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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.
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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.
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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.
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Nanopartículas , Petróleo , Celulosa , Plásticos , Suelo/química , Agricultura , Biodegradación AmbientalRESUMEN
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.
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Celulosa , Embalaje de Productos , Embalaje de Medicamentos , Resistencia a la Tracción , Embalaje de AlimentosRESUMEN
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.
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Celulosa , Nanopartículas , Celulosa/química , Cristalización , Poliésteres/química , Resistencia a la Tracción , Nanopartículas/químicaRESUMEN
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.
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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.
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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 â¼90%), excellent tensile strength (â¼122 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.
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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.
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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 (66.2â¯%) and extended slow-release performance (288â¯h), effectively enhancing the fertilizer's release ability. Compared to traditional fertilizers, the bifunctional L-UX significantly improves soil water retention capacity (824.3â¯%), plant growth, and germination percentage in challenging soil conditions (133â¯%). 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. The assessment 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.
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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.
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Celulosa , Fibroínas , Polifenoles , Cementos de Resina , Vendajes , Antibacterianos/farmacología , Hidrogeles , AguaRESUMEN
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.
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Nanocompuestos , Óxido de Zinc , Celulosa/química , Calor , Óxido de Zinc/química , Nanocompuestos/química , Interacciones Hidrofóbicas e Hidrofílicas , Embalaje de AlimentosRESUMEN
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.
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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.
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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.
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Celulosa , Nanopartículas , Humanos , Liberación de Fármacos , Microesferas , CinéticaRESUMEN
Nowadays, non-degradable plastic packaging materials have caused serious environmental pollution, posing a threat to human health and development. Renewable eco-friendly nanocellulose hybrid (NCs-hybrid) composites as an ideal alternative to petroleum-based plastic food packaging have been extensively reported in recent years. NCs-hybrids include metal, metal oxides, organic frameworks (MOFs), plants, and active compounds. However, no review systematically summarizes the preparation, processing, and multi-functional applications of NCs-hybrid composites. In this review, the design and hybridization of various NCs-hybrids, the processing of multi-scale nanocomposites, and their key properties in food packaging applications were systematically explored for the first time. Moreover, the synergistic effects of various NCs-hybrids on several properties of composites, including mechanical, thermal, UV shielding, waterproofing, barrier, antimicrobial, antioxidant, biodegradation and sensing were reviewed in detailed. Then, the problems and advances in research on renewable NCs-hybrid composites are suggested for biodegradable food packaging applications. Finally, a future packaging material is proposed by using NCs-hybrids as nanofillers and endowing them with various properties, which are denoted as "PACKAGE" and characterized by "Property, Application, Cellulose, Keen, Antipollution, Green, Easy."
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Embalaje de Alimentos , Nanocompuestos , Humanos , Antioxidantes , Biodegradación Ambiental , CelulosaRESUMEN
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.
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Antiinfecciosos , Quitosano , Películas Comestibles , Frutas/microbiología , Contención de Riesgos Biológicos , Antibacterianos , Conservación de Alimentos/métodos , Quitosano/química , Embalaje de AlimentosRESUMEN
There is a growing interest in the synthesis of electrically conductive cellulose nanocrystal (CNC) for advanced applications, such as supercapacitor, batteries, sensor, and printed electronics. CNC is recognized as an attractive template for the fabrication of functional nanomaterials. Since CNC possesses many attractive properties, it is a sustainable template to prepare conductive nanomaterials, by either coating it with a conductive material or transforming it into carbon nanorods. This review summarizes the utilization of a sustainable and low-cost CNC to produce conductive nanocomposites via an environmentally friendly process. Electroconductive CNCs with enhanced electrical properties, lower electrical percolation threshold, and better mechanical properties can be produced and are attractive systems for many new applications.
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Nanocompuestos , Nanopartículas , Metabolismo de los Hidratos de Carbono , Celulosa/química , Conductividad Eléctrica , Nanocompuestos/química , Nanopartículas/químicaRESUMEN
Bending multi-walled carbon nanotubes (MWCNTs) into rings and structuring them into aerogels is difficult. In this study, cellulose nanofiber (CNF)-MWCNT composite fibers with chain-ring structures were prepared by covalently interconnecting carboxylated CNF and aminated MWCNT by dehydration condensation, solving the problems of the formation of MWCNT aerogels and their phase separation during the compounding process and providing CNF-based aerogels with electrical conductivity. The covalently interconnected aerogels (CAs) had hierarchical porous structures with mechanical resilience and chain-ring fibers, which drove the CNF and MWCNT to form a continuous homogeneous network resulting in a high compression resistance of 269.02 kPa. The CA-based flexible all-solid-state supercapacitor had a quality specific capacitance of 114.8 F g-1, a capacitance retention rate of 94.78% and a Coulomb efficiency of 100%. The CA-based flexible sensor can sense different pressures with a stable response for 1000 cycles. This first study of pulling and bending MWCNT through CNF is expected to inspire more applications of MWCNTs in the fields of flexible supercapacitors and sensors.
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If a person comes into contact with pathogens on public facilities, there is a threat of contact (skin/wound) infections. More urgently, there are also reports about COVID-19 coronavirus contact infection, which once again reminds that contact infection is a very easily overlooked disease exposure route. Herein, we propose an innovative implantation strategy to fabricate a multi-walled carbon nanotube/polyvinyl alcohol (MWCNT/PVA, MCP) interpenetrating interface to achieve flexibility, anti-damage, and non-contact sensing electronic skin (E-skin). Interestingly, the MCP E-skin had a fascinating non-contact sensing function, which can respond to the finger approaching 0-20 mm through the spatial weak field. This non-contact sensing can be applied urgently to human-machine interactions in public facilities to block pathogen. The scratches of the fruit knife did not damage the MCP E-skin, and can resist chemical corrosion after hydrophobic treatment. In addition, the MCP E-skin was developed to real-time monitor the respiratory and cough for exercise detection and disease diagnosis. Notably, the MCP E-skin has great potential for emergency applications in times of infectious disease pandemics. Electronic Supplementary Material: Supplementary material (fabrication of MCP E-skin, laser confocal tomography, parameter optimization, mechanical property characterization, finite element simulation, sensing mechanism, signal processing) is available in the online version of this article at 10.1007/s12274-021-3831-z.