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Porous PEDOT:PSS Particles and their Application as Tunable Cell Culture Substrate
Due to its biocompatibility, electrical conductivity, and tissue-like elasticity, poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) constitutes a highly promising material regarding the fabrication of smart cell culture substrates. However, until now, high-throughput synthesis of pure PEDOT:PSS geometries was restricted to flat sheets and fibers. In this publication, the first microfluidic process for the synthesis of spherical, highly porous, pure PEDOT:PSS particles of adjustable material properties is presented. The particles are synthesized by the generation of PEDOT:PSS emulsion droplets within a 1-octanol continuous phase and their subsequent coagulation and partial crystallization in an isopropanol (IPA)/sulfuric acid (SA) bath. The process allows to tailor central particle characteristics such as crystallinity, particle diameter, pore size as well as electrochemical and mechanical properties by simply adjusting the IPA:SA ratio during droplet coagulation. To demonstrate the applicability of PEDOT:PSS particles as potential cell culture substrate, cultivations of L929 mouse fibroblast cells and MRC-5 human fibroblast cells are conducted. Both cell lines present exponential growth on PEDOT:PSS particles and reach confluency with cell viabilities above 95 vol.% on culture day 9. Single cell analysis could moreover reveal that mechanotransduction and cell infiltration can be controlled by the adjustment of particle crystallinity.
Porous PVDF Monoliths with Templated Geometry
Additive manufacturing of complex porous polymer geometries is a new field of advanced materials processing. Such new geometries can be used to fabricate porous polymer monoliths serving as a support for other material functions. Here, a novel fabrication technology to manufacture tailored 3D porous monoliths via additive manufacturing and templating is presented. The method is based on replicating a 3D-printed mold with a polymer solution of polyvinylidenfluorid-triethyl phosphate (PVDF-TEP) and induce phase separation of the polymer solution subsequently. In a second step, the mold is removed without affecting the porous PVDF phase. As a result, porous monoliths with a templated 3D architecture are successfully fabricated. The manufacturing process is successfully applied to complex structures and can be applied to any conceivable geometry. Coating the porous 3D monoliths with another PVDF solution allows applying a skin layer yielding an asymmetric membrane monolith. As a showcase, a polydimethylsiloxane coating even leads to a smooth and dense layer of micrometer size. The methodology enables a new generation of complex porous polymer monoliths with tailored surface coatings. For the combination of poly(dimethylsiloxane) on a porous support, gas/liquid mass transfer is used in blood oxygenation with reduced diffusion limitation is within reach.
Unravelling colloid filter cake motions in membrane cleaning procedures
The filtration performance of soft colloid suspensions suffers from the agglomeration of the colloids on the membrane surface as filter cakes.Backflushing of fluid through the membrane and cross-flow flushing across the membrane are widely used methods to temporally remove the filter cake and restore the flux through the membrane. However, the phenomena occurring during the recovery of the filtration performance are not yet fully described. In this study, we filtrate poly(N-isopropylacrylamide) microgels and analyze the filter cake in terms of its composition and its dynamic mobility during removal using on-line laser scanning confocal microscopy. First, we observe uniform cake build-up that displays highly ordered and amorphous regions in the cake layer. Second, backflushing removes the cake in coherent pieces and their sizes depend on the previous cake build-up. And third, cross-flow flushing along the cake induces a pattern of longitudinal ridges on the cake surface, which depends on the cross-flow velocity and accelerates cake removal. These observations give insight into soft colloid filter cake arrangement and reveal the cake’s unique behaviour exposed to shear-stress. © 2020, The Author(s).
Biocompatible Micron-Scale Silk Fibers Fabricated by Microfluidic Wet Spinning
For successful material deployment in tissue engineering, the material itself, its mechanical properties, and the microscopic geometry of the product are of particular interest. While silk is a widely applied protein-based tissue engineering material with strong mechanical properties, the size and shape of artificially spun silk fibers are limited by existing processes. This study adjusts a microfluidic spinneret to manufacture micron-sized wet-spun fibers with three different materials enabling diverse geometries for tissue engineering applications. The spinneret is direct laser written (DLW) inside a microfluidic polydimethylsiloxane (PDMS) chip using two-photon lithography, applying a novel surface treatment that enables a tight print-channel sealing. Alginate, polyacrylonitrile, and silk fibers with diameters down to 1 µm are spun, while the spinneret geometry controls the shape of the silk fiber, and the spinning process tailors the mechanical property. Cell-cultivation experiments affirm bio-compatibility and showcase an interplay between the cell-sized fibers and cells. The presented spinning process pushes the boundaries of fiber fabrication toward smaller diameters and more complex shapes with increased surface-to-volume ratio and will substantially contribute to future tailored tissue engineering materials for healthcare applications. © 2021 The Authors. Advanced Healthcare Materials published by Wiley-VCH GmbH
Direct Observation of Deformation in Microgel Filtration
Colloidal filtration processes using porous membranes suffer from productivity loss due to colloidal matter retention and continuous build-up by the retained matter. Especially during filtration of soft matter, the deformation of the individual colloids that make up the filter cake may be significant; however, this deformation and its impact remain unresolved so far. Yet, understanding the deformation on the single colloid level as well as on the ensemble level is important to be able to deconvolute filter cake properties from resistance increase of the membrane either by simultaneous internal adsorption or blocking of pores. Here, we report on the compression of a filter cake by filtrating soft microgels in a microfluidic channel in front of a model membrane. To study the single colloid deformation amorphous and crystalline domains were built up in front of the membrane and visualized on-line using confocal fluorescence microscopy while adjusting the degree of permeation, i.e., the transmembrane flux. Results show locally pronounced asymmetric deformation in amorphous domains, while the microgels in colloidal crystals approached regular polyeder shape. Increasing the flux beyond the maximum colloid deformation results in non-isochoric microgel behavior. The presented methodology enables a realistic description of complex colloidal matter deposits during filtration.
Templating the morphology of soft microgel assemblies using a nanolithographic 3D-printed membrane
Filter cake formation is the predominant phenomenon limiting the filtration performance of membrane separation processes. However, the filter cake’s behavior at the particle scale, which determines its overall cake behavior, has only recently come into the focus of scientists, leaving open questions about its formation and filtration behavior. The present study contributes to the fundamental understanding of soft filter cakes by analyzing the influence of the porous membrane’s morphology on crystal formation and the compaction behavior of soft filter cakes under filtration conditions. Microfluidic chips with nanolithographic imprinted filter templates were used to trigger the formation of crystalline colloidal filter cakes formed by soft microgels. The soft filter cakes were observed via confocal laser scanning microscopy (CLSM) under dead-end filtration conditions. Colloidal crystal formation in the cake, as well as their compaction behavior, were analyzed by optical visualization and pressure data. For the first time, we show that exposing the soft cake to a crystalline filter template promotes the formation of colloidal crystallites and that soft cakes experience gradient compression during filtration.
Wetting-Induced Polyelectrolyte Pore Bridging
Active layers of ion separation membranes often consist of charged layers that retain ions based on electrostatic repulsion. Conventional fabrication of these layers, such as polyelectrolyte deposition, can in some cases lead to excess coating to prevent defects in the active layer. This excess deposition increases the overall membrane transport resistance. The study at hand presents a manufacturing procedure for controlled polyelectrolyte complexation in and on porous supports by support wetting control. Pre-wetting of the microfiltration membrane support, or even supports with larger pore sizes, leads to ternary phase boundaries of the support, the coating solution, and the pre-wetting agent. At these phase boundaries, polyelectrolytes can be complexated to form partially freestanding selective structures bridging the pores. This polyelectrolyte complex formation control allows the production of membranes with evenly distributed polyelectrolyte layers, providing (1) fewer coating steps needed for defect-free active layers, (2) larger support diameters that can be bridged, and (3) a precise position control of the formed polyelectrolyte multilayers. We further analyze the formed structures regarding their position, composition, and diffusion dialysis performance.
Microfluidic colloid filtration
Filtration of natural and colloidal matter is an essential process in today’s water treatment processes. The colloidal matter is retained with the help of micro- and nanoporous synthetic membranes. Colloids are retained in a “cake layer” – often coined fouling layer. Membrane fouling is the most substantial problem in membrane filtration: colloidal and natural matter build-up leads to an increasing resistance and thus decreasing water transport rate through the membrane. Theoretical models exist to describe macroscopically the hydrodynamic resistance of such transport and rejection phenomena; however, visualization of the various phenomena occurring during colloid retention is extremely demanding. Here we present a microfluidics based methodology to follow filter cake build up as well as transport phenomena occuring inside of the fouling layer. The microfluidic colloidal filtration methodology enables the study of complex colloidal jamming, crystallization and melting processes as well as translocation at the single particle level.
Particle movements provoke avalanche-like compaction in soft colloid filter cakes
During soft matter filtration, colloids accumulate in a compressible porous cake layer on top of the membrane surface. The void size between the colloids predominantly defines the cake-specific permeation resistance and the corresponding filtration efficiency. While higher fluxes are beneficial for the process efficiency, they compress the cake and increase permeation resistance. However, it is not fully understood how soft particles behave during cake formation and how their compression influences the overall cake properties. This study visualizes the formation and compression process of soft filter cakes in microfluidic model systems. During cake formation, we analyze single-particle movements inside the filter cake voids and how they interact with the whole filter cake morphology. During cake compression, we visualize reversible and irreversible compression and distinguish the two phenomena. Finally, we confirm the compression phenomena by modeling the soft particle filter cake using a CFD-DEM approach. The results underline the importance of considering the compression history when describing the filter cake morphology and its related properties. Thus, this study links single colloid movements and filter cake compression to the overall cake behavior and narrows the gap between single colloid events and the filtration process.