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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., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

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., Competing Interests: Declaration of competing interest Authors have no declaration of interest in publishing this review article., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

In this study, a novel hydrogel, β-cyclodextrin/carbon dots-grafted cellulose nanofibrils hydrogel (βCCH), was fabricated for removal and fluorescence determination of levofloxacin (LEV). A comprehensive analysis was performed to characterize its physicochemical properties. Batch adsorption experiments were conducted, revealing that βCCH reached a maximum adsorption capacity of 1376.9 mg/g, consistent with both Langmuir and pseudo-second-order models, suggesting that the adsorption process of LEV on βCCH was primarily driven by chemical adsorption. The removal efficiency of βCCH was 99.2 % under the fixed conditions (pH: 6, initial concentration: 20 mg/L, contact time: 300 min, temperature: 25 °C). The removal efficiency of βCCH for LEV still achieved 97.3 % after five adsorption-desorption cycles. By using βCCH as a fluorescent probe for LEV, a fast and sensitive method was established with linear ranges of 1-120 mg/L and 0.2-1.0 μg/L and a limit of detection (LOD) as low as 0.09 μg/L. The viability of βCCH was estimated based on the economic analysis of the synthesis process and the removal of LEV, demonstrating that βCCH was more cost-effective than commercial activated carbon. This study provides a novel approach for preparing a promising antibiotic detection and adsorption material with the advantages of stability, and cost-effectiveness., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

In this study, an antibacterial material (CNF@CoMn-NS) with oxidase-like activity was created using ultrathin cobalt‑manganese nanosheets (CoMn-NS) with a larger specific surface area grown onto pineapple peel cellulose nanofibrils (CNF). The results showed that the CoMn-NS grew well on the CNF, and the obtained CNF@CoMn-NS exhibited good oxidase-like activity. The imidazole salt framework of the CNF@CoMn-NS contained cobalt and manganese in multiple oxidation states, enabling an active redox cycle and generating active oxygen species (ROS) such as singlet molecular oxygen atoms ( 1 O 2 ) and superoxide radical (·O 2 - ), resulting in the significant inactivation of Staphylococcus aureus (74.14%) and Escherichia coli (54.87%). Importantly, the CNF@CoMn-NS did not exhibit cytotoxicity. The CNF@CoMn-NS further self-assembled into a CNF@CoMn-NS paper with flexibility, stability, and antibacterial properties, which can effectively protect the wound of two varieties of pears from decay caused by microorganisms. This study demonstrated the potential of using renewable and degradable CNF as substrate combined with artificial enzymes as a promising approach to creating antibacterial materials for food preservation and even extending to textiles and biomedical applications., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

The high structural anisotropy and colloidal stability of cellulose nanofibrils' enable the creation of self-standing fibrillar hydrogel networks at very low solid contents. Adding methacrylate moieties on the surface of TEMPO oxidized CNFs allows the formation of more robust covalently crosslinked networks by free radical polymerization of acrylic monomers, exploiting the mechanical properties of these networks more efficiently. This technique yields strong and elastic networks but with an undefined network structure. In this work, we use acrylate-capped telechelic polymers derived from the step-growth polymerization of PEG diacrylate and dithiothreitol to crosslink methacrylated TEMPO-oxidized cellulose nanofibrils (MATO CNF). This combination resulted in flexible and strong hydrogels, as observed through rheological studies, compression and tensile loading. The structure and mechanical properties of these hydrogel networks were found to depend on the dimensions of the CNFs and polymer crosslinkers. The structure of the networks and the role of individual components were evaluated with SAXS (Small-Angle X-ray Scattering) and photo-rheology. A thorough understanding of hybrid CNF/polymer networks and how to best exploit the capacity of these networks enable further advancement of cellulose-based materials for applications in packaging, soft robotics, and biomedical engineering., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier Ltd.. All rights reserved.)

A novel photocatalytic adsorbent, a cellulose nanofibrils based hydrogel incorporating carbon dots and Bi 2 O 3 /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 Bi 2 O 3 /BiOCOOH. The superior photocatalytic performance of CCHBi was due to the Z-scheme photocatalytic system constructed by carbon dots-loaded cellulose nanofibrils and Bi 2 O 3 /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 Bi 2 O 3 /BiOCOOH. This study validates the potential of CCHBi for high-performance lignin removal and promotes the application of CNs in developing new photocatalytic adsorbents., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

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 N 2 -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 SiCH 3 , originating from the polysiloxanes-based substrate, as well as complementary CNH 2 groups formation. First-principles calculations show that NH 2 groups moderately increase hydrophobicity, while various SiCH 3 substitutions wholly change the character of the surface to repel water. Using nitrogen is shown to be crucial, as N(H)Si(CH 3 ) 3 groups induce greater hydrophobicity than simple OSi(CH 3 ) 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., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Cellulose-based humidity sensors have attracted great research interest due to their hydrophilicity, biodegradability, and low cost. However, they still suffer from relatively low humidity sensitivity. Due to the presence of negatively charged carboxylate groups, 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibril (CNF) exhibits enhanced hydrophilicity and ion conductivity, which is considered a promising candidate for humidity sensing. In this work, we developed a facile strategy to improve the humidity sensitivity of CNF films by regulating their surface charge density. With the increase in surface charge density, both water uptake and charge carrier densities of the CNF films can be improved, enabling a humidity sensitivity of up to 44.5 % (%RH) -1 , higher than that of most polymer-based humidity sensors reported in the literature. Meanwhile, the sensor also showed good linearity (R 2  = 0.998) over the 15-75 % RH at 1 kHz. With these features, the CNF film was further demonstrated for applications in noncontact sensing, such as human respiration, moisture on fingertips, and water leakage, indicating the great potential of CNF film in humidity monitoring., Competing Interests: Declaration of competing interest The authors declare that they have no financial interests/personal relationships which may be considered as potential competing interests., (Copyright © 2024 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Cellulose nanofibrils (CNF) isolation based on a catalyst-free maleic anhydride esterification has proven to be effective, however, the effects of pulp hornification on CNF isolation by this strategy have yet to be explored, which could present significant impacts for CNF isolation. Herein, dried northern bleached softwood Kraft pulp (D-NBSK) and never-dried northern bleached softwood Kraft pulp (ND-NBSK) were selected as the substrates. After esterification with maleic anhydride (MA), the esterified ND-NBSK pulp (E-ND) shows a significantly smaller size and more fragmented structure than the esterified D-NBSK pulp (E-D). Meanwhile, higher degree of esterification can be realized for the never dried pulp as compared to the dried pulp, which is corroborated by the significantly stronger characteristic peaks of CO (1720 cm -1 ) and -COO - (1575 cm -1 ) from the FTIR spectra and the higher surface charge content (0.86 ± 0.04 mmol/g vs. 0.55 ± 0.05 mmol/g). A comparison of the characteristics of the resulting CNF similarly demonstrated the negative impact of hornification. Overall, this work indicates that hornification tends to reduce the accessibility of chemical reagents to the pulp, leading to insufficient deconstruction. Such negative impact of hornification should be considered when performing nanocellulose isolation, especially when using pulp as feedstock., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Emulsions with reduced fat and natural stabilizers are currently prevalent. Herein, semisolid emulsions with an oil phase of 50 % were successfully prepared using cellulose nanofibrils from mushroom stipes as stabilizers. Cellulose nanofibrils obtained by high-pressure homogenization were dendritic-like and possessed a contact angle of 70.50 ± 0.41°. The rheological properties and stability of emulsions increased significantly as nanocellulose concentrations increased from 5 to 20 mg/mL, while nanocellulose at 25-30 mg/mL significantly reduced the storage stability and anti-lipid oxidation ability of emulsions. The microstructure of semisolid emulsions demonstrated that nanocellulose fibers at 20 mg/mL could stabilize emulsions by forming compact interfacial films around droplets and creating intensive bridging networks between neighboring droplets, while nanofibers at concentrations over 20 mg/mL easily clustered in the aqueous phase, making the droplets more susceptible to aggregation and demulsification. The results demonstrate that cellulose nanofibrils from mushroom byproducts have the potential to stabilize semisolid food-grade emulsions., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Nanocellulose is a sustainable nanomaterial and a versatile green platform that has attracted increasing attention. Although the wide applications of its aqueous suspensions are closely related to rheology, comprehensive studies of their rheological behavior, especially the yielding behavior, are still limited. Herein, to investigate the relationship between structure and rheological properties, the viscoelasticity, thixotropy and yielding behavior of two commonly used nanocelluloses, rod-shaped cellulose nanocrystals (CNCs) and filamentous cellulose nanofibrils (CNFs), were systematically investigated. The viscosity, viscoelasticity and thixotropic behavior of the suspensions were analyzed by steady-state shear, frequency sweep, creep-recovery, hysteresis loop, and three-interval thixotropic recovery tests. The yielding behaviors were evaluated through creep, steady-state shear, step shear rate, stress ramps, amplitude sweep, and large amplitude oscillatory shear tests. The rheological properties of the two typical suspensions showed a strong dependence on concentration and time. However, compared to CNC suspensions, CNF suspensions exhibited stronger thixotropy and higher yield stress due to the higher aspect ratio of CNF and the stronger structural skeleton of the suspensions as supported by Simha's equation and micromorphology analysis. This work provides a theoretical rheology basis for the practical applications of nanocellulose suspensions in various fields., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Motivated by the quest for biocompatibility, we report on oil-in-water (O/W), high-internal-phase Pickering emulsions stabilized via complexes of mechanical cellulose nanofibrils (CNF) and food-grade cationic surfactant ethyl lauroyl arginate (LAE). The complexation of oppositely charged CNF and LAE can be held together by electrostatic interaction. Their effect on suspensions electrostatic stabilization, heteroaggregation state, and emulsifying ability was studied and related to properties of resultant interfacial tension between oil and water and 3D printing of emulsions. The Pickering system with adjustable droplet diameter and stability against creaming and oiling-off during storage was achieved resting with LAE loading. Complexes formed by LAE adjustment act as Pickering stabilizers and three-dimensional networks in emulsion system, forming a scaffold with elastoplastic rheological properties that flows above critical stress while, without any additional treatment, exhibiting the required self-standing properties for 3D printing. By understanding the properties of CNF/LAE behavior in bulk and on interfaces, printing edible functional foods of CNF/LAE-based emulgel inks has been demonstrated to enable regulation of oil release., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Nanocellulose-based aerogels have been considered as one of the ideal candidates for CO 2 capture in practical applications owing to their lightweight and porous properties. Additionally, various adsorbents with amine groups have been widely used as effective CO 2 capture and storage strategies. Herein, amino-functionalized aerogels were prepared by sol-gel and freeze-drying methods using two typical nanocelluloses (cellulose nanofibrils (CNFs) and cellulose nanocrystals (CNCs)) as substrates. In addition, the reaction parameters for grafting and amino functionalization were optimized. The CNC and CNF aerogels could be easily modified by the hydrothermal growth of the amino group, and they exhibited attractive properties in terms of CO 2 adsorption, recyclability, thermal stability, hydrophobicity, and CO 2 /CH 4 mixture separation. The amino-functionalized CNF aerogel exhibited superior performance to the CNC aerogel, which was attributed to the increased cross-linking binding sites for hydrogen bonding in the CNF aerogel. The results of this study indicated that amino-functionalized nanocellulose aerogels can be considered a promising biodegradable, sustainable, and environmentally friendly material for CO 2 capture and removal of CO 2 from CH 4 ., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023. Published by Elsevier Ltd.)

The use of nanocellulose (NC) has increased significantly in the food industry, as subtypes such as cellulose nanofibrils (CNF) or bacterial cellulose (BC) have been demonstrated to be a source of insoluble fiber with important benefits for human health. Despite these advantages, and due to its nanoscale size, NC must be assessed from a safety perspective that considers its exposure, fate, and biological effects in order to help more accurately estimate its potential hazards. The exposure routes of humans to NC include (i) ingestion during consumption of foods that contain cellulose as a food ingredient or (ii) contact of food with cellulose-containing materials, such as its packaging. That is why it is important to understand the potentially toxic effects that nanomaterials can have on human health, understanding that the different types of NC behave differently in terms of their ingestion, absorption, distribution, metabolism, and excretion. By analysing both in vitro and in vivo studies, the purpose of this paper is to present the most recent findings on the different types of NC and their safety when used in food. In addition, it provides an overview of relevant studies into NC and its health benefits when used as a food additive., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Author A. Cañas-Gutiérrez, received fees for research support from Instituto Tecnológico Metropolitano. The other authors declare having received hours in their work plan to carry out the investigation in your institution., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

In order to alleviate the resource and environmental problems caused by plastic film materials, the development of biodegradable cellulose-based films is crucial. Inspired by the strengthening mechanism of cellulose-lignin network from wood, carboxylated lignin (CL) was isolated using maleic acid (MA) pretreatment catalyzed by metal chlorides. Compared with pure MA, the presence of metal ions yielded CL with high carboxyl content (0.34 mmol/g), small size and good dispersibility. CL was then composited with CNF to prepare various CL/cellulose nanofibrils (CNF) composite films. When the addition of ferric chloride was 0.3 mmol/g maleic acid, the corresponding composite films exhibited highest tensile strength (180.0 MPa), Young's modulus (13.0 GPa) and excellent ultraviolet blocking rate (97.0 %). Meanwhile, the interaction forces measured by atomic force microscope showed that the binding between CNF and various CLs (276-406 nN) was higher than that between pure CNFs (202 nN), verifying that CL enhanced the mechanical properties of composite films. In summary, this work constructs a super-strong network between CL and CNF synergistically mediated by metal ion crosslinking and hydrogen bonding, which can be a promising alternative to replace conventional plastics in multiple areas., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023. Published by Elsevier Ltd.)

Non-sustainable single-use plastics used for food packaging needs to be phased out. Films made from cellulose nanofibrils (CNFs) are suitable candidates for biodegradable and recyclable packaging materials as they exhibit good mechanical properties, excellent oxygen barrier properties and high transparency. Yet, their poor water vapour barrier properties have been a major hindrance in their commercialisation. Here, we describe the preparation of 25 μm thick CNF films with significantly improved water vapour barrier properties after deposition of ultrathin polymeric and metallic coatings, parylene C and aluminium, respectively. When first adding a 40 nm aluminium layer followed by an 80 nm parylene layer, i.e. with a combined thickness of less than one percent of the CNF film, a water vapour transmission rate of 2.8 g m -2 d -1 was achieved at 38 °C and 90 % RH, surpassing a 25 μm polypropylene film (4-12 g m -2 d -1 ). This is an improvement of more than 700 times compared to uncoated CNF films, under some of the harshest possible conditions a packaging material will need to endure in commercial use. The layers showed a good and even coverage, as assessed by atomic force microscopy, and the parylene-coated surfaces were hydrophobic with a contact angle of 110°, providing good water repellency., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 The Authors. Published by Elsevier Ltd.. All rights reserved.)

The target of this study is to gain a deeper understanding of the micro-dissolution process of cellulose in alkaline aqueous solutions and to develop a novel method for extracting cellulose nanofibrils (CNFs). Herein, the dissolution process of cellulose in alkaline aqueous solutions will be controlled by varying the temperature, and the undissolved cellulose will be analyzed to reveal the microscopic dissolution process of cellulose, and a novel process for extracting cellulose nanofibrils (CNFs) will be developed based on the findings. The crystalline structure of cellulose was gradually disrupted as the dissolution progressed, and the crystal form of cellulose changed gradually from cellulose I to cellulose II during the dissolution process, while all undissolved cellulose crystals remained as cellulose I. Cellulose, after its structure is disrupted during the dissolution process, will inevitably decompose into CNFs, and the microscopic dissolution process of cellulose follows a "top-down" dissolution sequence. The CNFs extraction method developed in this study can extract CNFs with high yield (>60 %) in a stable manner, as well as narrow particle size distribution, high crystallinity (>77 %), and good thermal stability. This study enhances the comprehension of the dissolution process of cellulose and paves a possible way for industrialization of CNFs production., Competing Interests: Declaration of competing interest We would like to submit the enclosed manuscript entitled “Microscopic dissolution process of cellulose in alkaline aqueous solvents and its application in CNFs extraction - investigating temperature as a variable”, which we wish to be considered for publication in Carbohydrate Polymers. No conflict of interest exits in the submission of this manuscript, and manuscript is approved by all authors for publication. The work was original research that has not been published previously, and not under consideration for publication elsewhere. I have not submitted my manuscript to a preprint server before submitting it to Carbohydrate Polymers., (Copyright © 2023. Published by Elsevier Ltd.)

In recent years, there has been a lot of interest in developing composite hydrogels with superior mechanical and conductive properties. In this study, triple-network (TN) cellulose nanofiber hydrogels were prepared by using cellulose nanofiber as the first network, isotropic poly(acrylamide-co-acrylic acid) as the second network, and polyvinyl alcohol as the third network via a cyclic freezing-thawing process. The strong (9.43 ± 0.14 MPa tensile strength, (445.5 ± 7.0)% elongation-at-break), tough (15.12 ± 0.14 MJ/m 3 toughness), and conductive (0.0297 ± 0.00021 S/cm ionic conductivity) TN cellulose nanofiber hydrogels were effectively created after being pre-stretched in an external force field, cross-linked by Fe 3+ and added Li + . The produced composite TN cellulose nanofiber hydrogels were successfully used as a flexible sensor for real-time monitoring and detecting human movements, highlighting their potential for wearable electronics, medical technology, and human-machine interaction. CHEMICAL COMPOUNDS STUDIED IN THIS ARTICLE: Acrylamide (PubChem CID: 6579); Acrylic acid (PubChem CID: 6581); Ammonium persulfate (PubChem CID: 6579); N, N'-methylene bisacrylamide (PubChem CID: 17956053); Sodium bromide (PubChem CID: 253881); Sodium hydroxide (PubChem CID: 14798); Sodium hypochlorite (PubChem CID: 23665760); Sodium chlorite (PubChem CID: 23668197); 2,2,6,6-tetramethylpiperidinyl-1-oxide (PubChem CID: 2724126); Polyvinyl alcohol (PubChem CID: 11199); Lithium chloride (PubChem CID: 433294); Iron nitrate nonahydrate (PubChem CID: 129774236)., Competing Interests: Declaration of competing interest There are no conflicts to declare., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Developing new agricultural products, such as new fertilizers with high use efficiency and less negative impact on the environment, is required in sustainable agriculture. In this vein, controlled-release fertilizers (CRFs) have been designed to decrease nutrient waste and increase nutrients' availability to plants. Various CRFs have been developed based on petroleum-derived polymers with many advantages over conventional fertilizers. Although, their use is limited due to their adverse effects on the soil and environment. To overcome these issues, CRFs based on biopolymers represent a new generation of fertilizers developed by encapsulating nutrients with cellulose nanofibrils (CNFs). CNFs and the hydrogels based on CNFs have great potential to be applied as CRFs matrix as they are biodegradable, minimize environmental pollution, and exhibit a great controlled-release potential and water/nutrient retention capacity. In order to gain a better understanding of the potential benefits of these new fertilizers in agricultural systems, this review summarizes the recent advances in CNFs in CRFs, the coating methods, hydrogel preparation techniques, and their impact on plant growth and soil. By examining these factors in depth, a better understanding can be gained on how these novel fertilizers can help improve agricultural productivity and sustainability., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023. Published by Elsevier Ltd.)

Carboxymethyl cellulose modified with norbornene groups (NorCMC) and cellulose nanofibrils (CNFs) produced through mechanical refining without chemical pretreatment formed interpenetrating network hydrogels through a UV-light initiated thiol-ene reaction. The molar ratio of thiols in crosslinkers to norbornene groups off the NorCMC (T:N), total polymer weight percent in the hydrogel, and weight percent of CNFs of the total polymer content of the hydrogels were varied to control hydrogel properties. This method enabled orders of magnitude changes to behavior. Swelling in aqueous environments could be significant (>150 %) without CNFs to minimal (<15 %) with the use of 50 % CNFs. NorCMC and CNF networks interacted synergistically to create hydrogels with compression modulus values spanning 1 to 150 kPa - the values of most biological tissues. T:N and total polymer weight percent could be varied to create hydrogels with different CNF content, but the same compression modulus, targeting 10 and 100 kPa hydrogels and providing a system that can independently vary fibrillar content and bulk modulus. Analysis of the effective crosslinks, thiol-ene network mesh size, and burst release of the polymer indicated synergistic interactions of the NorCMC thiol-ene and CNFs networks. These interactions enhanced modulus and degradation control of the network under physiological conditions., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

The usage of low-cost, readily available, or even disposable, single-use membranes in macromolecules' purification and separation is still in the development phase. In this research, highly porous (>95 %), water- and compression stable cation-exchange membranes were prepared by freeze-casting using cellulose nanofibrils (CNF) and citric acid (CA) acting as a crosslinker and source of weak anionic (carboxylic) surface groups arising from the mono-esterified CA. The membranes were characterized by different analytical techniques, and evaluated for the ionic adsorption efficacy of different proteins in dead-end filtration mode using a Tri-buffer of pH 8. The membrane's internal microstructure (porosity and density) with the available (quantity and access) carboxylic groups was confirmed, to determine not only the proteins' specific (related to the net charged and molecular weight) adsorption dynamic (>52 % of positive Lysozyme/Cytochrome, <8 % of negative BSA/Myoglobin; ≤0.5 g/L) at extremely high flow rates (>3.000 hL/h*MPa*m 2 ), but also their desorption (>97 %) and re-equilibration (using NaCl) with flux recovery (>80 %). Such efficiency was achieved with up to 5 consecutive filtering cycles. The high permeability (>87 %) of the spherical and negatively surface charged microparticles (used as models) also suggests the likelihood of removing larger microbial species, which, while retaining relatively smaller and positively charged proteins, further increases their potential in biopharma applications., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Cellulose nanofibrils (CNFs) are increasingly used as precursors for foams, films and composites, where water interactions are of great importance. In this study, we used willow bark extract (WBE), an underrated natural source of bioactive phenolic compounds, as a plant-based modifier for CNF hydrogels, without compromising their mechanical properties. We found that the introduction of WBE into both native, mechanically fibrillated CNFs and TEMPO-oxidized CNFs increased considerably the storage modulus of the hydrogels and reduced their swelling ratio in water up to 5-7 times. A detailed chemical analysis revealed that WBE is composed of several phenolic compounds in addition to potassium salts. Whereas the salt ions reduced the repulsion between fibrils and created denser CNF networks, the phenolic compounds - which adsorbed readily on the cellulose surfaces - played an important role in assisting the flowability of the hydrogels at high shear strains by reducing the flocculation tendency, often observed in pure and salt-containing CNFs, and contributed to the structural integrity of the CNF network in aqueous environment. Surprisingly, the willow bark extract exhibited hemolysis activity, which highlights the importance of more thorough investigations of biocompatibility of natural materials. WBE shows great potential for managing the water interactions of CNF-based products., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023. Published by Elsevier Ltd.)

Bioplastics are considered as potential alternatives to non-renewable and non-biodegradable petroleum-based plastics. Inspired by ionic and amphiphilic properties of mussel protein, we proposed a versatile and facile strategy for the fabrication of a high-performance chitosan (CS) composite film. This technique incorporates a cationic hyperbranched polyamide (QHB) and a supramolecular system based on the lignosulphonate (LS)-functionalized cellulose nanofibrils (CNF) (LS@CNF) hybrids. The cationic QHB was synthesized by a one-step process from hyperbranched polyamide and quaternary ammonium salt. Meanwhile, the functional LS@CNF hybrids act as a well-dispersed and rigid cross-linked domain in CS matrix. Owing to the interconnected hyperbranched and enhanced supramolecular network, the toughness and tensile strength of the CS/QHB/LS@CNF film simultaneously increased to 19.1 MJ/m 3 and 50.4 MPa, 170.2 % and 72.6 % higher than the pristine CS film. Additionally, the functional QHB/LS@CNF hybrids endow the films with superior antibacterial activity, water resistance, UV shielding, and thermal stability. This bioinspired strategy provides a novel and sustainable method for the production of multifunctional CS films., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Bacterial nanocellulose (BNC), due to its inherent nanometric scale and strength properties, can be considered as a good candidate to be used in papermaking. This work explored the possibility of using it in the production of fine paper as a wet-end component and for the paper coating. Filler-containing handsheet production was performed with and without the presence of common additives typically used in the furnish of office papers. It was found that, under optimized conditions, BNC mechanically treated by high-pressure homogenization could improve all the evaluated paper properties (mechanical, optical and structural) without impairing the filler retention. However, paper strength was improved only to a small extent (increase in the tensile index of 8 % for a filler content of ca. 27.5 %). On the other hand, when used at the paper surface, remarkable improvements in the gamut area of >25 % in comparison to the base paper and of >40 % in comparison to starch-only coated papers were achieved for a formulation having 50 % BNC and 50 % of carboxymethylcellulose. Overall, the present results highlight the possibility of using BNC as a paper component, particularly when applied at the paper substrate as a coating agent aiming at improving printing quality., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Dialdehyde cellulose nanofibrils (CNF) and nanocrystals (CNC) were prepared via periodate oxidation (CNF/CNC-ox) and subsequently functionalized with hexamethylenediamine (HMDA) via a Schiff-base reaction, resulting in partially crosslinked micro-sized (0.5-10 μm) particles (CNF/CNC-ox-HMDA) with an aggregation and sedimentation tendency in an aqueous media, as assessed by Dynamic Light Scattering and Scanning Electron Microscopy. The antibacterial efficacy, aquatic in vivo (to Daphnia magna) and human in vitro (to A594 lung cells) toxicities, and degradation profiles in composting soil of all forms of CNF/CNC were assessed to define their safety profile. CNF/CNC-ox-HMDA exhibited higher antibacterial activity than CNF/CNC-ox and higher against Gram-positive S. aureus than Gram-negative E. coli, yielding a bacteria reduction of >90 % after 24 h of exposure at the minimum (≤2 mg/mL), but potentially moderately/aquatic and low/human toxic concentrations (≥50 mg/L). The presence of anionic, un/protonated amino-hydrophobized groups in addition to unconjugated aldehydes of hydrodynamically smaller (<1 μm) CNC-ox-HMDA increased the reduction of both bacteria to log 9 at ≥4 mg/mL and their bactericidal activity. While only CNF/CNC-ox can be considered as biosafe and up to >80 % biodegradable within 24 weeks, this process was inhibited for the CNF/CNC-ox-HMDA. This indicated their different stability, application and disposal after use (composting vs. recycling)., Competing Interests: Declaration of competing interest The authors declare that they have no conflicts of interest to reveal., (Copyright © 2023 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Having competitive compressive strength and resilience as well as biocompatibility simultaneously still remains a challenge for composite hydrogels, which is critical if they are aimed for use as functional biomaterials. In the present work, a facile and green method was designed for producing a composite hydrogel based on polyvinyl alcohol (PVA) and xylan with sodium tri-metaphosphate (STMP) as cross-linker, aiming to specially enhance its compressive properties with the aid of eco-friendly produced formic acid esterified cellulose nanofibrils (CNFs). The CNF addition caused a compressive strength decrease of the hydrogels, although the values (2.34-4.57 MPa at a compressive strain of 70 %) were still at a high level among the reported PVA (or polysaccharide) based hydrogels so far. However, the compressive resilience of the hydrogels was enhanced significantly by the CNF addition, with maximal compressive strength retention of 88.49 % and 99.67 % in height recovery after 1000 compression cycles at a strain of 30 %, which reflects the significant influence of CNFs on the compressive recovery ability of the hydrogel. All materials used in the present work are naturally non-toxic with good biocompatible, which makes the synthesized hydrogels with great potential in biomedical applications, e.g., soft-tissue engineering., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

Hydrogels with prominent flexibility, versatility, and high sensitivity play an important role in the design and fabrication of wearable sensors. In particular, these flexible conductive hydrogels exhibit elastic modulus that is highly compatible with human skin, demonstrating the great potential for flexible sensing. However, the preparation of high-performance hydrogel-based sensors that can restrain extreme cold conditions is still challenging. Herein, a novel anti-freezing composite hydrogel with superior conductivity based on polyacrylamide (PAM), LiCl, and PEDOT:PSS coated cellulose nanofibrils (PAM/PEDOT:PSS/CNF) is constructed. The addition of CNF increased the hydrogen bonding sites of the molecular chains in the micro, thus improving the mechanical strength and the conductivity of the hydrogel in the macro. The hydrogels achieve a high tensile strength of 0.19 MPa, compressive strength of 0.92 MPa, and dissipation energy of 41.9 kJ/m 3 . Otherwise, LiCl increases the interactions between the colloidal phase and water molecules, endowing the hydrogels with excellent freezing tolerance. Specifically, the optimized hydrogel of 45 % LiCl exhibited stable mechanical properties at -40 °C. Finally, the composite hydrogel was used to assemble flexible sensors with high sensitivity of 10.3 MPa -1 , which can detect a wide range of human movements and physiological activities., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023. Published by Elsevier Ltd.)

Functional metal oxide particles are often added to the polymers to prepare flexible functional polymer composites with adequate mechanical properties. ZnO and cellulose nanofibrils (CNF) outstand among these metal oxides and the polymer matrices respectively due to their various advantages. Herein, we in situ prepare ZnO microrods in the presence of CNF, which resultes in a layered composite structure. The ZnO microrods are sandwiched between the CNF layers and strongly bind to highly charged CNF, which provides a better stress transfer during mechanical activity. Digital image correction (DIC) and finite element analysis-based computational homogenization methods are used to investigate the relationship between mechanical properties and composite structure, and the stress transfer to the ZnO microrods. Full-field strain measurements in DIC reveal that the in situ ZnO microrods preparation leads to their homogenous distribution in the CNF matrix unlike other methods, which require external means such as ultrasonication. The computational homogenization technique provides a fairly good insight into the stress transfer between constituents in microstructure as well as a good prediction of macroscopic mechanical properties, which otherwise, would be challenging to be assessed by any ordinary mechanical testing in the layered composites. Finally, we also demonstrate that these composites could be used as physiological motion sensors for human health monitoring., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Nanoscale infrared (IR) spectroscopy and microscopy, enabling the acquisition of IR spectra and images with a lateral resolution of 20 nm, is employed to chemically characterize individual cellulose nanocrystals (CNCs) and cellulose nanofibrils (CNFs) to elucidate if the CNCs and CNFs consist of alternating crystalline and amorphous domains along the CNF/CNC. The high lateral resolution enables studies of the nanoscale morphology at different domains of the CNFs/CNCs: flat segments, kinks, twisted areas, and end points. The types of nanocellulose investigated are CNFs from tunicate, CNCs from cotton, and anionic and cationic wood-derived CNFs. All nano-FTIR spectra acquired from the different samples and different domains of the individual nanocellulose particles resemble a spectrum of crystalline cellulose, suggesting that the non-crystalline cellulose signal observed in macroscopic measurements of nanocellulose most likely originate from cellulose chains present at the surface of the nanocellulose particles., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Adrian Cernescu is employed at Attocube Systems AG that manufactures nano-FTIR spectroscopy instruments., (Copyright © 2022. Published by Elsevier Ltd.)

An effective method based on Fe 2+ assisted cold plasma (CP) to pretreat pineapple peel cellulose for the preparation of cellulose nanofibrils (CNF) was proposed in this study. The mechanism underlying Fe 2+ assisted CP pretreatment based on the structural changes of cellulose was investigated. Results showed that the cellulose preabsorbed Fe 2+ , followed by 60 min of CP treatment, and then was nanofibrillated into CNF via ultrasonication. Fe 2+ assisted CP treatment exhibited strong capacity to significantly decrease the degree of polymerization of cellulose and to enhance electrostatic repulsion of fibrils. Furthermore, the roughness and breakage were observed on the surface of pretreated cellulose. The content of inter-molecular hydrogen bonds and average crystallite size (D hkl ) also decreased significantly. The current results provided useful fundamental insights into Fe 2+ assisted CP and cellulose interaction, which should be beneficial to developing new pretreatment methods for disintegrating cellulose into CNF., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Cellulose nanofibrils (CNFs) have gained much attention as part of biocompatible soft hydrogels used in various biomedical applications such as biodegradable scaffolds, biomedicine, tissues, and regenerative medicine. The CNF hydrogels were mediated with metal cations for improved mechanical strength and structural reversibility. Intermolecular interactions in these CNF hydrogels are controlled by metal cation-carboxylate coordination bonding, leading to the creation of interconnected three-dimensional nanofibril structures that produce high structural reversibility. The nonlinear inter- and intra-cycle were investigated viscoelastic responses of these CNF hydrogels by quantitative nonlinear viscoelastic parameters and transient responses. The dynamic and transitional analyses conducted indicate that the structural deformation and recovery characteristics of the CNF hydrogels are affected by the valency number of the metal cations. This property can be carefully chosen to tune the intermolecular interactions between the cellulose nanofibrils to create an efficient interwoven network structure with high structural reversibility that can go through repeated cycles of reformation and yielding., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Improving the redispersion and recycling of dried cellulose nanofibrils (CNFs) without compromising their nanoscopic dimensions and inherent mechanical properties are essential for their large-scale applications. Herein, mixed-linkage (1,3;1,4)-β-d-glucan (MLG) was studied as a rehydration medium for the redispersion and recycling of dried CNFs, benefiting from the intrinsic affinity of MLG to both cellulose and water molecules as inspired from plant cell wall. MLG from barley with a lower molar ratio of cellotriosyl to cellotetraosyl units was found homogeneously coated on CNFs, facilitating rehydration of the network of individualized CNFs. The addition of barley MLG did not impair the mechanical properties of the CNF/MLG composites as compared to neat CNFs nanopaper. With the addition of 10 wt% barley MLG, dry CNF/MLG composite film was successfully redispersed in water and recycled with well-maintained mechanical properties, while lichenan from Icelandic moss, cationic starch, and xyloglucan could not help the redispersion of dried CNFs., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022. Published by Elsevier Ltd.)

TEMPO-oxidized cellulose nanofibril (CNF) hydrogels or cellulose nanocrystal (CNC) hydrogels can now be obtained at high concentrations (>10 wt%) and used to fabricate biobased materials and structures. Thus, it is required to control and model their rheology in process-induced multiaxial flow conditions using 3D tensorial models. For that purpose, it is necessary to investigate their elongational rheology. Thus, concentrated TEMPO-oxidized CNF and CNC hydrogels were subjected to monotonic and cyclic lubricated compression tests. These tests revealed for the first time that the complex compression rheology of these two electrostatically stabilised hydrogels combines viscoelasticity and viscoplasticity. The effect of their nanofibre content and aspect ratio on their compression response was clearly emphasised and discussed. The ability of a non-linear elasto-viscoplastic model to reproduce the experiments was assessed. Even if some discrepancies were observed at low or high strain rates, the model was consistent with the experiments., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

In this study, a series of pretreatment methods (pectin extraction) were employed to prepare cellulose nanofibrils (CNFs) with different pectin composition and contents from ramie fibers. The comprehensive effects of residual pectin on the final properties of CNFs were investigated. The residual pectin did not have a significant effect on the size distribution of the obtained CNFs. While the presence of pectin led to higher zeta potential value, improved dispersion stability and enhanced storage modulus of the CNF dispersion, with the sodium carbonate extraction method showing the greatest impact. The possible mechanism for enhanced dispersion stability of CNFs is the formation of self-assembled hierarchical pectin-hemicellulose/lignin-cellulose nanostructures, offering abundant electrostatic repulsion and steric hindrance between the nanoparticles. This work provides guidelines for the tailored production of CNFs to meet the requirements for different applications., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

The structure and dynamics of networks formed by rod-shaped particles can be indirectly investigated by measuring the diffusion of spherical tracer particles. This method was used to characterize cellulose nanofibril (CNF) networks in both dispersed and arrested states, the results of which were compared with coarse-grained Brownian dynamics simulations. At a CNF concentration of 0.2 wt% a transition was observed where, below this concentration tracer diffusion is governed by the increasing macroscopic viscosity of the dispersion. Above 0.2 wt%, the diffusion of small particles (20-40 nm) remains viscosity controlled, while particles (100-500 nm) become trapped in the CNF network. Sedimentation of silica microparticles (1-5 μm) in CNF dispersions was also determined, showing that sedimentation of larger particles is significantly affected by the presence of CNF. At concentrations of 0.2 wt%, the sedimentation velocity of 5 μm particles was reduced by 99 % compared to pure water., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022. Published by Elsevier Ltd.)

Processing cellulose nanofibril (CNF) hydrogels with a high concentration is a solution to reduce logistics costs and drying energy and to produce CNF-based materials with good dimensional stability. However, the rheology of concentrated and highly concentrated CNF hydrogels is poorly understood due to the difficulties to characterise them using standard shear rheometers. In this study, enzymatic CNF hydrogels in the concentrated and highly concentrated regimes (3-13.6 wt%) were subjected to lubricated compression at various strain rates. At low strains, compression curves exhibited a linear regime. At higher strains and low strain rates, a heterogeneous and marked hardening of stress levels was observed and accompanied with a two-phase flow with significant fluid segregation and network consolidation. At high strain rates, a homogeneous and incompressible one-phase plateau-like regime progressively established. In this regime, a yield stress was measured and compared with literature data, showing a good agreement with them., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Generally, the thermal conductivity (TC) of composite based on cellulose nanofibrils (CNF) is improved by adding thermal conductive filler, which inevitably leads to the loss of its mechanical properties. In this work, it is the first to simultaneously improve the toughness and TC of CNF/boron nitride nanosheets (BNNS) composite from the perspective of thermal conductive filler addition and CNF crystal change. The hydrophilic-modified BNNSs were successfully prepared by xylose-assisted ball-milling prior to adding into CNF. Compared with that of CNF film (1.34 W/(m·K)), the in-plane TC of CNF/BNNS composite (12.68 W/(m·K)) increased significantly by 846 % with loading 30 % BNNS. Afterwards, both toughness (8.0 MJ·m -3 , increased ~250 %) and TC (14.7 W/(m·K), increased ~16 %) of CNF/BNNS composite were further enhanced significantly by mercerization with 12.5 % NaOH solution. The simultaneously improvement of toughness and TC is unprecedented in related studies, which contributes to the effective preparation of thermal management materials., Competing Interests: Declaration of competing interest The authors declare no competing interest., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Nanocellulose (NC), including cellulose nanocrystals (CNCs), cellulose nanofibrils (CNFs), and bacterial cellulose (BC), has attracted a great deal of attention as a green packaging material. NC can protect food from pathogen adhesion and can be degraded by microorganisms after being discarded. In this review, we introduce preparations of NC-based film, including layer by layer (LbL) assembly, electrospinning, coating, extrusion, casting, vacuum filtration, and immersion. We summarize the interaction between microorganisms and NC, and focused on the impact of NC on microbial adhesion to surfaces and the influence of microorganisms on degradation of NC-based film. We put forward the challenges of NC faces in packaging, such as hydrophobicity, antibacterial properties, and industrialization. We finally propose future perspectives of NC-based film as the packaging material., (Copyright © 2022. Published by Elsevier Ltd.)

Post-fibrillation endoglucanase treatment was employed to reduce the entanglement of cellulose nanofibrils (CNFs) produced with low extent of mechanical milling. The results showed that post-fibrillation endoglucanase treatment can effectively reduce the fibril degree of polymerization (DP) values and therefore entanglement. Cellulose DP was reduced from 520 for CNFs prepared by milling using a SuperMassColloider with 1 pass to 225 after endoglucanase treatment at a low dosage of 1 mg protein/g fibril for 24 h. Endoglucanase treatment can also effectively reduce the fibril mean diameter from 66 nm to 25 nm. Applying post-fibrillation endoglucanase treatment produced more uniform CNFs than the feed CNFs from pure mechanical treatment. All CNFs suspensions prepared by post-fibrillation endoglucanase treatment were non-Newtonian (except at very low concentrations below 0.5 wt%) with shear thinning behavior. Post-fibrillation endoglucanase treatment reduced the viscosity of CNF suspensions due to decreasing fibril DP values and the extent of entanglement., (Copyright © 2022. Published by Elsevier Ltd.)

Uncontrolled hemorrhage poses a severe life-threatening situation. However, traditional hemostats still have various limitations. It is urgent to develop a material with excellent biocompatibility and hemostatic ability. Evidence has shown that carboxymethyl chitosan (CMCS) has hemostatic properties and good compatibility. Herein, we develop an expandable hemostatic sponge by modifying CMCS with cellulose nanofibrils (CNFs) through the CO-NH cross-linking method. We verified its potential as a hemostatic agent both in vivo and in vitro. The results demonstrated that the prepared carboxymethyl chitosan/cellulose nanofiber composite (CNF-CMCS) sponges could absorb blood, quickly expand to exert pressure in the wound, and exhibit an excellent coagulation ability. The CNF-CMCS sponges significantly decreased the bleeding time and blood loss in several hemorrhage models and possessed a significant advantage in treating the deep penetrating injury hemorrhage. Therefore, the sponges provide a unique application prospect and potential as a penetrating trauma hemostatic agent., (Copyright © 2022. Published by Elsevier Ltd.)

TEMPO-oxidized cellulose nanofibrils (CNFs) possess lots of attractive properties. However, recycling of TEMPO is desirable because of ecological and economic demands. In this study, a novel strategy integrating direct reuse and extraction recovery of TEMPO was developed. 50 % of filtrates after TEMPO oxidation were directly reused and half of the fresh TEMPO was added to maintain a constant dosage, the obtained CNFs within 2 cycles shared similar carboxylate contents, crystallinity, and homogeneous width compared to the original ones. Furthermore, TEMPO in another 50 % of filtrates was extracted by ethyl acetate followed by distillation. The CNFs produced using the extracted TEMPO had almost the same properties compared to those of original ones, suggesting a negligible loss of activity of the recovered catalyst. Compared to the traditional route, the combined strategy exhibited a 31.3 % reduction in production costs, which enables clean and cost-effective production of CNFs and shows a promising industrial feasibility., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Phase change materials (PCM) have been increasingly used over the past decades in applications requiring thermal energy storage or maintaining temperature uniformity, in particular in the textile industry. Organic PCM is desired in temperature control, but it suffers from thermal leaking and unstable form during phase transition. Here, cellulose nanofibrils (CNFs) were used as emulsifiers to stabilize paraffin Pickering emulsion by ultrasonication. Results indicated uniform PCM emulsion particles of 4.2 ± 2.1 μm could be obtained using 0.8 wt% CNF suspension sonicated at 100%A and 7 mins with 2:8 paraffin to CNF ratio. The CNF-stabilized paraffin emulsion showed excellent long-term stability with unchanged particle size when stored at 45 °C for 28 days. In addition, differential scanning calorimetry (DSC) results showed high thermal stability after 51 heating-cooling cycles with high latent heat of 117.6 J/g. The CNF-stabilized paraffin emulsion can be facilely spray-coated onto fabric to prepare thermal regulating textile., (Copyright © 2022. Published by Elsevier Ltd.)

Lignin-containing cellulose nanofibrils (LCNFs) with tunable lignin contents from sugarcane bagasse were directly prepared by low-temperature soda‑oxygen pulping combined with simple mechanical treatment. The residual lignin structure, morphology and physical dimensions of LCNFs, and properties of the relevant cellulose nanopapers (CNPs) were investigated. In situ 2D Heteronuclear Single Quantum Coherence (HSQC) NMR spectra showed β-O-4 linkages, ferulate, and para-coumarate were well preserved in the LCNFs. Compared with the cellulose nanofibrils (CNFs), LCNFs displayed a more uniform size and narrow diameter distribution. The corresponding CNPs exhibited outstanding mechanical properties (tensile strength reached 152.9 MPa), and excellent combined optical properties both in the UV blocking and visible light transparency. Moreover, the water contact angles (50.0-80.2°) of LCNFs were much higher than that of CNFs (21.7°). Direct preparation of LCNFs under mild condition would unlock the full potential of cellulosic materials and provide enhanced opportunities for cellulose to fabricate multi-functional and high-value materials., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Mineral fillers hinder cellulosic fiber bonding and thus limit the increase of filler content in paper. Herein, precipitated calcium carbonate (PCC)/cellulose nanofibrils (CNF) composites were fabricated by a facile and efficient strategy, i.e., co-refining process (CRP). During this process, CNF and PCC were activated by mechanochemical effect and formed encapsulation structure by calcium ion coordination and hydrogen bonding. The encapsulation structure and H-bond/ionic coordination interactions not only endowed the composite with excellent size stability but also enhanced interfacial interaction between composite fillers and cellulosic fibers. Compare with the paper filled with only PCC, PCC + CNF mixture, the tensile index of the cellulosic paper containing PCC/CNF composite was increased by 44.48% and 12.14%, respectively. These results not only provide a facile and scalable approach to increase interaction between cellulosic fiber and mineral filler but also create more possibilities for special paper-based materials with requiring high content of inorganic materials., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Alginate has been used for decades for cell encapsulation. Cellulose nanofibrils (CNF) from tunicates are desirable in biomedicine due to high molecular weight, purity, crystallinity, and sustainable production. We prepared microbeads of 400-600 μm of alginate and tunicate CNF. Greater size, dispersity and aspect ratio were observed in microbeads with higher fractions of CNF. CNF content in Ca-crosslinked alginate microbeads decreased stability upon saline exposure, whereas crosslinking with calcium (50 mM) and barium (1 mM) yielded stable microbeads. The Young's moduli of gel cylinders decreased when exchanging alginate with CNF, and slightly increased permeability to dextran was observed in microbeads containing CNF. Encapsulation of MC3T3 cells revealed high cell viability after encapsulation (83.6 ± 0.4%) in beads of alginate and CNF. NHDFs showed lower viability but optimizing mixing and production techniques of microbeads increased cell viability (from 66.2 ± 5.3% to 72.7 ± 7.5%)., (Copyright © 2022 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Environmental pollution is increasingly becoming a serious global challenge due to various pollutants. Cellulose nanomaterials (CNMs) based membranes originated from green resources and sustainable processes are expected to have great potential in environmental applications due to their nanoscale dimension, high surface area, biodegradability, and biocompatibility as well as renewable capability. To fully unlock this potential, fundamental understandings of the interplay between various tunable parameters of CNMs and the substances to be separated, are required for the rational design and fabrication of CNMs based membranes. This review highlights the recent advances in CNMs membranes for environmental remediation in achieving clean air, water, and green energy. Key parameters that dominate the performances of CNMs membranes are critically assessed. The interactions of CNMs with pollutants, molecules, and ions are analyzed and their selective transport mechanisms in different membrane separation processes are discussed. The challenges and future directions for CNMs membranes are also outlined., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Creating a low-cost, highly efficient, and recyclable superabsorbent for spilled-oil cleanup is of great significance but remains a big challenge. Herein, we report a facile strategy to produce economic, environmentally friendly, and reusable foam from agricultural waste kapok fibers. These kapok-derived cellulose nanofibrils foams (KNFs) demonstrate a hierarchically porous structure at micro-level with ultra-low density (2.7 mg·cm -3 ). The superhydrophobic KNFs (150.5°) show outstanding oil absorption (126.8-320.4 g·g -1 ) and oil-water separation performance. Notably, a facile approach is designed to reuse KNFs easily by a homemade oil release system. The release behavior of the KNFs is quantitatively analyzed and confirmed by the Rigter-Peppas model, indicating that the oil release followed the Fickian diffusion. The KNFs exhibit desirable reusability, and can be recycled for at least 50 times while keeping excellent oil absorption, and release performance. These advantages prove that the KNF is a desirable substitute for spilled-oil treatment., (Copyright © 2021. Published by Elsevier Ltd.)

This study was designed to improve the stability of medium internal phase emulsion by adjusting the electrostatic interaction between gelatin (GLT) and TEMPO-oxidized bacterial cellulose nanofibrils (TOBC). The influences of polysaccharide-protein ratio (1:10, 1:5, and 1:2.5) and pH (3.0, 4.7, 7.0, and 11.0) on the emulsion properties were investigated. The droplet size of TOBC/GLT-stabilized emulsion was increased with the TOBC proportion increasing at pH 3.0-11.0. Additionally, emulsion had a larger droplet size at pH 4.7 (the electrical equivalence point pH of mixtures). However, the addition of TOBC significantly improved the emulsion stability. The emulsions prepared with TOBC/GLT mixtures (mixing ratio of 1:2.5) at pH 3.0-7.0 were stable without creaming during the storage. It was because the formation of nanofibrils network impeded the droplet mobility, and the emulsion viscosity and viscoelastic modulus were increased with the addition of TOBC. These findings were meaningful to modulate the physical properties of emulsions., (Copyright © 2021. Published by Elsevier Ltd.)

Cellulose nanofibril (CNF) paper has various applications due to its unique advantages. Herein, we present the intrinsic mechanical properties of CNF papers, along with the preparation and properties of nanoparticle-reinforced CNF composite papers. The literature on CNF papers reveals a strong correlation between the intrafibrillar network structure and the resulting mechanical properties. This correlation is found to hold for all primary factors affecting mechanical properties, indicating that the performance of CNF materials depends directly on and can be tailored by controlling the intrafibrillar network of the system. The parameters that influence the mechanical properties of CNF papers were critically reviewed. Moreover, the effect on the mechanical properties by adding nanofillers to CNF papers to produce multifunctional composite products was discussed. We concluded this article with future perspectives and possible developments in CNFs and their bionanocomposite papers., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

In this study, we fabricate physically dual-crosslinked cellulose-based hydrogels by varying coordination bonding effects with the addition of either divalent or trivalent metal cations. The first crosslinked network is created by metal-carboxylate coordination bonds between the cellulose nanofibrils that have abundant carboxyl groups and the metal cations. The second crosslinked network is formed by the reaction of tetra-functional borate ion complex and the hydroxyl groups in polyvinyl alcohol. These physically dual-crosslinked networks are strongly interwoven by non-sacrificial hydrogen bonds, this dual-crosslinked network leads to enhanced recovery characteristics in the resulting hydrogels. We use three interval thixotropic testing to investigate the deformation and recovery behaviors of the hydrogels and plot their structural deformation parameters in phase diagrams to understand the underlying complexity of energy dissipation and viscoelastic dynamics of the dual-crosslinked hydrogels., (Copyright © 2021 Elsevier Ltd. All rights reserved.)