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Diffusion of Polyelectrolytes in Dispersions of Nanoparticles Caterina Dolce

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Diffusion of Polyelectrolytes in Dispersions of Nanoparticles Caterina Dolce Diffusion of polyelectrolytes in dispersions of nanoparticles Caterina Dolce To cite this version: Caterina Dolce. Diffusion of polyelectrolytes in dispersions of nanoparticles. Chemical Physics [physics.chem-ph]. Université Pierre et Marie Curie - Paris VI, 2016. English. NNT : 2016PA066569. tel-01537900 HAL Id: tel-01537900 https://tel.archives-ouvertes.fr/tel-01537900 Submitted on 13 Jun 2017 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. Thèse de doctorat Pour l’obtention du grade de Docteur de l’Université Pierre et Marie Curie École doctorale de Chimie Physique et Chimie Analytique de Paris Centre Diffusion of polyelectrolytes in dispersions of nanoparticles Caterina DOLCE Directeur de thèse : Guillaume MÉRIGUET Présentée et soutenue publiquement le 24 Novembre 2016 devant un jury composé de : M. Eric BUHLER ...................................................... Rapporteur M. Armel GUILLERMO ............................................... Rapporteur Mme Barbara HRIBAR LEE .......................................... Examinatrice M. François RIBOT ................................................... Examinateur Mme Véronique GILARD ............................................ Examinatrice M. Guillaume MÉRIGUET ....................................... Directeur de thèse You must do the thing you think you cannot do Eleanor Roosevelt i ii Remerciements Ce travail de thèse a été réalisé au sein du laboratoire PHENIX (PHysicochimie des Elec- trolytes et Nanosystèmes InterfaciauX) de l’Université Pierre et Marie Curie (UPMC) sous la direction de Guillaume Mériguet. Je souhaite le remercier, tout d’abord pour m’avoir donné l’opportunité de faire ce parcours de thèse, pour ses qualités d’encadrement assujetti par ses grandes connaissances scientifiques. J’ai beaucoup appris grâce à lui, profitant de sa disponibilité permanente qui m’a permis d’apporter de nombreuses réponses à mes questions, auxquelles il a toujours su répondre de façon très didactique et scientifiquement stimulante. Je le remercie également de m’avoir appris ce qu’est un travail scientifique, et de m’avoir apporté un éclairage sur la bonne façon d’aborder un problème scientifique. Par ailleurs, un grand merci pour ses qualités humaines qui ont contribué à faire de ces trois années un parcours si agréable, une grande expérience de vie, une croissance scientifique, professionnelle, et humaine. J’ai eu la chance de l’avoir eu en tant qu’encadrant. Je remercie sincèrement Eric Buhler et Armel Guillermo d’avoir accepté de rapporter ma thèse, et Barbara Hribar Lee, Véronique Gilard, et François Ribot d’avoir accepté de faire partie de ce jury de thèse. Je remercie Pierre Levitz directeur du laboratoire Phenix qui m’a permis de realiser ma thèse au sein du laboratoire. Je remercie le Professeur Marie Jardat, Directrice de l’équipe MEM, qui en plus d’avoir été un très bon guide pour cette équipe, a réussi tous les jours à créer, alimenter, et maintenir la cohésion de groupe. Je remercie les bureaux des projets européens de l’UPMC, de la délégation Paris B du CNRS, et de l’UTC de Compiègne. Pour m’avoir accueilli pendant ma mission doctorale de valorisation de la recherche en partenariat européen. En particulier, j’adresse mes remerciement les plus chaleureux à Stéphanie Rossard, responsable des projets européens de l’UTC, pour la passion et l’enthousiasme qu’elle m’a bien transmise. Je remercie Isabelle Grillo pour m’avoir accueilli à l’ILL et pour son aide et ses précieux conseils durant les manips sur D33 ; Un merci également à Isabelle Correia pour son aide précieuse et sa disponibilité pendant les mesures RMN. En ce qui concerne mon laboratoire d’accueil, la liste est longue et j’espère sincèrement que je n’oublierai personne. Vous avez tous contribué à mon enrichissement personnel pendant ce parcours. Dans le domaine de la gestion du laboratoire, je remercie beaucoup Brigitte et Gérard, pour leur efficacité dans l’organisation de toutes les missions auxquelles j’ai participé, ainsi que pour iii leur gentillesse et disponibilité quotidienne. Un grand merci à Anne-Laure pour ses conseils et son soutien sur la RMN ; Emmanuelle pour ses conseils utiles et sa disponibilité ; Jean pour ses intéressantes histoires, sa disponibilité pour répondre à toutes les questions scientifiques et techniques, et aussi pour avoir été présent pendant les longues journées au laboratoire ; Nicolas pour la bonne humeur apportée dans le laboratoire ; Natalie pour m’avoir initié aux petits angles, pour avoir permis de faire les premiers tests pendant son beam time ; Amandine pour l’aide dans le laboratoire et pour m’avoir aidé à améliorer mon français pendant les agréables déjeuners ensemble . Merci également à tous ceux avec qui j’ai pu partager mes pauses thé, déjeuner et couloir : Serge, Vincent, Damien, Virginie, Benjamin, Mathieu, Jean-Pierre, Olivier, Ana, Augusta, José, et tous les autres. Enfin je remercie tous mes collègues et amis pour les bons moments passés, le soutien, la compréhension, l’aide, les conseils, et les échanges sur les plus différents sujets. Tout d’abord Steph, pour avoir été un parfait compagnon de bureau pour ces trois années, pour m’avoir bien supporté, ainsi que pour sa présence durant tous les moments que ce soit dans le laboratoire ou en dehors (la liste sera trop longue) ; Willy, ami et collègue, toujours prêt à écouter, à aider avec sa gentillesse et sa bonne humeur qui ont permis à rendre si agréable les journées ; Pauline B. pour sa gentillesse permanente, sa disponibilité et sa force tranquille qui m’ont beaucoup encouragé ; Pauline S. pour ses nombreuses contributions pour le laboratoire et pour tous ; Adelchi pour sa gentillesse, sa disponibilité et pour son aide dans la traduction de nombreux mots en français que je ne connaissais pas ; Anastacia chère amie et compagnon de laboratoire. Maintenant, je dois arrêter avec les périphrases et me contenter des faire une liste de tous mes chères col- lègues et amis qui m’ont accompagnée et ont été présents pendant cette période passée au laboratoire : Xu, Fabien, Sébastien, Vivien, Lisa, Allan, Yasine, Jamoowantee, Nadia, Véronica, Nebewia, Alberto, Gabriele ; Aux anciens thésards : Clarisse, Antoine, Simon, Raphael, Amaël, Dario, Davide, Clément... et aux thésards venus de loin mais toujours si proche Clébert et Grégor. C’est avec une heureuse nostalgie que je repenserai à tous les moments passés ensemble et en général à l’ensemble de ces trois années. A Derek, la personne qui a été à mes côtés de moi tous les jours, qui m’a encouragé et donné le soutien dont j’avais, j’ai et j’aurai besoin. Infine un ringraziamento speciale alla mia famiglia che mi ha permesso di realizzare gli studi, che mi ha sempre supportato e accompagnato nelle mie scelte senza mai giudicare ed essendo sempre presente in ogni momento di questo percorso. iv Contents Introduction 1 1 Colloids and polyelectrolytes 7 1.1 Introduction . 8 1.2 Colloids . 8 1.2.1 Electrostatic potential around a macroion . 9 1.2.2 Van der Waals potential . 12 1.3 Polymer . 13 1.3.1 Concentration regimes . 15 1.3.2 Ideal chain . 16 1.3.3 Real chain . 18 1.4 Polyelectrolytes . 20 1.4.1 Definition and applications . 20 1.4.2 Chain conformation . 21 1.4.3 Counterion condensation . 23 1.5 Polymer-colloid mixtures . 24 1.5.1 Depletion effect . 25 1.6 Dynamics of polymers . 27 1.6.1 The Rouse model . 29 1.6.2 The Zimm Model . 29 1.6.3 Kirkwood-Zimm . 30 1.7 Dynamics of polyelectrolytes . 31 2 Diffusion in crowded colloidal systems 33 2.1 Introduction . 34 2.2 Model based on obstruction effects . 37 2.2.1 Cell models . 39 2.3 Models based on chemical binding . 43 2.4 Models based on other effects . 44 2.4.1 Free volume theories . 44 2.4.2 Colloidal approach . 45 2.5 Cell-model for the diffusion in the DLVO potential . 46 2.5.1 Method . 46 2.5.2 Applications . 47 v 3 Nuclear Magnetic Resonance 51 3.1 Introduction . 52 3.2 Magnetic momentum . 53 3.3 Chemical shifts . 54 3.4 Relaxation . 56 3.4.1 Methods . 57 3.4.2 Results . 58 3.5 Diffusion NMR . 59 3.5.1 Diffusion pulse sequences . 61 3.6 Implementation of the experiments . 65 3.6.1 Solvent signal suppression . 66 3.6.2 Non-Gaussian brownian diffusion . 66 3.6.3 Dispersity effects . 67 3.6.4 Sequence parameters . 69 4 Chemical and physical properties of the systems 73 4.1 Chemical systems . 74 4.1.1 Oligomers . 74 4.1.2 Polyelectrolytes . 74 4.1.3 Nanoparticles . 77 4.2 Physical properties of the experimental systems . 79 4.2.1 Size characterisation: light scattering . 79 4.2.2 Charge characterizations . 82 5 Small polyelectrolytes in dilute regime 93 5.1 Introduction . 94 5.2 Analysis of 1H spectra . 94 5.2.1 Effect of concentration on 1H spectra . 97 5.2.2 Effect of screening of electrostatic interactions . 97 5.2.3 Effect of the interactions: the pH . 100 5.3 Self-diffusion of polyelectrolytes and oligomers . 104 5.3.1 Molecular weight influence . 104 5.3.2 Influence of the concentration on the dynamics . 105 5.3.3 Influence of the interaction on the diffusion . 107 5.4 What is the impact of the chain length on the properties of short weak polyelec- trolytes? ......................................114 6 Diffusion of short polyelectrolytes in crowded charged media 117 6.1 Preliminary analysis of polyelectrolytes and nanoparticles mixtures .
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