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Cellulose nanofibrils are one of the keystone materials for sustainable future, yet their poor water repellency hinders their push into industrial applications. Due to complexity and poor economical outcome and/or processing toxicity of the existing hydrophobization methods, nanocellulose loses against its antagonist plastic in medical and food industries. Herein, we demonstrate for the first time the "one-side selective water-repellency activation" in nanocellulose membranes by the means of mild N2-plasma treatment, exhibiting lowest wettability after 20 s of treatment. Hydrophobicity and accompanying Janus character were justified by the topological, chemical and structural reorganizations in cellulose nanofibrils. The findings suggest that the mechanism behind the hydrophilic/hydrophobic change primarily relies on the interplay between OH removal and appearance of SiCH3, originating from the polysiloxanes-based substrate, as well as complementary CNH2 groups formation. First-principles calculations show that NH2 groups moderately increase hydrophobicity, while various SiCH3 substitutions wholly change the character of the surface to repel water. Using nitrogen is shown to be crucial, as N(H)Si(CH3)3 groups induce greater hydrophobicity than simple OSi(CH3)3. Finally, the obtained materials absorb water on the hydrophilic side, while remaining hydrophobic on the other, exhibit high tensile strength, and protection against UV light, demonstrating applicability over wide range of applications.

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Hydrogels are highly sought-after absorbent materials for absorbent pads; however, it is still challenging to achieve a satisfactory balance between mechanical performance, water absorption capacity, and active functionalities. In this work, we presented double-network hydrogels synthesized through acrylic acid (AA) polymerization in the presence of quaternized cellulose nanofibrils (QCNF) and Fe3+. Spectroscopic and microscopic analyses revealed that the combined QCNF and Fe3+ facilitated the formation of double-network hydrogels with combined chemical and physical crosslinking. The synergistic effect of QCNF and Fe3+ resulted in impressive mechanical properties, including tensile strength of 1.98 MPa, fracture elongation of 838.8 %, toughness of 7.47 MJ m-3, and elastic modulus of 0.35 MPa. In comparison to the single-network PAA hydrogel, the PAA/QCNF/Fe3+ (PQFe) hydrogels showed higher and relatively stable swelling ratios under varying pH levels and saline conditions. The PQFe hydrogels exhibited notable antioxidant activity, as evidenced by the 2,2-diphenyl-1-picrylhydrazyl (DPPH) assay, and demonstrated effective antibacterial activity against both Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). These hydrogels show promising potential as an absorbent interlayer in absorbent pads for active food packaging.

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Despite significant research into cellulose nanofibril (CNF) films as substitutes to synthetic plastic materials, commercial applications remain very limited. One major hindrance is the poor water vapor barrier properties of CNF films compared to polyolefins, a critical property for product protection, such as food safety and preservation. To date, it is unknown whether full moisture barrier properties can be achieved with materials made by the assembly of nanofibers and fibrils. A comprehensive understanding of the effect of film structure on water vapor transport properties is required. Here, over 200 films were produced with a wide range of grammages from 30 g/m2 to 580 g/m2 by casting and spray deposition. Their structures were quantified by µCT and SEM and related to their water vapor transmission rates (WVTRs). Porosity and pore connectivity decreased with increasing film grammage, which correlates with the exponential decrease in WVTR. However, the WVTR plateaued at 30 g/m2day, indicating that the known open space and adsorption diffusion mechanisms cannot be fully eliminated by producing high grammage films. Pure cellulose nanofibril films therefore cannot replace polyolefins in packaging applications, requiring modifications such as coating and nanofillers.

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Concerns about food safety and environmental impact from chemical surfactants have prompted interest in natural lignocellulosic materials as alternatives. In this study, we combined hydrated deep eutectic solvent (DES) pretreatment with ultrasound treatment to prepare lignocellulosic nanofibrils (LCNF) from bamboo shoot shells with appropriate surface properties for stabilizing Pickering emulsions. The pretreatment intensity effectively modulated the surface characteristics of LCNF, achieving desirable wettability through lignin retention and in-situ esterification. The resulting LCNF/curcumin Pickering emulsion (CPE) demonstrated curcumin protection and pH-responsive color changes, while the ensuing CPE/PVA composite film exhibited ultraviolet shielding, mechanical strength, oxygen barrier, and antioxidant properties. Furthermore, the CPE/PVA film showed promise as a real-time indicator for monitoring shrimp freshness, maintaining sensitivity to spoilage even after six months of storage. These findings advance the advancement of green LCNF technologies, providing eco-friendly solutions for valorizing bamboo shoot shells and enhancing the application of LCNF in Pickering emulsions.

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A novel photocatalytic adsorbent, a cellulose nanofibrils based hydrogel incorporating carbon dots and Bi2O3/BiOCOOH (designated as CCHBi), was developed to address lignin pollution. CCHBi exhibited an adsorption capacity of 435.0 mg/g, 8.9 times greater than that of commercial activated carbon. This enhanced adsorption performance was attributed to the 3D porous structure constructed using cellulose nanofibrils (CNs), which increased the specific surface area and provided additional sorption sites. Adsorption and photocatalytic experiments showed that CCHBi had a photocatalytic degradation rate constant of 0.0140 min-1, 3.1 times higher than that of Bi2O3/BiOCOOH. The superior photocatalytic performance of CCHBi was due to the Z-scheme photocatalytic system constructed by carbon dots-loaded cellulose nanofibrils and Bi2O3/BiOCOOH, which facilitated the separation of photoinduced charge carriers. Additionally, the stability of CCHBi was confirmed through consecutive cycles of adsorption and photocatalysis, maintaining a removal efficiency of 85 % after ten cycles. The enhanced stability was due to the 3D porous structure constructed by CNs, which safeguarded the Bi2O3/BiOCOOH. This study validates the potential of CCHBi for high-performance lignin removal and promotes the application of CNs in developing new photocatalytic adsorbents.

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High-strength, lightweight, ultrathin, and flexible electromagnetic interference (EMI) shielding materials with a high shielding effectiveness (SE) are essential for modern integrated electronics. Herein, cellulose nanofibrils (CNFs) are employed to homogeneously disperse graphene nanoplates (GNPs) into an aramid nanofiber (ANF) network and silver nanowire (AgNW) network, respectively, producing high-performance nanopapers. These nanopapers, featuring nacre-mimetic microstructures and layered architectures, exhibited high tensile strength (601.11 MPa) and good toughness (103.56 MJ m-3) with a thickness of only 24.58 µm. Their specific tensile strength reaches 447.59 MPa·g-1·cm3, which is 1.74 times that of titanium alloys (257 MPa·g-1·cm3). The AgNW/GNP composite conductive layers exhibit an electrical conductivity of 12010.00 S cm-1, providing the nanopapers with great EMI shielding performance, achieving an EMI SE of 63.87 dB and an EMI SE/t of 25978.80 dB cm-1. The nanopapers also show reliable durability, retaining a tensile strength of 500.96 MPa and an EMI SE of 57.59 dB after 120,000 folding cycles. Additionally, they have a good electrical heating performance with a fast response time, low driving voltage, effective deicing capability, and reliable heating capacity in water. This work presents a strategy to develop a high-performance nanopaper, showing great potential for applications in electromagnetic compatibility, national defense, smart electronics, and human health.

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Bacterial keratitis (BK) is a severe eye infection commonly associated with Staphylococcus aureus (S. aureus), posing a significant risk to vision, especially among contact lens wearers. This research introduces a novel smart nanoplatform (deMS@cNF), developed from demineralized mussel shells (deMS) and reinforced with chitin (CT) nanofibrils, specifically designed for portable photothermal disinfection of contact lenses. The nanoplatform leverages the photothermal properties of eumelanin in mussel shells (MS), which, when activated by a simple bike flashlight, rapidly heats to temperatures up to 95 °C, effectively destroying bacterial contamination. In vitro tests demonstrate that the nanoplatform is biocompatible and non-toxic, making it suitable for medical applications. This study highlights an innovative approach to converting marine biowaste into a safe, effective, and low-cost portable method for disinfecting contact lenses, showcasing the potential of the deMS@cNF platform for broader antimicrobial applications.

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Uranium is the most important fuel for nuclear power operations, and the safe supply of its resources is the key to the development of nuclear power in China. Because of the complex seawater environment and extremely low uranium concentration, extracting uranium from natural seawater poses a significant challenge. In this study, a polyamidoxime-phosphorylated cellulose nanofibril composite aerogel was prepared as an adsorbent for uranium extraction from seawater. An adsorption kinetics test, equilibrium adsorption isotherm model fitting, an adsorption-desorption cycle test, and a selectivity test were carried out to evaluate the adsorption performance of the composite aerogel for uranium extraction. The adsorption capacities for the initial concentrations of 4 and 8 ppm in uranium-spiked pure water were 96.9 and 204.3 mg-U/g-Ads, respectively. The equilibrium uranium adsorption capacities of uranium-spiked simulated seawater were 38.9 and 51.7 mg-U/g-Ads, respectively. The distribution coefficient KD of uranium was calculated to be 2.5 × 107 mL/g. The results show that the polyamidoxime-phosphorylated cellulose nanofiber composite aerogels prepared in this study have the advantages of low cost and high uranium selectivity for uranium extraction from seawater.

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Hydrogels prepared from self-assembled cellulose nanofibrils (CNFs) are widely used in biomedicine, electronics and environmental technology. Their ability to serve as inks for extrusion-based 3D printing is conventionally evaluated by means of rheological tests. A model is developed that describes the response of CNF gels in small- and large-amplitude oscillatory tests in a unified manner. The model involves a reasonably small number of material parameters, ensures good agreement between results of simulation and observations in oscillatory tests and correctly predicts the stress-strain Lissajous curves, experimental data in hysteresis loop tests, and measurements of the steady-state viscosity. The model is applied to analyze how composition and preparation conditions for CNF gels affect transition from shear thinning to weak strain overshoot in large-amplitude shear oscillatory tests. Based on the model, simple relations are derived for the fractal dimension of CNF clusters and the storage modulus of gels prepared in aqueous solutions of multivalent salts. The validity of these equations is confirmed by comparison of their predictions with observations in independent tests.

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Achieving the delicate balance required for both emulsion and gel characteristics, while also imparting biological functionality in gelled emulsions, poses a significant challenge. Herein, Pickering emulsion biogels stabilized is reported by novel biological nanofibrils assembled from natural glutathione (GSH) and a tripod cholic acid derivative (TCA) via electrostatic interactions. GSH, composed of tripeptides with carboxyl groups, facilitates the protonation and dissolution of TCA compounds in water and the electrostatic interactions between GSH and TCA trigger nanofibrillar assembly. Fibrous nuclei initially emerge, and the formed mature nanofibrils can generate a stable hydrogel at a low solid concentration. These nanofibrils exhibit efficient emulsifying capability, enabling the preparation of stable Pickering oil-in-water (O/W) emulsion gels with adjustable phase volume ratios. The entangled nanofibrils adsorbed at the oil-water interface restrict droplet movement, imparting viscoelasticity and injectability to the emulsions. Remarkably, the biocompatible nanofibrils and stabilized emulsion gels demonstrate promising scavenging properties against reactive oxygen species (ROS). This strategy may open new scenarios for the design of advanced emulsion gel materials using natural precursors and affordable building blocks for biomedical applications.

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Personalized three-dimensional (3D) printed foods rich in probiotics were investigated. Lactiplantibacillus plantarum (Lp), as a representative of probiotics, was used to investigate the 3D printing of probiotic-rich dysphagia foods. Here, whey protein isolate nanofibrils (WPNFs) were coated and anchored on bacterial surfaces via biointerfacial supramolecular self-assembly, providing protection against environmental stress and the 3D printing process. The optimized composite gels consisting of High acyl gellan gum (0.25 g), whey protein isolate (1.25 g), fructooligosaccharides (0.75 g), Lp-WPNFs-Glyceryl tributyrate emulsion (Φ = 40%, 3.75 mL) can realize 3D printing, and exhibit high resolution, and stable shape. The viable cell count is higher than 8.0 log CFU/g. They are particularly suitable for people with dysphagia and are classified as level 5-minced & moist in the international dysphagia diet standardization initiative framework. The results provide new insights into the development of WPNFs-coating on bacterial surfaces to deliver probiotics and 3D printed food rich in probiotics.

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Effective and practical cleanup of viscous crude oil spills is extremely important in real harsh marine environments. Herein, we designed a solar-driven, nanocellulose-based Janus aerogel (Janus-A) with excellent floating stability and dual function of oil-water separation and degradation of aqueous organic pollutants. Janus-A, with its amphiprotic nature, was prepared through polypyrrole (PPy) deposition, freeze-drying, octyltrichlorosilane (OTS) impregnation, TiO2 spraying on the bottom surface, and UV irradiation treatment. The photothermal conversion effect of PPy coating raised the surface temperature of aerogel to 75.8 °C within 6 min under one simulated solar irradiation, which greatly reduced the viscosity of the crude oil and increased the absorption capacity of the aerogel to 36.7 g/g. Benefiting from the balance between the buoyancy generated by the hydrophobic part and water absorption of the hydrophilic part, Janus-A showed excellent floating stability under simulated winds and waves. In addition, Janus-A exhibited high degradation efficiency for organic pollutants in water owing to the synergistic photocatalytic properties of TiO2 and PPy. These excellent performances make Janus-A ideal for integrated water-oil separation and water remediation.

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Extracellular matrix (ECM) is essential for tissue development, providing structural support and a microenvironment that is necessary for cells. As tissue engineering advances, there is a growing demand for ECM mimics. Polycaprolactone (PCL) is a commonly used synthetic polymer for ECM mimic materials. However, its biologically inactive surface limits its direct application in tissue engineering. Our study aimed to improve the biocompatibility of PCL by incorporating hemoglobin nanofibrils (HbFs) into PCL using an electrospinning technique. HbFs were formed from bovine hemoglobin (Hb) extracted from industrial byproducts and designed to offer PCL an improved cell adhesion property. The fabricated HbFs@PCL electrospun scaffold exhibits improved fibroblast adherence, proliferation, and deeper fibroblast infiltration into the scaffold compared with the pure PCL scaffold, indicating its potential to be an ECM mimic. This study represents the pioneering utilization of Hb-sourced nanofibrils in the electrospun PCL scaffolds for tissue engineering applications.

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Membranes are a selective barrier that allows certain species (molecules and ions) to pass through while blocking others. Some rely on size exclusion, where larger molecules get stuck while smaller ones permeate through. Others use differences in charge or polarity to attract and repel specific species. Membranes can purify air and water by allowing only air and water molecules to pass through, while preventing contaminants such as microorganisms and particles, or to separate a target gas or vapor, such as H2 and CO2, from other gases. The higher the flux and selectivity, the better a material is for membranes. The desirable performance can be tuned through material type (polymers, ceramics, and biobased materials), microstructure (porosity and tortuosity), and surface chemistry. Most membranes are made from plastic from petroleum-based resources, contributing to global climate change and plastic pollution. Cellulose can be an alternative sustainable resource for making renewable membranes. Cellulose exists in plant cell walls as natural fibers, which can be broken down into smaller components such as cellulose fibrils, nanofibrils, nanocrystals, and cellulose macromolecules through mechanical and chemical processing. Membranes made from reassembling these particles and molecules have variable pore architecture, porosity, and separation properties and, therefore, have a wide range of applications in nano-, micro-, and ultrafiltration and forward osmosis. Despite their advantages, cellulose membranes face some challenges. Improving the selectivity of membranes for specific molecules often comes at the expense of permeability. The stability of cellulose membranes in harsh environments or under continuous operation needs further improvement. Research is ongoing to address these challenges and develop advanced cellulose membranes with enhanced performance. This article reviews the microstructures, fabrication methods, and potential applications of cellulose membranes, providing some critical insights into processing-structure-property relationships for current state-of-the-art cellulosic membranes that could be used to improve their performance.

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Recent scientific interest has surged in the application of bioresources within nanotechnology, primarily because of their eco-friendly nature, wide availability, and cost-effectiveness. Jute is globally recognized as the second most prevalent source of natural cellulose fibers, and it produces a significant quantity of jute sticks as a byproduct. Nanocellulose (NC), which includes cellulose nanofibrils (CNF) and cellulose nanocrystals (CNC), exhibits exceptional properties such as high strength, toughness, crystallinity, thermal stability, and stiffness. These attributes enable its versatile use across various sectors. The extensive surface areas and abundant hydroxyl groups of nanocellulose allow for diverse surface modifications, facilitating the design of advanced functional materials. This comprehensive review provides an overview of recent advancements in the synthesis, characterization, and potential applications of nanocellulose derived from jute. As a versatile natural fiber, jute holds immense potential across various research domains, including nanocellulose synthesis, scaffold fabrication, nanocarbon material preparation, life sciences, electronics and energy storage devices, drug delivery systems, nanomaterial synthesis, food packaging and paper industries. Additionally, its use extends to polymeric nanocomposites, sensors, and coatings. This study summarizes the extensive utilization of jute, emphasizing its versatility and potential across diverse research fields.

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Standalone cellulose nanofibril (CNF) films have a natural tendency to shrink upon drying from wet conditions due to capillary drying stresses. This shrinkage happens in both the radial direction, and the vertical direction. In this study, we prepared two types of CNF films- one in a restrained condition that did not allow shrinkage in the radial direction but enabled it in the vertical direction and another with 11 % radial shrinkage but limited vertical shrinkage. The radial shrinkage led to a more porous structure than the vertical shrinkage, which brought about poorer oxygen/moisture barrier performance. However, the density and oxygen permeability of the films converged to a similar value upon a simple thermocompression process. Radial shrinkage resulted in 140 % and 90 % higher strain at break and toughness in films with a significant sacrifice in strength and modulus. Scanning electron microscopy revealed that radial shrinkage formed wavy layers in the core structure leaving more free space, whereas vertical shrinkage formed flatter layers. Radial shrinkage is likely to produce a thicker individual layer in the core structure of CNF films than vertical shrinkage. The insight from this study will help tune the mechanical and barrier performance of CNF films and their composites.

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Natural polymer-derived nanofibrils have gained significant interest in diverse fields. However, production of bio-nanofibrils with the hierarchical structures such as fibrillar structures and crystalline features remains a great challenge. Herein, an all-natural strategy for simple, green, and scalable top-down exfoliation silk nanofibrils (SNFs) in novel renewable deep eutectic solvent (DES) composed by amino acids and D-sorbitol is innovatively developed. The DES-exfoliated SNFs with a controllable fibrillar structures and intact crystalline features, novelty preserving the hierarchical structure of natural silk fibers. Owing to the amphiphilic nature, the DES-exfoliated SNFs show excellent capacity of assisting the exfoliation of several 2D-layered materials, i.e., h-BN, MoS2, and WS2. More importantly, the SNFs-assisted dispersion of BNNSs with a concentration of 59.3% can be employed to construct SNFs/BNNSs nanocomposite membranes with excellent mechanical properties (tensile strength of 416.7 MPa, tensile modulus of 3.86 GPa and toughness of 1295.4 KJ·m-3) and thermal conductivity (in-plane thermal conductivity coefficient of 3.84 W·m-1·K-1), enabling it to possess superior cooling efficiency compared with the commercial silicone pad.

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Bamboo is composed of thick-walled fibrous tissue and thin-walled parenchymal tissue. To compare the energy consumption of preparing lignocellulose nanofibrils (LCNF) from these bamboo tissues, the crystallinity, sol. viscosity, morphology and mechanical properties of LCNF at different preparation stages were characterized in detail. It required at least nine homogenization cycles for dissociating the fibrous tissue, but only six cycles for the parenchymal tissue. The average diameter of LCNF isolated from fibrous and parenchymal tissues was 45.1 nm and 36.2 nm, respectively. The tensile strength of the LCNF film prepared from parenchymal tissue reached 142.46 MPa, whereas the film from fibrous tissue reached only 122.82 MPa. Additionally, a metal organic framework (MOF) was used to produce MOF-LCNF film with enhanced UV protection and antibacterial properties. The results indicated that the energy consumption for preparing LCNF from parenchymal tissue is significantly lower than that for preparing LCNF from fibrous tissue. This study offers a low-cost and eco-friendly method for preparing LCNF, promoting the precise utilization of different tissues from bamboo based on their unique characteristics.

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In this paper, we develop high aspect ratio nanofibrils from a polycaprolactone-based thermoplastic polyurethane (TPU) and evaluate their performance as a toughening agent. Poly(methyl methacrylate) (PMMA) was chosen as the matrix material because of its inherent brittleness and low resistance to sudden shocks and impact. We show that the addition of as little as 3 wt % of TPU nanofibrils with an average diameter of ∼98 nm and very high aspect ratio can significantly improve both the tensile toughness (∼212%) and impact strength (∼40%) of the chosen matrix (i.e., PMMA) without compromising its original strength, stiffness, and transparency. We compare the performance of TPU nanofibrils with TPU spherical particles─the form TPU typically manifests into when melt-mixed with an immiscible polymer. Our findings highlight that the structure of TPU plays a crucial role in determining the critical concentration of TPU needed for the brittle-ductile transition of the matrix. We also provide new and valuable insights into the unique interfacial interaction (i.e., formation of fibrillar bridges) observed between the PMMA matrix and TPU. We also show that the inclusion of 3 wt % of TPU nanofibrils can notably enhance resistance to creep deformation, even at temperatures close to the glass transition temperature of the matrix. Finally, we evaluate recyclability and demonstrate that the composite containing 3 wt % of TPU nanofibrils can be mechanically recycled without losing any properties. The proposed TPU nanofibrils can withstand repeated reprocessing at temperatures up to 190 °C due to their very high melting point and thermal stability. This presents the opportunity for them to be utilized not just with amorphous PMMA, but also with a range of other materials that can be processed at or below this temperature to remarkably improve their toughness without sacrificing strength and stiffness.

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Lignocellulosic nanofibrils (LCNFs) isolation is recognized as an efficient strategy for maximizing biomass utilization. Nevertheless, achieving a 100% yield presents a formidable challenge. Here, an esterification strategy mediated by the equilibrium moisture in biomass is proposed for LCNFs preparation without the use of catalysts, resulting in a yield exceeding 100%. Different from anhydrous chemical thermomechanical pulp (CTMP0%), the presence of moisture (moisture content of 7 wt%, denoted as CTMP7%) introduces a notably distinct process for the pretreatment of CTMP, comprising the initial disintegration and the post-esterification steps. The maleic acid, generated through maleic anhydride (MA) hydrolysis, degrades the recalcitrant lignin-carbohydrate complex (LCC) structures, resulting in esterified CTMP7% (E-CTMP7%). The highly grafted esters compensate for the mass loss resulting from the partial removal of hydrolyzed lignin and hemicellulose, ensuring a high yield. Following microfluidization, favorable LCNF7% with a high yield (114.4 ± 3.0%) and a high charge content (1.74 ± 0.09 mmol g-1) can be easily produced, surpassing most previous records for LCNFs. Additionally, LCNF7% presented highly processability for filaments, films, and 3D honeycomb structures preparation. These findings provide valuable insights and guidance for achieving a high yield in the isolation of LCNFs from biomass through the mediation of equilibrium moisture.