Inferring biophysical properties of membranes during endocytosis using machine learning.

Endocytosis is a fundamental cellular process in eukaryotic cells that facilitates the transport of molecules into the cell. With the help of fluorescence microscopy and electron tomography, researchers have accumulated extensive geometric data of membrane shapes during endocytosis. These data contain rich information about the mechanical properties of membranes, which are hard to access via experiments due to the small dimensions of the endocytic patch. In this study, we propose an approach that combines machine learning with the Helfrich theory of membranes to infer the mechanical properties of membranes during endocytosis from a dataset of membrane shapes extracted from electron tomography. Our results demonstrate that machine learning can output solutions that both match the experimental profile and satisfy the membrane shape equations derived from Helfrich theory. The learning results show that during the early stage of endocytosis, the inferred membrane tension is negative, indicating the presence of strong compressive forces at the boundary of the endocytic invagination. Our method presents a generic framework for extracting membrane information from super-resolution imaging.

Effect of Al2Cu constituent layer thickness discrepancy on the tensile mechanical behavior of Cu/Al2Cu/Al layered composites: a molecular dynamics simulation.

Nano-polycrystalline Cu/Al2Cu/Al layered composites with different layer thicknessesdof single-crystal Al2Cu constituent are constructed. The effects ofdon the strength and fracture modes of nano-polycrystalline Cu/Al2Cu/Al layered composites are systematically investigated by molecular dynamics simulations. The uniaxial tensile results show that the ultimate strength and fracture mode of the nano-polycrystalline Cu/Al2Cu/Al layered composites do not change monotonically with the change of single crystal Al2Cu constituent layer thicknessd, the ultimate strength peaking atd= 2.44 nm, and the toughness reaching the optimum atd= 4.88 nm. The improvement of deformation incompatibility between Cu, Al and Al2Cu components increases the ultimate strength of polycrystalline Cu/Al2Cu/Al laminated composites. Due to the high activity of Cu dislocation and the uniformity of strain distribution of single crystal Al2Cu, the fracture of nano-crystalline Cu/Al2Cu/Al layered composites changes from brittleness to toughness. This study is crucial to establish the organic connection between microstructure and macroscopic properties of Cu/Al layered composites. To provide theoretical basis and technical support for the application of Cu/Al layered composites in high-end fields, such as automotive and marine, aerospace and defense industries.

Mussel-inspired adhesive gelatin-polyacrylamide hydrogel wound dressing loaded with tetracycline hydrochloride to enhance complete skin regeneration.

Even though the global wound care market size was valued at USD 19.83 billion in 2020, it is still a challenge to develop a hydrogel-based wound dressing with a good mechanical property, adhesiveness and antibacterial property. This study established and validated a mussel-inspired adhesive hydrogel wound dressing with antibacterial activity by dispersing tetracycline hydrochloride into hydrogel based polydopamine, gelatin and polyacrylamide. A tough hydrogel with a fracture stress of 0.42 MPa was prepared by changing the contents of the gelatin and polyacrylamide. With the addition of polydopamine and tetracycline hydrochloride, the hydrogel was endowed with an adhesive property (with a tissue adhesive strength of 4.13 kPa) and antibacterial activity against both Escherichia coli and Staphylococcus aureus. Finally, a rat full-thickness skin defect wound model was used to evaluate the performance of the hydrogels in wound repair. The hydrogel group showed a significantly reduced wound area (95.72%) compared with the blank group (86.34%) on day 14. The hydrogel promoted the collagen deposition, weakened the inflammatory response and enhanced wound healing. Therefore, the hydrogel with multifunctional properties is a promising candidate for complete skin regeneration.

Robust Fabrication of Fluorescent Cellulosic Materials via Hantzsch Reaction.

Hantzsch reaction is one of the typical multicomponent reactions (MCRs), and it is employed herein to endow cellulosic materials with fluorescent properties. For example, acetoacetyl (ACAC)-bearing cotton fabric prepared via transesterification with tert-butyl acetoacetate is subjected to an aqueous Hantzsch reaction with formaldehyde and ammonium acetate at ambient temperature. A strong fluorescent emission around 460 nm is achieved within 10 min. XPS, fluorescent spectroscopy, and elemental analysis are used to confirm the presence of 1,4-dihydropyridine (DHP) rings on the surface of the fabric. TGA, SEM, XRD, and mechanical testing results show that the modification process has minimum impact on intrinsic properties of the fabric. The strategy is also shown to be generally applicable to various forms of cellulosic materials and different aldehydes. This fast and simple approach enriches the application of MCR in modification of cellulose and cellulose derivatives.

Chiral Spiro-Axis Induced Blue Thermally Activated Delayed Fluorescence Material for Efficient Circularly Polarized OLEDs with Low Efficiency Roll-Off.

A spiro-axis skeleton not only introduces circularly polarized luminescence (CPL) into thermally activated delayed fluorescence (TADF) molecules but also enhances the intramolecular through space charge transfer (TSCT) process. Spiral distributed phenoxazine and 2-(trifluoromethyl)-9H-thioxanthen-9-one-10,10-dioxide act as donor and acceptor units, respectively. The resulting TADF enantiomers, (rac)-OSFSO, display emission maxima at 470 nm, small singlet-triplet energy gap (ΔEST ) of 0.022 eV and high photoluminescence quantum yield (PLQY) of 81.2 % in co-doped film. The circularly polarized OLEDs (CP-OLEDs) based on (R)-OSFSO and (S)-OSFSO display obvious circularly polarized electroluminescence (CPEL) signals with dissymmetry factor up to 3.0×10-3 and maximum external quantum efficiency (EQEmax ) of 20.0 %. Moreover, the devices show remarkably low efficiency roll-off with an EQE of 19.3 % at 1000 cd m-2 (roll-off ca. 3.5 %), which are among the top results of CP-OLEDs.

Multi-responsive, self-healing and adhesive PVA based hydrogels induced by the ultrafast complexation of Fe3+ ions.

Herein, a PVA (polyvinyl alcohol)-based multi-responsive hydrogel was prepared by introducing the dynamic and reversible supramolecular complexation between polyvinyl alcohol acetoacetate (PVAA) and Fe3+ ions within 20 s at room temperature. PVAA-Fe hydrogels could be achieved by the simple mixing process of a PVAA aqueous solution with FeCl3 aqueous solution. The soluble PVAA was synthesized by the reaction of PVA with tert-butyl acetoacetate (t-BAA) via transesterification in dimethyl sulfoxide (DMSO). The chemical structure of PVAA was systematically characterized by FT-IR and 1H NMR spectroscopy. The resulting hydrogel showed excellent self-healing behavior without other external stimuli. It was also demonstrated that the PVAA-Fe hydrogel exhibited multi-responsive properties, such as responsiveness to pH, redox, light irradiation and temperature. In addition, the presence of Fe3+ ions and Cl- ions in the gel imparted the PVAA-Fe hydrogel with favorable conductivity. Therefore, the strategy for the facile preparation of the hydrogel in this work could provide a benign and versatile method for achieving multi-functional soft materials for various applications such as smart devices, logic gates, and sensors.

Synthesis of fibrous LaFeO3 perovskite oxide for adsorption of Rhodamine B.

The LaFeO3 perovskite oxide decorated active carbon fibers (LFO-ACFs) based on cotton fabric waste were successfully synthesized through sol-gel loading and thermal treatment. LaFeO3 perovskite and cotton fabric waste were combined to an eco-friendly and cheap adsorbent, which could reuse the leftover materials of textile industry and realize their functional modification. The structural, morphology/microstructure and functional groups were investigated through X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), Energy Dispersive X-ray (EDX), Fourier Transform Infrared spectroscopy (FTIR), respectively. The XRD pattern suggested the cotton fabric matrix didn't influence the structure of LaFeO3 perovskite oxide. In SEM studies, LFO-ACFs still maintained fibrous shape of the raw cotton fibers, and the EDX analysis showed that the main elements of the prepared LFO-ACFs were La, Fe, O and C. The synthesized LFO-ACF was employed for adsorption of cational dye of Rhodamine B (RhB), and the effects of adsorption parameters, i.e. pH, contact time, solution temperature and initial concentration of dye, on adsorption behavior were investigated. Results suggested the adsorption performance of LFO-ACF for RhB was nearly not affected by solution pH and its maximum adsorption capacity fitted by the Langmuir isothermal model could attain 182.6 mg/g at 293 K. The adsorption kinetics followed the pseudo-second-order equation and the regeneration of LFO-ACF could be well realized through an easy pyrolysis method.

Electrothermal Phase Change Composite with Flexibility over a Wide Temperature Range for Wearable Thermotherapy.

Flexible electrothermal composite phase change materials (PCMs) are promising candidates for portable thermotherapy. However, a great challenge remains to achieve high PCM loading while maintaining reasonable flexibility. Herein, the polypyrrole-decorated melamine foam (PPy@MF) was fabricated and thereafter applied to confine binary PCM mixtures composed of a high-enthalpy long-chain polyethylene glycol (PEG4000) and its short-chain homologue (PEG200) to make the novel PPy@MF-PEG4000+200 composite PCM. At a high loading of up to 74.1% PEG4000 and a high latent heat energy storage density of 150.1 J/g, the composite PCM remained flexible at temperature (-20 °C) far below its phase transition point thanks to the plasticine effect of PEG200. The composite also demonstrated good Joule heating performance, providing fast heating from 28 to 70 °C at low applied voltages (4.5-6.0 V). The energy could be stored efficiently and released to maintain the composites at the proper temperature. The electrothermal performance of the composite remained undisturbed during curved or repeated bending, showing good potential to be used for personal thermal management and thermotherapy.

Study of reactive dyes and their hydrolyzed forms in a real trichromatic dyeing process by capillary electrophoresis with UV detection.

Detecting the concentration of reactive dyes and their hydrolyzed products is essential for controlling the dyeing process and is an important guide for upgrading and improving textile dyeing technology. In this study, capillary electrophoresis (CE) with UV detection was for the first time applied in a real trichromatic dyeing process to provide qualitative and quantitative determination of reactive dyes and their hydrolyzed forms. Here, three original reactive dyes (SES-Cl-red-195, SES-Cl-yellow-145, and SES-Cl-blue-194), their vinyl sulfone forms (VS-Cl-red-195, VS-Cl-yellow-145, and VS-Cl-blue-194), and complete hydrolyzed forms (HES-OH-red-195, HES-OH-yellow-145, and HES-OH-blue-194) could be baseline separated in our developed BGE comprised of 10.0 mol/L Na2B4O7, 15% (V/V) ACN at pH 8.50 that adjusted by 0.50 mol/L H3BO3. The LODs (S/N = 3) of nine analytes ranged from 0.3 to 1.3 mg/L, and high sensitivities were achieved with UV detection. The RSDs of peak area and migration time were in the ranges of 1.4-3.8% and 0.39-1.29%, which indicated the CE methods were reliable for studying different dye forms in complex dye baths, and for evaluating dyeing process quality. Thus, the percentage of dye-uptake in single and trichromatic combination dyes was calculated based on the concentration of the original and their vinyl sulfone and hydrolyzed forms, and the result was consistent with the traditional UV-Vis method.

Green, chemical-free, and high-yielding extraction of nanocellulose from waste cotton fabric enabled by electron beam irradiation.

Recycling and high-value reutilization of waste cotton fabrics (WCFs) has attracted a widespread concern. One potential solution is to extract nanocellulose. Sulfuric acid hydrolysis is a conventional method for the production of nanocellulose with high negative charge from WCFs. However, the recycling and disposal of chemicals in nanocellulose production, along with low yields, remain significant challenges. Consequently, there is a pressing need for a sustainable method to produce nanocellulose at higher yield without the use of chemicals. Herein, we propose a green, sustainable and chemical-free method to extract nanocellulose from WCFs. The nanocellulose displayed a rod-like shape with a length of 50-300 nm, a large aspect ratio of 18.4 ± 2 and the highest yield of up to 89.9 %. The combined short-time and efficient two-step process, involving electron beam irradiation (EBI) and high-pressure homogenization (HPH), offers a simple and efficient alternative approach with a low environmental impact, to extract nanocellulose. EBI induced a noticeable degradation in WCFs and HPH exfoliated cellulose to nano-size with high uniformity via mechanical forces. The as-prepared nanocellulose exhibits excellent emulsifying ability as the Pickering emulsion emulsifier. This work provides a facile and efficient approach for nanocellulose fabrication as well as a sustainable way for recycle and reutilization of the waste cotton fabrics.

Lightweight and robust cellulose/MXene/polyurethane composite aerogels as personal protective wearable devices for electromagnetic interference shielding.

The increasing electromagnetic pollution is urgently needed as an electromagnetic interference shielding protection device for wearable devices. Two-dimensional transition metal carbides and nitrides (MXene), due to their interesting layered structure and high electrical conductivity, are ideal candidates for constructing efficient conductive networks in electromagnetic interference shielding materials. In this work, lightweight and robust cellulose/MXene/polyurethane composite aerogels were prepared by mixing cellulose nanofiber (CNF) suspensions with MXene, followed by freeze-drying and coating with polyurethane. In this process, CNF effectively assembled MXene nanosheets into a conductive network by enhancing the interactions between MXene nanosheets. The prepared aerogel exhibited the shielding effectiveness of 48.59 dB in the X-band and an electrical conductivity of 0.34 S·cm-1. Meanwhile, the composite aerogel also possessed excellent thermal insulation, infrared stealth, mechanical and hydrophobic properties, and can be used as a wearable protective device to protect the human body from injuries in different scenarios while providing electromagnetic interference shielding protection.

Preparation of high antioxidant nanolignin and its application in cosmetics.

Lignin, as a natural polyphenol, displays anti-oxidant activity by trapping and binding free radicals through its free phenolic hydroxyl groups. However, the most accessible form, industrial lignins, generally has low phenolic hydroxyl content, which severely limits their application value and scenarios. Herein, we showed that potassium-glycerate deep eutectic solvent (PG-DES) treatment can be combined with laccase oxidation to afford prepared high antioxidant lignin nanoparticles (HA-LNPs) with notably improved anti-oxidant activities benefiting from both the enhanced phenolic hydroxyl content 170.8 % and reduced average particle size (59.0 nm). At concentrations as low as 60 µg/mL, HA-LNPs showed favorable effects in promoting collagen formation. When HA-LNPs were used as an active ingredient in the anti-aging mask formulation, the reactive oxygen species (ROS) scavenging activity of mask samples containing 0.4 % HA-LNPs reached 37.2 %. The data suggest great promise of HA-LNPs as a natural antioxidant for formulating in anti-aging skin care products.

A fast and effective way to measure the inner pore size distributions of wetted cotton fibers and their pretreatment performance using time-domain nuclear magnetic resonance.

This study reports the findings from using time-domain nuclear magnetic resonance (TD-NMR) to analyze the pore structures of cotton fibers. Cotton fibers, which swell and soften in water, present challenges for conventional pore measurement techniques. TD-NMR overcomes these by measuring the transverse relaxation time (T2) of water protons within the fibers, indicative of internal pore sizes. We established a T2-to-pore size conversion equation using mixed cellulose ester membranes. This enabled differentiation between strongly bound, loosely bound, and free water within the fibers, and detailed the water distribution. A method for measuring the pore size distribution of wet cotton fiber was developed using TD-NMR. We then examined how various pretreatments affect the fibers' internal pores by comparing their pore size distribution and porosity. Specifically, caustic mercerization primarily enlarges the porosity and size of larger pores, while liquid ammonia treatment increases porosity but reduces the size of smaller pores. This research confirms TD-NMR's utility in assessing cotton fabrics' wet processing performance.

High-tensile chitin films regenerated from cryogenic aqueous phosphoric acid.

The abuse of non-renewable fossil resources and the resulting plastic pollution have posed a great burden on the environment. Fortunately, renewable bio-macromolecules have shown great potential to replace synthetic plastics in fields ranging from biomedical applications, and energy storage to flexible electronics. However, the potential of recalcitrant polysaccharides, such as chitin, in the above-mentioned fields have not been fully exploited because of its poor processability, which is ultimately due to the lack of suitable, economical, and environmentally friendly solvent for it. Herein, we demonstrate an efficient and stable strategy for the fabrication of high-strength chitin films from concentrated chitin solutions in cryogenic 85 wt% aqueous phosphoric acid (aq. H3PO4). The regeneration conditions, including the nature of the coagulation bath and its temperature are important variables affecting the reassembly of chitin molecules and hence the structure and micromorphology of the films. Uniaxial orientation of the chitin molecules by applying tension to the RCh hydrogels further endows the films with enhanced mechanical properties of up to 235 MPa and 6.7 GPa in tensile strength and Young's modulus, respectively.

Photoinduced Absorption Spectroscopy of Photoelectrocatalytic Methylene Blue Oxidation on Titania and Hematite: The Thermodynamic and Kinetic Impacts on Reaction Pathways.

Photoelectrochemical oxidation of methylene blue is investigated, with particular focus on the difference in kinetics and thermodynamics of decoloration and mineralization employing photoinduced absorption spectroscopy. Hematite and titania photoanodes are used for the comparison of both reactions, which is determined to be associated with the depth of the valence band (3.2 vs 2.5 V for titania and hematite, respectively). Methylene blue is mineralized by the titania photoanode, however it is only oxidized to small fragments by hematite. Such difference is related to the valence band potential that provides the thermodynamic driving force for photogenerated holes in both materials. In addition, the kinetic competition of water oxidation is found to occur on titania by controlling the pH of the electrolyte. In the pH 14 electrolyte, mineralization of methylene blue is suppressed due to the faster and dominant kinetics of water oxidation, in contrast to the complete mineralization in the near neutral electrolyte where water oxidation kinetics are modest. These results clearly address the importance considering both thermodynamic and kinetic challenges of methylene blue oxidation, which has been thought to be an easy molecule to oxidize, as the model reaction in the application of photo(electro)catalysis using metal oxides.

Rapid activation of peroxymonosulfate with iron(â ¢) complex for organic pollutants degradation via a non-radical pathway.

Developing high-performance catalytic systems for eliminating contaminants effectively in water has received a lot of attention. However, the complexity of practical wastewater poses a challenge for degrading organic pollutants. Non-radical active species with strong resistance to interference have shown great advantages in degrading organic pollutants under complex aqueous conditions. Herein, a novel system was constructed by Fe(dpa)Cl2 (FeL, dpa = N, N'-(4-nitro-1,2-phenylene) dipicolinamide) activating peroxymonosulfate (PMS). The mechanism study verified that the FeL/PMS system had high efficiency in producing high-valent iron-oxo and singlet oxygen (1O2) to degrade various organic pollutants. In addition, the chemical bonding between PMS and FeL was elucidated by the density functional theory (DFT) calculations. The FeL/PMS system could remove 96% Reactive Red 195 (RR195) in 2 min, which was much higher than other systems involved in this study. More attractively, the FeL/PMS system demonstrated general resistance to interference from common anions (Cl-, HCO3-, NO3- and SO42-), humic acid (HA) and pH changes and were thus compatible with various natural waters. This work provides a new approach for producing non-radical active species, which is a promising catalytic system for water treatment.

Fabrication of Fe-BTC on aramid fabrics for repeated degradation of isoproturon.

Catalytic degradation is a promising and ideal technology in environmental remediation. Among them, catalytic oxidation and photocatalysis respectively based on catalysts and photocatalysts both trigger broad interests because of their high removal activity. However, the reusability of the powder catalysts still faces substantial challenges. Here, a simple strategy is proposed to load Fe-BTC catalyst on aramid fabrics (AF) to construct Fe-BTC MOF @ aramid fabric (Fe-BTC@AF) composite materials with layer-by-layer in situ self-assembly methods. The experimental results illustrated that 98% isoproturon could be removed by Fe-BTC@AF20 with oxidant H2O2, while the single Fe-BTC@AF20 could photo-degrade 99% isoproturon within 7 h. Meanwhile, it could sustain a high degradation rate of more than 80%, even if it had gone through 5 degradation cycles. Thus, the Fe-BTC@AF composite has a significant advantage in the recycling ability for degradation of isoproturon, which will have potential applications in the efficient removal of organic contaminants in water.

Facile construction of photocatalytic cellulose-based sponge with stable flotation properties as efficient and recyclable photocatalysts for sewage treatment.

Dispersion and recycling of powdered nano-photocatalysts for water purification is still not an easy task. The self-supporting and floating photocatalytic cellulose-based sponges ware conveniently prepared by anchoring BiOX nanosheet arrays on cellulose-based sponge's surface. The introduction of sodium alginate into the cellulose-based sponge significantly enhanced the electrostatic adsorption of bismuth oxygen ions and promoted the formation of bismuth oxyhalide (BiOX) crystal nuclei. Among the photocatalytic cellulose-based sponges, the sponge (BiOBr-SA/CNF) modified with bismuth oxybromide displayed excellent photocatalytic ability for photodegrading 96.1 % rhodamine B within 90 min under 300 W Xe lamp irradiation (λ > 400 nm). The loading of bismuth oxybromide on cellulose-based sponge's surface improves the flotation stability of the cellulose-based sponge. Benefiting from excellent load fastness of bismuth oxybromide nanosheet and flotation stability of BiOBr-SA/CNF sponge, after 5 cycles of recycling, the photodegradation rates of BiOBr-SA/CNF sponge to rhodamine B remained above 90.2 % (90 min), and it also has excellent photocatalytic degradation effect on methyl orange and herbicide isoproteron. This work may provide a convenient and efficient method to construct self-supporting and floating photocatalytic sponges using cellulose based materials as substrates for sewage treatment.

Highly stretchable porous regenerated silk fibroin film for enhanced wound healing.

Silk fibroin (SF) has received interest in tissue engineering owing to its biocompatibility, biodegradability, and favorable mechanical properties. However, the complex preparation, brittleness, and lack of pores in the structure of the silk fibroin film limit its application. Herein, we show that facile dissolution of SF in aqueous phosphoric acid followed by regeneration in aqueous ammonium sulfate ((NH4)2SO4) could afford highly stretchable films with nano-pores formed in the nonsolvent-induced phase separation process. The named phase separation, which determines the morphology and mechanical properties of the regeneration silk fibroin (RSF) films, is highly dependent on the (NH4)2SO4 concentration as well as the initial concentration of the SF solution. Therefore, the RSF films exhibit a tunable pore size ranging from 230 to 510 nm and excellent stretchability with tensile strain up to 143 ± 16%. Most interestingly, the RSF films were shown to support the proliferation of human skin fibroblasts in vitro as well as speed up full-thickness skin wound healing in a rat model. This work establishes an easy and feasible method to access porous RSF membranes that can be used for wound dressing in clinical settings.

Customizable High-Contrast Optical Responses: Dual Photosensitive Colors for Smart Textiles.

Smart textiles demonstrating optical responses to external light stimuli hold great promise as functional materials with a wide range of applications in personalized decoration and information visualization. The incorporation of high-contrast, vivid, and real-time optical signals, such as color change or fluorescence emission, to indicate light on/off states is both crucial and challenging. In this study, we have developed a dual output photosensitive dye system possessing photochromic and photofluorescent properties, which was successfully applied to the dyeing and finishing processes of cotton fabrics. The design and fabrication of this dye system were based on the unique photoinduced proton transfer (PPT) principle exhibited by the water-soluble spiropyran (trans-MCH) molecule. The dual output response relies on the open-/closed-loop mechanism, wherein light regulates the trans-MCH molecule. Upon excitation by UV or visible light, the dye system and dyed fabrics display significant color changes and fluorescence switching in a real-time and highly reversible manner. Moreover, diverse photosensitive color systems can be tailored by direct blending with commercially available water-soluble dyes. By integrating high-contrast dual optical outputs into this scalable, versatile, and reversible dye system, we envisage the development and design of smart textiles capable of producing high-end products.