Cellulose nanofiber (CNF) has been widely used as a flexible and lightweight polymer matrix for electromagnetic shielding and thermally conductive composite films because of its excellent mechanical strength, environmental performance, and low cost. However, the lack of flame retardancy seriously hinders its further application. Herein, renewable and biomass-sourced l-arginine (AR) was used to surface-modify ammonium polyphosphate (APP) and an environmentally friendly biobased flame retardant was synthesized by the coordination of zinc sulfate heptahydrate (ZnSO4·7H2O), which was named AAZ. AAZ was deposited on the surface of CNF by electrostatic adsorption and Zn2+ complexation. The biobased compatibilizer Triton X-100 was employed to assist the exfoliation of graphene nanoplatelets (GNPs) and their dispersion in the CNF matrix. Due to the formation of a dense lamellar layer resembling a shell structure, the CNF/GNPs composite films with a tensile strength of 52 MPa were obtained via vacuum-assisted filtration. Because the phosphorus-containing group produces a protective layer of PxOy compound and promotes the formation of a carbon layer by CNF and the combustion releases ammonia gas, the fire-resistant performance of the composite films was greatly improved. Compared with the pure CNF film, the composite film exhibits 33% reduction in PHRR value and 40% reduction in THR. In addition, the CNF/GNPs composite film with 20 wt % GNPs possessed high conductivity (2079.2 S/m) and electromagnetic interference (EMI) shielding effectiveness (37 dB). The ultrathin CNF/GNPs composite films have excellent potential for use as efficient flame retardant and EMI shielding materials.

Jiuzao is the main solid by-products of Baijiu industry, which contain a high amount of underutilized cellulose and proteins. In recent years, cellulose nanofibers mixed with proteins to prepare biodegradable bio-based film materials have received widespread attention. In this study, we propose a novel method to simultaneously extract kafirin and cellulose from strong-flavor type of Jiuzao, and modify cellulose to prepare cellulose nanofibers by the TEMPO (2,2,6,6-tetramethylpiperidine-1-oxide) oxidation-pressure homogenization technique, and finally mix kafirin with cellulose nanofibers to prepare a new biodegradable bio-based composite film. Based on the analysis of one-way and response surface experiments, the highest purity of cellulose was 82.04 %. During cellulose oxidation, when NaClO was added at 25 mmol/g, cellulose nanofibers have a particle size of 80-120 nm, a crystallinity of 65.8°. Finally, kafirin and cellulose nanofibers were mixed to prepare films. The results showed that when cellulose nanofibers were added at 1 %, the film surface was smooth, the light transmittance was 60.8 %, and the tensile strength was 9.17 MPa at maximum, which was 104 % higher than pure protein film. The contact angle was 34.3°. This paper provides new ideas and theoretical basis for preparing biodegradable bio-based composite film materials, and improves the added value of Jiuzao.

Flexible hybrid hydrogels (GO/AC/CNFn) with a 3D porous network structure and superhydrophilic property are synthesized by cross-linking and self-assembling graphene oxide (GO) and activated carbon (AC) with cellulose nanofiber (CNF) during microwave hydrothermal process. In this ternary composite hydrogel, CNF molecular chains bridge GO sheets to build the 3D skeleton and anchor AC particles within GO nanosheets, forming ordered architecture of GO/AC/CNFn hydrogel that simultaneously possesses high flexibility and excellent mechanical integrity. When using this hydrogel as additive-free electrode, the presence of AC provides developed porous structure and density to promote high volumetric capacitance, while the heteroatom nitrogen groups tune the surface property of the composite with increased electrical conductivity. Benefited from the optimized structure, GO/AC/CNF1 electrode delivers an ultra-high mass specific capacitance of 627 F/g and volume specific capacitance of 618 F/cm3 at 0.5 A/g in three-electrode system in 1 M H2SO4 electrolyte, which is kinetically demonstrated to be essentially originated from the capacitive contributions. The energy density reaches 32.2 Wh/kg at a power density of 150 W/kg for the fabricated flexible solid-state symmetric supercapacitor. Moreover, the obtained flexible device could sensitively response at varied physiological signals, shedding fresh lights on their potential applications in signal sensors and portable electronics.

The effects of carboxylation degree (0.3-2.4 mmol/g) of cellulose nanofiber (CNF) on the microstructure and mechanical properties of edible walnut oleogels were comprehensively examined. The oleogels were well prepared by emulsion-templated approach for potential substitute of conventional saturated or trans-fats in food products. The results demonstrated that the oil-binding capacity (OBC) and textural strength of oleogels enhanced with the increase of CNF carboxyl content, while the structural strength (G\' in rheological measurement) and the resistance to shear thinning was first decreased and then increased. It possibly reflected the competition on the dominant structuring mechanism by hydrogen bonding from cellulose hydroxyl groups and electrostatic interactions from -COONa function. With the combined mechanism, oleogel with low structural strength and relatively high OBC (CNF carboxyl content of 1.2 mmol/g, OBC >83 %, G\' ≈ 7 × 104 Pa and firmness of 0.30 N) and oleogel with enough structural rigidity and high OBC (CNF carboxyl content of 1.8 mmol/g, OBC >89 %, G\' of up to 1.7 × 105 Pa, and firmness of up to 0.66 N) were both fabricated. This reveals the feasibility of regulating oleogel structure and textual properties by using CNF as the unique oleogelator and simply changing its surface carboxyl function.

We developed a highly sensitive solid-state sensor for mercury detection by stabilizing red-sub-nanometric fluorescent gold nanoclusters (AuNC, 0.9 ± 0.1 nm diameter) with bovine serum albumin in a matrix composed of cellulose nanofibrils (CNF) (BSA-AuNC/CNF). The main morphological and optical features of the system were investigated via atomic force/transmission electron microscopy and UV-Vis/fluorescence spectroscopy. The hybrid film (off-white and highly transparent) showed strong photoluminescene under UV irradiation. The latter is assigned to the AuNC, which also increase the ductility of the emitting film, which was demonstrated for high sensitivity Hg2+ detection. When used as a sensor system, following AuNC printing on CNF hybrid films, a limit of detection <10 nM was confirmed. What is more, nanocellulose films have a high pore structure and selective separation properties, showcasing a wide range of potential applications in many fields such as water treatment and oil-water separation.

Extreme environmental conditions often lead to irreversible structural failure and functional degradation in hydrogels, limiting their service life and applicability. Achieving high toughness, self-healing, and ionic conductivity in cryogenic environments is vital to broaden their applications. Herein, we present a novel approach to simultaneously enhance the toughness, self-healing, and ionic conductivity of hydrogels, via inducing non-freezable water within the zwitterionic cellulose-based hydrogel skeleton. This approach enables resulting hydrogel to achieve an exceptional toughness of 10.8 MJ m-3, rapid self-healing capability (98.9 % in 30 min), and high ionic conductivity (2.9 S m-1), even when subjected to -40 °C, superior to the state-of-the-art hydrogels. Mechanism analyses reveal that a significant amount of non-freezable water with robust electrostatic interactions is formed within zwitterionic cellulose nanofibers-modified polyurethane molecular networks, imparting superior freezing tolerance and versatility to the hydrogel. Importantly, this strategy harnesses the non-freezable water molecular state of the zwitterionic cellulose nanofibers network, eliminating the need for additional antifreeze and organic solvents. Furthermore, the dynamic Zn coordination within these supramolecular molecule chains enhances interfacial interactions, thereby promoting rapid subzero self-healing and exceptional mechanical strength. Demonstrating its potential, this hydrogel can be used in smart laminated materials, such as aircraft windshields.

In order to achieve an aerogel with both rigid pore structures and desired flexibility, stiff carboxyl-functionalized cellulose nanofiber (CNFs) were introduced into a flexible polyvinyl alcohol-polyethyleneimine (PVA-PEI) crosslinking network, with 4-formylphenylboronic acid (4FPBA) bridging within the PVA-PEI network to enable dynamic boroxine and imine bond formation. The strong covalent bonds and hydrogen connections between CNF and the crosslinking network enhanced the wet stability of the aerogel while also contributed to its thermal stability. Importantly, the harmonious coordination between the stiff CNF and the flexible polymer chains not only facilitated aerogel flexibility but also enhanced its increased specific surface area by improving pore structure. Moreover, the inclusion of CNF enhanced the adsorption capacity of the aerogel, rendering it effective for removing heavy metal ions. The specific surface area and adsorption capacity for copper ions of the aerogel increased significantly with a 3 wt% addition CNF suspension, reaching 19.74 m2 g-1 and 60.28 mg g-1, respectively. These values represent a remarkable increase of 590.21 % and 213.96 %, respectively, compared to the blank aerogel. The CNF-enhanced aerogel in this study, characterized by its well-defined pore structures, and desired flexibility, demonstrates versatile applicability across multiple domains, including environmental protection, thermal insulation, electrode fabrication, and beyond.

In this work, effects of cellulose nanofiber/dihydromyricetin (CNF/DMY) ratio on the structural, antioxidant and emulsifying properties of the CNF/DMY mixtures were investigated. CNF integrated with DMY via hydrogen bonding and the antioxidant capacity of mixtures increased with decreasing CNF/DMY ratio (k). The oxidative stability of emulsions enhanced as the DMY content increased. Emulsions formed at Φ = 0.5 displayed larger size (about 25 μm), better viscoelasticity and centrifugal stability than those at Φ = 0.3 (about 23 μm). The emulsions at k = 17:3 and Φ = 0.5 exhibited the most excellent viscoelasticity. In conclusion, the DMY content in mixtures and the oil phase fraction exhibited distinct synergistic effects on the formation and characteristics of emulsions, and the emulsions could demonstrate superior oxidative and storage stability. These findings could provide a novel strategy to extend the shelf life of cellulose-based emulsions and related products.

In order to obtain a flexible aerogel substrate for conductive materials used in the electrode, polydopamine-anchored cellulose nanofiber (PDA@CNF) was introduced into a polyethylene imine-poly(vinyl alcohol) (PEI-PVA) cross-linking network which used 4-formylphenylboronic acid (4FPBA) as bridge. The incorporation of rigid CNF as a structural scaffold effectively improved the pore architecture of the aerogel, potentially providing substantial advantages for the infiltration and deposition of conductive materials. Additionally, the outstanding stability and flexibility exhibited by the aerogel in aqueous solutions suggest its significant potential for applications in flexible electrodes. Furthermore, electrochemical experiments showed that the rapid pathway formed between PDA and PEI could enhance the charge-transfer rate within the aerogel substrate. It is anticipated that such an enhancement would significantly benefit the electrochemical attributes of the electrode. Inspired by mussels, our introduced PDA-anchored rigid CNF into flexible polymer networks to fabricate aerogel substrates for electrode materials. This study would contribute to the development and utilization of flexible electrodes while reducing carbon footprint in energy production and conversion processes.

Cellulose nanofiber (CNF) holds great promise in applications such as surface-enhanced Raman scattering (SERS), catalysis, esthesia, and detection. This study aimed to build novel CNF-based SERS substrates through a facile synthetic method. Citrate-reduced gold nanoparticles (AuNPs) were adsorbed on the cationized CNF surface due to electrostatic interactions, and uniform AuNPs@(2,3-epoxypropyl trimethylammonium chloride)EPTMAC@CNF flexible SERS substrates were prepared by a simple vacuum-assisted filtration method. The probe molecule methylene blue was chosen to assess the performance of the CNF-based SERS substrate with a sensitivity up to 10-9 M, superior signal reproducibility (relative standard deviation (RSD) = 4.67%), and storage stability (more than 30 days). Tensile strength tests indicated that the CNF-based films had good mechanical properties. In addition, CNF-based substrates can easily capture and visually identify microplastics in water. These results demonstrate the potential application of the flexible, self-assembled AuNPs@EPTMAC@CNF flexible SERS substrate for prompt and sensitive detection of trace substances.