INMdok (Leibniz Institute for New Materials)
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Nanocellulose and PEDOT:PSS composites and their applications
Get PDFThe need for achieving sustainable technologies has encouraged research on renewable and biodegradable materials for novel products that are clean, green, and environmentally friendly. Nanocellulose (NC) has many attractive properties such as high mechanical strength and flexibility, large specific surface area, in addition to possessing good wet stability and resistance to tough chemical environments. NC has also been shown to easily integrate with other materials to form composites. By combining it with conductive and electroactive materials, many of the advantageous properties of NC can be transferred to the resulting composites. Conductive polymers, in particular poly(3,4-ethylenedioxythiophene:poly(styrene sulfonate) (PEDOT:PSS), have been successfully combined with cellulose derivatives where suspensions of NC particles and colloids of PEDOT:PSS are made to interact at a molecular level. Alternatively, different polymerization techniques have been used to coat the cellulose fibrils. When processed in liquid form, the resulting mixture can be used as a conductive ink. This review outlines the preparation of NC/PEDOT:PSS composites and their fabrication in the form of electronic nanopapers, filaments, and conductive aerogels. We also discuss the molecular interaction between NC and PEDOT:PSS and the factors that affect the bonding properties. Finally, we address their potential applications in energy storage and harvesting, sensors, actuators, and bioelectronics
PIEZO1-mediated mechanosensing governs NK cell killing efficiency in 3D
Get PDFNatural killer (NK) cells play a vital role in eliminating tumorigenic cells. Efficient locating and killing of target cells in complex three-dimensional (3D) environments is critical for their functions under physiological conditions. Recent studies have shown that NK cell activation is regulated by substrate stiffness. However, the role of mechanosensing in regulating NK cell killing efficiency in physiologically relevant scenarios is poorly understood. In this study, we report that the responsiveness of NK cells is regulated by tumor cell stiffness. NK cell killing efficiency in 3D is impaired against softened tumor cells, while it is enhanced against stiffened tumor cells. Notably, the durations required for NK cell killing and detachment are significantly shortened for stiffened tumor cells. Furthermore, we have identified PIEZO1 as the predominantly expressed mechanosensitive ion channel in NK cells. Perturbation of PIEZO1 by GsMTx4 abolishes stiffness-dependent NK cell responsiveness, significantly impairs the killing efficiency of NK cells in 3D, and substantially reduces NK cell infiltration into 3D collagen matrices. Conversely, PIEZO1 activation enhances NK killing efficiency as well as infiltration. In conclusion, our findings demonstrate that PIEZO1-mediated mechanosensing is crucial for NK killing functions, highlighting the role of mechanosensing in NK cell killing efficiency under physiological conditions and the influence of environmental physical cues on NK cell functions
Polyacrylonitrile-containing amphiphilic block copolymers: self-assembly and porous membrane formation
Get PDFThe development of hierarchically porous block copolymer (BCP) membranes via the application of the self-assembly and non-solvent induced phase separation (SNIPS) process is one important achievement in BCP science in the last decades. In this work, we present the synthesis of polyacrylonitrile-containing amphiphilic BCPs and their unique microphase separation capability, as well as their applicability for the SNIPS process leading to isoporous integral asymmetric membranes. Poly(styrene-co-acrylonitrile)-b-poly(2-hydroxyethyl methacrylate)s (PSAN-b-PHEMA) are synthesized via a two-step atom transfer radical polymerization (ATRP) procedure rendering PSAN copolymers and BCPs with overall molar masses of up to 82 kDa while maintaining low dispersity index values in the range of Đ = 1.13–1.25. The polymers are characterized using size-exclusion chromatography (SEC) and NMR spectroscopy. Self-assembly capabilities in the bulk state are examined using transmission electron microscopy (TEM) and small-angle X-ray scattering (SAXS) measurements. The fabrication of isoporous integral asymmetric membranes is investigated, and membranes are examined by scanning electron microscopy (SEM). The introduction of acrylonitrile moieties within the membrane matrix could improve the membranes’ mechanical properties, which was confirmed by nanomechanical analysis using atomic force microscopy (AFM)
Advanced Materials Safety 2023
Get PDFFunctionality of advanced materials, their impact on humans and the environments as well as the acceptance of the technologies are the focus of the conference. With the Advanced Materials Safety 2023, we bring together researchers with different relevant expertise and identify possible interfaces for joint research projects that allow us to investigate such complex challenges
2D nanolamellar materials toward water-energy nexus applications
Get PDFElectrochemical water desalination is an emerging technology known for its high efficiency and low energy consumption in removing ions from aqueous media. The present thesis begins by explaining the fundamentals of a typical electrochemical water desalination system and presenting relevant performance metrics. The significance and limitations of the latter metrics are then discussed based on the generations of the electrodes developed during the past few decades. This report seeks to expand the scope by investigating MXene (titanium carbide) as a purely pseudocapacitive material characterized by a capacitor-like electric response achieved through ion intercalation. Afterward, the merit of MXene when utilized as an electrode in electrochemical desalination is investigated for both single-salt and multi-salt aqueous solutions, ultimately establishing qualitative insights into the relationship between MXene properties and its electrochemical desalination behavior. Finally, the thesis goes beyond MXene and explores its sibling materials, such as MBene (transition metal boride), for lithium-ion battery electrodes. As another application of 2D nanolamellar materials at the water-energy nexus, we have explored MXene conversion into transition metal dichalcogenides by sulfidation heat treatment and its merit as electrodes for hydrogen electrocatalysis. These findings can contribute to developing more efficient and sustainable energy storage, conversion, and desalination technologies.Elektrochemische Wasserentsalzung ist eine vielversprechende Technologie, die für ihre hohe Effizienz und ihren geringen Energieverbrauch bei der Entfernung von Ionen aus wässrigen Medien bekannt ist. Die vorliegende Arbeit beginnt mit der Erläuterung der Grundlagen eines typischen elektrochemischen Wasserentsalzungssystems und der Darstellung relevanter Leistungskennzahlen. Die Bedeutung und Einschränkungen der letztgenannten Metriken werden dann anhand der in der Vergangenheit entwickelten Generationen von Elektroden diskutiert. Die vorliegende Arbeit untersucht MXene (Titankarbid) als rein pseudokapazitives Material, das durch eine kondensatorähnliche elektrische Reaktion gekennzeichnet ist, die durch Ioneninterkalation erreicht wird. Anschließend wird der Nutzen von MXene bei der Verwendung als Elektrode bei der elektrochemischen Entsalzung sowohl für wässrige Lösungen mit einem Salz als auch mit mehreren Salzen untersucht, um schließlich qualitative Erkenntnisse über die Beziehung zwischen den Eigenschaften von MXen und seinem elektrochemischen Entsalzungsverhalten zu gewinnen. Letztlich erforscht die Arbeit auch MBene (Übergangsmetallborid) sowie die Derivatisierung von MXenen hin zu Übergangsmetalldichalkogeniden durch Sulfidierung für den Einsatz in der Wasserstoffelektrokatalyse untersucht. Die Ergebnisse dieser Studien können zur Entwicklung effizienterer und nachhaltigerer Technologien zur Energiespeicherung, -umwandlung und -entsalzung beitragen
Analysis of the compressible, isotropic, neo-Hookean hyperelastic model
Get PDFThe most widely-used representation of the compressible, isotropic, neo-Hookean hyperelastic model is considered in this paper. The version under investigation is that which is implemented in the commercial finite element software ABAQUS, ANSYS and COMSOL. Transverse stretch solutions are obtained for the following homogeneous deformations: uniaxial loading, equibiaxial loading in plane stress, and uniaxial loading in plane strain. The ground-state Poisson’s ratio is used to parameterize the constitutive model, and stress solutions are computed numerically for the physically permitted range of its values. Despite its broad application to a number of engineering problems, the physical limitations of the model, particularly in the small to moderate stretch regimes, are not explored. In this work, we describe and analyze results and make some critical observations, underlining the model’s advantages and limitations. For example, a snap-back feature of the transverse stretch is identified in uniaxial compression, a physically undesirable behavior unless validated by experimental data. The domain of this non-unique solution is determined in terms of the ground-state Poisson’s ratio and the state of stretch and stress. The analyses we perform are essential to enable the understanding of the characteristics of the standard, compressible, isotropic, neo-Hookean model used in ABAQUS, ANSYS and COMSOL. In addition, our results provide a framework for the parameter-fitting procedure needed to characterize this standard, compressible, isotropic neo-Hookean model in terms of experimental data
Human glabrous skin contains crystallized urea dendriform structures in the stratum corneum which affect the hydration levels
Get PDFGlabrous skin is hair-free skin with a high density of sweat glands, which is found on the palms, and soles of mammalians, covered with a thick stratum corneum. Dry hands are often an occupational problem which deserves attention from dermatologists. Urea is found in the skin as a component of the natural moisturizing factor and of sweat. We report the discovery of dendrimer structures of crystalized urea in the stratum corneum of palmar glabrous skin using laser scanning microscopy. The chemical and structural nature of the urea crystallites was investigated in vivo by non-invasive techniques. The relation of crystallization to skin hydration was explored. We analysed the index finger, small finger and tenar palmar area of 18 study participants using non-invasive optical methods, such as laser scanning microscopy, Raman microspectroscopy and two-photon tomography. Skin hydration was measured using corneometry. Crystalline urea structures were found in the stratum corneum of about two-thirds of the participants. Participants with a higher density of crystallized urea structures exhibited a lower skin hydration. The chemical nature and the crystalline structure of the urea were confirmed by Raman microspectroscopy and by second harmonic generated signals in two-photon tomography. The presence of urea dendrimer crystals in the glabrous skin seems to reduce the water binding capacity leading to dry hands. These findings highlight a new direction in understanding the mechanisms leading to dry hands and open opportunities for the development of better moisturizers and hand disinfection products and for diagnostic of dry skin
Cytocompatibility evaluation of PEG-methylsulfone hydrogels
Get PDFMethylsulfone derivatized poly(ethylene) glycol (PEG) macromers can be biofunctionalized with thiolated ligands and cross-linked with thiol-based cross-linkers to obtain bioactive PEG hydrogels for in situ cell encapsulation. Methylsulfonyl-thiol (MS-SH) reactions present several advantages for this purpose when compared to other thiol-based cross-linking systems. They proceed with adequate and tunable kinetics for encapsulation, they reach a high conversion degree with good selectivity, and they generate stable reaction products. Our previous work demonstrated the cytocompatibility of cross-linked PEG-MS/thiol hydrogels in contact with fibroblasts. However, the cytocompatibility of the in situ MS-SH cross-linking reaction itself, which generates methylsulfinic acid as byproduct at the cross-linked site, remains to be evaluated. These studies are necessary to evaluate the potential of these systems for in vivo applications. Here we perform an extensive cytocompatibility study of PEG hydrogels during in situ cross-linking by the methylsulfonyl-thiol reaction. We compare these results with maleimide–thiol cross-linked PEGs which are well established for cell culture and in vivo experiments and do not involve the release of a byproduct. We show that fibroblasts and endothelial cells remain viable after in situ polymerization of methylsulfonyl-thiol gels on the top of the cell layers. Cell viability seems better than after in situ cross-linking hydrogels with maleimide–thiol chemistry. The endothelial cell proinflammatory phenotype is low and similar to the one obtained by the maleimide–thiol reaction. Finally, no activation of monocytes is observed. All in all, these results demonstrate that the methylsulfonyl-thiol chemistry is cytocompatible and does not trigger high pro-inflammatory responses in endothelial cells and monocytes. These results make methylsulfonyl-thiol chemistries eligible for in vivo testing and eventually clinical application in the future
How to steer active colloids up a vertical wall
Get PDFAn important challenge in active matter lies in harnessing useful global work from entities that produce work locally, e.g., via self-propulsion. We investigate here the active matter version of a classical capillary rise effect, by considering a non-phase separated sediment of self-propelled Janus colloids in contact with a vertical wall. We provide experimental evidence of an unexpected and dynamic adsorption layer at the wall. Additionally, we develop a complementary numerical model that recapitulates the experimental observations. We show that an adhesive and aligning wall enhances the pre-existing polarity heterogeneity within the bulk, enabling polar active particles to climb up a wall against gravity, effectively powering a global flux. Such steady-state flux has no equivalent in a passive wetting layer
Encapsulation of bacteria in bilayer Pluronic thin film hydrogels: A safe format for engineered living materials
Get PDFIn engineered living materials (ELMs) non-living matrices encapsulate microorganisms to acquire capabilities like sensing or biosynthesis. The confinement of the organisms to the matrix and the prevention of overgrowth and escape during the lifetime of the material is necessary for the application of ELMs into real devices. In this study, a bilayer thin film hydrogel of Pluronic F127 and Pluronic F127 acrylate polymers supported on a solid substrate is introduced. The inner hydrogel layer contains genetically engineered bacteria and supports their growth, while the outer layer acts as an envelope and does not allow leakage of the living organisms outside of the film for at least 15 days. Due to the flat and transparent nature of the construct, the thin layer is suited for microscopy and spectroscopy-based analyses. The composition and properties of the inner and outer layer are adjusted independently to fulfil viability and confinement requirements. We demonstrate that bacterial growth and light-induced protein production are possible in the inner layer and their extent is influenced by the crosslinking degree of the used hydrogel. Bacteria inside the hydrogel are viable long term, they can act as lactate-sensors and remain active after storage in phosphate buffer at room temperature for at least 3 weeks. The versatility of bilayer bacteria thin-films is attractive for fundamental studies and for the development of application-oriented ELMs