INMdok (Leibniz Institute for New Materials)
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Sodium-ion diffusion coefficients in tin phosphide determined with advanced electrochemical techniques
Get PDFSodium ion insertion plays a critical role in developing robust sodium-ion technologies (batteries and hybrid supercapacitors). Diffusion coefficient values of sodium (DNa+) in tin phosphide between 0.1 V and 2.0 V vs. Na/Na+ are systematically determined by galvanostatic intermittent titration technique (GITT), electrochemical impedance spectroscopy (EIS), and potentiostatic intermittent titration technique (PITT). These values range between 4.55 × 10−12 cm2 s−1 and 1.94 × 10−8 cm2 s−1 and depend on the insertion/de-insertion current and the thickness of the electrode materials. Additionally, DNa+ values differ between the first and second cation insertion because of the solid electrolyte interface (SEI) formation. DNa+ vs. insertion potential alters non-linearly in a “W” form due to the strong interactions of Na+ with tin phosphide particles. The results reveal that GITT is a more appropriate electrochemical technique than PITT and EIS for evaluating DNa+ in tin phosphide
Toward a Li-Ion Battery Ontology Covering Production and Material Structure
Get PDFAn ontology for the structured storage, retrieval, and analysis of data on lithium-ion battery materials and electrode-to-cell production is presented. It provides a logical structure that is mapped onto a digital architecture and used to visualize, correlate, and make predictions in battery production, research, and development. Materials and processes are specified using a predetermined terminology; a chain of unit processes (steps) connects raw materials and products (items) of battery cell production. The ontology enables the attachment of analytical methods (characterization methods) to items. Workshops and interviews with experts in battery materials and production processes are conducted to ensure that the structure is conformable both for industrial-scale and laboratory-scale data generation and implementation. Raw materials and intermediate products are identified and defined for all steps to the final battery cell. Steps and items are defined based on current standard materials and process chains using terms that are in common use. Alternative structures and the connection of the ontology to other existing ontologies are discussed. The contribution provides a pragmatic, accessible way to unify the storage of materials-oriented lithium-ion battery production data. It aids the linkage of such data with domain knowledge and the automation of data analysis in production and research
A Photoreceptor-Based Hydrogel with Red Light-Responsive Reversible Sol-Gel Transition as Transient Cellular Matrix
Get PDFHydrogels with adjustable mechanical properties have been engineered as matrices for mammalian cells and allow the dynamic, mechano-responsive manipulation of cell fate and function. Recent research yields hydrogels, where biological photoreceptors translated optical signals into a reversible and adjustable change in hydrogel mechanics. While their initial application provides important insights into mechanobiology, broader implementation is limited by a small dynamic range of addressable stiffness. Herein, this limitation is overcome by developing a photoreceptor-based hydrogel with reversibly adjustable stiffness from ≈800 Pa to the sol state. The hydrogel is based on star-shaped polyethylene glycol, functionalized with the red/far-red light photoreceptor phytochrome B (PhyB), or phytochrome-interacting factor 6 (PIF6). Upon illumination with red light, PhyB heterodimerizes with PIF6, thus crosslinking the polymers and resulting in gelation. However, upon illumination with far-red light, the proteins dissociate and trigger a complete gel-to-sol transition. The hydrogel's light-responsive mechanical properties are comprehensively characterized and it is applied as a reversible extracellular matrix for the spatiotemporally controlled deposition of mammalian cells within a microfluidic chip. It is anticipated that this technology will open new avenues for the site- and time-specific positioning of cells and will contribute to overcome spatial restrictions
Self-Assembly of Polymer-Modified FePt Magnetic Nanoparticles and Block Copolymers
Get PDFThe fabrication of nanocomposites containing magnetic nanoparticles is gaining interest as a model for application in small electronic devices. The self-assembly of block copolymers (BCPs) makes these materials ideal for use as a soft matrix to support the structural ordering of the nanoparticles. In this work, a high-molecular-weight polystyrene-b-poly(methyl methacrylate) block copolymer (PSb-PMMA) was synthesized through anionic polymerization. The influence of the addition of different ratios of PMMA-coated FePt nanoparticles (NPs) on the self-assembled morphology was investigated using transmission electron microscopy (TEM) and small-angle X-ray scattering (SAXS). The selfassembly of the NPs inside the PMMA phase at low particle concentrations was analyzed statistically, and the negative effect of higher particle ratios on the lamellar BCP morphology became visible. The placement of the NPs inside the PMMA phase was also compared to theoretical descriptions. The magnetic addressability of the FePt nanoparticles inside the nanocomposite films was finally analyzed using bimodal magnetic force microscopy and proved the magnetic nature of the nanoparticles inside the microphase-separated BCP films
Interlaboratory study assessing the analysis of supercapacitor electrochemistry data
Get PDFSupercapacitors are fast-charging energy storage devices of great importance for developing robust and climate-friendly energy infrastructures for the future. Research in this field has seen rapid growth in recent years, therefore consistent reporting practices must be implemented to enable reliable comparison of device performance. Although several studies have highlighted the best practices for analysing and reporting data from such energy storage devices, there is yet to be an empirical study investigating whether researchers in the field are correctly implementing these recommendations, and which assesses the variation in reporting between different laboratories. Here we address this deficit by carrying out the first interlaboratory study of the analysis of supercapacitor electrochemistry data. We find that the use of incorrect formulae and researchers having different interpretations of key terminologies are major causes of variability in data reporting. Furthermore we highlight the more significant variation in reported results for electrochemical profiles showing non-ideal capacitive behaviour. From the insights gained through this study, we make additional recommendations to the community to help ensure consistent reporting of performance metrics moving forward
Alignment interaction and band formation in assemblies of auto-chemorepulsive walkers
Get PDFChemotaxis, i.e. motion generated by chemical gradients, is a motility mode shared by many living species that has been developed by evolution to optimize certain biological processes such as foraging or immune response. In particular, auto-chemotaxis refers to chemotaxis mediated by a cue produced by the chemotactic particle itself. Here, we investigate the collective behavior of auto-chemotactic particles that are repelled by the cue and therefore migrate preferentially towards low-concentration regions. To this end, we introduce a lattice model inspired by the true self-avoiding walk which reduces to the Keller-Segels model in the continuous limit, for which we describe the rich phase behavior. We first rationalize a the chemically-mediated alignment interaction between walkers in the limit of stationary concentration fields, and then describe the various large-scale structures that can spontaneously form and the conditions for them to emerge, among which we find stable bands traveling at constant speed in the direction transverse to the band
Stationary particle currents in sedimenting active matter wetting a wall
Get PDFRecently it was predicted, on the basis of a lattice gas model, that scalar active matter in a gravitational field would rise against gravity up a confining wall or inside a thin capillary - in spite of repulsive particle-wall interactions [Phys. Rev. Lett. 124, 048001 (2020)]. In this paper we confirm this prediction with sedimenting active Brownian particles (ABPs) in a box and elucidate the mechanism leading to the formation of a meniscus rising above the bulk of the sedimentation region. The height of the meniscus increases with the activity of the system, algebraically with the Péclet number. The formation of the meniscus is determined by a stationary circular particle current, a vortex, centered at the base of the meniscus, whose size and strength increases with the ABP activity. The origin of these vortices can be traced back to the confinement of the ABPs in a box: already the stationary state of ideal (non-interacting) ABPs without gravitation displays circular currents that arrange in a highly symmetric way in the eight octants of the box. Gravitation distorts this vortex configuration downward, leaving two major vortices at the two side walls, with a strong downward flow along the walls. Repulsive interactions between the ABPs change this situation only as soon as motility induced phase separation (MIPS) sets in and forms a dense, sedimented liquid region at the bottom, which pushes the center of the vortex upwards towards the liquid-gas interface. Self-propelled particles therefore represent an impressive realization of scalar active matter that forms stationary particle currents being able to perform visible work against gravity or any other external field, which we predict to be observable experimentally in active colloids under gravitation
Chemical and Structural Comparison of Different Commercial Food Supplements for Silicon Uptake
Get PDFVarious food supplements for silicon uptake were compared in terms of their structures and chemical compositions. In particular, we analyzed the silanol group content, which can be an indicator of the uptake of the siliceous species in the human body. We analyzed the commercial products Original Silicea Balsam®, Flügge Siliceous Earth Powder, Pure Colloidal Silicon, and BioSil® by applying various methods such as FTIR, 29Si NMR, and TGA. The Si-OH group content of the samples containing pure silica was the highest for the Original Silicea Balsam followed by the Pure Colloidal Silicon. The siliceous earth powder revealed the lowest content of such groups and the densest structure. BioSil® contained a considerable concentration of organic molecules that stabilized orthosilicic acid. The study may help to understand the silicon uptake behavior of different food supplements depending on their chemical structure
When Like Destabilizes Like: Inverted Solvent Effects in Apolar Nanoparticle Dispersions
Get PDFWe report on the colloidal stability of nanoparticles with alkanethiol shells in apolar solvents. Small angle X-ray scattering and molecular dynamics simulations were used to characterize the interaction between nanoparticles in linear alkane solvents ranging from hexane to hexadecane, including \SI{4}{\nano\meter} gold cores with hexadecanethiol shells and \SI{6}{\nano\meter} cadmium selenide cores with octadecanethiol shells. We find that the agglomeration is enthalpically driven and that, contrary to what one would expect from classical colloid theory, the temperature at which the particles agglomerate increases with increasing solvent chain length. We demonstrate that the inverted trend correlates with the temperatures at which the ligands order in the different solvents, and show that the inversion is due to a combination of enthalpic and entropic effects that enhance the stability of the ordered ligand state as the solvent length increases. We also explain why cyclohexane is a better solvent than hexane, despite having very similar solvation parameters to hexadecane
Engineered living materials for the conversion of a low-cost foodgrade precursor to a high-value flavonoid
Get PDFMicrobial biofactories allow the upscaled production of high-value compounds in biotechnological processes. This is particularly advantageous for compounds like flavonoids that promote better health through their antioxidant, antibacterial, anticancer and other beneficial effects but are only produced in small quantities in their natural plant-based hosts. Bacteria like E. coli have been genetically modified with enzyme cascades to produce flavonoids like naringenin and pinocembrin from coumaric or cinnamic acid. Despite advancements in yield optimization, the production of these compounds still involves high costs associated with their biosynthesis, purification, storage and transport. An alternative production strategy could involve the direct delivery of the microbial biofactories to the body. In such a strategy, ensuring biocontainment of the engineered microbes in the body and controlling production rates are major challenges. In this study, these two aspects are addressed by developing engineered living materials (ELMs) consisting of probiotic microbial biofactories encapsulated in biocompatible hydrogels. Engineered probiotic E. coli Nissle 1917 able to efficiently convert cinnamic acid into pinocembrin were encapsulated in poly(vinyl alcohol)-based hydrogels. The biofactories are contained in the hydrogels for a month and remain metabolically active during this time. Control over production levels is achieved by the containment inside the material, which regulates bacteria growth, and by the amount of cinnamic acid in the medium