Yildirim, Turgay | Bali, Aghiad | Koch, Marcus | Paul, Pascal | Latta, Lorenz | Scheider-Daum, Nicole | Gallei, Markus | Lehr, Claus-Michael
DOI:
Pseudomonas aeruginosa (PA) is a major healthcare concern due to its tolerance to antibiotics when enclosed in biofilms. Tobramycin (Tob), an effective cationic aminoglycoside antibiotic against planktonic PA, loses potency within PA biofilms due to hindered diffusion caused by interactions with anionic biofilm components. Loading Tob into nano-carriers can enhance its biofilm efficacy by shielding its charge. Polyion complex vesicles (PIC-somes) are promising nano-carriers for charged drugs, allowing higher drug loadings than liposomes and polymersomes. In this study, a new class of nano-sized PIC-somes, formed by Tob-diblock copolymer complexation is presented. This approach replaces conventional linear PEG with brush-like poly[ethylene glycol (methyl ether methacrylate)] (PEGMA) in the shell-forming block, distinguishing it from past methods. Tob paired with a block copolymer containing hydrophilic PEGMA induces micelle formation (PIC-micelles), while incorporating hydrophobic pyridyldisulfide ethyl methacrylate (PDSMA) monomer into PEGMA chains reduces shell hydrophilicity, leads to the formation of vesicles (PIC-somes). PDSMA unit incorporation enables unprecedented dynamic disulfide bond-based shell cross-linking, significantly enhancing stability under saline conditions. Neither PIC-somes nor PIC-micelles show any relevant cytotoxicity on A549, Calu-3, and dTHP-1 cells. Tob's antimicrobial efficacy against planktonic PA remains unaffected after encapsulation into PIC-somes and PIC-micelles, but its potency within PA biofilms significantly increases.
Wu, Xixi | Li, Wenjian | Herlah, Lara | Koch, Marcus | Wang, Hui | Schirhagl, Romana | Włodarczyk-Biegun
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Multifunctional wound dressings, enriched with biologically active agents for preventing or treating infections and promoting wound healing, along with cell delivery capability, are highly needed. To address this issue, composite scaffolds with potential in wound dressing applications were fabricated in this study. The poly-lactic acid/nanodiamonds (PLA/ND) scaffolds were first printed using melt electrowriting (MEW) and then coated with quaternized β-chitin (QβC). The NDs were well-dispersed in the printed filaments and worked as fillers and bioactive additions to PLA material. Additionally, they improved coating effectiveness due to the interaction between their negative charges (from NDs) and positive charges (from QβC). NDs not only increased the thermal stability of PLA but also benefitted cellular behavior and inhibited the growth of bacteria. Scaffolds coated with QβC increased the effect of bacteria growth inhibition and facilitated the proliferation of human dermal fibroblasts. Additionally, we have observed rapid extracellular matrix (ECM) remodeling on QβC-coated PLA/NDs scaffolds. The scaffolds provided support for cell adhesion and could serve as a valuable tool for delivering cells to chronic wound sites. The proposed PLA/ND scaffold coated with QβC holds great potential for achieving fast healing in various types of wounds.
Van Impelen, David | González-García, Lola | Kraus, Tobias
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Silver-coated copper microparticles combine the oxidation resistance of silver with the low cost of copper. They are interesting components for printed conductive structures. We studied whether printed films of such particles can be printed and sintered at low temperatures in air to create highly conductive films and whether it is possible to recover the particles from them for recycling. Pastes containing 1.5 μm to 5 μm spheres and 3 μm flakes with L-ascorbic acid were prepared, screen-printed, and treated at temperatures of 110 °C to 300 °C in air. The bulk resistance of films treated below 160 °C were two orders of magnitude higher than that of bulk copper, ρCu, and limited by particle-particle contact resistances. They were reduced by treating the prints at 160 °C to 250 °C, leading to bulk film resistances down to 41ρCu. We demonstrate that the high mobility of silver enables the formation of necks that bridge the copper cores and reduce resistivity in this temperature window. The sintered prints retained their conductivity for at least 6 months. Treatments at higher temperatures in air were detrimental: resistances increased above 250 °C. These temperatures led to dewetting of the silver coating and fast copper oxidation, resulting in a continuously increasing resistance. In a final study, we demonstrated that films treated below 200 °C can be recycled by recovering the metal powder from the printed conductors and that the powder can be printed again.
Silina, Yulia E. | Butyrskaya, E. V. | Koch, Marcus | Fink-Straube, Claudia | Korkmaz, Nuriye | Levchenko, M. G. | Zolotukhina, E. V.
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Herein, a study dealing with a progress on palladium (Pd) electrocatalysts for an efficient glycerol electrooxidation in model aqueous and real fermentation solutions with special focus on some physicochemical parameters (e.g., the impact of adsorption stage of multiple species, presence of oxygen, influence of anodic limits and Pd-size) was conducted. During the course of investigations by tandem of an optical oxygen minisensor and cyclic voltammetry a significant impact of oxygen on the efficiency of glycerol electrooxidation on Pd electrocatalysts at alkaline pH in model aqueous and yeast fermentation media was revealed. The obtained knowledge was used for the optimization of an assay utilizing Pd-sensing layers for glycerol determination and quantification in yeast fermentation medium. Received results showed a satisfactory agreement with a control measurement carried out by gas chromatography mass-spectrometry.
De Andrade Ruthes, Jean G. | Arnold, Stefanie | Prenger, Kaitlyn | Jaski, Ana C. | Klobukoski, Vanessa | Riegel-Vidotti, Izabel C. | Presser, Volker
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The development of flexible and wearable electronics has grown in recent years with applications in different fields of industry and science. Consequently, the necessity of functional, flexible, safe, and reliable energy storage devices to meet this demand has increased. Since the classical electrochemical systems face structuration and operational limitations to match the needs of flexible devices, novel approaches have been in the research spotlight: gel polymer electrolytes (GPEs). Combining comparable ionic conductivity with liquid electrolytes with desirable mechanical stability, GPEs have been investigated in various electrochemical applications in sensors, actuators, and energy storage. This versatile class of quasi-solid material finds applications in the different components of energy storage devices. They are being investigated as electrodes, binders, electrolytes, and stand-alone systems due to desirable physical-chemical characteristics such as a wider potential operational window and high adhesion to solid electrode materials. Coalescing a liquid phase occluded into an entangled 3D polymeric matrix, these materials withstand elevated mechanical stress such as strain and compression, and they are also interesting materials for various applications. Moreover, they allow further functionalization to match the specific requirements of various energy storage systems. In this review, we summarize different applications of GPEs in energy storage devices, highlighting many valuable properties and emphasizing their enhancements compared to classical liquid electrochemical energy storage systems.
Lopez, Esmeralda | Gómez, Mauricio | Becar, Ian | Zapata, Paula | Pizarro, Jaime | Navlani-García | Cazorla-Amorós, Diego | Presser, Volker | Gómez, Tatiana | Cárdenas, Carlos
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Environmentally friendly polymers such as cellulose acetate (CA) and chitosan (CS) were used to obtain electrospun fibers for Cu2+, Pb2+, and Mo6+ capture. The solvents dichloromethane (DCM) and dimethylformamide (DMF) allowed the development of a surface area of 148 m2 g−1 for CA fibers and 113 m2 g−1 for cellulose acetate/chitosan (CA/CS) fibers. The fibers were characterized by IR-DRIFT, SEM, TEM, CO2 sorption isotherms at 273 K, Hg porosimetry, TGA, stress-strain tests, and XPS. The CA/CS fibers had a higher adsorption capacity than CA fibers without affecting their physicochemical properties. The capture capacity reached 102 mg g−1 for Cu2+, 49.3 mg g−1 for Pb2+, and 13.1 mg g−1 for Mo6+. Furthermore, optimal pH, adsorption times qt, and C0 were studied for the evaluation of kinetic models and adsorption isotherms. Finally, a proposal for adsorbate-adsorbent interactions is presented as a possible capture mechanism where, in the case of Mo6+, a computational study is presented. The results demonstrate the potential to evaluate the fibers in tailings wastewater from copper mining.
Liang, Kun | Wu, Tao | Misra, Sudhajit | Dun, Chaochao | Husmann, Samantha | Prenger, Kaitlyn | Urban, Jeffrey J. | Presser, Volker | Unocic, Raymond R. | Jiang, De-en | Naguib, Michael
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MXene is investigated as an electrode material for different energy storage systems due to layered structures and metal-like electrical conductivity. Experimental results show MXenes possess excellent cycling performance as anode materials, especially at large current densities. However, the reversible capacity is relatively low, which is a significant barrier to meeting the demands of industrial applications. This work synthesizes N-doped graphene-like carbon (NGC) intercalated Ti3C2Tx (NGC-Ti3C2Tx) van der Waals heterostructure by an in situ method. The as-prepared NGC-Ti3C2Tx van der Waals heterostructure is employed as sodium-ion and lithium-ion battery electrodes. For sodium-ion batteries, a reversible specific capacity of 305 mAh g−1 is achieved at a specific current of 20 mA g−1, 2.3 times higher than that of Ti3C2Tx. For lithium-ion batteries, a reversible capacity of 400 mAh g−1 at a specific current of 20 mA g−1 is 1.5 times higher than that of Ti3C2Tx. Both sodium-ion and lithium-ion batteries made from NGC-Ti3C2Tx shows high cycling stability. The theoretical calculations also verify the remarkable improvement in battery capacity within the NGC-Ti3C2O2 system, attributed to the additional adsorption of working ions at the edge states of NGC. This work offers an innovative way to synthesize a new van der Waals heterostructure and provides a new route to improve the electrochemical performance significantly.
Kök, Cansu | Wang, Lei | Ruthes, Jean Gustavo A. | Quade, Antje | Suss, Matthew E. | Presser, Volker
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The demand for electronic devices that utilize lithium is steadily increasing in this rapidly advancing technological world. Obtaining high-purity lithium in an environmentally friendly way is challenging by using commercialized methods. Herein, we propose the first fuel cell system for continuous lithium-ion extraction using a lithium superionic conductor membrane and advanced electrode. The fuel cell system for extracting lithium-ion has demonstrated a twofold increase in the selectivity of Li+/Na+ while producing electricity. Our data show that the fuel cell with a titania-coated electrode achieves 95% lithium-ion purity while generating 10.23 Wh of energy per gram of lithium. Our investigation revealed that using atomic layer deposition improved the electrode's uniformity, stability, and electrocatalytic activity. After 2000 cycles determined by cyclic voltammetry, the electrode preserved its stability.
Klos, Michael | González-García, Lola | Kraus, Tobias
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Hybrid core–shell nanoparticles with metal cores and conductive polymer shells yield materials that are sinter-free and highly conductive but mechanically weak. Conventional composites of such nanoparticles are electrically insulating. Here, we introduce microscale phase-separated nanocomposites of hybrid gold-PEDOT:PPS particles in insulating poly(vinyl alcohol) (PVA). They combine electrical conductivities of up to 2.1 × 105 S/m at 10 vol % PVA with increased mechanical adhesion on polyethylene terephthalate and glass substrates. We studied the effects of the PVA molecular weight, hydrolyzation degree, and volume fraction. Composites with 10 vol % highly hydrolyzed PVA at a MW of 89–98 kDa had the highest conductivities and stabilities; highly hydrolyzed PVA even increased the conductivity of the hybrid particle layers. We propose the formation of hydrogen bonds between PVA and PEDOT:PSS that lead to demixing and the formation of stable, structured composites. Finally, we demonstrated the inkjet-printability of inks containing PVA in water with viscosities of 1.6–2.0 Pa s at 50.1 s–1 and prepared bending-resistant electrical leads.
Karmakar, Mintu | Chatterjee, Swarnajit | Paul, Raja | Rieger, Heiko
DOI:
We numerically study a discretized Vicsek model (DVM) with particles orienting in q possible orientations in two dimensions. The study investigates the significance of anisotropic orientation and microscopic interaction on macroscopic behavior. The DVM is an off-lattice flocking model like the active clock model (ACM; Chatterjee et al 2022 Europhys. Lett.138 41001) but the dynamical rules of particle alignment and movement are inspired by the prototypical Vicsek model (VM). The DVM shows qualitatively similar properties as the ACM for intermediate noise strength where a transition from macrophase to microphase separation of the coexistence region is observed as q is increased. But for small q and noise strength, the liquid phase appearing in the ACM at low temperatures is replaced in the DVM by a configuration of multiple clusters with different polarizations, which does not exhibit any long-range order. We find that the dynamical rules have a profound influence on the overarching features of the flocking phase. We further identify the metastability of the ordered liquid phase subjected to a perturbation.
