Scientific publications

Translocation across barriers and through constrictions is a mechanism that is often used in vivo for transporting material between compartments. A specific example is apicomplexan parasites invading host cells through the tight junction that acts as a pore, and a similar barrier crossing is involved in drug delivery using lipid vesicles penetrating intact skin. Here, we use triangulated membranes and energy minimization to study the translocation of vesicles through pores with fixed radii. The vesicles bind to a lipid bilayer spanning the pore, the adhesion-energy gain drives the translocation, and the vesicle deformation induces an energy barrier. In addition, the deformation-energy cost for deforming the pore-spanning membrane hinders the translocation. Increasing the bending rigidity of the pore-spanning membrane and decreasing the pore size both increase the barrier height and shift the maximum to smaller fractions of translocated vesicle membrane. We compare the translocation of initially spherical vesicles with fixed membrane area and freely adjustable volume to that of initially prolate vesicles with fixed membrane area and volume. In the latter case, translocation can be entirely suppressed. Our predictions may help rationalize the invasion of apicomplexan parasites into host cells and design measures to combat the diseases they transmit.

Electrocoagulation (EC) technology features a promising prospect for coping with the formidable microplastics (MPs) pollution challenge, albeit the underlying abatement mechanism still needs to be further clarified. Accordingly, in this work, we evaluated the removal performance by EC for four typical MPs, including polyvinyl chloride (PVC), polystyrene (PS), polypropylene (PP), and polyethylene (PE). The Fourier transform infrared spectroscopies of MPs confirmed the presence of electrochemical oxidation during EC process, owing to its hydroxyl radical generation ability as demonstrated by the detected fluorescence spectroscopies and electron paramagnetic resonance results, which has been rarely reported in other works. Specifically, 21.2 ± 0.8 %, 10.8 ± 1.8 %, 15.6 ± 1.6 %, and 7.6 ± 1.4 % abatement efficiency for PVC, PS, PP, and PE, respectively, originated from the oxidation effect, and these values for flocculation effect were 77.2 ± 0.8 %, 74.0 ± 1.6 %, 70.8 ± 1.2 %, and 69.2 ± 1.2 %, successively. Many factors influence these differences, especially the MPs’ hydrophilicity, as it facilitates the mass transfer efficiency between MPs (like PVC and PP) and the generated flocs or radicals. To lay a foundation for practical application, we also optimized the operation parameters, demonstrating the wise choice of pH 7 to maintain a balance between the oxidation and flocculation effect. Therefore, we believe our work provides a good reference for promoting MPs abatement efficiency and elucidating the corresponding mechanism, especially the contribution of the oxidation part by EC.

Materials that can be switched between a polycationic/antimicrobial and a polyzwitterionic/protein-repellent state have important applications, e.g., as biofilm-reducing coatings in medical devices. However, the lack of stability under storage and application conditions so far restricts the lifetime and efficiency of such materials. In this work, a polynorbornene-based polycarboxybetaine with an optimized molecular structure for improved hydrolytic stability is presented. The polymer is fully characterized on the molecular level. Surface-attached polymer networks are obtained by spin-coating and UV cross-linking. These coatings are highly uniform and demonstrate charge-switching in zeta-potential studies. Storage stability in the dry state, as well as in aqueous systems at pH 4.5 and 7.4 for 28 days, is demonstrated. At pH 8, hydrolytic degradation is observed. Overall, the materials are substantially more stable than the corresponding ester-based systems.

The water dynamics in a nanocomposite film that consists of the electrically conductive poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and cellulose nanofibrils (CNFs) have been investigated during three cycles of exposure to low and high relative humidity (RH = 5% and 85%, respectively) using quasi-elastic neutron scattering (QENS). The obtained dynamical structure factors are transformed into the imaginary part of the dynamic susceptibility to better differentiate between the individual relaxation processes. In a humid environment, two different water species are present inside the films: fast-moving bulk water and slow-moving hydration water. During the first cycle, a large amount of hydration water enhances the polymer chain mobility, eventually leading to irreversible structural rearrangements within the film. In the subsequent cycles, we observed a release of all bulk water and portions of hydration water upon drying, along with an uptake of both water species in a humid environment. The relaxation times of hydration water diffusion as a function of momentum transfer can be described by a jump-diffusion model. The obtained jump lengths, residence times, and diffusion coefficients of hydration water suggest a change in the hydration layer upon drying: water molecules around hydrophobic groups are released from the film, while the hydrogen bonds between water and hydrophilic groups are sufficiently strong to keep these molecules inside the films, even in a dry state. The QENS results can be correlated to the structural and conductive properties. In the dry state, the low hydration water content and the absence of bulk water allow for improved wetting of the CNFs by PEDOT:PSS, which eventually increases the electrical conductivity of the films.

Wound healing is a dynamic biological process that leads to the repair of damaged body tissues and restores their ability to function as protective barriers. There are several approaches to handling and treating skin wounds; however, new and efficient procedures must be developed to cope with the inadequacies of the current methods, such as longer recovery time. In our novel research, we used NiSe NPs ointment and NiSe-incorporated PANI/PEO fibers for wound healing. The materials-related characteristics were studied by UV/visible spectroscopy, FTIR, SEM, DLS, and XRD. SEM images illustrate the rod-like structure of the NiSe, while bead-free NiSe-based PANI/PEO fibers are conformed from SEM with an average diameter of 330 nm. An average crystal size of 6.2 nm is measured from the XRD pattern. The antibacterial and antioxidant properties showed that NiSe-incorporated PANI/PEO fibers exhibited better response than NiSe NPs with less toxicity. NiSe NPs and NiSe-based PANI/PEO fibers give excellent wound healing potential of 89.5% ± 1.18% and 95.6% ± 0.25%, respectively. Healing response and tissue regeneration by NiSe-incorporated PANI/PEO fibers were evaluated clinically by using histopathology and interleukin-6, which indicated efficient and effective wound recovery.

Lithium-ion batteries play a crucial role in powering electric vehicles and portable electronics, making them indispensable in modern technology and driving a significant increase in global lithium demand. With more and more batteries reaching their end of life and the challenges of lithium extraction, including rising prices, geopolitical constraints, and environmental concerns, the efficient recovery of lithium from spent battery cells is crucial for sustainable battery recycling. While state-of-the-art battery recycling focuses mainly on pyro- and hydrometallurgical methods, electrochemical recycling methods can be an environmentally friendly, energy-efficient, and cost-effective alternative. This study optimizes an energy-efficient electrochemical method for selective LiCl extraction from leaching solutions derived from cathode materials of a typical battery cell format (lithium cobalt oxide (LCO)). This places our electrochemical separation within the hydrometallurgical processing of spent battery materials (black mass) and prior to subsequent lithium refining steps. Applying carbon-coated lithium iron phosphate (LFP) electrodes for selective lithium recovery yielded an average uptake capacity of 11.4 mgLi gLFP/C-1 over 300 cycles, maintaining a significant discharge capacity (30 mAh g-1) after 500 cycles.

This report is about the chemical formation of gels from ultrathin gold nanowires (AuNWs) and the gels’ properties. An excess of triphenylphosphine (PPh3) initiated the gelation of AuNWs with core diameters below 2 nm and an oleylamine (OAm) ligand shell dispersed in cyclohexane. The ligand exchange of OAm by PPh3 changes the AuNW-solvent interactions and leads to phase separation of the solvent to form a macroscopic gel. Small angle X-ray scattering and transmission electron microscopy indicate that hexagonal bundles in the original dispersion are dispersed, and the released nanowires entangle. Rheological analyses indicate that the resulting gel is stabilized both by physical entanglement and crosslinking of AuNWs by Van der Waals and π–π interactions. Chemically formed AuNW gels have solid-like properties and crosslinks that distinguish them from highly concentrated non-crosslinked AuNW dispersions. The AuNW gel properties can be tuned via the Au:PPh3 ratio, where smaller ratios led to stiffer gels with higher storage moduli.

Melt Electrowriting (MEW) is a powerful technique in tissue engineering, enabling the precise fabrication of scaffolds with complex geometries. One of the most important parameters of MEW is collector speed, which has been extensively studied in relation to critical translation speed. However, its influence on crystallinity was overlooked. Crystallinity is crucial for the mechanical properties and degradation behavior of the scaffolds. Therefore, in this study, we present how printing affects the crystallinity of fibers and the resulting mechanical properties of MEW scaffolds. In systematic analysis, we observed a significant reduction in scaffold crystallinity with increased speed, as evidenced by wide-angle X-ray scattering. This decrease in crystallinity was attributed to differences in cooling rates, impacting the polycaprolactone molecular orientation within the fibers. By using tensile testing, we observed the decrease in scaffold Young's modulus with increasing collector speed. Given the relation between crystallinity and mechanical properties of the material, we developed a finite element analysis model that accounts for changes in crystallinity by employing distinct bulk Young's modulus values to help characterize scaffold mechanical behavior under tensile loading. The model reveals insights into scaffold stiffness variation with different architectural designs. These insights offer valuable guidance for optimizing 3D printing to obtain scaffolds with desired mechanical properties.

Encapsulation of microbes in natural or synthetic matrices is a key aspect of engineered living materials, although the influence of such confinement on microbial behavior is poorly understood. A few recent studies have shown that the spatial confinement and mechanical properties of the encapsulating material significantly influence microbial behavior, including growth, metabolism, and gene expression. However, comparative studies within different bacterial species under identical confinement conditions are limited. In this study, Gram-negative Escherichia coli Nissle 1917 and Gram-positive Lactiplantibacillus plantarum WCFS1 were encapsulated in hydrogel matrices, and their growth, metabolic activity, and recombinant gene expression were examined under varying degrees of hydrogel stiffness, achieved by adjusting the polymer concentration and chemical cross-linking. Both bacteria grow from single cells into confined colonies, but more interestingly, in E. coli gels, mechanical properties influenced colony growth, size, and morphology, whereas this did not occur in L. plantarum gels. However, with both bacteria, increased matrix stiffness led to higher levels of recombinant protein production within the colonies. By measuring metabolic heat from the bacterial gels using the isothermal microcalorimetry technique, it was inferred that E. coli adapts to the mechanical restrictions through multiple metabolic transitions and is significantly affected by the different hydrogel properties. Contrastingly, both of these aspects were not observed with L. plantarum. These results revealed that despite both bacteria being gut-adapted probiotics with similar geometries, mechanical confinement affects them considerably differently. The weaker influence of matrix stiffness on L. plantarum is attributed to its slower growth and thicker cell wall, possibly enabling the generation of higher turgor pressures to overcome restrictive forces under confinement. By providing fundamental insights into the interplay between mechanical forces and bacterial physiology, this work advances our understanding of how matrix properties shape bacterial behavior. The implications of these findings will aid the design of engineered living materials for therapeutic applications.