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La première partie de cette thèse constitue une introduction aux différentes méthodes de conversion d'énergie et de dessalement qui seront évoquées dans cet ouvrage. Dans une deuxième partie, nous montrons que la conductance ionique d'un réseau de nanopores est sous-additive avec le nombre de pores. La contribution individuelle de chaque pore à la conductance globale tend vers une valeur nulle, pour un réseau suffisamment grand. On note que seuls des rapports de longueurs interviennent, et que le choix d'une échelle nanométrique n'a pas d'influence dans l'effet observé. Ensuite, dans une troisième partie, nous mesurons la perméabilité d'un réseau de pores à une échelle macroscopique. Là aussi, l'influence du réseau ne dépend pas de l'échelle du système. La perméabilité évolue en sens inverse de la conductance : elle est augmentée par la présence de pores voisins, mais dans une faible proportion. La quatrième partie se sert des résultats des deux parties précédentes, dans le but de déterminer une loi d'échelle pour la puissance électrique produite par courant d'écoulement et diffusio-osmose, deux méthodes de conversion d'énergie osmotique. On montre que les effets d'entrée ont un effet délétère sur cette conversion ; ils nécessitent des études plus approfondies. La dernière partie est un travail numérique sur un nouveau procédé de dessalement par osmose via une phase gaz, piégée dans des nanotubes hydrophobes. Son intérêt principal est l'utilisation de nanotubes plus gros que les pores des matériaux actuellement utilisés, donc moins susceptibles de s'encrasser. Par dynamique moléculaire, nous étudions la perméabilité et la sélectivité du dispositif / The first part of this thesis is an introduction to the different energy conversion and desalination methods that will be invoked in this work. In a second part, we show that the ionic conductance of a nanopore array is sub-additive with the number of pores. Individal contributions of each pore to the global conductance tend to a null value, if the network is big enough. We note that this phenomenon only involves length ratios, and that working at a nanometric scale does not have any influence. Then, in a third part, we measure the permeability of a pore array at a macroscopic scale. There too, the effect of the array does not depend on the scale of the system. Permeability evolves inversely to conductance: permeability is enhanced by the presence of neighboring pores, but in a smaller proportion than the ionic conductance falls under the same cause. The fourth part uses the results of the two preceding ones, to determine a scaling law for the electric power produced by streaming current and diffusio-osmosis, two methods of osmotic energy conversion. We show that entrance effects have a negative impact on such conversion, more efforts are needed to understand them better and circumvent them. The fifth and last part of this thesis is a numerical work on a new desalination device. It relies on osmosis through a gas phase which is trapped within a hydrophobic nanotube. Its main interest is to use nanotubes bigger than the pores of currently used materials, thus less prone to fouling. We use molecular dynamics methods to study the permeability and selectivity of this device

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Within the scope of this thesis, a theoretical study of liquid flow in graphitic nanopores was performed. More precisely, a combination of numerical simulations and analytic approach was used to establish the special properties of carbon nanotubes for fluid transport: Molecular dynamics flow simulations of different liquids in carbon nanotubes exhibited flow velocities that are 1-3 orders of magnitude higher than predicted from the continuum hydrodynamics framework and the no-slip boundary condition. These results support previous experiments performed by several groups reporting exceptionally high flow rates for water in carbon nanotube membranes. The reason for this important flow enhancement with respect to the expectation was so far unclear. In this work, a careful investigation of the water/graphite friction coefficient which we identified as the crucial parameter for fast liquid transport in the considered systems, was carried out. In simulations, the friction coefficient was found to be very sensitive to wall curvature: friction is independent of confinement for water between flat graphene walls with zero curvature, while it increases with increasing negative curvature (water at the outside of the tube), and it decreases with increasing positive curvature (water inside the tube), eventually leading to quasi frictionless flow for water in a single file configuration in the smallest tubes. A similar behavior was moreover found with several other liquids, such as alcohol, alcane and OMCTS. Furthermore, a theoretical approximate expression for the friction coefficient is presented which predicts qualitatively and semi-quantitatively its curvature dependent behavior. Moreover, a deeper analysis of the simulations according to the proposed theoretical description shed light on the physical mechanisms at the origin of the ultra low liquid/solid friction in carbon nanotubes. In fine, it is due to their perfectly ordered molecular structure and their atomically smooth surface that carbon nanotubes are quasi-perfect liquid conductors compared to other membrane pores like, for example, nanochannels in amorphous silica. The newly gained understanding constitutes an important validation that carbon nanotubes operate as fast transporters of various liquids which makes them a promising option for different applications like energy conversion or filtration on the molecular level.

Today, the growing and aging population, and the rise of new global threats on human health puts an increasing demand on the healthcare system and calls for preventive actions. To make existing medical treatments more efficient and widely accessible and to prevent the emergence of new threats such as drug-resistant bacteria, improved diagnostic technologies are needed. Potential solutions to address these medical challenges could come from the development of novel lab-on-chip (LoC) for point-of-care (PoC) diagnostics. At the same time, the increasing demand for sustainable energy calls for the development of novel approaches for energy conversion and storage systems (ECS), to which micro- and nanotechnologies could also contribute. This thesis has for objective to contribute to these developments and presents the results of interdisciplinary research at the crossing of three disciplines of physics and engineering: electrokinetic transport in fluids, manufacturing of micro- and nanofluidic systems, and surface control and modification. By combining knowledge from each of these disciplines, novel solutions and functionalities were developed at the macro-, micro- and nanoscale, towards applications in PoC diagnostics and ECS systems. At the macroscale, electrokinetic transport was applied to the development of a novel PoC sampler for the efficient capture of exhaled breath aerosol onto a microfluidic platform. At the microscale, several methods for polymer micromanufacturing and surface modification were developed. Using direct photolithography in off-stoichiometry thiol-ene (OSTE) polymers, a novel manufacturing method for mold-free rapid prototyping of microfluidic devices was developed. An investigation of the photolithography of OSTE polymers revealed that a novel photopatterning mechanism arises from the off-stoichiometric polymer formulation. Using photografting on OSTE surfaces, a novel surface modification method was developed for the photopatterning of the surface energy. Finally, a novel method was developed for single-step microstructuring and micropatterning of surface energy, using a molecular self-alignment process resulting in spontaneous mimicking, in the replica, of the surface energy of the mold. At the nanoscale, several solutions for the study of electrokinetic transport toward selective biofiltration and energy conversion were developed. A novel, comprehensive model was developed for electrostatic gating of the electrokinetic transport in nanofluidics. A novel method for the manufacturing of electrostatically-gated nanofluidic membranes was developed, using atomic layer deposition (ALD) in deep anodic alumina oxide (AAO) nanopores. Finally, a preliminary investigation of the nanopatterning of OSTE polymers was performed for the manufacturing of polymer nanofluidic devices. / <p>QC 20140509</p> / Rappid / NanoGate / Norosensor

<p>Particle suspensions in viscoelastic fluids (e.g., polymeric fluids, liquid crystalline solutions, gels) are ubiquitous in industrial processes and in biology. In such fluids, particles often acquire lift forces that push them to preferential streamlines in the flow domain. This lift force depends greatly on the fluid’s rheology, and plays a vital role in many applications such as particle separations in microfluidic devices, particle rinsing on silicon wafers, and particle resuspension in enhanced oil recovery. Previous studies have provided understanding on how fluid rheology affects the motion of spherical particles in simple viscoelastic fluid flows such as shear flows. However, the combined effect of more complex flow profiles and particle shape is still under-explored. The main contribution of this thesis is to: (a) provide understanding on the migration and rotation dynamics of an arbitrary-shaped particle in complex flows of a viscoelastic fluid, and (b) develop guidelines for designing such suspensions for general applications.</p> <p><br></p> <p>In the first part of the thesis, we develop theories based on the second-order fluid (SOF) constitutive model to provide solutions for the polymeric force and torque on an arbitrary-shaped solid particle under a general quadratic flow field. When the first and second normal stress coefficients satisfy  <strong>Ψ</strong>₁  = −2 <strong>Ψ</strong> ₂ (corotational limit), the fluid viscoelasticity modifies only the fluid pressure and we provide exact solutions to the polymer force and torque on the particle. For a general SOF with  <strong>Ψ</strong> ₁ ≠  −2 <strong>Ψ</strong> ₂, fluid viscoelasticity modifies the shear stresses, and we provide a procedure for numerical solutions. General scaling laws are also identified to quantify the polymeric lift based on different particle shapes and orientation. We find that the particle migration speed is directly proportional to the length the particle spans in the shear gradient direction (L_sg), and that polymeric torques lead to unique orientation behavior under flow.</p> <p><br></p> <p>Secondly, we investigate the migration and rotational behavior of prolate and oblate spheroids in various viscoelastic, pressure-driven flows. In a 2-D slit flow, fluid viscoelasticity causes prolate particles to transition to a log-rolling motion where the particles orient perpendicular to the flow-flow gradient plane. This behavior leads to a slower overall migration speed (i.e., lift) of prolate particles towards the flow centerline compared to spherical particles of the same volume. In a circular tube flow, prolate particles align their long axis along the flow direction due to the extra polymer torque generated by the velocity curvature in all radial directions. Again, this effect causes prolate particles to migrate slower to the flow centerline than spheres of the same volume. For oblate particles, we quantify their long-time orientation and find that they migrate slower than spheres of the same volume, but exhibit larger migration speeds than prolate particles. Lastly, we examine the effect of normal stress ratio ? <strong>α</strong>  = <strong>Ψ</strong> ₂ /<strong>Ψ</strong>₁on the particle motion and find that this parameter only quantitatively impacts the particle migration velocity but has negligible effect on the rotational dynamics. We therefore can utilize the exact solution derived under the corotational limit (?<strong>α</strong> = −1/2) for a quick and reasonable prediction on the particle dynamics.</p> <p><br></p> <p>We next experimentally investigate the migration behavior of spheroidal particles in microfluidic systems and draw comparisons to our theoretical predictions. A dilute suspension of prolate/oblate microparticles in a density-matched 8% aqueous polyvinylpyrrolidone (PVP) solution is used as the model suspension system. Using brightfield microscopy, we qualitatively confirm our theoretical predictions for flow Deborah numbers 0 < De < 0.1 – i.e., that spherical particles show faster migration speed than prolate and oblate particles of the same volume in tube flows.</p> <p><br></p> <p>We finally design a holographic imaging method to capture the 3-D position and orientation of dynamic microparticles in microfluidic flow. We adopt in-line holography setup and propose a straightforward hologram reconstruction method to extract the 3-D position and orientation of a non-spherical particle. The method utilizes image moment to locate the particle and localize the detection region. We detect the particle position in the depth direction by quantifying the image sharpness at different depth position, and uses principal component analysis (PCA) to detect the orientation of the particle. For a semi-transparent particle that produces complex diffraction patterns, a mask based on the image moment information can be utilized during the image sharpness process to better resolve the particle position.</p> <p><br></p> <p>In the last part of this thesis, we conclude our work and discuss the future research perspectives. We also comment on the possible application of current work to various fields of research and industrial processes.</p> <p><br></p>