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Abstract Separation and classification are important operations in particle technology, but they are still limited in terms of suspended particles in the micrometer and nanometer size-range. Electrical fields can be beneficial for sorting such particles according to material properties. A mechanism based on strong and inhomogeneous fields is dielectrophoresis (DEP). It can be used to separate microparticles according to their material properties, such as conductivity and permittivity, by selectively trapping one particle type while the other can pass the separator. Conventional DEP-separators show either a limitation in throughput or frequency bandwidth. A low throughput limits the economical feasibility in many cases. A lower frequency bandwidth limits the variety of materials that can be sorted by DEP. To separate semiconducting particles from a mixture containing particles with higher conductivity according to their material, high frequencies are required. Possible applications are the separation of semiconducting and metallic carbon nanotubes or the separation of carbon-coated lithium iron phosphate particles from graphite in the recycling process of spent lithium-ion batteries. In this publication, we aim to display how to tune the electrical impedance of a high-throughput DEP separator based on custom-designed printed circuit boards to increase its frequency bandwidth. By adding inductors to the electrical circuit, we were able to increase the frequency bandwidth from 500 kHz to over 11 MHz. The experiments in this study act as proof-of-principle. Furthermore, a non-deterministic way to increase the impedance of the setup is shown, yielding a maximum frequency of 39.16 MHz.

The sorting of nano- and microparticles according to different properties is an industrially highly relevant but partly unsolved problem. In this study, we investigate the sorting of a complex microparticle mixture on the basis of their different properties by insulator-based dielectrophoretic filtration at high throughput. We demonstrate here that such a high selectivity demanding sorting process is possible in a single device thanks to recent advances in the development of dielectrophoretic filters, which has been shown using simple binary mixtures in a previous study. In that study, a filter with a regular structure (mesh) is introduced with pores several orders of magnitude larger than the target particles so that the particles are trapped solely by the action of positive dielectrophoresis. In this work, we demonstrate the improvement of the filter design, by comparing the trapping behavior to an alternative, irregular porous ceramic structure as a filter medium. A significantly higher selectivity for positive dielectrophoresis could be reached using the regular mesh structure. This high selectivity enables a stepwise operation mode, combining a selective trapping step and several subsequent selective remobilization steps. A mixture of polystyrene-based particles could be sorted by size, shape, and surface coating in one pass of the filter. The proposed method is therefore a promising technique to efficiently create highly specific particle systems in the future.

Abstract The interaction of rarefied gases with functionalized surfaces is of great importance in technical applications such as gas separation membranes and catalysis. To investigate the influence of functionalization and rarefaction on gas flow rate in a defined geometry, pressure-driven gas flow experiments with helium and carbon dioxide through plain and alkyl-functionalized microchannels are performed. The experiments cover Knudsen numbers from 0.01 to 200 and therefore the slip flow regime up to free molecular flow. To minimize the experimental uncertainty which is prevalent in micro flow experiments, a methodology is developed to make optimal use of the measurement data. The results are compared to an analysis-based hydraulic closure model (ACM) predicting rarefied gas flow in straight channels and to numerical solutions of the linearized S-model and BGK kinetic equations. The experimental data shows that if there is a difference between plain and functionalized channels, it is likely obscured by experimental uncertainty. This stands in contrast to previous measurements in smaller geometries and demonstrates that the surface-to-volume ratio of 0.4 $$\upmu$$ μ m $$^{-1}$$ - 1 seems to be too small for the functionalization to have a strong influence and highlights the importance of geometric scale for surface effects. These results also shed light on the molecular reflection characteristics described by the TMAC.

The development of highly selective separation processes is a focus of current research. In 2016, the German Science Foundation funded a priority program SPP 2045 “MehrDimPart—highly specific multidimensional fractionation of fine particles with technical relevance” that aims to develop new or enhance existing approaches for the separation of nano- and micrometer-sized particles. Dielectrophoretic separators achieve highly selective separations of (bio-)particles in microfluidic devices or can handle large quantities when non-selective separation is sufficient. Recently, separator designs were developed that aim to combine a high throughput and high selectivity. Here, we summarize the development from a microfluidic fast chromatographic separation via frequency modulated dielectrophoretic particle chromatography (DPC) toward a macrofluidic high throughput separation. Further, we provide a starting point for future work by providing new experimental data demonstrating for the first time the trapping of 200 nm polystyrene particles in a dielectrophoretic high-throughput separator that uses printed circuit boards as alternatives for expensive electrode arrays.

Abstract NADH plays a crucial role in many enzymatically catalysed reactions. Due to the high costs of NADH a regeneration mechanism of this cofactor can enlarge the applications of enzymatic reactions dramatically. This paper gives a thorough system analysis of the mediated electrochemical regeneration of active NADH using cyclic voltammograms and potentiostatic measurements with varying pH, electrode potential, and electrolyte solution, highlighting the system’s limiting conditions, elucidating optimal working parameters for the electrochemical reduction of NAD+, and bringing new insight on the oxidation of inactive reduction products. Using [Cp*Rh(bpy)Cl]+ as an electron mediator dramatically increases the percentage of enzymatically active electrochemically reduced NADH from 15% (direct) to 99% (mediated) with a faradaic efficiency of up to 86%. Furthermore, investigations of the catalytic mechanisms of [Cp*Rh(bpy)Cl]+ clarifies the necessary conditions for its functioning and questions the proposed reaction mechanism by two-step reduction where first the mediator is reduced and then brought in contact with NAD+.

Lithium-ion batteries (LIB) are integrated in a wide range of electronic devices that are an integral part of our modern world. Growing number of LIBs that reach their end of life demands development of effective recycling strategies to recover rare and/or expensive battery materials. Dielectrophoresis (DEP) is an electrokinetic particle manipulation technique that allows for selective particle separation based on properties, such as material, size, and shape. Here, we demonstrate separation of lithium iron phosphate (LFP) and graphite using dielectrophoretic filtration. Graphite and LFP are two common LIB anode and cathode materials. We demonstrate both: non-selective separation using pure suspensions of both graphite and uncoated LFP and an isolation of graphite from a mixture of uncoated LFP and graphite. We confirmed that LFP shows negative DEP while graphite shows positive DEP. We determined the conductivity at which material-selective polarisability-based separation becomes possible, thus, proofing the concept of sorting of non-carbon coated lithium iron phosphate (LiFePO4) and graphite. Graphite generally shows high separation efficiency of 70–100 %. Using atomic absorption spectroscopy (AAS), we found a low separation efficiency of LFP between 1 and 15 % from a mixture of graphite and LFP. These results reinforce one possibility of using DEP filtration as a potential method for direct physical recycling of battery material waste.

Abstract Particle separation is an essential part of many processes. One mechanism to separate particles according to size, shape, or material properties is dielectrophoresis (DEP). DEP arises when a polarizable particle is immersed in an inhomogeneous electric field. DEP can attract microparticles toward the local field maxima or repulse them from these locations. In biotechnology and microfluidic devices, this is a well-described and established method to separate (bio-)particles. Increasing the throughput of DEP separators while maintaining their selectivity is a field of current research. In this study, we investigate two approaches to increase the overall throughput of an electrode-based DEP separator that uses selective trapping of particles. We studied how particle concentration affects the separation process by using two differently-sized graphite particles. We showed that concentrations up to 800 mg/L can be processed without decreasing the collection rate depending on the particle size. As a second approach to increase the throughput, parallelization in combination with two four-way valves, relays, and stepper motors was presented and successfully tested to continuously separate conducting from non-conducting particles. By demonstrating possible concentrations and enabling a semi-continuous process, this study brings the low-cost DEP setup based on printed circuit boards one step closer to real-world applications. The principle for semi-continuous processing is also applicable for other DEP devices that use trapping DEP.

The generation of high-quality volume meshes out of µCT data can be a challenging task that is mandatory to perform CFD simulations of fluid flows within or around scanned objects. Despite the growing relevance of CT-based CFD simulations, there is still a lack of a standardized, free-to-use workflow. In this work, an open-source based workflow is presented, which covers all steps from the CT image stack to a volume mesh in the end. The software packages ImageJ, ParaView, and Blender are used for surface reconstruction and processing of µCT data; resulting meshes are evaluated regarding geometric parameters, surface fidelity, and used memory. For volume meshing, the mesh generator snappyHexMesh implemented in OpenFOAM is used. A detailed description of this workflow is provided in the Supplementary Materials. We demonstrate how potential pitfalls and shortcomings can be avoided and how surface smoothing is especially important to preserve the surface area of scanned objects. We use CT data of a 10 ppi open cell foam to illustrate that data decimation can reduce the required time for the volume meshing by up to 45% and RAM up to 75%. The resulting meshes are used to simulate flow fields and heat transport with a surface heat source. The resulting temperature fields show that differences in the surface area and recesses in an unsmoothed mesh can affect the outcome of heat transport simulations, highly relevant for reactive CFD simulations. The results highlight the quality of our workflow’s outcome, which can help engineers that rely on CT reconstruction processes, also for other applications.

Abstract Electrochemical NAD+ reduction is a promising method to regenerate NADH for enzymatic reactions. Many different electrocatalysts have been tested in the search for high yields of the 1,4-isomer of NADH, the active NADH, but aside from electrode material, other system parameters such as pH, electrode potential and educt concentration also play a role in NADH regeneration. The effect of these last three parameters and the mechanisms behind their influence on NADH regeneration was systematically studied and presented in this paper. With percentages of active NADH ranging from 10 to 70% and faradaic efficiencies between 1 and 30%, it is clear that all three system parameters drastically affect the reaction outcome. As a proof of principle, the NAD+ reduction in the presence of pyruvate and lactate dehydrogenase was performed. It could be shown that the electrochemical NADH regeneration can also be done successfully in parallel to enzymatically usage of the regenerated cofactor.

This study outlines the design, construction and characterization of a tailored low-cost linear birdcage (BC) resonator for magnetic resonance imaging at 7T. Typically, different BC designs found in literature are well described in theory but lack crucial information for practical realization. This is challenging, as theoretical and practical aspects often differ greatly from each other, especially in the field of high frequency technology. We propose a simple and open-source 3D printable design which results in a working BC if the instructions in this publication are followed. The aim is to open up the possibility of building a functioning BC with simple means and a budget below 750€, even for users without a great deal of expertise in MRI coil building. We demonstrate that the BC can achieve a good B1 field homogeneity using the double angle method. The proposed design is qualitatively compared to a commercially available resonator. Both perform equally well in terms of SNR and image quality.

Abstract Separation of (biological) particles ( $$\ll {10}~{\upmu }\text {m}$$ ≪ 10 μ m ) according to size or other properties is an ongoing challenge in a variety of technical relevant fields. Dielectrophoresis is one method to separate particles according to a diversity of properties, and within the last decades a pool of dielectrophoretic separation techniques has been developed. However, many of them either suffer selectivity or throughput. We use simulation and experiments to investigate retention mechanisms in a novel DEP scheme, namely, frequency-modulated DEP. Results from experiments and simulation show a good agreement for the separation of binary PS particles mixtures with respect to size and more importantly, for the challenging task of separating equally sized microparticles according to surface functionalization alone. The separation with respect to size was performed using 2 $${\upmu }$$ μ m and 3 $${\upmu }$$ μ m sized particles, whereas separation with respect to surface functionalization was performed with 2 $${\upmu }$$ μ m particles. The results from this study can be used to solve challenging separation tasks, for example to separate particles with distributed properties.

There is an increasing interest in algae-based raw materials for medical, cosmetic or nutraceutical applications. Additionally, the high diversity of physicochemical properties of the different algal metabolites proposes these substances from microalgae as possible additives in the chemical industry. Among the wide range of natural products from red microalgae, research has mainly focused on extracellular polymers for additive use, while this study also considers the cellular components. The aim of the present study is to analytically characterize the extra- and intracellular molecular composition from the red microalga Dixoniella grisea and to evaluate its potential for being used in the tribological industry. D. grisea samples, fractionated into extracellular polymers (EPS), cells and medium, were examined for their molecular composition. This alga produces a highly viscous polymer, mainly composed of polysaccharides and proteins, being secreted into the culture medium. The EPS and biomass significantly differed in their molecular composition, indicating that they might be used for different bio-additive products. We also show that polysaccharides and proteins were the major chemical compounds in EPS, whereas the content of lipids depended on the separation protocol and the resulting product. Still, they did not represent a major group and were thus classified as a potential valuable side-product. Lyophilized algal fractions obtained from D. grisea were found to be not toxic when EPS were not included. Upon implementation of EPS as a commercial product, further assessment on the environmental toxicity to enchytraeids and other soil organisms is required. Our results provide a possible direction for developing a process to gain an environmentally friendly bio-additive for application in the tribological industry based on a biorefinery approach.

Heat Treatment of martensitic stainless steels is used to increase the hardness that is caused by several microstructure changes. But such a treatment does affect both mechanical properties and corrosion resistance. Existing studies about the effect of austenitizing on the material properties and the corrosion resistance show contradictory results. Here we reveal the different effects of austenitizing on the passive layer of stainless steel and thus the corrosion resistance, thermodynamic phase calculations, microstructure investigations and various electrochemical measurements are performed. By potentiodynamic polarization scans the pitting potential, the critical pitting potential and the corrosion current are determined. Impedance spectroscopy are used to gain deeper insight into the passive layer properties. The results show a strong dependency of the corrosion behavior on the heat treatment where the governing corrosion mechanism are affected differently.

Structured open-cell foam reactors are promising for managing highly exothermic reactions such as CO2 methanation due to their excellent heat transport properties. Especially at low flow rates and under dynamic operation, foam-based reactors can be advantageous over classic fixed-bed reactors. To efficiently design the catalyst carriers, a thorough understanding of heat transport mechanisms is needed. So far, studies on heat transport in foams have mostly focused on the solid phase and used air at atmospheric pressure as fluid phase. With the aid of pore-scale 3d CFD simulations, we analyze the effect of the fluid properties on heat transport under conditions close to the CO2 methanation reaction for two different foam structures. The exothermicity is mimicked via volumetric uniformly distributed heat sources. We found for foams that are designed to be used as catalyst carriers that the working pressure range and the superficial velocity influence the dominant heat removal mechanism significantly. In contrast, the influence of fluid type and gravity on heat removal is small in the range relevant for heterogeneous catalysis. The findings might help to facilitate the design-process of open-cell foam reactors and to better understand heat transport mechanisms in foams.

The heat transport management in catalytic reactors is crucial for the overall reactor performance. For small-scale dynamically-operated reactors, open-cell foams have shown advantageous heat transport characteristics over conventional pellet catalyst carriers. To design efficient and safe foam reactors as well as to deploy reliable engineering models, a thorough understanding of the three heat transport mechanisms, i.e., conduction, convection, and thermal radiation, is needed. Whereas conduction and convection have been studied extensively, the contribution of thermal radiation to the overall heat transport in open-cell foam reactors requires further investigation. In this study, we simulated a conjugate heat transfer case of a µCT based foam reactor using OpenFOAM and verified the model against a commercial computational fluid dynamics (CFD) code (STAR-CCM+). We further explicitly quantified the deviation made when radiation is not considered. We studied the effect of the solid thermal conductivity, the superficial velocity and surface emissivities in ranges that are relevant for heterogeneous catalysis applications (solid thermal conductivities 1–200 W m−1 K−1; superficial velocities 0.1–0.5 m s−1; surface emissivities 0.1–1). Moreover, the temperature levels correspond to a range of exo- and endothermal reactions, such as CO2 methanation, dry reforming of methane, and methane steam reforming. We found a significant influence of radiation on heat flows (deviations up to 24%) and temperature increases (deviations up to 400 K) for elevated temperature levels, low superficial velocities, low solid thermal conductivities and high surface emissivities.

The separation of microparticles with respect to different properties such as size and material is a research field of great interest. Dielectrophoresis, a phenomenon that is capable of addressing multiple particle properties at once, can be used to perform a chromatographic separation. However, the selectivity of current dielectrophoretic particle chromatography (DPC) techniques is limited. Here, we show a new approach for DPC based on differences in the dielectrophoretic mobilities and the crossover frequencies of polystyrene particles. Both differences are addressed by modulating the frequency of the electric field to generate positive and negative dielectrophoretic movement to achieve multiple trap-and-release cycles of the particles. A chromatographic separation of different particle sizes revealed the voltage dependency of this method. Additionally, we showed the frequency bandwidth influence on separation using one example. The DPC method developed was tested with model particles, but offers possibilities to separate a broad range of plastic and metal microparticles or cells and to overcome currently existing limitations in selectivity.

The formation and breakdown of passive layers due to pitting corrosion are a major cause of failure of metal structures. The investigation of passivation and pitting corrosion requires two different electrochemical measurements and is therefore a time consuming process. To reduce time in material characterization and to study the interactions of both mechanisms, here, a combined experiment addressing both phenomena is introduced. In the presented electrolyte the different corrosion mechanisms are distinguished and investigated by cyclic voltammograms and polarization scans. The measurements show a passive area, metastable pit growth, and pitting corrosion as well as repassivation. The pitting corrosion is separated from additional dissolution processes and the standard deviation of the corrosion potential is smaller than in other electrolytes. Both passivation and pitting corrosion can be observed in one measurement without additional corrosion attacks. The deviation between different measurements of the same steel is small; this is helpful for the screening of similar materials.

Microscopic multiphase flows have gained broad interest due to their capability to transfer processes into new operational windows and achieving significant process intensification. However, the hydrodynamic behavior of Taylor droplets is not yet entirely understood. In this work, we introduce a model to determine the excess velocity of Taylor droplets in square microchannels. This velocity difference between the droplet and the total superficial velocity of the flow has a direct influence on the droplet residence time and is linked to the pressure drop. Since the droplet does not occupy the entire channel cross-section, it enables the continuous phase to bypass the droplet through the corners. A consideration of the continuity equation generally relates the excess velocity to the mean flow velocity. We base the quantification of the bypass flow on a correlation for the droplet cap deformation from its static shape. The cap deformation reveals the forces of the flowing liquids exerted onto the interface and allows estimating the local driving pressure gradient for the bypass flow. The characterizing parameters are identified as the bypass length, the wall film thickness, the viscosity ratio between both phases and the C a number. The proposed model is adapted with a stochastic, metaheuristic optimization approach based on genetic algorithms. In addition, our model was successfully verified with high-speed camera measurements and published empirical data.

The physicochemical nature of chitin and chitosan, which influences the biomedical activity of these compounds, is strongly related to the source of chitin and the conditions of the chitin/chitosan production process. Apart from widely described key factors such as weight-averaged molecular weight (MW) and degree of N-acetylation (DA), other physicochemical parameters like polydispersity (MW/MN), crystallinity or the pattern of acetylation (PA) have to be taken into consideration. From the biological point of view, these parameters affect a very important factor—the solubility of chitin and chitosan in water and organic solvents. The physicochemical properties of chitosan solutions can be controlled by manipulating solution conditions (temperature, pH, ionic strength, concentration, solvent). The degree of substitution of the hydroxyl and the amino groups or the degree of quaternization of the amino groups also influence the mechanical and biological properties of chitosan samples. Finally, a considerable research effort has been directed towards developing safe and efficient chitin/chitosan-based products because many factors, like the size of nanoparticles, can determine the biomedical characteristics of medicinal products. The influence of these factors on the biomedical activity of chitin/chitosan-based products is presented in this report in more detail.

A frontier to be conquered in the field of membrane technology is related to the very limited scientific base for the rational and task-specific design of membranes. This is especially true for nanofiltration membranes with properties that are based on several solute-membrane interaction mechanisms. “Thinking in terms of Structure-Activity-Relationships” (T-SAR) is a methodology which applies a systematic analysis of a chemical entity based on its structural formula. However, the analysis become more complex with increasing size of the molecules considered. In this study, T-SAR was combined with classical membrane characterization methods, resulting in a new methodology which allowed us not only to explain membrane characteristics, but also provides evidence for the importance of the chemical structure for separation performance. We demonstrate an application of the combined approach and its potential to discover stereochemistry, molecular interaction potentials, and reactivity of two FilmTec nanofiltration membranes (NF-90 and NF-270). Based on these results, it was possible to predict both properties and performance in the recovery of hydrophobic ionic liquids from aqueous solution.

Chitin, the second most important natural polymer in the world, and its N-deacetylated derivative chitosan, have been identified as versatile biopolymers for a broad range of applications in medicine, agriculture and the food industry. Two of the main reasons for this are firstly the unique chemical, physicochemical and biological properties of chitin and chitosan, and secondly the unlimited supply of raw materials for their production. These polymers exhibit widely differing physicochemical properties depending on the chitin source and the conditions of chitosan production. The presence of reactive functional groups as well as the polysaccharide nature of these biopolymers enables them to undergo diverse chemical modifications. A complete chemical and physicochemical characterization of chitin, chitosan and their derivatives is not possible without using spectroscopic techniques. This review focuses on the application of spectroscopic methods for the structural analysis of these compounds.

The aggregation behavior of thirteen 1-alkyl-3-methylimidazolium based ionic liquids in aqueous solution is presented, considering variations of the alkyl side chain length as well as the anionic moiety. Cation and anion molecular volumes are selected as appropriate molecular descriptors. Additionally, the existing relationship between critical micelle concentration (CMC) and electrolyte concentration in solution is established, aiming to clarify ion effects. CMC values were obtained by measuring electrical conductivity and surface tension. It was confirmed that aggregation of ionic liquids in aqueous solution and in presence of inorganic salts is affected by the factors developed in this study.