Cellulose-based electrolytes are promising solid electrolyte candidates for low-cost and eco-friendly batteries owing to their natural characteristics of being renewable and biodegradable. Unfortunately, they have strong reactivity and high crystallinity, leading to critical challenges when used in Li-ion batteries, including poor high-voltage tolerance, slow Li-ion conduction and heterogeneous Li-ion flux. Here, we report a functional grafting modification to regulate Li-ion conduction within cellulose-based solid electrolytes. In-situ sol-gel self-assembly accompanied by amino-siloxane grafting is developed to achieve the homogeneous integration of cellulose-amino-siloxane-ionic liquid composites, forming a compact solid-state electrolyte membrane. Such functional design establishes continuous and uniform Li-ion transport highways through amino coordination while disrupting native crystallinity of cellulose, endowing a rapid Li-ion conductivity (1 & times;10-3 S cm-1) and a high electrochemical oxidation potential (5 V). The obtained electrolyte membrane features a homogenous microstructure with high mechanical elasticity and thermodynamic stability, exhibiting high compatibility with Li metal and enabling excellent electrochemical performance. Consequently, solid-state Li-metal batteries exhibit exceptional cycle-life, whereas LiFePO4 cells run 592 cycles and LiNi0.8Co0.1Mn0.1O2 cells run 403 cycles at 0.5 C rate until the capacity reduces to 80%. Notably, a comprehensive life-cycle assessment verifies its advantages in energy conservation and carbon reduction. It presents a sustainable development of high-performance cellulose-based solid-state electrolytes.

High-quality solid-state electrolytes with excellent ionic conductivity and interface compatibility are essential for high-performance solid-state batteries. However, at present, all-solid-state electrolytes severely suffer from low intrinsic ionic conductivity and high interface impedance, while quasi-solid-state electrolytes face great challenges of structural metastability due to the heterogeneity. Here, we propose a new metal-organic ionogel concept for extending solid-state electrolytes and investigate their electrochemical properties in Li metal batteries. A simple sol-gel method is used for metal-organic ionogel self-assembly, in which ferric nitrate trimer reacts with trimeric acid to form ordered mesoporous metal-organic frameworks, while ionic liquid electrolyte is in-situ confined within mesoporous channels. The resulting metal-organic ionogel exhibits a glassy homogeneous structure with fast room-temperature Li-ion conduction (1.02 & times; 10- 3 S cm- 1), high electrochemical oxidation potential (4.8 V vs Li/Li+), and excellent thermal stability (300 degrees C), accordingly demonstrating great potential for Li batteries, where both LiFePO4//Li and LiNi0.8Co0.1Mn0.1O2//Li cells display high initial capacities (160 and 202 mAh g- 1) and excellent capacity retention (98.6% and 85.4%) after 200 cycles.

Nano-/micro-cellulose has attracted significant attention in advanced materials due to its cellulosic properties as well as the important hallmarks of nano-/micro-materials. However, current approaches for the preparation of them are predominantly limited to “top-down” strategies which yield mostly whisker-/fiber-like morphologies. Therefore, it is imperative to develop cellulose-based nano-/micro-materials with diversified architectures. Here, we report the preparation of cellulose nanosheets composed of cellulose nanofibrous network, using cellulose solution as the precursor, via a “bottom-up” strategy. Due to its excellent water dispersibility and stability, these cellulose nanosheets can be assembled to form cellulose hollow microspheres through an ice-melting-induced lyophilization technique. The property and application of the cellulose microspheres can be further expanded by preparing composite microspheres via co-assembling cellulose nanosheets with functional nanomaterials. This work not only provides a simple, mild, and green approach through a new type of “bottom-up” strategy which may shed light on the design and preparation of nano-/micro-materials, but also offers novel cellulose-based nano-/micro-materials which may find wide applications in various fields due to the distinct architectures.

Plant secondary cell walls constitute the dominant reservoir of renewable biomass, comprising tightly packed cellulose, hemicellulose, and lignin at the nanoscale. Recent advances in solid-state NMR spectroscopy and the availability of small-angle X-ray scattering for biomass characterization have led to an accumulation of experimental data on cell wall organization, yet no explicit structure model has simultaneously satisfied both X-ray and NMR observations. Using wheat straw as a model system, we propose a structural framework consistent with current knowledge of cellulose biosynthesis, X-ray scattering data, and one- and two-dimensional 13C solid-state NMR spectra. In this model, 18-chain elementary fibrils align in parallel and populate the cross-section at random. Arabinose-substituted xylan shows no conformational dependence for cellulose-binding in wheat, and only a minor fraction of 2-fold xylan appears in close proximity to cellulose, unlike in Arabidopsis, where xylan is more tightly attached to the cellulose surface. While NMR data cannot unambiguously resolve the internal arrangement of the 18 glucan chains, X-ray scattering profiles uniquely constrain the fibril size and exclude the possibility of tight bundling in the intact walls. The specific interaction between the matrix polymers and the cellulose elementary fibrils must be reconsidered in light of the small interfibril spaces, which bring the matrix components into spatial proximity with cellulose even in the absence of attractive interactions. These findings provide fundamental molecular-level insight into cellulose fibril architecture and matrix-polymer interactions, resolving longstanding discrepancies between spectroscopic and scattering data and advancing our understanding of biopolymer assembly into structurally and functionally versatile lignocellulosic biomaterials.

A covalent–supramolecular multivalent synergy strategy is proposed to construct cellulose-based high-temperature phosphorescent materials with multi-stimulus responsiveness. Integrated TS-FRET and processability enable advanced photonic applications.

Cellulose dissolution remains a fundamental challenge due to its recalcitrant crystalline structure, governed by interchain hydrogen bonds and dispersion interactions. Hydroxide-based systems are industrially relevant but require energy-intensive subzero temperatures. This study employs molecular dynamics simulations to elucidate the molecular mechanisms underlying the dissolution performance of benzyltrimethylammonium hydroxide (BzMe3NOH) and NaOH. Na+ binds to cellulose primarily through electrostatic interactions, whereas the amphiphilic benzyltrimethylammonium cation (BzMe3N+) engages predominantly via vdW interactions, accumulating along the hydrophobic backbone. Both systems exhibit anion-cellulose interactions with hydroxide ions, forming bifurcated hydrogen bonds that facilitate transient deprotonation of hydroxyl groups. A key thermodynamic advantage of BzMe3N+ is that each cation displaces more water molecules away from cellulose's solvation shell than Na+ does, reducing the entropic penalty of dissolution. This work establishes that effective dissolution in hydroxide systems requires a synergistic combination of anion-driven hydrogen-bonding disruption and cation-driven dispersion compensation.

Hydrogels hold great potential for osmotic energy conversion due to their inherent low resistance, yet their application is limited by weak mechanical properties, low charge density, and unstable pore structures. To address these challenges, we propose a Hofmeister effect-mediated strategy to develop a tough and highly conductive nanofluidic hydrogel from carboxymethyl cellulose and polyvinyl alcohol. The resulting hydrogel exhibits a tensile strength of 17.7 MPa and achieves an osmotic power density of 12.6 W m-2 under a 50-fold salinity gradient, representing a 3402% and 368% increase over conventional hydrogels. This enhancement is attributed to the formation of a nanophase separation structure, where hydrophobic regions serve as physical crosslinks for excellent mechanical strength and swelling resistance, and hydrophilic channels function as "ion highways" for high ionic conductivity. Moreover, the highly charged nanopores induced by the salting-out effect boost ion selectivity. This design overcomes the traditional trade-off between mechanical stability and ion transport. Under a 500-fold salinity gradient, the power density reaches 38.4 W m-2, surpassing most state-of-the-art nanochannel membranes. This strategy demonstrates broad applicability across various hydrogel systems. This work offers a versatile, scalable route to fabricate high-performance nanofluidic hydrogel for efficient and durable osmotic energy conversion.

Polydopamine-functionalized cellulose nanofibers (PDCCNF) were incorporated into polyethersulfone ultrafiltration membranes to elucidate the interfacial regulation mechanism of nanofillers during nonsolvent-induced phase separation. The incorporation of PDCCNF significantly altered the rheological behavior and phase inversion kinetics of the casting solution by enhancing polymer–nanofiller interfacial interactions and facilitating solvent–nonsolvent exchange. Consequently, the modified phase inversion behavior promoted the formation of more continuous asymmetric finger-like pore structures with improved pore connectivity and enhanced surface hydrophilicity. Mechanistic analysis revealed that PDCCNF-functionalized interfacial regulation synergistically governed phase inversion behavior, asymmetric pore evolution, and membrane surface hydration. The optimized membrane (PC-M0.15) exhibited enhanced permeability, improved dye/protein rejection, and superior antifouling performance during long-term water filtration. This work provides new insights into nanofiller-functionalized interfacial regulation during membrane formation and offers an effective strategy for fabricating high-performance PES ultrafiltration membranes for water treatment applications.

Organic ferroelectrics offer solution processability, mechanical flexibility and promising applications in sensing, energy storage and actuation. However, their polarization and Curie temperatures are typically lower than those of inorganic ferroelectrics because weak intermolecular interactions hinder efficient dipole alignment. The development of organic materials that integrate dipole units, long-range dipole ordering and switchable polarization may enable the design of high-performance organic ferroelectrics. Here we report a donor-acceptor cocrystal in which V-shaped donor molecules pack into a gear-like arrangement, enabled by supramolecular interactions. Within this binary confined lattice, a cooperative in-plane rotation of 42° by the donor molecules-triggered by an external electric field-enables reversible polarization switching. This rotational mechanism yields a remanent polarization of 58 μC cm-2, stable ferroelectricity up to 479 K and a low coercive field of 0.022 MV m-1, exhibiting superior performance compared with previously reported organic ferroelectrics. These findings provide a pathway towards the design of high-performance organic ferroelectrics.

The development of sustainable, high-performance elastomers with multifunctional capabilities is pivotal for the next-generation of eco-friendly technologies. Here, we overcome the intrinsic rigidity of cellulose, by orchestrating its molecular chains into dynamic, chiral-nematic ordered liquid crystal elastomers using hydroxypropyl cellulose. Precise control over elasticity and optical properties was achieved via a salt-induced Hofmeister effect, which modulates the interchain hydrogen-bond network. This network acts as a reversible softness regulator, while the embedded right-handed helical structures produce vivid, stimuli-responsive structural colors. Crucially, mechanical strain unwinds the helix in liquid crystal elastomer, resulting in a real-time, naked-eye mechanochromic response that directly visualizes the local stress. This dynamic color change enables real-time monitoring of mechanical stress for practical applications in rehabilitation training. Moreover, owing to the biocompatibility and biodegradability nature of cellulose, the obtained elastomer can be completely degraded within 30 days in soil. This work provides a scalable design route for sustainable elastomers that simultaneously offer high performance, multifunctionality, and embodied intelligence, paving the way for a distinct class of smart eco-friendly materials.

Lightweight multifunctional aerogels hold great promise in applications, e.g., electromagnetic microwave absorption, thermal insulation, and acoustic damping. However, conventional aerogels often suffer from limited functionalities, complicated manufacturing, and poor sustainability. Metal-organic frameworks (MOFs), with tunable porosity and abundant active sites, offer a compelling route to high-performance multifunctional aerogels, but it has remained a grand challenge to develop sustainable multifunctional MOF-based aerogels. Here, we report a sustainable multifunctional bio-aerogel (Ni-CCA) by integrating hierarchical scale-like topological Ni-MOF-NH2 with cellulose through simple pretreatment using deep eutectic solvent followed by stepwise assembly–carbonization. The resulting aerogel features an ultralow density and a 3-dimensional layered porous structure. With 5 wt.% filler loading, Ni-CCA achieves a minimum reflection loss (RLmin) of −53.47 dB and an effective absorption bandwidth of 4.42 GHz, along with a radar cross-section suppression of 27.90 dB·m2. Additionally, Ni-CCA shows enhanced flame retardancy (64.3% reduction in peak heat release), low thermal conductivity [33.3 mW/(m·K)] and improved acoustic damping (NRC of 0.31, 15 to 23 dB attenuation). The multifunctionalities of this bio-aerogel stem from its hierarchical architecture and synergistic loss mechanisms, offering a promising strategy for creating the next generation of lightweight multifunctional protective materials.

Printable aqueous carbon nanotube (CNT) inks are promising for scalable, flexible, and wearable electronics, yet it remains challenging to simultaneously achieve high electrical performance, long-term dispersion stability, and reliable processability in water. A one-pot ternary deep eutectic solvent (TDES) pretreatment enables lignin depolymerization and functionalization with ammonium phytate/sulfate groups, followed by spontaneous self-assembly into P/N/S-containing lignin nanoparticles (PLNPs). The resulting PLNPs exhibit tunable particle sizes (from 24 nm to 100 nm) and high negative surface charge (up to -62.6 mV). PLNPs adsorb uniformly onto CNT surfaces without forming large aggregates. Molecular dynamics (MD) simulations reveal an "anchor-and-disperse" interfacial mechanism, in which PLNPs anchor on CNT surfaces with heteroatom-enabled noncovalent interactions, while surface charge and hydration provide electrosteric and steric stabilization that suppresses reaggregation. The PLNPs/CNT inks show pronounced shear-thinning and rapid thixotropic recovery, making them suitable for screen printing of conductive patterns on paper. The inks exhibit excellent colloidal stability (>100 days) and achieve conductivities up to 34.9 S·cm-1 without additional synthetic additives. Furthermore, cotton textiles can be dip-coated to fabricate wearable piezoresistive sensors capable of monitoring diverse human motions. This work provides a renewable, waterborne CNT ink platform for sustainable printed and wearable textile electronics.

Aqueous zinc-ion batteries (ZIBs) are regarded as a promising candidate for the next-generation energy storage system. As a gel electrolyte with tunable chemistry, polyacrylamide hydrogels suffer from insufficient mechanical strength and limited capability to regulate Zn2+ transport. Herein, we address this challenge by incorporating 2D cellulose nanosheets (CNS) into a polyacrylamide network, constructing a composite gel electrolyte with heterogeneous synergistic effects. The CNS reinforces the gel through physical cross-linking with polyacrylamide chains, significantly improving its mechanical properties, while the CNS increases the transference number of Zn2+ and suppresses side reactions, thereby favoring uniform zinc deposition and reversible stripping. Benefiting from this cooperative mechanism, the composite hydrogel enables stable cycling in Zn||Zn symmetric cells, operating for over 2800 h at 0.5 mA cm-2 and 0.5 mAh cm-2, and the assembled Zn||MnO2 full cell demonstrates a high-capacity retention of 88.5% after 2500 cycles at 0.5 A g-1. Furthermore, the assembled flexible battery exhibited stable specific capacity under repeated bending, confirming its excellent mechanical flexibility. This work establishes a novel system for long-life and high-safety gel electrolyte for ZIBs, while validating the considerable promise of 2D biomass-derived nanomaterials for advanced energy storage systems.

Nanofluidic membranes possess unique ion-selective transport properties, offering considerable potential for energy harvesting and sensing applications. However, the scarcity of anion-selective membranes has significantly hindered progress in these fields. Herein, the energy disparities among chitin crystalline planes are exploited to selectively cleave the low-energy (020) plane, facilitating the directional exfoliation of Bouligand-structured chitin into 2D sub-nanosheets (CSs) with an average thickness of 0.7 nm and lateral dimensions of 50-100 nm. Simulations and experiments demonstrate that a reduction in thickness significantly enhances both the ion transport flux (1.53 times) and selectivity (1.14 times), which in turn boosts the power output density to 12.95 W m-2 under a 50-fold salinity gradient surpassing all-existing biomass-based nanofluidic membranes (max. 2.87 W m-2) and the commercial benchmark (5.0 W m-2). Furthermore, the membranes' extreme ion management capabilities facilitate real-time nanofluidic sensing, as demonstrated in jellyfish cultivation monitoring. This study presents a cost-effective strategy for developing high-performance, positively-charged nanofluidic membranes with exceptional energy harvesting and sensing capabilities, laying the foundation for advanced energy and sensing technologies.

Solid electrolytes are a key enabling technology for the safe operation of Li-metal batteries, as they can suppress side reactions and Li dendrites. However, their microstructural heterogeneity and metastability largely restrict their mechanical and electrochemical properties. Herein we report a one-pot sol-gel self-assembly for in-situ constructing silica-cellulose-ether nanocomposite as solid-state electrolytes in Li-metal batteries. The obtained composite features mesoporous silica nanoparticles grafted to functional cellulose nanofibers to form crosslinked frameworks, in which liquid ether electrolytes are in-situ immobilized. By regulating chemical interactions between three nanocomponents for optimizing electrolyte's distribution and ionic conduction, such composite design enables excellent electrochemical properties, showing rapid Li+ ionic conductivity (6.9 x 10-4 S cm- 1) and high electrochemical oxidation tolerance (4.87 V vs Li/Li+). Notably, the quasi-solid-state Li-metal batteries using composite membranes exhibit outstanding battery performance: Li//LiFePO4 cell delivers an ultra-high capacity retention of 97.5 % after 200 cycles, and Li//RuO2-O2 cell exhibits an extended cycle-life over 300 cycles.

Passive cooling permits thermal management of near-zero energy consumption and low CO2 emissions. Herein, cellulose/wood chip composite foam (CWF) with anisotropic porous structure was prepared via freeze-casting strategy. The CWF displayed an average reflectance of up to 95.2 % in the UV to NIR light range (0.2-2.5 mu m), as well as with an average emissivity of 94.8 % in the atmospheric transparent window (8-13 mu m). The theoretical cooling power reaches approximately 130 W/m2, thus making it suitable for applications in fields such as passive cooling building materials. In addition, hydrophobic coating was further applied to the CWF, which not only endowed the CWF with moisture resistance, but also enhanced the reflectivity. This novel CWF composed of natural polymer and forest wastes will pave the way for smart passive coolers of high efficiency, sustainability and low cost.

Chirality transfer across length scales is a fascinating phenomenon that has intrigued researchers across disciplines. This is especially the case with cellulose, where, despite being one of the most exploited materials in our society, such as paper and cotton, it remains elusive when it comes to the transfer of intrinsic chirality at the molecular scale to larger hierarchical structures. Here, we show that in the case of cellulose nanocrystals (CNCs), allomorphic transformation from cellulose I to cellulose II can lead to chirality inversions in chiral nematic suspensions. This phenomenon allows the fabrication of right-handed chiral photonic films using CNCs extracted from standard plant biomass, which is first mercerized and then subjected to sulfuric acid hydrolysis, followed by desulfation. Similar to standard cellulose I-based CNC self-assembly, the twist chirality and aspect ratio of the left-handed CNCs in cellulose II can be significantly modified through crystallite aggregation engineering. In contrast to molecular liquid crystals, chirality inversion has never been presented in colloidal liquid crystals, and our findings present a step toward the development of so far inaccessible cellulose materials beyond the native crystallinity.

Novel cellulose solvents, including polybasic inorganic salt hydrates (ISH), have been exploited for cellulose swelling, dissolution and functionalization. The ZnCl2-based hydrate is deemed to one of effective cellulose solvents. However, the role of water ratio for tunning cellulose swelling or dissolution remains unclear. In this work, a series of binary ISH with variable water ratios are designed for this purpose. The effects of water on the hydrogen bond interactions and cellulose swelling or dissolution behaviors were comprehensively investigated via Kamlet-Taft parameters (i.e., β and π*) analyses and molecular dynamic simulation. Results show that such ISH only contributes to the fiber swelling when the molar ratio of water is 2.5, ascribed to the destruction of surface hydroxyl group for cellulose molecule under an unsaturated zinc hydrate. Upon the cellulose swelling in ZnCl2-based ISH, followed by the regeneration in ethanol/water, a flexible yet robust specialty paper can be roll-to-roll prepared, and the tailored paper has an ultrahigh strength (107.5 MPa), toughness (18.8 %), enhanced dielectric strength (48.8 kV/mm) and good hydrophobicity (73.6°).

Impact sensitivity and elasticity are among the most important properties of energetic materials. Both properties are related to the mechanical stress. Understanding elasticity and impact sensitivity is crucial for predicting the mechanical response and failure of energetic materials, thus establishing a correlation between the elasticity mechanics and the initiation and detonation of energetic materials. However, it is unclear how elasticity influences the impact sensitivity of energetic crystals. Herein, the elastic properties of 19 typical energetic crystals with impact sensitivity varying from low to high are studied by using dispersion-corrected density functional theory. We demonstrate that the elastic stiffness tensors predicted in this work satisfy the necessary and sufficient stability conditions for elastic stability. A thorough comparison with literature data further shows that while the results are in general agreement with literature data, large discrepancies are found for certain elastic tensor elements. By probing the correlation between impact sensitivity and elasticity, we show that higher elastic moduli and elastic anisotropy generally lead to lower impact sensitivity. The underlying mechanism is that higher elastic moduli and higher elastic anisotropy lead to easy absorption of impact energy in the form of elastic deformation and dissipation of impact energy through thermal conductivity and shear sliding, thus lowering the probability of impact-induced formation and growth of hotspots. These findings facilitate our fundamental understanding of the elastic properties and structure-property relationships of energetic crystals.

Interface evaporation-driven hydroelectric systems integrating water purification and energy collection offer the potential for sustainable agricultural irrigation. However, achieving high evaporation rates and efficient energy harvesting poses challenges, particularly in optimizing evaporation and water transport. This study develops a gradient-aligned structured aerogel (GA aerogel), composed of biomass materials such as cellulose and chitosan, which utilizes efficient water transport through aligned cellulose channels, unique ion management in nanoscale channels, and chitosan's ability to reduce evaporation energy consumption, thereby enhancing water and energy harvesting performance. The GA aerogel achieves a solar absorption rate of 91.4%, an evaporation rate of 2.5 kg m-2 h-1, an output power of 680 nW cm-2, and stable operation for over 120 h. Furthermore, by integrating a series array with capacitive energy storage, the system utilizes harvested electrical energy to irrigate plants with purified water, promoting sustainable agriculture and providing insights for designing biomass-based solar evaporators.