SearcharxivSearch

arXiv subjects

Matthias Wessling

Publications and source records attributed to Matthias Wessling.

At least 19 recordsLinked to original sources

Morphology Engineering of Mixed Ionic Electronic Conductors through Aqueous Phase Separation

The performance of organic electrochemical transistors (OECTs) is fundamentally governed by the interplay between ionic accessibility and electronic transport within organic mixed ionic-electronic conductors. Although increasing channel thickness enhances transconductance, it also prolongs ion transport, resulting in the well-known gain-speed trade-off. Here, we demonstrate that engineering the internal morphology of PEDOT:PSS:PEI films through pH-induced aqueous phase separation provides an effective route to mitigate this limitation. The resulting interconnected pore network promotes electrolyte penetration and increases the electrochemically addressable volume, while DMSO treatment and annealing enhance the continuity and ordering of the PEDOT-rich electronic phase. Consequently, porous OECT channels achieve a transconductance of 30 mS and a response time of 13 ms at an ultralow gate voltage of 0.05 V despite channel thicknesses exceeding 100 um. Comparison of films with comparable electronic conductivity but different pore architectures identifies morphology as the dominant factor governing device performance, supporting a transition from predominantly surface-limited modulation toward spatially distributed mixed ionic-electronic transport. Beyond demonstrating a scalable water-based fabrication strategy, this work establishes internal morphology as a design parameter that complements molecular structure and device geometry in organic mixed conductors, providing a general framework for the development of high-performance OECTs, soft bioelectronics, and future neuromorphic materials.

cond-mat.mtrl-sci

Towards a Physics Foundation Model

Foundation models have revolutionized natural language processing through a ``train once, deploy anywhere'' paradigm, where a single pre-trained model adapts to countless downstream tasks without retraining. Access to a Physics Foundation Model (PFM) would be transformative - democratizing access to high-fidelity simulations, accelerating scientific discovery, and eliminating the need for specialized solver development. Yet current physics-aware machine learning approaches remain fundamentally limited to single, narrow domains and require retraining for each new system. We present the General Physics Transformer (GPhyT), trained on 1.8 TB of diverse simulation data, that demonstrates foundation model capabilities are achievable for physics. Our key insight is that transformers can learn to infer governing dynamics from context, enabling a single model to simulate fluid-solid interactions, shock waves, thermal convection, and multi-phase dynamics without being told the underlying equations. GPhyT achieves three critical breakthroughs: (1) superior performance across multiple physics domains, outperforming specialized architectures by more than 7x, (2) plausible zero-shot generalization to entirely unseen physical systems through in-context learning, and (3) more stable long-term predictions through long-horizon rollouts. By establishing that a single model can learn generalizable physical principles from data alone, this work opens the path toward a universal PFM that could transform computational science and engineering.

cs.LG

PECVD and PEALD on polymer substrates (Part II): Understanding and tuning of barrier and membrane properties of thin films

This feature article presents insights concerning the correlation of PECVD and PEALD thin film structures with their barrier or membrane properties. While in principle similar precursor gases and processes can be applied, the adjustment of deposition parameters for different polymer substrates can lead to either an effective diffusion barrier or selective permeabilities. In both cases the understanding of the film growth and the analysis of the pore size distribution and the pore surface chemistry is of utmost importance for the understanding of the related transport properties of small molecules. In this regard the article presents both concepts of thin film engineering and analytical as well as theoretical approaches leading to a comprehensive description of the state of the art in this field. Moreover, based on the presented correlation of film structure and molecular transport properties perspectives of future relevant research in this area is presented.

cond-mat.soft

Reminding Forgetful Organic Neuromorphic Device Networks

Organic neuromorphic device networks can accelerate neural network algorithms and directly integrate with microfluidic systems or living tissues. Proposed devices based on the bio-compatible conductive polymer PEDOT:PSS have shown high switching speeds and low energy demand. However, as electrochemical systems, they are prone to self-discharge through parasitic electrochemical reactions. Therefore, the network's synapses forget their trained conductance states over time. This work integrates single-device high-resolution charge transport models to simulate neuromorphic device networks and analyze the impact of self-discharge on network performance. Simulation of a single-layer nine-pixel image classification network reveals no significant impact of self-discharge on training efficiency. And, even though the network's weights drift significantly during self-discharge, its predictions remain 100\% accurate for over ten hours. On the other hand, a multi-layer network for the approximation of the circle function is shown to degrade significantly over twenty minutes with a final mean-squared-error loss of 0.4. We propose to counter the effect by periodically reminding the network based on a map between a synapse's current state, the time since the last reminder, and the weight drift. We show that this method with a map obtained through validated simulations can reduce the effective loss to below 0.1 even with worst-case assumptions. Finally, while the training of this network is affected by self-discharge, a good classification is still obtained. Electrochemical organic neuromorphic devices have not been integrated into larger device networks. This work predicts their behavior under nonideal conditions, mitigates the worst-case effects of parasitic self-discharge, and opens the path toward implementing fast and efficient neural networks on organic neuromorphic hardware.

cs.ET

Multi-scale membrane process optimization with high-fidelity ion transport models through machine learning

Innovative membrane technologies optimally integrated into large separation process plants are essential for economical water treatment and disposal. However, the mass transport through membranes is commonly described by nonlinear differential-algebraic mechanistic models at the nano-scale, while the process and its economics range up to large-scale. Thus, the optimal design of membranes in process plants requires decision making across multiple scales, which is not tractable using standard tools. In this work, we embed artificial neural networks~(ANNs) as surrogate models in the deterministic global optimization to bridge the gap of scales. This methodology allows for deterministic global optimization of membrane processes with accurate transport models -- avoiding the utilization of inaccurate approximations through heuristics or short-cut models. The ANNs are trained based on data generated by a one-dimensional extended Nernst-Planck ion transport model and extended to a more accurate two-dimensional distribution of the membrane module, that captures the filtration-related decreasing retention of salt. We simultaneously design the membrane and plant layout yielding optimal membrane module synthesis properties along with the optimal plant design for multiple objectives, feed concentrations, filtration stages, and salt mixtures. The developed process models and the optimization solver are available open-source, enabling computational resource-efficient multi-scale optimization in membrane science.

physics.comp-ph

Cell barrier characterization in transwell inserts by electrical impedance spectroscopy

We describe an impedance-based method for cell barrier integrity testing. A four-electrode electrical impedance spectroscopy (EIS) setup can be realized by simply connecting a commercial chopstick-like electrode (STX-1) to a potentiostat allowing monitoring cell barriers cultivated in transwell inserts. Subsequent electric circuit modeling of the electrical impedance results the capacitive properties of the barrier next to the well-known transepithelial electrical resistance (TEER). The versatility of the new method was analyzed by the EIS analysis of a Caco-2 monolayer in response to (a) different membrane coating materials, (b) two different permeability enhancers ethylene glycol-bis(2-aminoethylether)-N,N,N',N'-tetraacetic acid (EGTA) and saponin, and (c) sonoporation. For the different membrane coating materials, the TEERs of the standard and new protocol coincide and increase during cultivation, while the capacitance shows a distinct maximum for three different surface materials (no coating, Matrigel, and collagen I). The permeability enhancers cause a decline in the TEER value, but only saponin alters the capacitance of the cell layer by two orders of magnitude. Hence, cell layer capacitance and TEER represent two independent properties characterizing the monolayer. The use of commercial chopstick-like electrodes to access the impedance of a barrier cultivated in transwell inserts enables remarkable insight into the behavior of the cellular barrier with no extra work for the researcher. This simple method could evolve into a standard protocol used in cell barrier research.

physics.app-ph

Flow-electrode capacitive deionization enables continuous and energy-efficient brine concentration

Many industrial and agricultural applications require the treatment of water streams containing high concentrations of ionic species for closing material cycles. High concentration factors are often desired, but hard to achieve with established thermal or membrane-based water treatment technologies at low energy consumptions. Capacitive deionization processes are normally assumed as relevant for the treatment of low salinity solutions only. Flow-electrode capacitive deionization (FCDI), on the other hand, is an electrically driven water desalination technology, which allows the continuous desalination and concentration of saline water streams even at elevated salinities. Ions are adsorbed electrostatically in pumpable carbon flow electrodes, which enable a range of new process designs. In this article, it is shown that continuously operated FCDI systems can be applied for the treatment of salt brines. Concentrations of up to 291.5~g/L NaCl were reached in the concentrate product stream. Based on this, FCDI is a promising technology for brine treatment and salt recovery. Additionally, a reduction of the energy demand by more than 70% is demonstrated by introducing multiple cell pairs into a continuous FCDI system. While the economic feasibility is not investigated here, the results show that FCDI systems may compete with established technologies regarding their energy demand.

physics.app-ph

Membrane-electrode assemblies for flow-electrode capacitive deionization

Scale-up of flow-electrode capacitive deionization is hindered due to the reliance on thick brittle graphite current collectors. Inspired by developments of electrochemical technologies we present the use of flexible membrane electrode assemblies (MEA) to solve these limitations. We tested different carbon-fiber fabrics as current collectors and laminated them successfully with ion-exchange membranes. The use of thinner ion-exchange membranes is now possible due to the reinforcement with the carbon fiber fabric. Desalination experiments reveal that a MEA setup can achieve salt transfer rates equal to standard setups. Hence, we deduce that charge percolation also acts outside the electric field. In a single point of contact, ionic and electric charges are exchanged at the carbon surface of the MEA. The use of thinner membranes leads to a reduced potential drop. Together with a more homogeneous electric field across the feed water section, this can compensate for the reduction of contact surface between flow electrode and current collector.

physics.app-ph

A mini-module with built-in spacers for high-throughput ultrafiltration

Ultrafiltration membrane modules suffer from a permeate flow decrease arising during filtration and caused by concentration polarization and fouling in, e.g., fermentation broth purification. Such performance losses are frequently mitigated by manipulating the hydrodynamic conditions at the membrane-fluid interface using, e.g., mesh spacers acting as static mixers. This additional element increases manufacturing complexity while improving mass transport in general, yet accepting their known disadvantages such as less transport in dead zones. However, the shape of such spacers is limited to the design of commercially available spacer geometries. Here, we present a methodology to design an industrially relevant mini-module with an optimized built-in 3D spacer structure in a flat-sheet ultrafiltration membrane module to eliminate the spacer as a separate part. Therefore, the built-in structures have been conceptually implemented through an in-silico design in compliance with the specifications for an injection molding process. Ten built-in structures were investigated in a digital twin of the mini-module by 3D-CFD simulations to select two options, which were then compared to the empty feed channel regarding mass transfer. Subsequently, the simulated flux increase was experimentally verified during bovine serum albumin (BSA) filtration. The new built-in sinusoidal corrugation outperforms conventional mesh spacer inlays by up to 30% higher permeation rates. The origin of these improvements is correlated to the flow characteristics inside the mini-module as visualized online and in-situ by low-field and high-field magnetic resonance imaging velocimetry (flow-MRI) during pure water permeation.

physics.flu-dyn

In-situ investigation of wetting patterns in polymeric multibore membranes via magnetic resonance imaging

Wetting of the membrane to displace air or conditioning liquids is important to exploit the complex porosity of a filtration membrane. This study reveals the details of wetting in multibore membrane-based filtration modules. Using magnetic resonance imaging (MRI), we quantify the fluid distribution patterns during initial membrane wetting in dead-end permeation mode. The spatio-temporal evolution of aqueous copper sulfate solution wetting the membrane fibers was investigated as a function of the applied flux, packing density, and position along the membrane module length. Three initial wetting conditions were examined: delivery-state membranes, ethanol-washed and dried (air-filled) membranes, and ethanol-filled membranes. Significant changes in wetting patterns were observed due to interfacial and polymer swelling effects. This in-situ investigation reveals a slow wetting progression over six hours and more to obtain complete wetting, even at high fluxes of 200 LMH. However, an increased flux leads to faster wetting kinetics as the evolving wetting patterns are flux dependent. The packing density of the multibore fibers additionally impacts the wetting kinetics by shifting the prevalent pressure conditions. Although in dead-end mode, the wetting progression is non-uniform along the membrane module length. In addition to this parameter study, different pre-wetting agents' effect on the displacement behavior was investigated in depth. This study helps to understand (a) complex wetting phenomena inside multibore membranes in dead-end filtration, (b) the membranes' interaction with their surroundings due to neighboring membranes, and (c) the effect of the used fluid system for displacement on the resulting wetting patterns.

physics.app-ph

How does porosity heterogeneity affect the transport properties of multibore filtration membranes?

The prediction of pressure and flow distributions inside porous membranes is important if the geometry deviates from single-bore tubular geometries. This task remains challenging, especially when considering local porosity variations caused by lumen- and shell-side membrane skins and macro- and micro-void structures, all of them present in multibore membranes. This study analyzes pure water forward and reverse permeation and backwashing phenomena for a polymeric multibore membrane with spatially-varying porosity and permeability properties using computational fluid dynamics simulations. The heterogeneity of porosity distribution is experimentally characterized by scanning electron microscopy scans and reconstructed cuboids of X-ray micro-computed tomography scans. The reconstructed cuboids are used to determine porosity, pore size distribution, and intrinsic permeability in the membrane's porous structure in all spatial directions. These position-dependent properties are then applied to porous media flow simulations of the whole membrane domain with different properties for separation layer, support structure, and outside skin layer. Various cases mimicking the pure water permeation, fouling, and backwashing behavior of the membrane are simulated and compared to previously obtained MRI measurements. This work reveals (a) anisotropic permeability values and isoporosity in all directions and (b) differing contributions of each lumen channel to the total membrane performance, depending on the membrane-skin's properties. This study encourages to pertain the quest of understanding the interaction of spatially distributed membrane properties and the overall membrane module performance of multibore membranes.

physics.flu-dyn

Direct 3D observation and unraveling of electroconvection phenomena during concentration polarization at ion-exchange membranes

A decade ago, two-dimensional microscopic flow visualization proved the theoretically predicted existence of electroconvection roles as well as their decisive role in destabilizing the concentration polarization layer at ion-selective fluid/membrane interfaces. Electroconvection induces chaotic flow vortices injecting volume having bulk concentration into the ion-depleted diffusion layer at the interface. Experimental quantification of these important flow patterns have so far only been carried out in 2D. Numerical direct simulations suggest 3D features, yet experimental proof is lacking. 3D simulations are also limited in covering extended spacial and temporal scales. This study presents a new comprehensive experimental method for the time-resolved recording of the 3D electroconvective velocity field near a cation-exchange membrane. For the first time, the spatio-temporal velocity field can be visualized in 3D at multiples of the overlimiting current density. In contrast to today's simulations, these experiments cover length and time scales typical for actual electrodialytic membrane processes. We visualize coherent vortex structures and reveal the changes in the velocity field and its statistics during the transition from vortex rolls to vortex rings with increasing current density. The transition is characterized by changes in the rotational direction, mean square velocity, and temporal energy spectrum with only little influence on the spatial spectrum. These findings indicate a more significant impact of EC's structural change on the mean square velocities and temporal spectra than on the spatial spectra. This knowledge is a prerequisite for engineering ion-selective surfaces that will enable the operation of electrically driven processes beyond the diffusion-limited Nernst regime.

physics.flu-dyn

3D Nanofabrication inside rapid prototyped microfluidic channels showcased by wet-spinning of single micrometre fibres

Microfluidics is an established multidisciplinary research domain with widespread applications in the fields of medicine, biotechnology and engineering. Conventional production methods of microfluidic chips have been limited to planar structures, preventing the exploitation of truly three-dimensional architectures for applications such as multi-phase droplet preparation or wet-phase fibre spinning. Here the challenge of nanofabrication inside a microfluidic chip is tackled for the showcase of a spider-inspired spinneret. Multiphoton lithography, an additive manufacturing method, was used to produce free-form microfluidic masters, subsequently replicated by soft lithography. Into the resulting microfluidic device, a threedimensional spider-inspired spinneret was directly fabricated in-chip via multiphoton lithography. Applying this unprecedented fabrication strategy, the to date smallest printed spinneret nozzle is produced. This spinneret resides tightly sealed, connecting it to the macroscopic world. Its functionality is demonstrated by wet-spinning of single-digit micron fibres through a polyacrylonitrile coagulation process induced by a water sheath layer. The methodology developed here demonstrates fabrication strategies to interface complex architectures into classical microfluidic platforms. Using multiphoton lithography for in-chip fabrication adopts a high spatial resolution technology for improving geometry and thus flow control inside microfluidic chips. The showcased fabrication methodology is generic and will be applicable to multiple challenges in fluid control and beyond.

physics.app-ph

Fouling mitigation in tubular membranes by 3D-printed turbulence promoters

Despite intensive research, fouling remains a severe problem in membrane filtration. It is often controlled by applying turbulent flow which requires a higher energy consumption. So-called turbulence promoters or static mixers can be inserted into the flow channel of tubular membranes. They deflect the fluid, induce vortices, enhance particle back-transport and increase the shear rate at the membrane surface, thus mitigating fouling. However, little is known how the geometry of such turbulence promotors affects the reduction of fouling. We investigate how different 3D-printed mixer geometries affect fouling and improve the flux during filtration with humic acid. Most mixer geometries used in the present study are based on a twisted tape; a Kenics static mixer is investigated as well. Static mixers with changing diameter prove to be less effective than twisted tape mixers with constant diameter which lead to an increase in permeate flux of around 130%. The highest flux improvement of 140% can be reached by applying a Kenics mixer. Regardless of their geometry, all investigated static mixer cause higher permeate fluxes at same specific energy consumption. Again, the Kenics mixer proves to be the most efficient static mixer. The presented mixer geometries can be fabricated with undercut injection molding techniques and represent a simple and viable option to make tubular membrane based filtration processes more efficient.

physics.flu-dyn

3D-printed conductive static mixers enable all-vanadium redox flow battery using slurry electrodes

State-of-the-art all-vanadium redox flow batteries employ porous carbonaceous materials as electrodes. The battery cells possess non-scalable fixed electrodes inserted into a cell stack. In contrast, a conductive particle network dispersed in the electrolyte, known as slurry electrode, may be beneficial for a scalable redox flow battery. In this work, slurry electrodes are successfully introduced to an all-vanadium redox flow battery. Activated carbon and graphite powder particles are dispersed up to 20 wt% in the vanadium electrolyte and charge-discharge behavior is inspected via polarization studies. Graphite powder slurry is superior over activated carbon with a polarization behavior closer to the standard graphite felt electrodes. 3D-printed conductive static mixers introduced to the slurry channel improve the charge transfer via intensified slurry mixing and increased surface area. Consequently, a significant increase in the coulombic efficiency up to 95% and energy efficiency up to 65% is obtained. Our results show that slurry electrodes supported by conductive static mixers can be competitive to state-of-the-art electrodes yielding an additional degree of freedom in battery design. Research into carbon properties (particle size, internal surface area, pore size distribution) tailored to the electrolyte system and optimization of the mixer geometry may yield even better battery properties.

physics.app-ph

Sinusoidal shaped hollow fibers for enhanced mass transfer

Inducing secondary flows and vortices is known to enhance mass transport. They can be imposed by structured flow channels for instance. In particular, these vortices reduce fouling and concentration polarization. In this work we present a new method of producing hollow fiber membranes with a sinusoidal change in diameter over the fiber length. We engineered a pulsation module that imposes a sinusoidally fluctuating bore liquid flow rate. Harmonic bore flow conditions can be varied over a wide range. The fluctuating bore liquid flow rate translates into axial membrane properties varying with respect to inner bore diameter and wall thickness. The resulting narrowing and widening of the membrane lumen channel are hypothesized to induce secondary vortices to the liquid inside the membrane lumen known as the Bellhouse effect. Improved oxygen transport from shell-to-lumen side prove superiority over straight hollow fiber membranes in G/L absorption process. We anticipate the dynamic flow module to be easily integrated into currently existing hollow fiber membrane spinning processes.

physics.flu-dyn

Flow and filtration imaging of single use sterile membrane filters

Sterile filters incorporating endotoxin adsorption function emerged recently to pretreat dialysate liquids fed to a hemodialysis filtration process. Their application significantly enhances the survival rate during dialysis treatment as they function as sterile filters as well as an endotoxin adsorber. Little is known about the fluid flow distribution in such single use membrane modules. We report a detailed analysis of the local 3D flow field distribution in such membrane modules using magnetic resonance flow imaging. Next to pure water filtration representing the application case of endotoxin adsorption from an already pure liquid, we also used the module as a filtration device rejecting for instance colloidal silica. Such experiments performed in-situ allow the quantification of cake layer development and its concomitant redistribution of the flow field. Particularly novel is the quantification of the time evolution of local permeate flux distribution. These detailed insights of this study encourage the use of flow-MRI when designing and applying new membrane module configurations.

physics.ins-det

What are the microscopic events of colloidal membrane fouling?

Due to the complex interplay between surface adsorption and hydrodynamic interactions, representative microscopic mechanisms of colloidal membrane fouling are still not well understood. Numerical simulations overcome experimental limitations such as the temporal and spatial resolution of microscopic events during colloidal membrane fouling: they help to gain deeper insight into fouling processes. This study uses coupled computational fluid dynamics - discrete element methods (CFD-DEM) simulations to examine mechanisms of colloidal fouling in a microfluidic architecture mimicking a porous microfiltration membrane. We pay special attention to how particles can overcome energy barriers leading to adsorption and desorption with each other and with the external and internal membrane surface. Interparticle interaction leads to a transition from the secondary to the primary minimum of the DLVO potential. Adsorbed particles can show re-entrainment or they can glide downstream. Since particles mainly re-suspend as clusters, the inner pore geometry significantly affects the fouling behavior. The findings allow a basic understanding of microscopic fouling events during colloidal filtration. The methodology enables future systematic studies on the interplay of hydrodynamic conditions and surface energy contributions represented by potentials for soft and patchy colloids.

physics.comp-ph