Confined Chemical Transitions for Direct Extraction of Conductive Cellulose Nanofibers with Graphitized Carbon Shell at Low Temperature and Pressure.

Cellulose is the most abundant renewable natural polymer on earth, but it does not conduct electricity, which limits its application expansion. The existing methods of making cellulose conductive are combined with another conductive material or high-temperature/high-pressure carbonization of the cellulose itself, while in the traditional method of sulfuric acid hydrolysis to extract nanocellulose, it is usually believed that a too high temperature will destroy cellulose and lead to experimental failure. Now, based on a new research perspective, by controlling the continuous reaction process and isolating oxygen, we directly extracted intrinsically conductive cellulose nanofiber (CNF) from biomass, where the confined range molecular chains of CNF were converted to highly graphitized carbon at only 90 °C and atmospheric pressure, while large-scale twisted graphene films can be synthesized bottom-up from CNFene suspensions, called CNFene (cellulose nanofiber-graphene). The conductivity of the best CNFene can be as high as 1.099 S/cm, and the generality of this synthetic route has been verified from multiple biomass cellulose sources. By comparing the conventional high-pressure hydrothermal and high-temperature pyrolysis methods, this study avoided the dangerous high-pressure environment and saved 86.16% in energy. These findings break through the conventional notion that nanocellulose cannot conduct electricity by itself and are expected to extend the application potential of pure nanocellulose to energy storage, catalysis, and sensing.

"Green" electrostatic droplet-assisted forming cellulose microspheres with excellent structural controllability and stability for efficient Cr(VI) removal.

This study presents a novel and environmentally friendly method for producing cellulose microspheres (CM) with controllable morphology and size using electrostatic droplets. The traditional droplet method for CM production requires complex equipment and harmful reagents. In contrast, the proposed method offers a simple electrostatic droplet approach to fabricate CM10 at 10 kV, which exhibited a smaller volume, linear microscopic morphology, and a larger specific surface area, with a 36.60 % improvement compared to CM0 (prepared at 0 kV). CM10 also demonstrated excellent underwater structural stability, recovering in just 0.5 s, and exhibited the highest adsorption capacity for Cr(VI) at 190.16 mg/g, a 72.15 % improvement over CM0. This enhanced adsorption capacity can be attributed to the unique structure of CM10 and the introduction of more amino groups. Moreover, CM10 displayed good cyclic adsorption capacity and high dynamic adsorption efficiency, making it highly suitable for practical applications. CM10 exhibited remarkable adsorption capacity, stability, and practical value in treating Cr(VI) wastewater. This work proposes a simple and eco-friendly method for producing CM with excellent structural controllability and stability, providing an effective route for wastewater treatment.

In situ growth of curcumin-loaded cellulose composite film for real-time monitoring of food freshness in smart packaging.

Visual pH-responsive packaging material is particularly important in food supply chain safety monitoring due to their non-destructive monitoring method and intuitive result. However, it has always been limited by the instability performance of pH-response components and carriers, which further hinders its wide food safety application. To address these challenges, we selected cellulose with remarkable biocompatibility and mechanical properties as the carrier, and high pH-responsive curcumin to develop a smart packaging material (RC/GC composite film) with real-time food safety monitoring. Compared with pure cellulose film, the RC/GC composite film exhibited excellent mechanical properties (4-fold enhancement) and thermal stability (100 °C increasing). Meanwhile, based on the first reported strategy of curcumin in-situ growth during cellulose film formation, the RC/GC composite film exhibited exceptional antioxidant activity (89.2 %), antimicrobial property (91.6 %), and significant pH-responsive sensitivity (within 15 s). This innovative approach offers a new strategy for easy-to-use and effective monitoring of food spoilage in packaging materials.

Highly efficient dissolution and reinforcement mechanism of robust and transparent cellulose films for smart packaging.

The packaging of fresh foods increasingly focuses on renewable and eco-friendly cellulose films, but their low dissolution efficiency and weak mechanical strength greatly limit their wide application, which also cannot be used for smart packaging. Here, a highly efficient synergistic chloride-salt dissolution method was proposed to fabricate robust, transparent, and smart cellulose films. Cellulose films with appropriate Ca2+ concentration exhibited robust mechanical strength, better thermal stability, high transparency and crystallinity. The metal chelation of Ca2+ with cellulose chains could induce cellulose chain arrangement during the cellulose regeneration process. Particularly, compared to pure cellulose films, the tensile strength and elongation at break of cellulose films with suitable Ca2+ were increased by 167 % and 200 %, respectively. Moreover, optimal cellulose films can be used to reflect the quality of the fruit by detecting changes in ethanol gas. Hence, a novel strategy is presented to fabricate robust and transparent cellulose films with great potential application for smart packaging.

Deep insights into biodegradability mechanism and growth cycle adaptability of polylactic acid/hyperbranched cellulose nanocrystal composite mulch.

The widespread use of petroleum-based plastic mulch in agriculture has accelerated white and microplastic pollution while posing a severe agroecological challenge due to its difficulty in decomposing in the natural environment. However, endowing mulch film with degradability and growth cycle adaptation remains elusive due to the inherent non-degradability of petroleum-based plastics severely hindering its applications. This work reports polylactic acids hyperbranched composite mulch (PCP) and measured biodegradation behavior under burial soil, seawater, and ultraviolet (UV) aging to understand the biodegradation kinetics and to increase their sustainability in the agriculture field. Due to high interfacial interactions between polymer and nanofiler, the resultant PCP mulch significantly enhances crystallization ability, hydrophilicity, and mechanical properties. PCP mulch can be scalable-manufactured to exhibit modulated degradation performance under varying degradation conditions and periods while concurrently enhancing crop growth (wheat). Thus, such mulch with excellent performance can reduce labor costs and the environmental impact of waste mulch disposal to replace traditional mulch for sustainable agricultural production.

Multiple noncovalent interactions tailored crystallization and performance reinforcement mechanisms of Biopolyester Composites with functional Cellulose Nanocrystals.

The slow crystallization and weak mechanical features of poly (butylene adipate-co-terephthalate) (PBAT) have become a severe industrial problem in food packaging. Inspired by principle of bionic structure, functional cellulose nanocrystals (CNC) modified with hexamethylene diisocyanate (HMDI) and toluene diisocyanate (TDI) can enhance the crystallization ability and mechanical properties of PBAT nanocomposites. Significantly, CNC-T (CNC modified by TDI) showed a stronger reinforced effect on PBAT properties than unmodified CNCs and CNC-H (CNC modified by HMDI) nanofillers due to hydrogen bonds, π-π interaction between PBAT matrix and CNC-T nanofillers with benzene ring structure. Thus, compared with pure PBAT, PBAT/5CNC-T composites displayed an enhancement of 34.5 % on the tensile strength and exhibited the most robust nucleation ability on PBAT crystallization than CNC and CNC-H. Meanwhile, the possible nucleation, crystallization, and performance reinforcement mechanisms of PBAT nanocomposites have been presented, which is very beneficial for designing robust PBAT nanocomposites with functional cellulose nanocrystals for potential green packaging.

Facile synthesis, release mechanism, and life cycle assessment of amine-modified lignin for bifunctional slow-release fertilizer.

Biomass-based slow-release fertilizers (SRFs) are a sustainable solution for addressing food scarcity, improving fertilizer efficiency, and reducing pollution, whereas they still face complex preparation, high costs, and low release characteristics. This study introduces a simple and innovative approach to producing bifunctional green SRFs with controlled release and conditioning properties for saline soils and harsh environments. The method involves a one-pot preparation of microsphere-structured amine-modified lignin slow-release fertilizer (L-UX) using biomass lignin as the starting material. The L-UX demonstrates an exceptional fertilizer loading rate (66.2 %) and extended slow-release performance (288 h), effectively enhancing the fertilizer's release ability. Compared to traditional fertilizers, the bifunctional L-UX significantly improves soil water retention capacity (824.3 %), plant growth, and germination percentage in challenging soil conditions (133 %). These findings highlight the potential of L-UX as a large-scale controlled-release fertilizer in harsh environments. A life cycle assessment (LCA) was also conducted to evaluate the environmental impact of L-UX from its production to disposal. This revealed that L-UX has a minimal environmental footprint compared to conventional inorganic fertilizers. This study further supports the widespread application of L-UX as an environmentally friendly alternative.

Highly sensitive and structure stable polyvinyl alcohol hydrogel sensor with tailored free water fraction and multiple networks by reinforcement of conductive nanocellulose.

The wearable composite hydrogel sensors with high stretchability have attracted much attention in recent years, while the traditional hydrogels have weak molecular (chain) interaction and contain a lot of free water, leading to poor mechanical properties, unstable environmental tolerance and sensing ability. Herein, a novel ice crystal extrusion-crosslinking strategy is used to obtain polyvinyl alcohol (PVA) hydrogel with conductive nanocellulose-poly (3,4-ethylenedioxythiophene) (CNC-PEDOT) as skeleton network, sodium alginate (SA) and Ca2+ as tough segment of multi-bonding network. This strategy synergistically enhanced the interaction of hydrogen bonds and calcium (Ca2+) ion chelation within the hydrogel, building highly sensitive and stable multiple tough-elastic networks. Therefore, the optimal hydrogel sensor (PVA/SA-CP45) shows good structural stability, robust mechanical performance, excellent compress (Sensitivity = 68.7), stretching sensitivity (Gauge factor = 4.16), ultra-wide application range (-105-60 °C), fast response/relaxation time and outstanding dynamic durability with 6000 stretching-releasing cycles. Especially, it can give good sensing performance for omnidirectional monitoring of human motion and weak signals. Moreover, it was also designed into multifunctional sensing systems for gait guidance of model training and real-time monitoring ammonia gas for food preservation and public environmental safety, demonstrating great potential in flexible sensors devices for health monitoring.

Two-response surface design optimization of carboxylated CNCs with super high thermal stability and dye removal capability.

Discharging wastewater from industrial dyeing and printing processes poses a significant environmental threat, necessitating green and efficient adsorbents. Cellulose nanocrystals (CNCs) have emerged as a promising option for dye adsorbing. However, the industrial production and commercialization of CNCs still faced low yield, time-consuming, and uneco-friendly. In this study, we proposed a facile hydrochloric/maleic acid (HCl/C4H4O4) hydrolysis method to synthesize carboxylated CNCs using Box-Behnken design and dual response surface design, which can systematically investigate the effect of experimental factors (temperature, time and HCl/C4H4O volume ratio) on the final products. The rod-liked carboxylated CNCs gave the highest yield of 90.50 %, maximum carboxyl content of 1.29 mmol/g, and efficient dye removal ratio of 91.5 %. Furthermore, compared to CNCs obtained by commonly sulfuric acid hydrolysis way (CNCs-S) with a Tmax of 242.6 °C, the CNCs extracted at 5 h exhibited significantly improved thermal stability with Tmax reaching 351.2 °C. The enriched carboxyl content and excellent thermal stability show potential wastewater treatment applications under harsh conditions.

Efficient cellulose dissolution and derivatization enabled by oxalic/sulfuric acid for high-performance cellulose films as food packaging.

The performance of cellulose-based materials is highly dependent on the choice of solvent systems. Exceptionally, cellulose dissolution and derivatization by efficient solvent have been considered as a key factor for large-scale industrial applications of cellulose. However, cellulose dissolution and derivatization often requires harsh reaction conditions, high energy consumption, and complex solubilizing, resulting in environmental impacts and low practical value. Here we address these limitations by using a low-temperature oxalic acid/sulfuric acid solvent to enable cellulose dissolution and derivatization for high-performance cellulose films. The dissolution and derivatization mechanism of the mixed acid is studied, demonstrating that cellulose is firstly socked by oxalic acid, then more hydrogen bonds ionized by sulfuric acid break cellulose chain, and finally the esterification reaction between oxalic acid and cellulose is catalyzed by sulfuric acid. Solutions containing 8 %-10 % cellulose are obtained and can be stored for a long time at -18 °C without significant degradation. Moreover, the cellulose film exhibits a higher tensile strength of up to 66.1 MPa, thermal stability, and degree of polymerization compared to that fabricated by sulfuric acid. These unique advantages provide new paths to utilize renewable resources for alternative food packaging materials at an industrial scale.

Stiff gel-protected fiber-shaped supercapacitors based on CNFA/silk composite fiber with superhigh interference-resistant ability as self-powered temperature sensor.

The development of self-powered sensors with interference-resistant detection is a priority area of research for the next generation of wearable electronic devices. Nevertheless, the presence of multiple stimuli in the actual environment will result in crosstalk with the sensor, thereby hindering the ability to obtain an accurate response to a singular stimulus. Here, we present a self-powered sensor composed of silk-based conductive composite fibers (CNFA@ESF), which is capable of energy storage and sensing. The fabricated CNFA@ESF exhibits excellent mechanical performance, as well as flexibility that can withstand various deformations. The CNFA@ESF provides a good areal capacitance (44.44 mF cm-2), high-rate capability, and excellent cycle stability (91 % for 5000 cycles). In addition, CNFA@ESF also shows good sensing performance for multiple signals including strain, temperature, and humidity. It was observed that the assembly of the symmetrical device with a stiff hydrogel surface layer for protection enabled the real-time, interference-free monitoring of temperature signals. Also, the CNFA@ESF can be woven into fabrics and integrated with a solar cell to form a self-powered sensor system, which has been proven to convert and store solar energy to power electronic watches, indicating its huge potential for future wearable electronics.

Multiple covalent modification enables nylon fiber biosensor with robust scrub-resistant and signal-capture ability for multiscenario health monitoring and security warning.

Nylon fibers have great potentials in smart textiles due to their excellent wear resistance, resilience, and chemical stability, whereas poor combination between nylon fibers and conductive materials causes discontinuous signal capture. In this work, nylon fibers/di-aldehyde cellulose nanocrystals/polypyrrole (NFACP) biosensors with robust scrub-resistant and signal-capture ability were fabricated by interfacial multiple covalent reactions. The best NFACP0.2 biosensor exhibited high conductivity (354 S/m), robust mechanical strength and stretching-releasing dynamic durability. Especially, its textile sensors still possessed high sensitivity and excellent sensing performance after repeated washing and friction. Moreover, NFACP0.2 biosensor can be designed into various multifunctional health monitoring and security warning systems for "stress reducing exercise" enthusiasts, high-altitude activities, and deep-sea exploration, demonstating great potentials of conductive nylon fiber biosensor in flexible electronics.

Investigating interface adhesion of PLA-coated cellulose paper straws: Degradation, plant growth effects, and life cycle assessment.

Although bioplastics and paper straws have been introduced as alternatives to single-use plastic straws, their potential environmental, economic, and social impacts have not been analyzed. This study addresses this gap by designing a polylactic acid layer interface adhesion on cellulose paper-based (PLA-P) composite straws by a dip molding process. This process is simple, efficient, and scalable for massive production. Optimizing key manufacturing parameters, including ice bath ultrasonic, overlapping paper strips (2 strips), winding angle (60°), soaking time (5 min), and drying temperature (50 °C), were systematically evaluated to improve straw quality and manufacturing efficiency. PLA chains were found to deposit onto the cellulose network through intermolecular interactions to form a consistent "sandwich" structure, which can improve adhesion, water resistance, and mechanical properties. Interestingly, PLA-P straws effectively decomposed in soil and compost environments, with a 35-40 % degradation rate within 4 months. Besides, PLA-P straw residues affected seed germination and plant growth, but no significant toxic effects were detected. Further, microplastics were observed in soil and plant tissues (roots, stems, and leaves), and their possible diffusion mechanisms were explored. The results of a comprehensive life cycle assessment (LCA) and cost analysis showed that the process improvements reduced the ecological footprint of PLA-P straws and showed good prospects for commercial application. The study's findings contribute to the understanding of bioplastics and paper straws in effectively reducing environmental impact and fostering sustainable development.

Tailoring Hydronium ion Driven Dissociation-Chemical Cross-Linking for Superfast One-Pot Cellulose Dissolution and Derivatization to Build Robust Cellulose Films.

Concepts of sustainability must be developed to overcome the increasing environmental hazards caused by fossil resources. Cellulose derivatives with excellent properties are promising biobased alternatives for petroleum-derived materials. However, a one-pot route to achieve cellulose dissolution and derivatization is very challenging, requiring harsh conditions, high energy consumption, and complex solubilizing. Herein, we design a one-pot tailoring hydronium ion driven dissociation-chemical cross-linking strategy to achieve superfast cellulose dissolution and derivatization for orderly robust cellulose films. In this strategy, there is a powerful driving force from organic acid with a pKa below 3.75 to dissociate H+ and trigger the dissolution and derivatization of cellulose under the addition of H2SO4. Nevertheless, the driving force can only trigger a partial swelling of cellulose but without dissolution when the pKa of organic acid is above 4.26 for the dissociation of H+ is inhibited by the addition of inorganic acid. The cellulose film has high transmittance (up to ∼90%), excellent tensile strength (∼122 MPa), and is superior to commercial PE film. Moreover, the tensile strength is increased by 400% compared to cellulose film prepared by the ZnCl2 solvent. This work provides an efficient solvent, which is of great significance for emerging cellulose materials from renewable materials.

Next-generation self-adhesive dressings: Highly stretchable, antibacterial, and UV-shielding properties enabled by tannic acid-coated cellulose nanocrystals.

Hydrogels with excellent high-water uptake and flexibility have great potential for wound dressing. However, pure hydrogels without fiber skeleton faced poor water retention, weak fatigue resistance, and mechanical strength to hinder the development of the dressing as next-generation functional dressings. We prepared an ultrafast gelation (6 s) Fe3+/TA-CNC hydrogel (CTFG hydrogel) based on a self-catalytic system and bilayer self-assembled composites. The CTFG hydrogel has excellent flexibility (800% of strain), fatigue resistance (support 60% compression cycles), antibacterial, and self-adhesive properties (no residue or allergy after peeling off the skin). CTFG@S bilayer composites were formed after electrospun silk fibroin (SF) membranes were prepared and adhesive with CTFG hydrogels. The CTFG@S bilayer composites had significant UV-shielding (99.95%), tensile strain (210.9 KPa), and sensitive humidity-sensing properties. Moreover, the integrated structure improved the mechanical properties of electrospun SF membranes. This study would provide a promising strategy for rapidly preparing multifunctional hydrogels for wound dressing.

Robust and versatile superhydrophobic cellulose-based composite film with superior UV shielding and heat-barrier performances for sustainable packaging.

Replacing single-use plastic delivery bags (SPDBs) with cellulose-based materials is an effective strategy to reduce environmental pollution. However, the inherent hydrophilicity and ultralow mechanical strength of cellulose materials limit its development. In this study, zinc oxide (ZnO)-cellulose composite films were successfully prepared through "two-step strategy" of lotus leaves structure simulation, including deposition of micro-nano ZnO particles and stearic acid (STA) modification. Well-dispersed micro-nano ZnO particles with stick-like structure were anchored in the ZnO-cellulose composite film prepared at 90 °C (CF-90). Due to the special structural design and strong interaction between the cellulose and micro-nano ZnO particles, the CF-90 showed higher mechanical property (a 47.8 % improvement in the tensile strength). Impressively, CF-90 also exhibited great UV shielding properties with larger UPF value of 1603.98 and superhigh heat-barrier performance. Moreover, CF-90 obtained excellent superhydrophobicity with a water contact angle of 163.6° by further modification. Consequently, the versatile cellulose-based material bringing a dawn on application of sustainable packaging materials for express delivery industry.

One-pot strategy to fabricate conductive cellulose nanocrystal-polyethylenedioxythiophene nanocomposite: Synthesis mechanism, modulated morphologies and sensor assembly.

Simple preparation, good conductivity, and excellent hydrophilicity are in urgent demand due to fast growth of wearable intelligent devices. Cellulose nanocrystal-polyethylenedioxythiophene (CNC-PEDOT) nanocomposites with modulated morphology were prepared through Iron (III) p-toluenesulfonate hydrolysis of commercialized microcrystalline cellulose (MCC) and in situ polymerization of 3,4-ethylenedioxythiophene monomers (EDOT) through one-pot green synthesis, where preparation and modification of CNC were obtained for uses as templates to anchor PEDOT nanoparticles. The resultant CNC-PEDOT nanocomposite gave well-dispersed PEDOT nanoparticles with sheet-like structure on the CNC surface, possessing higher conductivity and improved hydrophilicity or dispersibility. Subsequently, a wearable non-woven fabrics (NWF) sensor was successfully assembled by dipping the conductive CNC-PEDOT, and showed excellent sensing response for multiple signals (subtle deformation from various human activities and temperature). This study provides a feasible and large-scale production of CNC-PEDOT nanocomposites and their applications in wearable flexible sensors and electronic devices.

Homogeneous wet-spinning construction of skin-core structured PANI/cellulose conductive fibers for gas sensing and e-textile applications.

Fiber-based wearable electronic textiles have broad applications, but non-degradable substrates may contribute to electronic waste. The application of cellulose-based composite fibers as e-textiles is hindered by the lack of fast and effective preparation methods. Here, we fabricated polyaniline (PANI)/cellulose fibers (PC) with a unique skin-core structure through a wet-spinning homogeneous blended system. The conductive network formation was enabled at a mere 1 wt% PANI. Notably, PC15 (15 wt% PANI) shows higher electrical conductivity of 21.50 mS cm-1. Further, PC15 exhibits excellent ammonia sensing performance with a sensitivity of 2.49 %/ppm and a low limit of detection (LOD) of 0.6 ppm. Cellulose-based composite fibers in this work demonstrate good gas sensing and anti-static properties as potential devices for smart e-textiles.

All-naturally structured tough, ultrathin, and washable dual-use composite for fruits preservation with high biosafety evaluation.

This work develops a sustainable and global strategy to enhance fruit preservation efficacy. The dual-use composite coating or film comprises silk fibroin/cellulose nanocrystals (SF/CNC) with superior ductility through a synergistic plasticizing effect of glycerol and natural aloe-emodin powder (AE) as antimicrobial agents. To confirm our strategy, two common fruit preservation materials (edible surface coating-SCA-CS; packaging film-SCA-PF) and five different fruits (strawberries, bananas, apples, blueberries, and guavas) have been used. Moreover, SCA-CS coating with antibacterial and antioxidant activities formed an ultrathin layer on the fruit's surfaces with a thickness of 7.7 µm and could be easily washable. Therefore, bananas and strawberries' shelf-life with SCA-CS coating can be extended for 9 days and 6 days, respectively. The discharge water of SCA-CS has excellent biosafety in an indoor environment with no threat to plant health (microgreens bean sprouts germination as a case study). The plant exhibited positive results within 15 days, and leaves maintained their green color with a germination rate of 97.6 %. The toughness of SCA-PF film increased by 14,685.7 % with a water vapor transmission rate (WPTR) of 17 g mm m-2 day-1, which confirms that the concept of SCA-PF film and SCA-CS coating are feasible to be used for fruit preservation/packaging.

Thermo-sensitive composite microspheres incorporating cellulose nanocrystals for regulated drug release kinetics.

Thermo-sensitive composite microspheres (TPCP) were developed to achieve the on-demand release of drugs. The TPCP microspheres were synthesized using Oil-in-Water (O/W) emulsion evaporation technique and then impregnated with thermo-sensitive polyethylene glycol (PEG). The addition of cellulose nanocrystals (CNCs) significantly enhance thermal stability, crystallization ability, and surface hydrophilicity of TPCP microspheres due to heterogeneous nucleation effect and hydrogen bonding interaction, resulting in stable microsphere structure. The thermal degradation temperature (Tmax) increased by 13.8 °C, and the crystallinity improved by 20.9 % for 10 % TPCP. The thermo-sensitive composite microspheres showed the regulated cumulative release according to in vitro human physiological temperature changes. Besides, four release kinetics and possible release mechanism of TPCP microspheres were provided. Such thermo-responsive composite microspheres with control microsphere sizes and high encapsulation rate may have the potential to the development of on-demand and advanced controlled-release delivery systems.