1 Acid-base properties of polyaminophosphonates ligands ......................................... 56 1.1 Potentiometric study ........................................................................................... 56 1.2 Spectrophotometric study according to the pH .................................................. 60 1.3 Conclusion .........................................................................................................
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