Ionogels have garnered significant attention in fields such as flexible electronics and energy storage. However, simultaneously achieving high strength, excellent stretchability, and strong reversible adhesion for ionogels remains a major challenge. To address this, we propose a strategy that involves introducing a flexible segment capable of forming dense interactions with various components into a rigid segment-dominated macro-phase separated system. Specifically, hydroxyethyl acrylate as the flexible segment was incorporated into a strong macro-phase separation system composed of benzyl methacrylate (BzMA) as the rigid segment and ionic liquid. Benefiting from the preserved small entanglement regions of BzMA that serve as stress-dispersing zones, as well as the reversible interactions within the system that impart stretchability, the resulting ionogel exhibits a high tensile strength of 8.4 MPa, a fracture strain of 396%, and an outstanding toughness of 17.8 MJ m-3. This modulation process also enhances the optical transmittance of the ionogel to 87%. Moreover, the ionogel exhibits strong reversible adhesion (7.46 MPa on glass) through heating-cooling cycles in both air and underwater environments. Leveraging these high mechanical properties and reversible underwater adhesion, the ionogel is successfully applied in an underwater transfer monitoring device, highlighting its great potential for applications that demand both robust mechanical performance and strong adhesive capability. (c) 2026 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.
The development of flexible wearable electronics (FWE) that integrate high sensitivity, excellent strain tolerance, and multi-signal decoupling capability is of great significance, yet remains challenging. Herein, a rigid-flexible supramolecular unit is constructed by incorporating flexible demethylated lignin (DL) onto the surface of rigid cellulose nanofibers (CNF) framework (DL@CNF). This supramolecular unit integrates high-strength rigid load-bearing with a high-efficiency energy dissipation mechanism at the nanoscale, which confers high fatigue resistance and stable signal transmission. The presence of rigid crystalline regions and the sufficient dynamic interaction sites on the DL@CNF endow the eutectogel with superior mechanical properties (approximate to 343 kPa, 5000%), robust adhesion (approximate to 110 kPa), good self-healing property, and excellent UV shielding capability (99.5%). Benefiting from the above integrated features, the wearable sensors that harness the eutectogel as the generation of high-fidelity electrical signals in response to strain, pressure, and temperature over a broad temperature range (-80 degrees C to 60 degrees C). This work unlocks immense potential as a generic platform for biomass-derived supramolecular engineering, offering a unique opportunity to create tailored materials for advanced bio-based flexible electronics.
Abstract This research examines recycling potassium hydroxide-based pretreatment black liquor in wheat straw chemi-thermo-mechanical pulping (CTMP) to improve process sustainability and cut operational expenses. By reusing the black liquor across five cycles, the solid content increased from 6.2 % to 14.8 %, concentrating both organic and inorganic elements without adding new chemicals. About 80 % of the solids were degradation products of cellulose, hemicellulose, and lignin, with potassium and silicon making up the remaining 20 %. The recycling did not harm fiber structure, pulp strength, or papermaking ability, as shown by FTIR, SEM, and Micro-CT analyses. No new functional groups appeared, though slight increases in hydroxyl and carbonyl bands were noticed. These findings reveal that black liquor recycling in wheat straw CTMP is a viable method to boost liquor concentration, reduce freshwater use, and lower energy and costs associated with evaporation and transportation. This study supports cleaner production in non-wood pulping by enabling effluent reuse and valorization within a circular process.
Driven by the principles of ecological sustainability, this study presents an integrated biorefinery strategy for the rapid deconstruction and integrated valorization of moso bamboo. A novel lactic acid-based ternary deep eutectic solvent (DES), composed of tetrabutylammonium chloride, lactic acid, and p-toluenesulfonic acid (TBAC/LA/PTSA), was developed to achieve rapid fractionation. Under optimized conditions (130 degrees C, 30 min), the ternary DES achieved a high removal efficiency of lignin (86.28%) and hemicellulose (95.23%), significantly reducing pretreatment time and energy consumption. The resulting cellulose-rich residue exhibited an exceptional enzymatic hydrolysis efficiency of 98.28%, maintaining a robust performance of 76.75% even after five DES recycling cycles. Structural characterization revealed that the isolated lignin possessed high purity, moderate molecular weight, and superior antioxidant activity (IC50 = 0.66 mg/mL), outperforming the commercial antioxidant BHT (IC50 = 0.96 mg/mL). Furthermore, the pretreatment liquid was directly transformed into a high-performance functional eutectogel via a seamless in situ gelation process. The resulting eutectogel displayed outstanding mechanical properties (747% tensile strain and 954 kPa compressive strength) and exceptional environmental adaptability across a wide temperature range (-70 to 65 degrees C). This integrated approach not only demonstrates the efficient deconstruction of bamboo biomass but also provides a sustainable pathway for synthesizing wearable flexible electronics, ensuring the comprehensive utilization of all lignocellulosic components.
Developing skin-adhesive hydrogel sensors that balance robust, stable signal detection with comfortable, painless removal remains a formidable challenge in wearable electronics. Here, we present a temperature-responsive, skin-adhesive (TRSA) hydrogel integrating fast temperature response, visually reversible adhesion, and antifreezing properties. The hydrogel is fabricated via the random copolymerization of [2-(methacryloyloxy)ethyl] dimethyl-(3-sulfopropyl) ammonium hydroxide (DMAPS) and acrylic acid (AA), with lithium chloride (LiCl) acting as a conductive and anti-freezing agent. By finely tuning the DMAPS/AA ratio, the phase transition temperature of the TRSA hydrogel is precisely adjusted to match human body temperature. Above the phase transition temperature, the hydrogel exhibits high transparency and strong adhesion to the skin. Below it, phase transition occurs, turning opaque with greatly weakened adhesion, enabling visual adhesion monitoring and painless, non-irritating detachment. Furthermore, the incorporation of LiCl disrupts the hydrogen bonds between water molecules, endowing the hydrogel with robust flexibility and ionic conductivity even at sub-zero temperatures. As a flexible strain sensor, the TRSA hydrogel demonstrates high sensitivity (Gauge Factor = 3.62 at 0-100% strain). Our hydrogels provide a highly promising paradigm for next-generation flexible electronic skins, intelligent wearable devices, and human-computer interaction systems.
The rapid development of wearable electronics, self-powered systems, and the Internet of Things urgently requires efficient thermal management (TM) technologies and sustainable energy solutions. However, triboelectric nanogenerator (TENG) and their integrated electronic components inevitably generate or accumulate Joule thermal. It led to performance degradation or even device failure. This review focuses on the research progress in integrating advanced TM technologies into TENGs, aiming to provide comprehensive insights for constructing high-performance and highly stable self-powered systems. The scope of this review encompasses: (i) systematically summarizing the design and development of TM-TENG systems based on key materials, such as graphene, carbon nanotubes, MXene, cellulose, and phase change materials, (ii) elucidating the bidirectional coupling mechanism between triboelectric charge generation and thermal management, along with a critical analysis of existing theoretical models, and (iii) detailing the multifunctional integration and applications potential of TM-TENGs in the fields including thermal conversion, thermal energy harvesting, storage, actuation, and conduction. The bidirectional coupling mechanisms between triboelectric charge generation and thermal management are thoroughly dissected at a theoretical level. The predominant physical models explaining the interaction phenomena between frictional heating and thermal management are reviewed, with critical analysis of their applicability and limitations. Furthermore, this work discusses the current challenges and future directions in this field and proposes strategic recommendations for realizing more advanced TM-TENG systems. The primary objectives of this review are to synthesize existing knowledge, clarify interaction mechanisms, and promote interdisciplinary development at the intersection of thermal management and energy harvesting.
Lignin condensation and the recalcitrance of lignocellulose during conventional fractionation limit their valorization. Herein, we develop a tunable ternary deep eutectic solvent (TDES) composed of guanidine hydrochloride, lactic acid, and ethylene glycol for efficient fractionation of moso bamboo. By modulating the EG content, 74.3% delignification was achieved while preserving lignin structure, as confirmed by a β‑O‑4 content of 26.3/100 Ar (61.3% retention). Lignin nanoparticles self‑assembled into uniform lignin nanobottles (LNBs) with size controlled by lignin structure. Moreover, the preserved structural integrity enabled a high bio‑oil yield of 39.7 wt%. 4‑Vinylphenol was identified by Py‑GC/MS as the dominant product. Strong positive correlations were observed between β‑O‑4 content and both LNBs size and bio‑oil yield. Enzymatic saccharification of the treated residue achieved up to 94.4% glucose conversion. This work establishes a clear structure‑property relationship and presents a "structure‑first" strategy for dual‑pathway lignin valorization into nanomaterials and fuels.
The interface reflection loss severely constrains the light-harvesting efficiency in solar technologies. Conventional anti-reflective coatings face limitations such as narrow wavelength, angular dependence, and complicated fabrication process. Here, we propose an omnidirectional light-harvesting biomimetic design based on refractive index tunable core-shell particles. The carboxyl groups-containing polymers aggregate into nanocluster as the core and tetraethyl orthosilicate hydrolyzes into SiO2 shell. The gradient refractive index of core-shell particles can be achieved by regulating the composition of core and shell, as well as the pH value during the hydrolysis process. The broadband omnidirectional anti-reflection (BOAR) coating can be prepared by a scalable dip-coating process, providing flexibility for the adaptation of different substrates. The BOAR coating has an average transmittance of over 80% across a broad spectral range of 300-2500 nm and a wide incidence angle range of 0 degrees- 85 degrees. Compared to bare cells, the solar cells with BOAR coating show a 2.5 mA cm-2 increase in short-circuit current density and an improvement in power conversion efficiency from 10.8% to 11.8%. Our work provides a scalable approach that integrates broadband angular stability, omnidirectional performance, and ambient temperature processability, making it suitable for applications in photovoltaic modules, solar energy collectors, and optical devices.
Non-timber resources pulping and papermaking can not only effectively make up for the shortage of timber resources, but also minimize their own pollution, which is derived to the high value utilization of natural resources. As a recently cultivated high-yield hybrid variety of Arundo, Chinese Arundo donax (CAD) demonstrated significant potential for pulping and papermaking. In this study, effects of alkali impregnation stage in chemimechanical pulping (CMP) process on the soluble substances including glucose, xylose and lignin of Chinese Arundo donax and subsequent pulping and papermaking performance were systematically investigated. It was found that CAD-based pulp and paper produced by chemi-mechanical pulping method exhibited excellent properties. Particularly, the yield of CAD-based pulp can reach as high as 64.27%. Moreover, the ring crush, tensile, bursting and tear indexes of CAD-based paper were 9.708 N center dot m/g, 23.190 N center dot m/g, 1.114 kPa center dot m2/g and 3.786 mN center dot m2/g, respectively. Additionally, a high-precision least squares regression model was established to predict the dissolution behavior of xylose during alkali impregnation process, which is helpful to describe and guide the process of pulping and papermaking. Therefore, this study provided a solid theoretical foundation and experimental support for valorization of Chinese Arundo donax in the field of pulping and papermaking.
To address plastic pollution and food preservation challenges through the valorization of industrial by-products, we developed a high-performance food packaging film incorporating beeswax and sodium lignosulfonate (LS). In this system, LS served a dual function: as a submicron emulsion stabilizer, it enabled the formation of a stable and uniform dispersion of hydrophobic beeswax, and as an interfacial compatibilizer, it strengthened adhesion between the cellulose matrix and the wax phase within the composite film. This synergistic design produced a film with a tensile strength of 107 MPa, representing a 133% increase over pure cellulose, along with exceptional barrier properties, including an oxygen permeability (OP) of 1.95 cm3 center dot & micro;m center dot m-2 center dot day-1 center dot kPa-1 and a water vapor permeability (WVP) of 6.98 & times; 10 3 g center dot & micro;m center dot m-2 center dot day-1 center dot kPa-1 , while maintaining high visible light transmittance (87%). The lignin incorporation also conferred antioxidant and antibacterial functionalities to the films and effectively extended the shelf life of cherry tomatoes under normal storage conditions. This design successfully reconciles the trade-off between in-use durability, as predicted by Arrhenius modeling, and rapid end-of-life biodegradability, providing a versatile blueprint for next-generation, circular bio-based packaging materials.
Multicolor luminescence modulation of lignin-derived carbon quantum dots (LD-CQDs) is a key prerequisite for anti-counterfeiting applications; however, achieving this through surface engineering using a single precursor remains challenging. This study develops a stepwise surface chemical modulation strategy using alkali lignin (AL) as the sole carbon source to achieve continuous photoluminescence (PL) tuning of LD-CQDs from blue to yellow. Blue-emitting LD-CQDs (L-CQDs) were first synthesized via choline chloride-assisted hydrothermal treatment. Subsequent synergistic nitrogen/sulfur (N/S)-codoping with 2,4-diaminobenzenesulfonic acid produced green emissive LD-CQDs (N-CQDs) with a markedly enhanced quantum yield of 16.3%. Controlled nitric acid oxidation of N-CQDs further yielded oxygen-doped LD-CQDs (O-CQDs) enriched with electron-withdrawing oxygen-containing moieties, resulting in a pronounced PL red shift to the yellow region. Comprehensive structural characterizations confirmed the progressive incorporation of N/S/O heteroatomic functional groups and elucidated their strong structure-property correlations with the sequential PL red shift. Polyvinyl alcohol (PVA) served as a dispersing stabilizer and film-forming matrix to fabricate carbon quantum dot/polyvinyl alcohol (CQDs/PVA) printed fluorescent films (CPPFs) and composite fluorescent films (CPCFs) via screen printing and template casting, respectively. The resulting films exhibited excellent fluorescence and ultraviolet-shielding performance, providing a robust basis for anti-counterfeiting packaging applications. Overall, this work establishes an efficient and generalizable surface-engineering strategy for precise PL regulation of LD-CQDs, underscoring their potential for rapid-response anti-counterfeiting technologies and functional packaging materials.
Developing flexible pressure sensors that combine ultralow detection limits, high sensitivity, and environmental sustainability remains challenging, particularly using bio-based alternatives to petroleum-derived polymers. We present ultra-sensitive pressure sensors based on multi-scale allyl cellulose ball (ACB) arrays. ACBs were fabricated through syringe-based droplet formation in a saturated NaCl bath and UV-mediated crosslinking of allyl cellulose (AC), yielding a dual-network architecture comprising physically entangled chains from salt-induced phase separation and covalently crosslinked allyl groups that imparts mechanical robustness with controlled diameters (1.2, 1.5, and 2.2 mm). The sensor features a gradient architecture where different-sized ACBs create sequential activation mechanisms: larger balls deform first under low pressure, followed by progressive engagement of smaller balls, achieving ultrahigh sensitivity (27.2% kPa-1), ultralow detection limit (8 Pa), rapid response/recovery (38/40 ms), broad detection range (8 Pa-10 kPa), and exceptional stability (less than 5% drift over 6500 cycles). The approach eliminates expensive lithographic fabrication while surpassing human tactile thresholds. We demonstrated practical applications including flexible electroluminescent devices with programmable patterns and an intelligent handwriting recognition system capable of real-time character classification with 99.3% accuracy. This work establishes a gradient architecture strategy for biodegradable cellulose-based flexible sensors, offering a scalable and cost-effective pathway toward next-generation sustainable wearable electronics and intelligent human-machine interfaces.
Achieving high sensitivity across a broad pressure range remains a critical challenge for wearable flexible triboelectric hydrogel sensors. Here, we report an electric-field-induced in-situ crosslinking strategy to fabricate a gradient porous hydrogel based on phosphorylated cellulose nanofibrils (P-CNF) colloid. Under the field, negatively charged P-CNF electrophoretically migrates toward the anode, establishing a stable concentration gradient. Subsequent UV polymerization and hydrogen-bond crosslinking between P-CNF and PAM yield a continuous transition from a PAM-rich macroporous layer to a P-CNF-reinforced dense microporous region, forming multi-level continuous interfaces without interfacial delamination. The resulting gradient architecture exhibits spatially graded modulus, which regulates local stress distribution and ion migration pathways. When configured as a triboelectric nanogenerator (TENG), this hydrogel achieves a high sensitivity of 14.24 V/kPa (0-10 kPa) and 1.55 V/kPa (10-65 kPa), with a fast response time of 14 ms and recovery time of 16 ms. The continuous multi-level interfaces effectively alleviate stress concentration and prevent structural collapse under a broad pressure range. This work demonstrates that electrophoretically controlled colloidal assembly combined with in-situ hydrogen-bonding network formation provides a general and scalable route to gradient hydrogels with continuous interfaces for mechanoelectric applications.
Achieving high temperature phosphorescence (HTP), particularly using biomass as precursors, is intriguing but faces significant challenges due to the violent non-radiative decay. Here, lignin is converted to carbon dots (L-CD) in the urea-boric acid (UB) matrix through an in situ double matrix confinement strategy. The rigid UB matrix can provide multiple chemical and non-covalent interactions with L-CD, thus the triplet excitons are protected against quenching by strong confinement effect. The L-CD-UB demonstrates outstanding room temperature phosphorescence (RTP) lifetime of 1256.99 ms and quantum yield of 7.43% at ambient environment. Because of the high stability of the triplet excitons and reduced energy gap between singlet state and triplet state, the L-CD-UB shows thermally activated delayed fluorescence (TADF) and high temperature phosphorescence dual emission phenomenon, with a striking phosphorescence lifetime of 304.33 ms at 453 K. The work provides an effective method to achieve HTP of lignin and affords a promising eco-friendly material for high temperature anti-counterfeiting, encryption and smart sensing.
Intelligent indicator films for food spoilage detection have emerged as an effective strategy to mitigate foodborne diseases and reduce food waste in modern life. However, large-scale fabrication of such intelligent films with integrated biosafety, biodegradability, and multifunctionality remains a significant challenge. Herein, a facile and feasible gel immersion technique was developed to prepare biodegradable cellulose/curcumin indicators with good antibacterial, antioxidant, and anti-ultraviolet properties by employing γ-CD-MOFs as curcumin carriers. The structure and performance of the cellulose/curcumin@γ-CD-MOFs films were found to be highly dependent on curcumin@γ-CD-MOFs concentration. Although the tensile strength of cellulose/curcumin@γ-CD-MOFs film decreased with increasing curcumin@γ-CD-MOFs content, the tensile strength of Film C-Cur5 (highest loading) still reached 94.26 MPa, maintaining good mechanical properties. Notably, the integration of curcumin@γ-CD-MOFs substantially enhanced the anti-ultraviolet, antioxidant, and antibacterial capacities of the cellulose composites. Specifically, the average transmittance of cellulose composites in UVA, UVB, and UVC regions was reduced from 86.15%, 80.24%, and 56.75% to 3.55%, 5.40%, and 3.18% for Film C-Cur5, respectively. Simultaneously, the radical scavenging rate of composite films reached a maximum of 95.90%. Meanwhile, the color of the composite films was strongly impacted by both curcumin concentration and pH value, and Film C-Cur5 exhibited the highest sensitivity to pH changes. Furthermore, the biosafe and biodegradable cellulose/curcumin@γ-CD-MOFs films were further applied to the real-time monitoring of strawberries and apricots freshness and packaging of fresh-cut apple. In conclusion, the pH-sensitive and biodegradable cellulose/curcumin@γ-CD-MOFs composite films with enhanced performance were successfully developed, demonstrating great potential for applications in fruit packaging and freshness detection.
Hard carbon anodes for sodium-ion batteries rely on Na+ insertion into graphite-like layers below 0.1 V, where closed-pore structures are critical for high energy density. However, controlling hard carbon microstructures remains challenging. Here, the industrial lignin precursor was simply pre-pyrolyzed and carbonized to synthesize high-performance hard carbon with curved graphite-like layers forming topological cavities. Through GITT and in situ TEM, we visualized Na+ (de)intercalation and demonstrated that closed pores (similar to 1 nm) enhance sodium storage. Even the FFT transform revealed the appearance of a new material lattice (C32Na). This work provides insights for tuning hard carbon microstructures and biomass bulk processing and value-added utilization.
Cellulose, rich in polar hydroxyl groups, readily loses electrons, making it an ideal positive triboelectric material. However, its insulating nature limits charge storage and increases energy loss, leading to poor charge retention and low output. To address this issue, this study proposes combining the charge confinement at the TEMPO-nanofiber/ferroelectric interface with the microcapacitive effect of carbon nanotubes. This strategy significantly enhances charge trapping and reduces dissipation, achieving a charge density of 308.4 μC/m2, a 452% increase over CNF films. The maximum power density reaches 2.32 W/m2 under load (2580% improvement), while the leakage current decreases to 1.64 × 10-12 A/cm2, a 6707% reduction. The resulting CS-TENG sensor exhibits high sensitivity and stable performance, offering an effective approach to high-density cellulose triboelectric materials in wearable electronics.
Developing high-performance lignocellulosic-based plastics as alternatives to non-biodegradable petroleum-based plastics is a crucial strategy to address white pollution. As an abundant, renewable, and biodegradable natural polysaccharide, xylan is an ideal candidate material for producing bioplastics. However, existing preparation methods often struggle to simultaneously enhance both the strength and flexibility of xylan-based film. To overcome this drawback, a two-birds-with-one-stone strategy was adopted, the dual-network was constructed by crosslinked xylan and nanocellulose via thiol-ene click reaction, followed by stepwise dehydrating and hot-pressing, to produce a xylan bioplastic (XAGP-CNFSH). Here, nanocellulose not only functions as a macromolecular crosslinking agent but also serves as a reinforcing agent, significantly enhancing the mechanical properties of xylan bioplastic. XAGP-CNFSH demonstrates outstanding mechanical performance, with a tensile strength reaching 143 ± 1.36 MPa and toughness up to 19.08 ± 0.44 MJ/m3, superior to most reported xylan-based film. Compared to polyethylene (PE), XAGP-CNFSH offers superior strength and toughness, coupled with a better oxygen barrier (OTR, 3.4 ml·μm/m2·d·Pa), good thermal stability, and biodegradability. This study offers a novel route to developing high-performance, biodegradable bioplastics from renewable xylan.
The pursuit of carbon neutrality and the replacement of highly polluting energy sources drive the imperative need for a novel electrode material system. In this study, a ternary composite hydrogel (LPGH) with promising electrochemical properties was synthesized using a facile one-step hydrothermal method. This material features a graphene-based conductive scaffold, with lignosulfonate (LS) serving as a multifunctional dispersant and potassium ferrate (K2FeO4) incorporated as a multifunctional precursor. The LPGH electrode delivers a remarkable areal capacitance of 799 mF cm-2 at 1 mA cm-2, which is 2.1 times greater than that of the pure graphene hydrogel (377 mF cm-2). Furthermore, a symmetric supercapacitor fabricated with LPGH electrodes achieved an energy density of 41.1 μWh·cm-2 at a power density of 500 μW·cm-2. Moreover, the device exhibited excellent long-term stability, retaining 84.46% of its initial capacitance after 10,000 cycles. This work thus presents a sustainable strategy for designing high-performance, environmentally compatible energy storage materials from biomass resources.
Acrolein, a major harmful substance in cigarettes, could induce cellular genetic mutations and impair cellular repair functions. Therefore, the development of a practical and effective method for detecting acrolein is essential. In this study, a modified polymeric fluorescent probe, Poly(NAP-SH-co-PEGMA400), exhibiting large Stokes shift (110 nm), good water solubility, high selectivity, rapid response time (10 min) and low biotoxicity, was synthesized using the reversible addition-fracture chain transfer polymerization (RAFT) method for the detection of acrolein. Poly(NAP-SH-co-PEGMA400) had been successfully used to detect acrolein in tobacco, cookies, and in gaseous form. Additionally, the result of experiment had been demonstrated remarkable responsiveness to acrolein in biosample imaging experiments involving cells, zebrafish, and rice seedlings.