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The development of halochromic textile materials could lead to interesting end-use applications as it offers the potential for flexible pH-sensors with a first warning signal. Research on halochromic textiles, especially on the development of these materials using a simple and economic beneficial dyeing process, is however very limited. Therefore, we studied color-changing textile materials with a pH-sensitivity based on the dyeing of conventional textiles with standard water-soluble pH-indicator dyes. In a first broad screening, a set of pH-indicators is evaluated on their dyeing performance and their color change with a change in pH. After this, some promising indicators (Brilliant Yellow and Alizarin) are selected and studied in more detail. It was found that the indicators show different characteristics on the textile materials compared with the solution due to dye--fiber interactions. The properties of the pH-indicator dyes are also dependant on the fiber type. Moreover, in case of Brilliant Yellow this thesis was confirmed by Raman spectroscopy. Generally, it can be concluded that it is feasible to develop a pH-sensor with pH-indicator dyes and conventional textile materials using a standard dyeing process. [ABSTRACT FROM AUTHOR]

This study investigates the effectiveness of polyether block amide (PEBA) thermoplastic elastomeric nanofibers in reducing low-velocity impact damage across three carbon fiber composite lay-up configurations: a cross-ply [0°/90°]2s (CP) and a quasi-isotropic [0°/45°/90°/-45°]s (QI) lay-up utilizing unidirectional plies, and a stacked woven [(0°,90°)]4s (W) lay-up using twill woven fabric plies. The flexural strength and interlaminar shear strength of the composites remained unaffected by the addition of nanofibers: around 750 MPa and 63 MPa for CP, 550 MPa and 58 MPa for QI, and 650 MPa and 50 MPa for W, respectively. The incorporation of nanofibers in the interlaminar regions resulted in a substantial reduction in projected damage area, ranging from 30% to 50% reduction over an impact energy range of 5-20 J. Microscopic analysis showed that especially the delamination damage decreased in toughened composites, while intralaminar damage remained similar for the cross-ply and quasi-isotropic lay-ups and decreased only in the woven lay-up. This agrees with the broad body of research that shows that interleaved nanofibers result in a higher delamination resistance due to toughening mechanisms related to nanofiber bridging of cracks. Despite their ability to mitigate delamination during impact, nanofibers showed limited positive effects on Compression After Impact (CAI) strength in quasi-isotropic and cross-ply composites. Interestingly, only the woven fabric composites demonstrated improved CAI strength, with a 12% improvement on average over the impact energy range, attributed to a reduction in both interlaminar and intralaminar damage. This study indicates the critical role of fiber integrity over delamination size in determining CAI performance, suggesting that the delaminations are not sufficiently large to induce buckling of sub-layers, thereby minimizing the effect of nanofiber toughening on the CAI strength.

The amniotic egg fulfils a critical role in reproduction by serving as an interface between the external environment and the embryo. Because non-avian reptiles are rarely incubated, they must be heated by, and absorb water from, the oviposition site for the developing embryo. The mechanisms by which they absorb sufficient, but not excess, water and how these mechanisms vary with local habitat is largely unknown, despite its significance to their evolution. Here, we first performed histology, Fourier-transform infrared spectroscopy and dynamic vapor sorption experiments to elucidate the mechanisms of eggshell absorption for 56 reptile species. Then, we used phylogenetic comparative analysis to test the hypothesis that the absorptive capacity of reptile eggshells increases with aridity of the environment. We found that water absorption increases in the presence of a superficial mucopolysaccharide layer and decreases with increased calcium content. We found that eggs from arid environments have highly absorbent eggshells, but only in species with weakly calcified shells. Our results suggest that reptile eggshells have over evolutionary time tuned absorptive capacity to environmental moisture level. Since these eggs often must sustain conflicting constraints, they may serve as inspirations for new biomimetic materials, such as water filtering membranes or humidity sensors., (© The Author(s) 2024. Published by Oxford University Press on behalf of the Society for Integrative and Comparative Biology.)

In this work, the feasibility of ultra-high drug loaded amorphous solid dispersions (ASDs) for the poorly soluble itraconazole, mebendazole and celecoxib via solvent electrospinning in combination with poly(2-ethyl-2-oxazoline) and fenofibrate in combination with polyvinylpyrrolidone is demonstrated. By lowering the polymer concentration in the electrospinning solution below its individual spinnable limit, ASDs with a drug content of up to 80 wt% are obtained. This is attributed to drug-polymer interactions not being limited by default to hydrogen bonds, as also Van der Waals interactions can result in high drug loadings. The theoretically predicted miscibility by the Flory-Huggins theory is corroborated by the experimental findings based on (modulated) differential scanning calorimetry and x-ray diffraction. Globally, the maximally obtained amorphous drug loadings are higher compared to the loadings found in literature. Additionally, non-sink dissolution tests demonstrate an increase in solubility of up to 50 times compared to their crystalline counterparts. Moreover, due to the lack of precipitation biocompatible PEtOx succeeds in stabilizing the dissolved drug and inhibiting its instant precipitation. The current work thus demonstrates the broader applicability of the electrospinning technique for the production of physically stable ASDs with ultra-high drug loadings, a result which has been validated for several Biopharmaceutics Classification System class II drugs., Competing Interests: Declaration of Competing Interest JB, CV, RH and KDC are listed as inventors on a filed patent application covering high drug-loading ASD nanofibers as presented in this work. R.H. is one of the founders of Avroxa BVBA that commercializes poly(2-oxazoline)s as Ultroxa®. The other authors have no conflicts to declare., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Nanofibrous scaffolds are widely investigated for tendon tissue engineering due to their porous structure, high flexibility, and the ability to guide cells in a preferred direction. Previous research has shown that providing a microenvironment similar to in vivo settings improves tissue regeneration. Therefore, in this work, ingenious multicomponent nanoyarn scaffolds that mimic the fibrillar and tubular structures of tendons are developed for the first time through electrospinning and bundling nanoyarns followed by electrospinning of a nanofibrous shell around the bundle. Multicomponent nanoyarn scaffolds out of poly(ε-caprolactone) with varying porosity, density, and diameter were successfully produced by coelectrospinning with water-soluble poly(2-ethyl-2-oxazoline) as a sacrificial component. The diameter and fiber orientation of the nanoyarns were successfully tuned based on parameter-morphology models obtained by the design of experiments. Cyclic bending tests were performed, indicating that the flexibility of the multicomponent nanoyarn scaffolds depends on the morphology and can be tuned through controlling the number of nanoyarns in the bundle and the porosity. Indirect and direct cell culture tests using mouse and equine tendon cells revealed excellent cytocompatibility of the nanofibrous products and demonstrated the potential of the nanoyarns to guide the growing cells along the nanofiber direction, which is crucial for tendon tissue engineering.

In recent years, ambient ionization mass spectrometry (AIMS) including laser ablation rapid evaporation IMS, has enabled direct biofluid metabolome analysis. AIMS procedures are, however, still hampered by both analytical, i.e., matrix effects, and practical, i.e., sample transport stability, drawbacks that impede metabolome coverage. In this study, we aimed at developing biofluid-specific metabolome sampling membranes (MetaSAMPs) that offer a directly applicable and stabilizing substrate for AIMS. Customized rectal, salivary, and urinary MetaSAMPs consisting of electrospun (nano)fibrous membranes of blended hydrophilic (polyvinylpyrrolidone and polyacrylonitrile) and lipophilic (polystyrene) polymers supported metabolite absorption, adsorption, and desorption. Moreover, MetaSAMP demonstrated superior metabolome coverage and transport stability compared to crude biofluid analysis and was successfully validated in two pediatric cohorts (MetaBEAse, n = 234 and OPERA, n = 101). By integrating anthropometric and (patho)physiological with MetaSAMP-AIMS metabolome data, we obtained substantial weight-driven predictions and clinical correlations. In conclusion, MetaSAMP holds great clinical application potential for on-the-spot metabolic health stratification.

Electrospun nanofiber membranes show high potential in various application fields (e.g., filtration, catalysis, and sensing). Nevertheless, knowledge of the mechanical behavior, and more specifically, the deformation of nanofiber membranes is still limited today which can complicate the appliance of nanofiber membranes in applications where they are mechanically loaded. In this paper, we, therefore, analyzed the mechanical behavior of polymeric nanofiber membranes with different fiber orientations (random and aligned) extensively. Polyamide 6 was used as a representative reference polymer for proof-of-concept. Mechanical tests show that all membranes have a coherent deformation behavior at the macroscale up to the point of fracture. Large variations in stiffness, ultimate strength, and ultimate strain were observed between membranes with different fiber orientations (Random: E-mod: 370 ± 34 MP; UTS: 38.5 ± 6.0 MPa; ε max : 30.0 ± 2.8%; Parallel aligned: E-mod: 753 ± 11 MPa; UTS: 55.4 ± 0.8 MPa; ε max : 12.0 ± 0.1%; Perpendicular aligned: E-mod: 24.1 ± 3.7 MPa; UTS:/; ε max : >40%). This shows the versatility and tunability of the mechanical behavior of these nanofiber membranes. At the microscale, the fibrous structure results in deformation mechanisms that resist failure formation and progression when the membrane is mechanically loaded. This results in a high fracture resistance, even for pre-damaged membranes. Realignment of the fibers along the loading direction causes crack tip blunting, locally reinforcing the membrane.

In this work, an important step is taken towards the bioavailability improvement of poorly water-soluble drugs, such as flubendazole (Flu), posing a challenge in the current development of many novel oral-administrable therapeutics. Solvent electrospinning of a solution of the drug and poly (2-ethyl-2-oxazoline) (PEtOx) is demonstrated to be a viable strategy to produce stable nanofibrous amorphous solid dispersions (ASDs) with ultrahigh drug-loadings (up to 55 wt% Flu) and long-term stability (at least one year). Importantly, at such high drug loadings, the concentration of the polymer in the electrospinning solution has to be lowered below the concentration where it can be spun in absence of the drug as the interactions between the polymer and the drug result in increased solution viscosity. A combination of experimental analysis and molecular dynamics simulations revealed that this formulation strategy provides strong, dominant and highly stable hydrogen bonds between the polymer and the drug, which is crucial to obtain the high drug-loadings and to preserve the long-term amorphous character of the ASDs upon storage. In vitro drug release studies confirm the remarkable potential of this electrospinning formulation strategy by significantly increased drug solubility values and dissolution rates (respectively tripled and quadrupled compared to the crystalline drug), even after storing the formulation for one year., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Many groundbreaking therapies for the treatment of blindness require delivery of biologics or cells to the inner retina by intravitreal injection. Unfortunately, the advancement of these therapies is greatly hampered by delivery difficulties where obstruction of the therapeutics at the inner limiting membrane (ILM) represents the dominant bottleneck. In this proof-of-principle study, we explore an innovative light-based approach to locally ablate the ILM in a minimally invasive and highly controlled manner, thus making the ILM more permeable for therapeutics. More specifically, we demonstrate that pulsed laser irradiation of ILM-bound indocyanine green (ICG), a clinically applied ILM dye, results in the formation of vapor nanobubbles which can disrupt the bovine ILM as well as the extraordinary thick human ILM. We have observed that this photodisruption allows for highly successful retinal delivery of model nanoparticles which are otherwise blocked by the intact ILM. Strikingly, this treatment is furthermore able of enhancing the efficacy of mRNA-loaded lipid nanoparticles within the bovine retina by a factor of 5. In conclusion, this study provides evidence for a light-based approach to overcome the ILM which has the potential to improve the efficacy of all retinal therapies hampered by this delivery barrier., Competing Interests: Declaration of Competing Interest None., (Copyright © 2022 Elsevier B.V. All rights reserved.)

The inner limiting membrane (ILM) represents a major bottleneck hampering efficient drug delivery to the retina after intravitreal injection. To overcome this barrier, we intend to perforate the ILM by use of a light-based approach which relies on the creation of vapor nanobubbles (VNBs) when irradiating photosensitizers with high intensity laser pulses. Upon collapse of these VNBs, mechanical effects can disrupt biological structures. As a photosensitizer, we explore indocyanine green (ICG) loaded nanoparticles (NPs) specifically designed for our application. In light of this, ICG liposomes and PLGA ICG NPs were characterized in terms of physicochemical properties, ICG incorporation and VNB formation. ICG liposomes were found to encapsulate significantly higher amounts of ICG compared to PLGA ICG NPs which is reflected in their VNB creating capacity. Since only ICG liposomes were able to induce VNB generation, this class of NPs was further investigated on retinal explants. Here, application of ICG liposomes followed by laser treatment resulted in subtle disruption effects at the ILM where zones of fully ablated ILM were alternated by intact regions. As the interaction between the ICG liposomes and ILM might be insufficient, active targeting strategies or other NP designs might improve the concept to a further extent.

Recent development in the field of additive manufacturing, also known as three-dimensional (3D) printing, has allowed for the incorporation of continuous fiber reinforcement into 3D-printed polymer parts. These fiber reinforcements allow for the improvement of the mechanical properties, but compared to traditionally produced composite materials, the fiber volume fraction often remains low. This study aims to evaluate the in-nozzle impregnation of continuous aramid fiber reinforcement with glycol-modified polyethylene terephthalate (PETG) using a modified, low-cost, tabletop 3D printer. We analyze how dimensional printing parameters such as layer height and line width affect the fiber volume fraction and fiber dispersion in printed composites. By varying these parameters, unidirectional specimens are printed that have an inner structure going from an array-like to a continuous layered-like structure with fiber loading between 20 and 45 vol%. The inner structure was analyzed by optical microscopy and Computed Tomography (µCT), achieving new insights into the structural composition of printed composites. The printed composites show good fiber alignment and the tensile modulus in the fiber direction increased from 2.2 GPa (non-reinforced) to 33 GPa (45 vol%), while the flexural modulus in the fiber direction increased from 1.6 GPa (non-reinforced) to 27 GPa (45 vol%). The continuous 3D reinforced specimens have quality and properties in the range of traditional composite materials produced by hand lay-up techniques, far exceeding the performance of typical bulk 3D-printed polymers. Hence, this technique has potential for the low-cost additive manufacturing of small, intricate parts with substantial mechanical performance, or parts of which only a small number is needed.

The three-dimensional arrangement of natural and synthetic network materials determines their application range. Control over the real-time incorporation of each building block and functional group is desired to regulate the macroscopic properties of the material from the molecular level onwards. Here we report an approach combining kinetic Monte Carlo and molecular dynamics simulations that chemically and physically predicts the interactions between building blocks in time and in space for the entire formation process of three-dimensional networks. This framework takes into account variations in inter- and intramolecular chemical reactivity, diffusivity, segmental compositions, branch/network point locations and defects. From the kinetic and three-dimensional structural information gathered, we construct structure-property relationships based on molecular descriptors such as pore size or dangling chain distribution and differentiate ideal from non-ideal structural elements. We validate such relationships by synthesizing organosilica, epoxy-amine and Diels-Alder networks with tailored properties and functions, further demonstrating the broad applicability of the platform., (© 2021. The Author(s), under exclusive licence to Springer Nature Limited.)

Wound dressings are high performance and high value products which can improve the regeneration of damaged skin. In these products, bioresorption and biocompatibility play a key role. The aim of this study is to provide progress in this area via nanofabrication and antimicrobial natural materials. Polyhydroxyalkanoates (PHAs) are a bio-based family of polymers that possess high biocompatibility and skin regenerative properties. In this study, a blend of poly(3-hydroxybutyrate) (P(3HB)) and poly(3-hydroxyoctanoate- co -3-hydroxy decanoate) (P(3HO- co -3HD)) was electrospun into P(3HB))/P(3HO- co -3HD) nanofibers to obtain materials with a high surface area and good handling performance. The nanofibers were then modified with silver nanoparticles (AgNPs) via the dip-coating method. The silver-containing nanofiber meshes showed good cytocompatibility and interesting immunomodulatory properties in vitro, together with the capability of stimulating the human beta defensin 2 and cytokeratin expression in human keratinocytes (HaCaT cells), which makes them promising materials for wound dressing applications.

Anthocyanins and pyranoanthocyanins are flavonoids that are present in various food products (e.g., fruit, vegetables, wine, etc.). The large chemical diversity amongst these molecules leads to compound-specific properties such as color and stability towards external conditions. These properties are also attractive for food and non-food applications. The photophysical experimental characterization is not easy as this generally demands advanced analytical techniques along with optimized separation procedures. Molecular modeling can provide insights into the fundamental understanding of the photophysical properties of these compounds in a uniform way for a broad set of compounds. However, the current literature is quite fragmented on this topic. Herein, a large set of 140 naturally derived anthocyanins was evaluated in a systematic way with three functionals (B3LYP, PBE0, and CAM-B3LYP). The accuracy of these functionals was determined with experimental literature λ max,vis values. In addition to λ max,vis values, time-dependent (TD)-DFT calculations also provided oscillator strengths, molar absorption coefficients, and orbital energies, which define whether specific natural anthocyanin-based compounds can be deployed in food and non-food applications such as food additives/colorants, textile dyeing, analytical standards, and dye-sensitized solar cells (DSSCs)., (© 2021 Wiley-VCH GmbH.)

Fiber reinforced composite materials are typically comprised of two phases, i.e., the reinforcing fibers and a surrounding matrix. At a high volume fraction of reinforcing fibers, the matrix is confined to a microscale region in between the fibers (1-200 µm). Although these regions are interconnected, their behavior is likely dominated by their micro-scale. Nevertheless, the characterization of the matrix material (without reinforcing fibers) is usually performed on macroscopic bulk specimens and little is known about the micro-mechanical behavior of polymer matrix materials. Here, we show that the microscale behavior of an epoxy resin typically used in composite production is clearly different from its macroscale behavior. Microscale polymer specimens were produced by drawing microfibers from vitrifying epoxy resin. After curing, tensile tests were performed on a large set of pure epoxy microfiber specimens with diameters ranging from 30 to 400 µm. An extreme ductility was observed for microscale epoxy specimens, while bulk scale epoxy specimens showed brittle behavior. The microsized epoxy specimens had a plastic deformation behavior resulting in a substantially higher ultimate tensile strength (up to 380 MPa) and strain at break (up to 130 %) compared to their bulk counterpart (68 MPa and 8%). Polarized light microscopy confirmed a rearrangement of the internal epoxy network structure during loading, resulting in the plastic deformation of the microscale epoxy. This was further accompanied by in-situ electron microscopy to further determine the deformation behavior of the micro-specimens during tensile loading and make accurate strain measurements using video-extensometry. This work thus provides novel insights on the epoxy material behavior at the confined microscale as present in fiber reinforced composite materials.

In the present study, poly(3-hydroxybuturate-co-3-hydroxyvalerate) (PHBV) and plasticized polylactide acid (PLA) blends were processed by melt extrusion with different weight ratio (up to 20 wt.% of PHBV). Bionanocomposites were obtained through the incorporation of an organomodified montmorillonite (C30B) at 3 wt.%. The main features of the processing and physico-chemical characterization of films and injected samples were assessed and the influence of the components on the chemical, thermal and mechanical properties of the bionanocomposites was investigated. The results indicated that plasticized PLA/PHBV/C30B bionanocomposites present optimal mechanical properties for sanitary applications. Moreover, plasticized PLA/PHBV could lead to finely tuned biomaterials able to form electrospun nanofibers.

Polyhydroxyalkanoates (PHAs) are a family of bio-based polyesters that have found different biomedical applications. Chitin and lignin, byproducts of fishery and plant biomass, show antimicrobial and anti-inflammatory activity on the nanoscale. Due to their polarities, chitin nanofibril (CN) and nanolignin (NL) can be assembled into micro-complexes, which can be loaded with bioactive factors, such as the glycyrrhetinic acid (GA) and CN-NL/GA (CLA) complexes, and can be used to decorate polymer surfaces. This study aims to develop completely bio-based and bioactive meshes intended for wound healing. Poly(3-hydroxybutyrate)/Poly(3-hydroxyoctanoate-co-3-hydroxydecanoate), P(3HB)/P(3HO- co -3HD) was used to produce films and fiber meshes, to be surface-modified via electrospraying of CN or CLA to reach a uniform distribution. P(3HB)/P(3HO- co -3HD) fibers with desirable size and morphology were successfully prepared and functionalized with CN and CLA using electrospinning and tested in vitro with human keratinocytes. The presence of CN and CLA improved the indirect antimicrobial and anti-inflammatory activity of the electrospun fiber meshes by downregulating the expression of the most important pro-inflammatory cytokines and upregulating human defensin 2 expression. This natural and eco-sustainable mesh is promising in wound healing applications.

Background: It is hypothesized that oxidative and epigenetic alterations to DNA induced by ovarian stimulation for in vitro fertilization (IVF) may be associated with an increased risk of diseases and cancer in the offspring and could possibly be attenuated by preconception food supplementation., Methods: In a prospective randomised open-label trial, 62 patients were randomly assigned to either 30 days of preconception treatment with the nutraceutical Fertility woman ® duo (Nutriphyt, Beernem, Belgium) (group 1), this nutraceutical complemented with selenomethionine (group 2), or folic acid only (group 3). Biochemical and epigenetic effects and pregnancy rates were assessed., Results: In all 3 groups the level of DNA oxidative damage, estimated by the concentration of 8-hydroxy- 2-deoxyguanosine over creatinine in early morning urine, and the concentration of homocysteine in the blood decreased after treatment. In group 2, the degree of methylation of the cancer-associated CpG2 dinucleotide of the human Telomerase Reverse Transcriptase (hTERT) promoter region, assessed by pyrosequence in follicular cells obtained at oocyte pick-up, was 18% lower than that of group 3. The pregnancy rate, including the transfer of fresh and frozen embryos, was significantly higher in group 2 (50%) than in group 3 (6%) with the result in group 1 being intermediate (30%)., Conclusion: The results suggest that preconception food supplementation using a specific nutraceutical significantly reduces oxidative and epigenetic DNA changes to follicular cells of women treated by IVF, and may optimize gene expression in the oocytes, thus increasing the pregnancy rate per cycle of ovarian stimulation., Competing Interests: Conflict of interest: Gabriël Devriendt is the CEO of Nutriphyt Ltd. producing the nutraceutical Fertility woman ® . F. Comhaire owns the patent protecting the formulation of QALY 1+2 ® . The remaining authors report no conflict of interest., (Copyright © 2020 Facts, Views & Vision.)

The present review had the aim of describing the methodologies of synthesis and properties of biobased pullulan, a microbial polysaccharide investigated in the last decade because of its interesting potentialities in several applications. After describing the implications of pullulan in nano-technology, biodegradation, compatibility with body and skin, and sustainability, the current applications of pullulan are described, with the aim of assessing the potentialities of this biopolymer in the biomedical, personal care, and cosmetic sector, especially in applications in contact with skin.

Based on differential scanning calorimetry (DSC), X-ray diffraction (XRD) analysis, polarizing microscope (POM), and scanning electron microscopy (SEM) analysis, strategies to close the gap on applying conventional processing optimizations for the field of 3D printing and to specifically increase the mechanical performance of extrusion-based additive manufacturing of poly(lactic acid) (PLA) filaments by annealing and/or blending with poly(3-hydroxybutyrate) (PHB) were reported. For filament printing at 210 °C, the PLA crystallinity increased significantly upon annealing. Specifically, for 2 h of annealing at 100 °C, the fracture surface became sufficiently coarse such that the PLA notched impact strength increased significantly (15 kJ m -2 ). The Vicat softening temperature (VST) increased to 160 °C, starting from an annealing time of 0.5 h. Similar increases in VST were obtained by blending with PHB (20 wt.%) at a lower printing temperature of 190 °C due to crystallization control. For the blend, the strain at break increased due to the presence of a second phase, with annealing only relevant for enhancing the modulus.

Nanofibrous membranes based on polycaprolactone (PCL) have a large potential for use in biomedical applications but are limited by the hydrophobicity of PCL. Blend electrospinning of PCL with other biomedical suited materials, such as gelatin (Gt) allows for the design of better and new materials. This study investigates the possibility of blend electrospinning PCL/Gt nanofibrous membranes which can be used to design a range of novel materials better suited for biomedical applications. The electrospinnability and stability of PCL/Gt blend nanofibers from a non-toxic acid solvent system are investigated. The solvent system developed in this work allows good electrospinnable emulsions for the whole PCL/Gt composition range. Uniform bead-free nanofibers can easily be produced, and the resulting fiber diameter can be tuned by altering the total polymer concentration. Addition of small amounts of water stabilizes the electrospinning emulsions, allowing the electrospinning of large and homogeneous nanofibrous structures over a prolonged period. The resulting blend nanofibrous membranes are analyzed for their composition, morphology, and homogeneity. Cold-gelling experiments on these novel membranes show the possibility of obtaining water-stable PCL/Gt nanofibrous membranes, as well as nanostructured hydrogels reinforced with nanofibers. Both material classes provide a high potential for designing new material applications.

Here, we introduce a novel concept for the fabrication of colored materials with significantly reduced dye leaching through covalent immobilization of the desired dye using plasma-generated surface radicals. This plasma dye coating (PDC) procedure immobilizes a pre-adsorbed layer of a dye functionalized with a radical sensitive group on the surface through radical addition caused by a short plasma treatment. The non-specific nature of the plasma-generated surface radicals allows for a wide variety of dyes including azobenzenes and sulfonphthaleins, functionalized with radical sensitive groups to avoid significant dye degradation, to be combined with various materials including PP, PE, PA6, cellulose, and PTFE. The wide applicability, low consumption of dye, relatively short procedure time, and the possibility of continuous PDC using an atmospheric plasma reactor make this procedure economically interesting for various applications ranging from simple coloring of a material to the fabrication of chromic sensor fabrics as demonstrated by preparing a range of halochromic materials.

With increasing toxicity and environmental concerns, electrospinning from water, i.e., waterborne electrospinning, is crucial to further exploit the resulting nanofiber potential. Most water-soluble polymers have the inherent limitation of resulting in water-soluble nanofibers, and a tedious chemical cross-linking step is required to reach stable nanofibers. An interesting alternative route is the use of thermoresponsive polymers, such as poly(N-isopropylacrylamide) (PNIPAM), as they are water-soluble beneath their lower critical solution temperature (LCST) allowing low-temperature electrospinning while the obtained nanofibers are water-stable above the LCST. Moreover, PNIPAM nanofibers show major potential to many application fields, including biomedicine, as they combine the well-known on-off switching behavior of PNIPAM, thanks to its LCST, with the unique properties of nanofibers. In the present work, based on dedicated turbidity and rheological measurements, optimal combinations of polymer concentration, environmental temperature, and relative humidity are identified allowing, for the first time, the production of continuous, bead-free PNIPAM nanofibers electrospun from water. More specifically, PNIPAM gelation was found to occur well below its LCST at higher polymer concentrations leading to a temperature regime where the viscosity significantly increases without compromising the polymer solubility. This opens up the ecological, water-based production of uniform PNIPAM nanofibers that are stable in water at temperatures above PNIPAM's LCST, making them suitable for various applications, including drug delivery and switchable cell culture substrates.