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Food safety is vital to human health, necessitating the development of nondestructive, convenient, and highly sensitive methods for detecting harmful substances. This study integrates cellulose dissolution, aligned regeneration, in situ nanoparticle synthesis, and structural reconstitution to create flexible, transparent, customizable, and nanowrinkled cellulose/Ag nanoparticle membranes (NWCM-Ag). These three-dimensional nanowrinkled structures considerably improve the spatial-electromagnetic-coupling effect of metal nanoparticles on the membrane surface, providing a 2.3 × 108 enhancement factor for the surface-enhanced Raman scattering (SERS) effect for trace detection of pesticides in foods. Notably, the distribution of pesticides in the apple peel and pulp layers is visualized through Raman imaging, confirming that the pesticides penetrate the peel layer into the pulp layer (â¼30 µm depth). Thus, the risk of pesticide ingestion from fruits cannot be avoided by simple washing other than peeling. This study provides a new idea for designing nanowrinkled structures and broadening cellulose utilization in food safety.
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Celulosa , Inocuidad de los Alimentos , Nanopartículas del Metal , Plaguicidas , Espectrometría Raman , Celulosa/química , Plaguicidas/análisis , Plaguicidas/química , Nanopartículas del Metal/química , Espectrometría Raman/métodos , Plata/química , Malus/química , Humanos , Frutas/química , Nanotecnología/métodos , Propiedades de Superficie , Contaminación de Alimentos/análisisRESUMEN
Micro(nano)plastics (MNPs) have become a significant environmental concern due to their widespread presence in the biosphere and potential harm to ecosystems and human health. Here, we propose for the first time a MNPs capture, utilization, and storage (PCUS) concept to achieve MNPs remediation from water while meeting economically productive upcycling and environmentally sustainable plastic waste management. A highly efficient capturing material derived from surface-modified woody biomass waste (M-Basswood) is developed to remove a broad spectrum of multidimensional and compositional MNPs from water. The M-Basswood delivered a high and stable capture efficiency of >99.1% at different pH or salinity levels. This exceptional capture performance is driven by multiscale interactions between M-Basswood and MNPs, involving physical trapping, strong electrostatic attractions, and triggered MNPs cluster-like aggregation sedimentation. Additionally, the in vivo biodistribution of MNPs shows low ingestion and accumulation of MNPs in the mice organs. After MNPs remediation from water, the M-Basswood, together with captured MNPs, is further processed into a high-performance composite board product where MNPs serve as the glue for utilization and storage. Furthermore, the life cycle assessment (LCA) and techno-economic analysis (TEA) results demonstrate the environmental friendliness and economic viability of our proposed full-chain PCUS strategy, promising to drive positive change in plastic pollution and foster a circular economy.
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The property of being stubborn and degradation resistant makes nanoplastic (NP) pollution a long-standing remaining challenge. Here, we apply a designed top-down strategy to leverage the natural hierarchical structure of waste crayfish shells with exposed functional groups for efficient NP capture. The crayfish shell-based organic skeleton with improved flexibility, strength (14.37 to 60.13 MPa), and toughness (24.61 to 278.98 MJ m-3) was prepared by purposefully removing the inorganic components of crayfish shells through a simple two-step acid-alkali treatment. Due to the activated functional groups (e.g., -NH2, -CONH-, and -OH) and ordered architectures with macropores and nanofibers, this porous crayfish shell exhibited effective removal capability of NPs (72.92 mg g-1) by physical interception and hydrogen bond/electrostatic interactions. Moreover, the sustainability and stability of this porous crayfish shell were demonstrated by the maintained high-capture performance after five cycles. Finally, we provided a postprocessing approach that could convert both porous crayfish shell and NPs into a tough flat sheet. Thus, our feasible top-down engineering strategy combined with promising posttreatment is a powerful contender for a recycling approach with broad application scenarios and clear economic advantages for simultaneously addressing both waste biomass and NP pollutants.
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Exoesqueleto , Astacoidea , Animales , Adsorción , Porosidad , Exoesqueleto/química , Microplásticos/química , Tamaño de la Partícula , Propiedades de SuperficieRESUMEN
Self-powered skin attachable and detachable electronics are under intense development to enable the internet of everything and everyone in new and useful ways. Existing on-demand separation strategies rely on complicated pretreatments and physical properties of the adherends, achieving detachable-on-demand in a facile, rapid, and universal way remains challenging. To overcome this challenge, an ingenious cellulose nanofiber-mediated manifold dynamic synergy strategy is developed to construct a supramolecular hydrogel with both reversible tough adhesion and easy photodetachment. The cellulose nanofiber-reinforced network and the coordination between Fe ions and polymer chains endow the dynamic reconfiguration of supramolecular networks and the adhesion behavior of the hydrogel. This strategy enables the simple and rapid fabrication of strong yet reversible hydrogels with tunable toughness ((Valuemax-Valuemin)/Valuemax of up to 86%), on-demand adhesion energy ((Valuemax-Valuemin)/Valuemax of up to 93%), and stable conductivity up to 12 mS cm-1. We further extend this strategy to fabricate different cellulose nanofiber/Fe3+-based hydrogels from various biomacromolecules and petroleum polymers, and shed light on exploration of fundamental dynamic supramolecular network reconfiguration. Simultaneously, we prepare an adhesive-detachable triboelectric nanogenerator as a human-machine interface for a self-powered wireless monitoring system based on this strategy, which can acquire the real-time, self-powered monitoring, and wireless whole-body movement signal, opening up possibilities for diversifying potential applications in electronic skins and intelligent devices.
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Rechargeable batteries, typically represented by lithium-ion batteries, have taken a huge leap in energy density over the last two decades. However, they still face material/chemical challenges in ensuring safety and long service life at temperatures beyond the optimum range, primarily due to the chemical/electrochemical instabilities of conventional liquid electrolytes against aggressive electrode reactions and temperature variation. In this regard, a gel polymer electrolyte (GPE) with its liquid components immobilized and stabilized by a solid matrix, capable of retaining almost all the advantageous natures of the liquid electrolytes and circumventing the interfacial issues that exist in the all-solid-state electrolytes, is of great significance to realize rechargeable batteries with extended working temperature range. We begin this review with the main challenges faced in the development of GPEs, based on extensive literature research and our practical experience. Then, a significant section is dedicated to the requirements and design principles of GPEs for wide-temperature applications, with special attention paid to the feasibility, cost, and environmental impact. Next, the research progress of GPEs is thoroughly reviewed according to the strategies applied. In the end, we outline some prospects of GPEs related to innovations in material sciences, advanced characterizations, artificial intelligence, and environmental impact analysis, hoping to spark new research activities that ultimately bring us a step closer to realizing wide-temperature rechargeable batteries.
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Inert inorganic nano-building blocks, such as carbon nanotubes (CNTs) and boron nitride (BN) nanosheets, possess excellent physicochemical properties. However, it remains challenging to build aerogels with these inert nanomaterials unless they are chemically modified or compounded with petrochemical polymers, which affects their intrinsic properties and is usually not environmentally friendly. Here, a universal biomacromolecule-enabled assembly strategy is proposed to construct aerogels with 90 wt% ultrahigh inorganic loading. The super-high inorganic content is beneficial for exploiting the inherent properties of inert nanomaterials in multifunctional applications. Taking chitosan-CNTs aerogel as a proof-of-concept demonstration, it delivers sensitive pressure response as a pressure sensor, an ultrahigh sunlight absorption (94.5%) raising temperature under light (from 25 to 71 °C within 1 min) for clean-up of crude oil spills, and superior electromagnetic interference shielding performance of up to 68.9 dB. This strategy paves the way for the multifunctional application of inert nanomaterials by constructing aerogels with ultrahigh inorganic loading.
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Millions of patients annually suffer life-threatening illnesses caused by bacterial infections of skin wounds. However, the treatment of wounds infected with bacteria is a thorny issue in clinical medicine, especially with drug-resistant bacteria infections. Therefore, there is an increasing interest in developing wound dressings that can efficiently fight against drug-resistant bacterial infections and promote wound healing. In this work, an anti-drug-resistant bacterial chitosan/cellulose nanofiber/tannic acid (CS/CNF/TA) hydrogel with excellent wound management ability was developed by electrospinning and fiber breakage-recombination. The hydrogel exhibited an outstanding antibacterial property exceeding 99.9 %, even for drug-resistant bacteria. This hydrogel could adhere to the tissue surface due to its abundant catechol groups, which avoided the shedding of hydrogel during the movement. Besides, it exhibited extraordinary hemostatic ability during the bleeding phase of the wound and then regulated the wound microenvironment by absorbing water and moisturizing. Moreover, the CS/CNF/TA also promoted the regrowth of vessels and follicles, accelerating the healing of infected wound tissue, with a healing rate exceeding 95 % within a 14-day timeframe. Therefore, the CS/CNF/TA hydrogel opens a new approach for the healing of drug-resistant bacterial infected wounds.
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Infecciones Bacterianas , Quitosano , Hemostáticos , Nanofibras , Polifenoles , Humanos , Hemostáticos/farmacología , Taninos , Celulosa/farmacología , Hidrogeles/farmacología , Bacterias , Antibacterianos/farmacologíaRESUMEN
Hepatectomy, a surgical procedure for liver cancer, is often plagued by high recurrence rates worldwide. The recurrence of liver cancer is primarily attributed to microlesions in the liver, changes in the immune microenvironment, and circulating tumor cells in the bloodstream. To address this issue, a novel intervention method that combines intraoperative hemostasis with mild photothermal therapy is proposed, which has the potential to ablate microlesions and improve the immune microenvironment simultaneously. Specifically, the integrated strategy is realized based on the fibrous chitosan/polydopamine sponge (CPDS), which is constructed from shearing-flow-induced oriented hybrid chitosan fibers and subsequent self-assembly of polydopamine. The CPDS demonstrates high elasticity, excellent water absorption, and photothermal conversion performance. The results confirm the efficient hemostatic properties of the fibrous CPDS in various bleeding models. Notably, in subcutaneous and orthotopic postoperative recurrence and metastasis models of hepatocellular carcinoma, the fibrous CPDS significantly inhibits local tumor recurrence and distant metastasis. Moreover, the combination with lenvatinib can substantially enhance the antitumor effect. This comprehensive treatment strategy offers new insights into hepatectomy of liver cancer, representing a promising approach for clinical management.
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Carcinoma Hepatocelular , Quitosano , Indoles , Neoplasias Hepáticas , Polímeros , Humanos , Carcinoma Hepatocelular/cirugía , Neoplasias Hepáticas/cirugía , Quitosano/farmacología , Recurrencia Local de Neoplasia/prevención & control , Hemostasis , Microambiente TumoralRESUMEN
The cellulose industry depends heavily on water owing to the hydrophilic nature of cellulose fibrils and its potential for sustainable and innovative production methods. The emergence of nanocellulose, with its excellent properties, and the incorporation of nanomaterials have garnered significant attention. At the nanoscale level, nanocellulose offers a higher exposure of hydroxyl groups, making it more intimate with water than micro- and macroscale cellulose fibers. Gaining a deeper understanding of the interaction between nanocellulose and water holds the potential to reduce production costs and provide valuable insights into designing functional nanocellulose-based materials. In this review, water molecules interacting with nanocellulose are classified into free water (FW) and bound water (BW), based on their interaction forces with surface hydroxyls and their mobility in different states. In addition, the water-holding capacity of cellulosic materials and various water detection methods are also discussed. The review also examines water-utilization and water-removal methods in the fabrication, dispersion, and transport of nanocellulose, aiming to elucidate the challenges and tradeoffs in these processes while minimizing energy and time costs. Furthermore, the influence of water on nanocellulose properties, including mechanical properties, ion conductivity, and biodegradability, are discussed. Finally, we provide our perspective on the challenges and opportunities in developing nanocellulose and its interplay with water.
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Its excellent renewability and biodegradability make cellulose an attractive resource to prepare fossil-based plastic alternatives. However, cellulose itself exhibits strong intermolecular hydrogen bond (H-bond) interactions, significantly restricting the mobility of cellulose chains, thus leading to poor thermo-processing performance. Here, we reconstructed the intermolecular interactions of cellulose chains via replacing the original H-bonds with dynamic covalent bonds. By this, cellulose can be easily thermo-processed into a cellulosic plastic under mild conditions (70 °C). Through adjusting the chemical structure of dynamic covalent networks, the cellulosic plastic shows tunable mechanical strength (3.0-33.5 MPa) and toughness (43-321 kJ m-2). The cellulosic plastic also exhibits excellent resistance to water, organic solvent, acid solution, alkali solution, and high temperature (>400 °C). Moreover, it owns good chemical and biological degradability and recyclability. This work provides an effective method to develop high-performance cellulosic plastics for fossil-based plastic substitution.
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Near-infrared (NIR) transparent optical filters show great promise in night vision and receiving windows. However, NIR optical filters are generally prepared by laborious, environmentally unfriendly processes that involve metal oxides or petroleum-based polymers. We propose a lignin capturing-fusing approach to manufacturing optical biofilters based on molecular collaboration between lignin and cellulose from waste agricultural biomass. In this process, lignin is captured via self-assembly in a cellulose network; then, the lignin is fused to fill gaps and hold the cellulose fibers tightly. The resulting optical biofilter featured a dense structure and smooth surface with NIR transmittance of ~90%, ultralow haze of close to 0%, strong ultraviolet-visible light blocking (~100% at 400 nm and 57.58% to 98.59% at 550 nm). Further, the optical biofilter has comprehensive stability, including water stability, solvent stability, thermal stability, and environmental stability. Because of its unique properties, the optical biofilter demonstrates potential applications in the NIR region, such as an NIR-transmitting window, NIR night vision, and privacy protection. These applications represent a promising route to produce NIR transparent optical filters starting from lignocellulose biomass waste.
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Ionic conductors (ICs) find widespread applications across different fields, such as smart electronic, ionotronic, sensor, biomedical, and energy harvesting/storage devices, and largely determine the function and performance of these devices. In the pursuit of developing ICs required for better performing and sustainable devices, cellulose appears as an attractive and promising building block due to its high abundance, renewability, striking mechanical strength, and other functional features. In this review, we provide a comprehensive summary regarding ICs fabricated from cellulose and cellulose-derived materials in terms of fundamental structural features of cellulose, the materials design and fabrication techniques for engineering, main properties and characterization, and diverse applications. Next, the potential of cellulose-based ICs to relieve the increasing concern about electronic waste within the frame of circularity and environmental sustainability and the future directions to be explored for advancing this field are discussed. Overall, we hope this review can provide a comprehensive summary and unique perspectives on the design and application of advanced cellulose-based ICs and thereby encourage the utilization of cellulosic materials toward sustainable devices.
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The growing environmental concern over petrochemical-based plastics continuously promotes the exploration of green and sustainable substitute materials. Compared with petrochemical products, cellulose has overwhelming superiority in terms of availability, cost, and biodegradability; however, cellulose's dense hydrogen-bonding network and highly ordered crystalline structure make it hard to be thermoformed. A strategy to realize the partial disassociation of hydrogen bonds in cellulose and the reassembly of cellulose chains via constructing a dynamic covalent network, thereby endowing cellulose with thermal processability as indicated by the observation of a moderate glass transition temperature (Tg = 240 °C), is proposed. Moreover, the cellulosic bioplastic delivers a high tensile strength of 67 MPa, as well as excellent moisture and solvent resistance, good recyclability, and biodegradability in nature. With these advantageous features, the developed cellulosic bioplastic represents a promising alternative to traditional plastics.
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There is an urgent need to develop sustainable, renewable, and environment-friendly adsorbents to rectify heavy metals from water. In the current study, a green hybrid aerogel was prepared by immobilizing yeast on chitin nanofibers in the presence of a chitosan interacting substrate. A cryo-freezing technique was employed to construct a 3D honeycomb architecture comprising the hybrid aerogel with excellent reversible compressibility and abundant water transportation pathways for the accelerated diffusion of Cadmium(II) (Cd(II)) solution. This 3D hybrid aerogel structure offered copious binding sites to accelerate the Cd(II) adsorption. Moreover, the addition of yeast biomass amplified the adsorption capacity and reversible wet compression of hybrid aerogel. The monolayer chemisorption mechanism explored by Langmuir and pseudo-second-order kinetic exhibited a maximum adsorption capacity of 127.5 mg/g. The hybrid aerogel demonstrated higher compatibility for Cd(II) ions as compared to the other coexisted ions in wastewater and manifested a better regeneration potential following four consecutive sorption-desorption cycles. Complexation, electrostatic attraction, ion-exchange and pore entrapment were perhaps major mechanisms involved in the removal of Cd(II) revealed by XPS and FT-IR. This study unveiled a novel avenue for efficient green-synthesized hybrid aerogel that may be sustainably used as an excellent purifying agent for Cd(II) removal from wastewater.
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Nanofibras , Contaminantes Químicos del Agua , Cadmio/metabolismo , Quitina/química , Saccharomyces cerevisiae/metabolismo , Aguas Residuales , Adsorción , Nanofibras/química , Biomasa , Espectroscopía Infrarroja por Transformada de Fourier , Iones/química , Agua , Cinética , Contaminantes Químicos del Agua/análisisRESUMEN
Biosafe antibacterial agents are urgently demanded in treating infection especially chronic infection. However, efficient and controlled release of those agents remains great challenging. Two nature-derived agents, lysozyme (LY) and chitosan (CS), are selected to establish a facile method for long-term bacterial inhibition. We incorporated LY into the nanofibrous mats, then deposited CS and polydopamine (PDA) on the surface by layer-by-layer (LBL) self-assembly. In this vein, LY is gradually released with the degradation of nanofibers, and CS is rapidly disassociated from the nanofibrous mats to synergistically result in a potent inhibition against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli) over a period of 14 days. Besides long-term antibacterial capacity, LBL-structured mats could readily achieve a strong tensile stress of 6.7 MPa with an increase percentage of up to 103%. The enhanced proliferation of L929 cells arrives at 94% with help of CS and PDA on the surface of nanofibers. In this vein, our nanofiber has a variety of advantages including biocompatibility, strong long-term antibacterial effect, and skin adaptability, revealing the significant potential to be used as highly safe biomaterial for wound dressings.
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Quitosano , Nanofibras , Quitosano/farmacología , Muramidasa/farmacología , Staphylococcus aureus , Escherichia coli , Antibacterianos/farmacologíaRESUMEN
Cryogels with extreme mechanical properties such as ultrahigh compressibility, fatigue resistance, and rapid recovery are attractive in biomedical, environmental remediation, and energy storage applications, which, however, are difficult to achieve in man-made materials. Here, inspired by the multiscale macro-/microfiber network structure of spider web, we construct an ultraelastic chitosan cryogel with interconnected hybrid micro-/nanofibers (CMNF cryogels) via freeze-induced physicochemical cross-linking. Chitosan chains are directionally assembled into high-aspect-ratio microfibers and nanofibers under shear-flow induction, which are further assembled into an interconnected three-dimensional (3D) network structure with staggered microfibers and nanofibers. In this multiscale network, nanofibers connecting the microfibers improve the stability, while microfibers improve the elasticity of the CMNF cryogels through long-range interaction. The synergy of the two-scale fibers endows the CMNF cryogel with extraordinary mechanical properties in comparison to those assembled with single-scale fibers, including its ultrahigh ultimate strain (97% strain with 50 cycles), excellent fatigue resistance (3200 compressing-releasing cycles at 60% compression strain), and rapid water-triggered shape recovery (recovering in â¼1 s). Moreover, the fibrous CMNF cryogel shows excellent functionalization capability via the rapid assembly of nanoscale building blocks for flexible electronics and environmental remediation. Our work thereby demonstrates the potential of this bioinspired strategy for designing gel materials with extreme mechanical properties.
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The strong reactivity of water in aqueous electrolytes toward metallic zinc (Zn), especially at aggressive operating conditions, remains the fundamental obstacle to the commercialization of aqueous zinc metal batteries (AZMBs). Here, a water-immiscible ionic liquid diluent 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)amide (EmimFSI) is reported that can substantially suppress the water activity of aqueous electrolyte by serving as a "water pocket", enveloping the highly active H2 O-dominated Zn2+ solvates and protecting them from parasitic reactions. During Zn deposition, the cation Emim+ and anion FSI- function respectively in mitigating the tip effect and regulating the solid electrolyte interphase (SEI), thereby favoring a smooth Zn deposition layer protected by inorganic species-enriched SEI featuring high uniformity and stability. Combined with the boosted chemical/electrochemical stability endowed by the intrinsic merits of ionic liquid, this ionic liquid-incorporated aqueous electrolyte (IL-AE) enables the stable operation of Zn||Zn0.25 V2 O5 ·nH2 O cells even at a challenging temperature of 60 °C (>85% capacity retention over 400 cycles). Finally, as an incidental but practically valuable benefit, the near-zero vapor pressure nature of ionic liquid allows the efficient separation and recovery of high-value components from the spent electrolyte via a mild and green approach, promising the sustainable future of IL-AE in realizing practical AZMBs.
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Heavy reliance on petrochemical-based plastic foams in both industry and society has led to severe plastic pollution (the so-called "white pollution"). In this work, we develop a biodegradable, recyclable, and sustainable cellulose/bentonite (Cel/BT) foam material directly from resource-abundant natural materials (i.e., lignocellulosic biomass and minerals) via ambient drying. The strong resistance to the capillary force-driven structural collapse of the preformed three-dimensional (3D) network during the ambient drying process can be ascribed to the purpose-designed cellulose-bentonite coordination interaction, which provides a practical way for the locally scalable production of foam materials with designed shapes without complex processing and intensive energy consumption. Benefiting from the strong cellulose-bentonite coordination interaction, the Cel/BT foam material demonstrates high mechanical strength and outstanding thermal stability, outperforming commercial plastic polystyrene foam. Furthermore, the Cel/BT foam presents environmental impacts much lower than those of petrochemical-based plastic foams as it can be 100% recycled in a closed-loop recycling process and easily biodegraded in the environment (natural cellulose goes back to the carbon cycle, and bentonite minerals return to the geological cycle). This study demonstrates an energy-efficient ambient drying approach for the local and scalable production of an all-natural cellulose/bentonite foam for sustainable packaging, buildings, and beyond, presenting great potential in response to "white pollution" and resource shortage.
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Bentonita , Celulosa , Celulosa/química , PoliestirenosRESUMEN
Ionic conductive hydrogels prepared from naturally abundant cellulose are ideal candidates for constructing flexible electronics from the perspective of commercialization and environmental sustainability. However, cellulosic hydrogels featuring both high mechanical strength and ionic conductivity remain extremely challenging to achieve because the ionic charge carriers tend to destroy the hydrogen-bonding network among cellulose. Here we propose a supramolecular engineering strategy to boost the mechanical performance and ionic conductivity of cellulosic hydrogels by incorporating bentonite (BT) via the strong cellulose-BT coordination interaction and the ion regulation capability of the nanoconfined cellulose-BT intercalated nanostructure. A strong (compressive strength up to 3.2 MPa), tough (fracture energy up to 0.45 MJ m-3), yet highly ionic conductive and freezing tolerant (high ionic conductivities of 89.9 and 25.8 mS cm-1 at 25 and -20 °C, respectively) all-natural cellulose-BT hydrogel is successfully realized. These findings open up new perspectives for the design of cellulosic hydrogels and beyond.