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Biointerfaces based on the combination of synthetic polymers and biomolecules

  • Autores: Anna Puiggalí Jou
  • Directores de la Tesis: Luís Javier del Valle Mendoza (dir. tes.), Carlos Alemán Llansó (dir. tes.), Raimon Jané Campos (tut. tes.)
  • Lectura: En la Universitat Politècnica de Catalunya (UPC) ( España ) en 2019
  • Idioma: español
  • Tribunal Calificador de la Tesis: Elisabet Engel López (presid.), Guillermo Revilla López (secret.), Laura Marcela Uribe-Calderón (voc.), Antonella Accardo (voc.), Ian W. Hamley (voc.)
  • Programa de doctorado: Programa de Doctorado en Ingeniería Biomédica por la Universidad Politécnica de Catalunya y la Universidad de Zaragoza
  • Materias:
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  • Resumen
    • During the last decades, research focused on the preparation of highly selective and smart materials has increased considerably. For instances, it has been possible to achieve intelligent drug nano-carriers, biomolecular sensors, platforms to promote cell growth and differentiation among many other striking applications. Two mentionable factors that helped such development are the incorporation of biological moieties onto this interfaces to gain specificity and the combination of more than one material in order to get a synergistic effect between the different components (i.e. conducting polymers suffer from poor mechanical strength, therefore its combination with polyesters can reduce their fragility).

      This thesis has been devoted to the design and development of high performance polymeric materials for multiple functions related to the biomedical field, such as passive ion transport membranes, drug delivery systems and the addition of selectivity in different surfaces. The work gives special emphasis to the characterization of these platforms, like its surface chemistry, topology, biocompatibility or its mechanical strength. Besides, these systems have been synthetized in a large variety of shapes, from free-standing nanomembranes to polymeric nanoparticles.

      The Thesis is divided in three blocs: Bloc A encloses all the studies realized for the generation of hybrid nanoperforated membranes in order to achieve controlled ion diffusion. Specifically, an outer membrane protein, Omp2a, was considered for these studies. Primarily, the protein was purified, folded and characterized in an ambient resembling to the one encountered in nature, its mechanical forces and conductivity were analysed. The project was followed by the immobilization of Omp2a into silicon microcantillevers to acquire greater knowledge of its folding and unfolding processes upon thermal stress. Next, artificial polymeric membranes containing nanofeatures were developed with the final purpose to immobilize Omp2a via protein confinement. Then, the conductivity of the membrane with different electrolyte media solutions was tested.

      Bloc B describes the state-of-the art of drug delivery systems prepared with intrinsically conducting polymers to achieve controlled drug release upon electrical stimuli. Furthermore, two systems based on poly(3,4-ethylenedioxythiophene) (PEDOT) nanoparticles are described. Particularly, curcumin was employed as a model neutral drug and incorporated within the PEDOT nanoparticles. The oxidation state of the PEDOT chains regulated the drug release. Later on, a similar system was generated with polyester microfibers loaded with curcumin and nanoparticles. The driving force for the later drug release was the actuation of the PEDOT nanoparticles.

      Lastly, Bloc C reports the immobilization of a pentapeptide called CREKA and its analog CR(NMe)EKA onto PEDOT and silicon surfaces. The addition of CREKA favoured the selectivity of those interfaces towards clotted plasma proteins such as fibrin and fibrinogen. PEDOT-peptide material allowed the electrochemical detection of the proteins by an increase in membrane resistance and these interactions were evaluated with microcantilevers by measuring the difference on weight when they were incubated with different protein concentrations.

      Overall, the compilation of the studies presented in this Thesis offer a comprehensive view on how modifying and generating hybrid materials is possible to optimize and exploit their capabilities for a wide range of applications.


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