Synthèse à différentes interfaces de films bio-inspirés du byssus de la moule : Influence de la nature de l'oxydant à l'interface solide-liquide et d'ajout de polymères à l'interface air-eau

Polydopamine (PDA) materials are inspired from mussels’ byssus strong adhesion underwater. The oligomerization of dopamine in a basic medium allows forming a PDA coating on virtually any materials. In addition to the simplicity, ecofriendly and versatility of the deposition method, PDA has properties similar to those of melanin pigments and displays many outstanding properties. Thus PDAis widely used in energy, environmental and biomedical sciences. However design of PDA based new materials with tailored properties is a challenge since its structure is still unknown. In that sense one of the aims of this thesis is to gain knowledge in PDA structure-property relationship in order to design PDA materials with new properties. By choosing the appropriate oxidant we deposited thick and superhydrophylic films on any materials for the elaboration of low fouling and biocompatible surfaces. Additionally we discovered the possibility to form PDA films at the air/water interface. The investigation of this phenomenon led to the formation of stimuli responsive free standing membranes.Les matériaux à base de polydopamine (PDA) s’inspirent de la forte adhésion du byssus de la moule sous l’eau. L’oligomérisation de la dopamine dans un milieu basique permet la formation de revêtement de PDA sur n’importe quel matériau. En plus de la simplicité du procédé celui-ci est vert et versatile. La PDA a des propriétés similaires aux mélanines, d’où son utilisation dans le domaine des phénomènes de conversion d’énergie, de l’environnement et du biomédical. Cependant la structure de la PDA étant inconnue, l’élaboration de matériaux basés sur la relation structure propriétés est difficile. L’un des buts de cette thèse a été de comprendre cette relation pour élaborer de nouveaux matériaux de PDA. En choisissant l’oxydant adéquat nous avons déposé un film épais, superhydrophile et biocompatible sur n’importe quels substrats. De plus nous avons découverts la possibilité de former des films de PDA à l’interface air/eau. L’étude de ce phénomène a permis de former des membranes autosupportées et stimuli responsives

Borohydride-functionalized polydopamine-coated open cell polyurethane foam as a reusable soft structured material for reduction reactions: application to the removal of a dye

International audienceOpen cell polyurethane foams coated with mussel-inspired polydopamine can be used as support for borohydride anions through their complexation by the catechol groups of the polydopamine layer. This strong interaction prevents borohydride hydrolysis and oxidation, and based on the redox mediator properties of polydopamine, the so-functionalized polydopamine-coated open cell polyurethane foams can act as efficient and reusable soft structured materials for the reduction of methylene blue in aqueous solution without additional sodium borohydride (NaBH4). Very low amounts of released boron sub-products and very small potential of hydrogen (pH) increase are observed in comparison to previous processes using dissolved NaBH4. This considerably reduces the environmental impact of the reducing structured material on the treated wastewater compared to the latter

Stable Bioactive Enzyme-Containing Multilayer Films Based on Covalent Cross-Linking from Mussel-Inspired Adhesives

The use of immobilized enzymes is mandatory for the easy separation of the enzyme, the unreacted substrates, and the obtained products to allow repeated enzymatic assays without cumbersome purification steps. The immobilization procedure is however critical to obtain a high fraction of active enzyme. In this article, we present an enzyme immobilization strategy based on a catechol functionalized alginate. We demonstrate that alkaline phosphatase (ALP) remains active in multilayered films made with alginate modified with catechol moieties (AlgCat) for long duration, that is, up to 7 weeks, provided the multilayered architecture is cross-linked with sodium periodate. This cross-linking reaction allows to create covalent bonds between the amino groups of ALP and the quinone group carried by the modified alginate. In the absence of cross-linking, the enzymatic activity is rapidly lost and this reduction is mainly due to enzyme desorption. We also show that NaIO₄ cross-linked (AlgCat-Alp)_<i>n</i> films can be freeze-dried and reused at least 3 weeks later without lost in enzymatic activity

Polydopamine Films from the Forgotten Air/Water Interface

The formation of polydopamine under mild oxidation conditions from dopamine solutions with mechanical agitation leads to the formation of films that can functionalize all kinds of materials. In the absence of stirring of the solution, we report the formation of polydopamine films at the air/water interface (PDA A/W) and suggest that it arises from an homogeneous nucleation process. These films grow two times faster than in solution and can be deposited on hydrophilic or hydrophobic substrates by the Langmuir–Schaeffer technique. Thanks to this new method, porous and hydrophobic materials like polytetrafluoroethylene (PTFE) membranes can be completely covered with a 35 nm thick PDA A/W film after only 3h of reaction. Finally the oxidation of a monomer followed by a polymerization in water is not exclusive to polydopamine since we also transferred polyaniline functional films from the air/water interface to solid substrates. These findings suggest that self-assembly from a solution containing hydrophilic monomers undergoing a chemical transformation (here oxidation and oligomerization) could be a general method to produce films at the liquid/air interface