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.

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.

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.

Association between systemic immune-inflammation index and metabolic syndrome and its components: results from the National Health and Nutrition Examination Survey 2011-2016.

BACKGROUND: Metabolic syndrome (MetS), a worldwide public health problem, affects human health and quality of life in a dramatic manner. A growing evidence base suggests that MetS is strongly associated with levels of systemic immune inflammation. The present study aimed to investigate the possible relationship between the systemic immune-inflammation index (SII), a novel inflammatory marker, and MetS to provide data support for effective MetS prevention by reducing the systemic inflammatory response. METHODS: We included adult participants with complete SII and MetS information from the 2011-2016 National Health and Nutrition Examination Survey (NHANES). MetS was defined as using the criteria developed by the Adult Treatment Program III of the National Cholesterol Education Program. The formula for SII was as follows: SII = platelet counts × neutrophil counts/ lymphocyte counts. Weighted linear regression was used to assess differences in variables across SII quartile groups after the SII score was divided into 4 quartiles. The independent interaction between SII and MetS was investigated using weighted multivariate logistic regression analysis and subgroup analysis, and the relationship between SII levels and 5 particular MetS items was further explored in depth. RESULTS: A total of 12,402 participants, 3,489 of whom were diagnosed with MetS, were included in this study. After correcting for covariates, the results of a logistic regression of multistage weighted complex sampling data revealed that participants with higher SII scores had a higher chance of developing MetS (odds ratio (OR) = 1.33, 95% confidence interval (CI): 1.14-1.55) and that SII levels could be used as an independent risk factor to predict that likelihood of MetS onset. In the Q1-Q4 SII quartile group, the risk of developing MetS was 1.33 times higher in the Q4 group, which had the highest level of systemic immune inflammation than in the Q1 group. After adjusting for all confounding factors, SII scores were found to have a negative correlation with high-density lipoprotein cholesterol (OR = 1.29; 95% CI, 0.99-1.67, P = 0.056) and a significant positive correlation with waist circumference (OR = 2.17; 95% CI, 1.65-2.87, P < 0.001) and blood pressure (BP) (OR = 1.65; 95% CI, 1.20-2.27, P = 0.003). Gender, age, and smoking status were shown to alter the positive association between SII and MetS in subgroup analyses and interaction tests (p for interaction < 0.05). Additionally, we demonstrated a nonlinear correlation between SII and MetS. The findings of the restricted cubic spline indicated that there was an inverted U-shaped association between SII and MetS. CONCLUSIONS: Our findings imply that increased SII levels are related to MetS, and SII may be a simple and cost-effective method to identify individuals with MetS. Therefore, protective measures such as early investigation and anti-inflammatory interventions are necessary to reduce the overall incidence of MetS.

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.

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.

Composite hydrogel based oxidated sodium carboxymethyl cellulose and gelatin loaded carboxymethylated cotton fabric for hemostasis and infected wound treatment.

The fabric-based wound dressings are hard to maintain a moist environment for wound healing while the hemostatic property and gas permeability of some hydrogel-based wound dressings are not ideal. This study first put forward a strategy of checkerboard-pattern wound dressing: 1) preparing the base fabric with hemostatic property, 2) printing multifunctional hydrogels onto one side of the base fabric to form checkerboard patterns, 3) modifying the other side of the base fabric to be hydrophobic. In this manner, the composite dressing not only maintained the advantages of hydrogels, but also inherited good mechanical property, hemostatic property, and gas permeability from the base fabric. Here, the cotton fabric was carboxymethylated to be MCF. To obtain multifunctional hydrogel, sodium carboxymethylcellulose was oxidated to introduce aldehyde groups to form Schiff base with amino groups in gelatin, besides, dopamine and Ag nanoparticles were introduced to endow the hydrogel with antioxidant property and antibacterial activity. The multifunctional hydrogel was printed onto one side of MCF, subsequently, the deposition of paraffin made the other side of this dressing become hydrophobic. The good performance of the obtained dressing in hemostatic process and wound healing demonstrated its potential in the field of wound treatment.

Clinical, Radiological and Pathological Characteristics Between Cerebral Small Vessel Disease and Multiple Sclerosis: A Review.

Cerebral small vessel disease (CSVD) and multiple sclerosis (MS) are a group of diseases associated with small vessel lesions, the former often resulting from the vascular lesion itself, while the latter originating from demyelinating which can damage the cerebral small veins. Clinically, CSVD and MS do not have specific signs and symptoms, and it is often difficult to distinguish between the two from the aspects of the pathology and imaging. Therefore, failure to correctly identify and diagnose the two diseases will delay early intervention, which in turn will affect the long-term functional activity for patients and even increase their burden of life. This review has summarized recent studies regarding their similarities and difference of the clinical manifestations, pathological features and imaging changes in CSVD and MS, which could provide a reliable basis for the diagnosis and differentiation of the two diseases in the future.

Lignocellulose Extraction from Sisal Fiber and Its Use in Green Emulsions: A Novel Method.

Regenerated lignocellulose nanofibrils (RLCNFs) have recently piqued the interest of researchers due to their widespread availability and ease of extraction. After dewaxing, we treated sisal fiber with alkali, followed by heating and agitation, to obtain RLCNFs, which were then vacuum oven-dried. We used a variety of characterization techniques, including XRD, SEM, and FT-IR, to assess the effects of the alkali treatment on the sisal fiber. Various characterizations demonstrate that lignocellulose fibrils have been successfully regenerated and contaminants have been removed. In addition, employing the RLCNFs as a stabilizer, stable Pickering emulsions were created. The effects of RLCNF concentration in the aqueous phase and water-to-oil volume ratio on stability were studied. The RLCNFs that have been produced show promise as a stabilizer in Pickering emulsions.

Morphology-Controlled Synthesis of Polyphosphazene-Based Micro- and Nano-Materials and Their Application as Flame Retardants.

Common flame retardants, such as halogen-based materials, are being phased-out owing to their harmful environmental and health effects. We prepared poly-(cyclotriphosphazene-co-4,4'-sulfonyldiphenol) (PZS) microspheres, nanotubes, capsicum-like nanotubes, and branched nanotubes as flame retardants. An increase in reaction temperature changed the morphology from nanotubes to microspheres. A PZS shape had a positive effect on the flame retardancy of polyethylene terephthalate (PET). The PZS with a capsicum-like nanotube morphology had the best flame retardancy, and the PET limiting oxygen index increased from 25.2% to 34.4%. The flame retardancy capability was followed by PZS microspheres (33.1%), branched nanotubes (32.8%), and nanotubes (32.5%). The capsicum-like nanotubes promote the formation of highly dense and continuous carbon layers, and they release a non-combustible gas (CO2). This study confirms polyphosphazene-based flame retardants as viable and environmentally-friendly alternatives to common flame retardants. It also presents a novel and facile design and synthesis of morphology-controlled nanomaterials with enhanced flame retardant properties.

Integrated Janus cellulosic composite with multiple thermal functions for personalized thermal management.

The effective integration of multiple thermal functions into one material is highly attractive in personal thermal management, taking the complex application environment into consideration. Herein, a multifunctional Janus cellulosic composite encompassing superior electrical heating, energy storage, thermal insulation, and infrared camouflage performance was firstly developed by integrating Janus cellulose nanofibers (CNF) aerogel, polypyrrole (PPy), and polyethylene glycol (PEG). In practice, the active heating-thermal regulation layer (PPy@CNFphilic-PEG) of multifunctional Janus cellulosic composite is faced inward to provide heating on-demand through the joint action of the electrically conductive PPy and thermally regulative PEG. The outward-facing hydrophobic aerogel layer (CNFphobic) serves as the thermal insulator, which simultaneously enables infrared camouflage by reducing heat loss to the environment via infrared radiation. This work presents an effective and facile strategy toward multifunctional Janus materials for efficient personal thermal management, showing great promise for potential applications, such as thermal comfort, infrared camouflage, and security protection.

Antibacterial thyme oil-loaded zwitterionic emulsion hydrogels.

Emulsion hydrogels are structurally composite materials combining the advantages of emulsions and hydrogels with the ability to accommodate hydrophobic and hydrophilic components in one system. It is a promising strategy for the excellent encapsulation and delivery of many bioactive ingredients. In this work, the thyme oil-loaded zwitterionic emulsion hydrogels are constructed by the cellulose acetoacetate-horseradish peroxidase-hydrogen peroxide-initiated (CAA-HRP-H2O2-initiated) ternary enzyme-mediated polymerization of the thyme oil-in-water (O/W) emulsions stabilized by cellulose acetoacetate (CAA). CAA is the key component in the system, acting as the emulsifier and the polymerization mediator simultaneously. The formed zwitterionic poly(sulfobetaine methacrylate) (PSBMA) hydrogel network provides emulsion hydrogels with good hydration capacity and potential anti-fouling performance. The thyme oil-loaded zwitterionic emulsion hydrogels exhibit interconnected, uniform, and adjustable porous structures with tunable mechanical properties, antifouling performance, good biocompatibility, and excellent antibacterial activity against S. aureus and E. coli. These results all demonstrate that the ternary enzyme-mediated polymerization of zwitterionic monomers in the continuous phase of O/W emulsion templates is a facile and efficient strategy to encapsulate hydrophobic bioactive ingredients.

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.

High-tensile regenerated cellulose films enabled by unexpected enhancement of cellulose dissolution in cryogenic aqueous phosphoric acid.

We have demonstrated, for the first time, high-efficient non-destructive and non-derivative dissolution of cellulose could be achieved in cryogenic aqueous phosphoric acid. Cellulose from different sources and of varying degree of polymerization from 200 (MCC) to 2200 (cotton fabric) could be dissolved completely to afford solutions containing 5 wt%-18 wt% cellulose, from which ultra-strong and tough cellulose films of tensile strength as high as 707 MPa could be obtained using water as the coagulant. These solutions can be stored at -18 °C for extended time without noticeable degradation while desired degree of polymerization is also attainable by tuning the storage conditions. The findings of this work call for renewal attention on phosphoric acid as a promising cellulose solvent for being non-toxic, non-volatile, easy to handle, and cost-effective.

A Nature-Inspired Monolithic Integrated Cellulose Aerogel-Based Evaporator for Efficient Solar Desalination.

Solar-driven seawater desalination is a prospective approach to tackle the problem of freshwater shortage. Establishing a robust, efficient solar-thermal water evaporator with great salt-resistance through a facile and scalable fabrication technique is still a challenge. In this study, a floatable and robust monolithic integrated cellulose aerogel-based evaporator (MiCAE) with high performance is fabricated by carefully designing and integrating three functional components, namely, a hydrophilic cellulose-PVA aerogel (CPA), hydrophobic silylated cellulose aerogel (SCA), and multiwalled carbon nanotube (MCNT) coating layer (CPA@CNT), through the heterogeneous mixing and freeze-drying aerogel fabrication step in situ. Inspired by woods and mushrooms, the incorporation of SCA with mushroom-shaped CPA possessing wood-like structures in MiCAE can realize heat localization and effectively suppress irreversible heat dissipation. Meanwhile, CPA endows the evaporator with the rapid water transportation and great salt excretion capability because of its low-tortuosity porous structure. Thanks to the synergistic effect of the integrated functional structures, in the highly concentrated brine (17.5 wt %), the MiCAE can still realize the combination of high efficiency and obvious salt-resistance behavior. This work offers a facile, efficient salt-resistance solution for seawater desalination.

Self-healing and acidochromic polyvinyl alcohol hydrogel reinforced by regenerated cellulose.

Recently, integration of self-healing, color-tunable, sol-gel converted properties into hydrogel has attracted interest for preparing a reinforced multifunctional hydrogel. Herein, acidochromic regenerated cellulose (ARC) was incorporated into the polyvinyl alcohol/borax (PB) matrix for constructing a tough, self-healing, multicolor and sol-gel converted smart hydrogel (PB/ARC). The mechanical properties of PB/ARC hydrogel were improved after introducing ARC, which could bear a weight of 200 g and had high maximum tensile strength (6.8 times) and compressive strength (2.3 times). PB/ARC hydrogel automatically fused within 15 s after being cut and quickly recovered to the original state after being subjected to high shear strain, showing excellent self-healing ability. The color of hydrogel could be tuned between yellow and purple by altering pH values (5-12). In addition, PB/ARC hydrogel exhibited reversible sol-gel conversion in response to the change of acidity and alkalinity. This study offers a new and facile strategy for developing multifunctional smart hydrogel.

In situ growth of CuS NPs on 3D porous cellulose macrospheres as recyclable biocatalysts for organic dye degradation.

Aiming at recyclable catalyst carriers, porous cellulose macrospheres from wood pulp dissolved in an alkaline urea system were regenerated by simple injection regeneration. After solvent exchange, porous cellulose macrospheres (CMs) with a high specific surface area of 325.3 m2 g-1 were obtained by lyophilization, and CuS nanoparticles (CuS NPs) were coated on CMs by in situ growth in the liquid phase to achieve CuS-supported CM macrospheres (CuS@CM). The results indicated that the CuS@CM biocatalyst was successfully prepared with an average diameter of approximately 1.2 mm. In addition, CuS@CM was further used as a heterogeneous catalyst for the catalytic degradation of methylene blue (MB) and methyl orange (MO) model dyes during the oxidation of hydrogen peroxide (H2O2). In the presence of low doses of H2O2, the degradation rate of MB reached 94.8% within 10 min, showing high catalytic activity under neutral and alkaline conditions. After five cycles, 90.1% of the original catalytic activity was still retained, indicating that the prepared CuS@CM composite possessed excellent catalytic activity and reusability.

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.

Synthetic semicrystalline cellulose oligomers as efficient Pickering emulsion stabilizers.

Nanocellulose are promising Pickering emulsion stabilizers for being sustainable and non-toxic. In this work, semicrystalline cellulose oligomers (SCCO), which were synthesized from maltodextrin using cellobiose as primer by in vitro enzymatic biosystem, were exploited as stabilizers for oil-in-water Pickering emulsions. At first, the morphology, structure, thermal and rheological properties of SCCO suspensions were characterized, showing that SCCO had a sheet morphology and typical cellulose-Ⅱ structure with 56 % crystallinity. Then the kinetic stabilities of emulsions containing various amounts of SCCO were evaluated against external stress such as pH, ionic strength, and temperature. Noting that SCCO-Pickering emulsions exhibited excellent stabilities against changes in centrifugation, pH, ionic strengths, and temperatures, and it was also kinetically stable for up to 6 months. Both SCCO suspensions and their emulsions exhibited gel-like structures and shear-thinning behaviors. These results demonstrated great potential of SCCO to be applied as nanocellulosic emulsifiers in food, cosmetic and pharmaceutical industries.

The effect of the degree of substitution on the solubility of cellulose acetoacetates in water: A molecular dynamics simulation and density functional theory study.

The effect of the degree of substitution (DS) on the aqueous solubility of cellulose acetoacetates (CAA) was investigated by molecular dynamics simulations and density functional theory calculations. Using average non-covalent interaction and the electrostatic potential analyses done on cellobiose as the model, it was showed both polar and non-polar areas of the system increased as the more hydroxyls were replaced by acetoacetate groups. Analyses of the solvation free energies of a celludecose (glucan containing 10 monosaccharide sugar units) at constant pressure and temperature showed the polar solvation free energies and the number of decose-water hydrogen bonds increased as DS was varied from 0.3 to 0.8, which contributes to higher solubility in water. When the DS of CAA increased from 0.8 to 1.5, it became insoluble again because the plateaued increase in solvation free energy could no longer compensate for the decreasing CAA-water hydrogen bonding interactions. The growing van der Waals interactions among CAA molecules as the molecule grows bigger with each attached AA group also contributes to the decreasing water solubility.