ABSTRACT Bio‐based adhesives are gaining traction by virtue of their tremendous potential for substituting petrochemical adhesives, yet the restricted adhesion performance, poor water retention, and intrinsic flammability severely hindered their scale‐up application. Herein, drew inspiration from gecko setae and biomineralization, a novel bio‐based adhesive derived from epoxidized HEC‐core hyperbranched polyester hybrid (EH), gelatin (G) and modified nano‐hydroxyapatite (γHA) is presented. In this system, the self‐synthesized EH features a setae‐like hyperbranched structure enriched with abundant active groups, which maximize interfacial effectiveness. Meanwhile the gelatin and hydroxyapatite act synergistically achieve marked enhancements in robust cohesion and durable water retention via biomineralization. The developed organic‐inorganic hybrid adhesive offers a unique combination of broad substrate universality, low‐temperature curability, satisfactory flame retardancy, outstanding environmental robustness, and superior storage stability. The integrated performance profile enables wide‐temperature on‐demand bonding, safe construction application, and extended practical utility with reliable long‐term performance. This bioinspired strategy represents a fresh and feasible insight for the promotion of bio‐based adhesive, and offers a prospective pathway toward robust, sustainable, and safety versatile bonding materials.

Eutectogels hold considerable promise soft electrodes for high-performance flexible triboelectric nanogenerator (TENG) due to their tunable mechanical properties and environmental stability. However, conventional eutectogels with single linear polymer chains often exhibit poor mechanical strength as well as undesirable migration of components (e.g., initiators), which compromise device stability and limit their environmental adaptability in high-performance energy harvesting. Here, lignin was molecularly engineered into branched lignin nanospheres (BLNS) functionalized with polymerizable acrylate groups. In a deep eutectic solvent system, BLNS simultaneously enabled rapid self-initiated UV polymerization (97.3% C--C conversion) and constructed a robust, nonmigrating crosslinked network, yielding triboelectric supramolecular eutectogels (SEG). Specifically, benefiting from branched backbone and nanoreinforcing effect of the BLNS, the resulting SEG achieved exceptional mechanical robustness (tensile strength of 1.76 MPa, toughness of 5.10 MJ/m3) and strong adhesion (1.21 MPa). The SEG-based sensor exhibited a high ionic conductivity of 4.50 mS m- 1 and a gauge factor of 3.3, while maintaining stable sensing performance over a wide temperature range (-30 to 80 degrees C) and under varying humidity conditions (30-90% RH), demonstrating excellent adaptability to harsh environmental conditions. As a proof-of-concept, a TENG was constructed using the SEG as the flexible electrode, with open-circuit voltage remaining stable over 6000 contact-separation cycles, underscoring the robustness and operational stability essential for reliable self-powered soft electronic systems. This work establishes a versatile strategy for designing multifunctional lignin-based materials for next-generation self-powered electronics.

Aqueous zinc ion batteries (AZIBs) utilizing hydrogel electrolytes have emerged as promising sustainable solutions for flexible energy storages owing to their intrinsic safety and mechanical stability. However, the inherent poor toughness, low Zn2+ transference number, and lacking electron field regulation capability in conventional hydrogel electrolytes exacerbate uncontrolled Zn dendrite growth and side reactions, posing a substantial challenge to interfacial stability between the Zn anode and the hydrogel electrolyte. To address this, here we present a novel biphasic hydrogel electrolyte capable of both multi-scale stress deconcentration and dual-field regulation via polymerization followed by salting-out and coordination strategy. The well-designed hydrogel electrolyte demonstrates high toughness of 17.5 kJ m(-2), an ionic conductivity of 60.6 mS cm(-1) and a Zn2+ transference number of 0.753, collectively achieving highly reversible Zn plating/stripping and exceptional interfacial stability. Consequently, the Zn||NaV3O8 center dot 1.5H(2)O (NVO) full cells equipped with this hydrogel electrolyte show remarkable electrochemical performance, including high capacity (375.4 mAh g(-1) at 0.5 A g(-1)), outstanding rate capability (188.9 mAh g(-1) at 8 A g(-1)) and long-term cycling stability (91.6 % capacity retention after 3000 cycles), with sustained performance under harsh conditions such as high temperature, high humidity, and low temperatures (-30 degrees C). Furthermore, the assembled flexible pouch cells demonstrate exceptional mechanical and environmental adaptability, reliably powering a circular lamp even under severe bending at both room and -30 degrees C. This work provides fundamental insights into Zn anodic chemistry in multifunctional hydrogel electrolyte and offers practical guidelines for constructing advanced zinc-based energy storage devices.

The practical application of wood-based materials in sustainable triboelectric nanogenerators (TENGs) is constrained by their mechanical weakness, poor environmental tolerance, and insufficient electrical output. Incorporating functional polymers offers potential for enhancing wood-based substrates, yet weak interfacial bonding often undermines structural stability. Herein, we develop an optimized wood-based substrate (WS) featuring superior mechanical toughness, water resistance, and transparency by constructing the biomimetic hierarchical structures. The filler matrix, engineered with reactive isocyanate groups, enables the formation of stable covalent bonds at hierarchical interfaces, thereby achieving exceptional mechanical toughness (3.38 MJ/m3), water resistance, and a high dielectric constant (5.33). Leveraging these properties, the WS serves as a sustainable substrate for a rotary TENG, enabling efficient wind and water flow energy harvesting, and achieving a significantly enhanced peak power density (300.7 mW/m2) compared with most of the reported wood-based TENGs. This work opens up new avenues for designing next-generation wood-based TENGs for efficient green energy harvesting.

Natural plant cells featuring polygonal honeycomb architectures exhibit exceptional load-bearing and energy dissipation capacities. The strategic incorporation of this biomimetic structure presents an effective reinforcement approach for composite materials. In this study, a fully biobased and sustainable soy protein adhesive with improved water resistance and bonding strength was developed through the integration of modified cork. The cork was modified via a two-step process: deep eutectic solvent treatment to partially remove lignin while preserving the unique cellular framework, followed by dopamine hydrochloride functionalization to improve interfacial reactivity and promote extensive hydrogen bonding with the soy protein matrix. The resulting composite adhesive demonstrated remarkable improvements in performance, achieving a wet shear strength of 1.15 MPa and a 111.8% increase in fracture toughness compared with unmodified soy protein adhesive. This work provides an effective strategy for fabricating high-performance, fully biobased adhesives and highlights the value-added utilization of cork as a functional reinforcement material.

Gel electrolytes are high-priority materials for solid-state Zn-ion hybrid capacitors, characterized by high ionic conductivity and intrinsic mechanical flexibility. However, because the existing gel electrolytes are relatively soft and do not contact intimately with rigid Zn anodes, they have inferior interfacial compatibility with Zn anodes, leading to device degradation. Here we develop a class of biogel electrolytes by in situ crystallizing gelatin triple helix units from the alginate polymer domain to form a unique hierarchical-heterogeneous structure. The biogel electrolyte demonstrates combined advantages of high toughness, temperature-triggered adhesion, high Zn2+ transference number and temperature-independent ionic conductivity. These notable features favor Zn2+ 3D diffusion and accommodate zinc anode volume changes, thus enabling the symmetric Zn||Zn cell to highlight a balance among high current density, high areal capacity and prolonged cycling life. Moreover, the assembled zinc||activated carbon hybrid capacitor performs exceptional capacitive behavior and stable operation across the temperature range from 25°C to -40°C, delivering competitive energy density of 125.5 Wh kg-1 with high capacity retention of 97.1% over 10 000 cycles even at -40°C. Finally, system-level demonstration based on the resulting hybrid capacitors can power portable electronics in a power cable-free manner, validating applicability for green power sources in outdoor activities.

The development of sustainable, high-performance bio-adhesives to replace formaldehyde-based resins remains a critical challenge for the wood industry. However, the low water resistance, poor penetration, and weak adhesion strength severely bottleneck the practical application of bio-adhesives. Here, we present a strong, tough, and flame-retardant soybean meal (SM)-based adhesive with high penetration through a hierarchical dual bio-inspired strategy, combining the hard-soft phase combination of bivalve hinges and the root-like topological entanglement of plants. In this system, calcium sulfoaluminate (CSA) acts as rigid fillers to prompt crack deflection and energy dissipation, while polyacrylamide (PAM) entanglement further enhances the toughness of the SM matrix and mechanical interlocking at the interface. The prepared SM-adhesive achieves significant enhancements in dry shear strengths and wet work of adhesive, which were 6.0 folds and 37.5 folds higher than those of the primary SM. Furthermore, prepared adhesive exhibits excellent flame retardancy with limiting oxygen index of 32.5%, attributing to the gas-phase protective layer and condensed-phase flame retardancy of CSA. This work establishes a sustainable pathway for replacing traditional petroleum-based adhesives in plywood, and it has potential to develop on industrial-scale and achieve eco-friendly alternatives in the future.

Eutectic gels as important conductive polymers have promising practical applications in wearable electronic devices. However, the development of the ultra-stretchable and self-adhesive eutectic gel for multifunctional flexible sensors remains a challenge. Here, a lignin-enabled ultra-stretchable eutectic gel (LEG) integrating with excellent self-adhesion and high conductivity is prepared through polymerizable deep eutectic solvents (PDES) treated lignin followed by in-situ polymerization. In this LEG, the lignin macromolecules are utilized as important mediators to build dynamic crosslinking points in the polyacrylic acid (PAA) networks via hydrogen bond interactions. The dynamic disruption and reconstruction of the hydrogen bonds between the mobile PAA chain and dynamic crosslinking points ensure the high integrity of the crosslinking network to realize the ultra-stretchability (about 4845 %). Additionally, the abundant phenol groups of lignin endow the LEG with robust self-adhesion, which allows the LEG to seamlessly adhere to the different substrates. Based on these features, the LEGs are assembled as wearable strain sensors with high sensitivity, fast response time, and long-term sensing stability, and this wearable strain sensor demonstrates promising applications in human motion monitoring and information encryption systems. This work develops an effective pathway to design lignin-enabled ultra-stretchable eutectic gels for multifunctional sensors.

Self-powered electronic textiles undergo repeated deformation and friction, which imposes higher demands on the mechanical durability and sustainability of the dielectric polymeric substrates. However, designing the ideal polymeric substrates simultaneously possessing high strength and toughness, and excellent reprocessing performance for highly durable electronic textiles remains a rigorous challenge due to the intrinsic conflict in the mechanisms. Herein, we present a design concept that cellulose-enabled reversible chemical micro-crosslinking combination with multiple hierarchical hydrogen bonds induced dynamic crosslinking microdomains to realize the superior strength and toughness, and reprocessable bio-elastomers. The disintegration of hierarchical hydrogen bonds dissipating energy combination with the orientation arrangement of dynamic crosslinking microdomains along the stretching direction miraculously realize the superior mechanical strength (55.58 MPa) and toughness (144.25 MJ/m3). The reversible breakage and reconstruction of the dynamic crosslinking microdomains allow the bio-elastomer to be reprocessed for several cycles with extremely high mechanical strength recovery efficiency of 91.54 %. The bio-elastomers are employed as dielectric layers to laminate with the PPy-modified cotton fabric for large-scale manufacture of TENG-based electronic textiles with high stability, durability, and washability. The application scenarios are demonstrated for energy harvesting, motion monitoring, and human-computer interaction, providing a novel paradigm for environmental friendliness and durable wearable electronics.

Soybean meal (SM)-based adhesive, which is sustainable and releases no aldehyde, can play an important role in the development of green adhesives. However, natural SM-based adhesives lack water retention ability, which makes it tedious to apply in engineered materials. This work designed a polymer entanglement system by free radical polymerization of acrylamide (AAm). As a small molecule filler, succinic acid (SA) entered the polyacrylamide (PAAm) cross-linking network. The hydrophilic amide groups of PAAm can adsorb water molecules through hydrogen bonding interactions, while the introduction of SA achieved hydrogen bonding interlocking between carboxyl and amide groups on water molecules, firmly locking water molecules in the three-dimensional network of PAAm. This not only improved the cohesion of the adhesive, but also achieved excellent water retention performance.The prepressing strength of the plywood with the prepared adhesive was 1.05 MPa, which grew by 104 times in contrast to unmodified one (0.01 MPa) after the veneer was once opened and evaporated in the air for 1 h. In addition, the water content of the modified adhesive was found to be multiplied by 69.5 % after 3 days, in contrast to the unmodified adhesive. The dry and wet shear strengths of the modified adhesive were 2.47 and 1.21 MPa, which were 61.8 % and 317.2 % higher than the SM adhesive. A SM-based adhesive system that enhanced water retention while increasing strength was created, achieving excellent water retention, high bonding strength, and excellent long-term prepressing performance. As a green adhesive, this is a good reference for the further development of soy protein adhesives in engineering applications.

The development of mechanically tunable and self-strengthening hydrogels for advanced electronic applications is highly desirable but remains a challenge. Muscles, as force-bearing tissues, could autonomously grow to adapt to the surrounding environment through cyclic disassembly and reconstruction of muscle fibers by mechanical training. Inspired by this biological feature, we presented a mechanical training enhancement strategy for preparing self-strengthening conductive composite hydrogels. The polyvinyl alcohol (PVA) acted as the hydrogel matrix, MXene serving as conductive medium realized high conductivity (679.6 mS/m), and the incorporation of carboxymethyl cellulose (CMC) not only prevented MXene self-stacking but also strengthened hydrogen bonding interactions and chain entanglement density. During mechanical training process, the nanocrystalline domains of the PVA chain were reoriented into a highly ordered structure, while the decrease in average distance between neighboring nanocrystalline domains increased the density of nanocrystalline domains in the cross-section. As a result, the prestretched composite hydrogel demonstrated enhanced tensile strength of 1356.1 kPa and toughness of 2962.2 kJ/m3, which were 4.4 and 6.4 times of the initial composite hydrogel, respectively. The composite hydrogels were successfully employed as strain sensors for monitoring human motions. This work demonstrated a promising approach to developing self-strengthening soft materials for advanced applications.

Conductive hydrogels have emerged as essential components in wearable electronics due to their intrinsic flexibility, stretchability, and electrical conductivity. However, the simultaneous realization of mechanical robustness, continuous conductive networks, strong adhesion, frost resistance, and structural tunability remains a formidable challenge. Herein, we fabricated a sulfated cellulose (SC) with a high degree of substitution, which acts as a green stabilizer and reactive template to induce the in-situ oxidative polymerization of 3,4-ethylene-dioxythiophene (EDOT) and formed PEDOT: SC dispersions. The resulting PEDOT:SC dispersions exhibit remarkable colloidal stability, high electrical conductivity (1.75 S/cm), and freeze-dry re-dispersibility without performance loss. Based on this stable dispersion, we developed multifunctional hydrogels through copolymerization with acrylamide and doping with lithium chloride. The resulting hydrogels exhibit exceptional stretchability (650 %), high conductivity (52.4 mS/cm), strong adhesion, and robust anti-freezing performance. Notably, the hydrogels maintain mechanical integrity and sensing accuracy at-20 degrees C, supporting stable motion detection and Morse code signal transmission under frozen conditions. This work demonstrates a green and efficient strategy for constructing high-performance conductive hydrogels and dispersions, offering significant potential for wearable electronics in extreme environments.

Hydrogel sensors are emerging as one promising device for wearable electronics by virtue of intrinsic flexibility and stimuli sensitivity. In particular, MXene hydrogel sensors possess superior properties of high sensitivity and wide strain sensing range, because MXene nanosheets have unique flake structure and metal-like electronic conductivity. However, the existing defects of aggregation and oxidation in MXene nanosheets would easily weaken the toughness and conductivity of hydrogel matrices, thus compromising the mechanical flexibility and strain sensitivity of hydrogel sensors. Here a class of MXene hydrogel sensors is proposed by in situ polymerization and non-covalent interactions. These hydrogel sensors exhibit high stretchability and high toughness simultaneously, reaching stretchability of 1100% and fracture energy of 5374 J m-2. Meanwhile, the introduced catechol groups of dopamine-grafted carboxymethyl cellulose sodium （DA@CMC） endow the hydrogel sensor with excellent anti-oxidation, adhesion, and long-term conductivity, enabling this sensor to show desirable strain sensitivity with a fast response time of 102 ms and a wide sensing scope of 0-800% strain. Moreover, the integration of a strain-sensitive hydrogel sensor with a multicolor display demonstrates system-level applications for real-time visual motion monitoring. This work paves the way for the development of body-conformable monitoring devices, holding great potential in wearable electronics that require visual functionalities.

Rechargeable aqueous zinc-ion batteries (ZIBs) have emerged as promising candidates for the next generation of energy storage technology by virtue of their high energy density, safety, and low cost. However, achieving rapid and stable zinc-ion transport and preventing dendrite growth between solid-state electrolyte and Zn anode remain significant challenges. Herein, we developed a biphasic hydrogel electrolyte consist of soybean protein isolate particle clusters phase and a highly entangled elastic network phase. This structure gives the hydrogel both high toughness and high elasticity, ensuring good fatigue resistance even at low temperatures (fatigue threshold of 403 J m-2 at -60 degrees C), and guide uniform electrodeposition to inhibit zinc dendrites. Thanks to commendable balance of excellent mechanical properties and high ionic conductivity of hydrogel electrolyte, symmetrical Zn cells prepared with the biphasic hydrogel electrolyte achieve highly reversible Zn plating/ stripping within 500 h, maintaining a stable overpotential of 81.9 mV at -60 degrees C. Furthermore, the full cell incorporating PANI as the cathode and the developed electrolyte demonstrates a specific capacity of 140 mAh g-1 and maintains cycling stability over 1500 cycles at -60 degrees C. We integrate Zn||PANI cells and biphasic hydrogel strain sensors into a system that accurately monitors muscle responses during dynamic body movements.

Starch-based adhesives have attracted considerable attention as sustainable alternatives to formaldehyde-based binders due to their renewability and environmental compatibility. However, their practical application is still limited by poor water resistance and reliance on hot-pressing. Herein, a swallow's nest-inspired biomimetic strategy is proposed to overcome these challenges and develop a room-temperature curing and multifunctional starch-based adhesive composed of corn starch (CS), diphenylmethane diisocyanate (MDI), polyvinyl alcohol (PVA), and choline phytate (CPA). Specifically, CS served as the rigid phase, while MDI anchored surface hydroxyl groups, forming a compact "hard-soft phase" structure with PVA. CPA endowed this adhesive with antibacterial and flame-retardant functions. The optimized starch-based adhesive cures at room temperature, exhibits outstanding bonding performance (dry/wet shear strengths of 1.36/0.84 MPa) and superior toughness in three-layer plywood. It also maintains excellent mildew resistance (no growth after 15 days) and antibacterial activity against Staphylococcus aureus and Escherichia coli under high temperature and humidity (30 degrees C, 90 %RH). Moreover, the adhesive achieves a limiting oxygen index (LOI) of 30.5 %, and could markedly reduce heat release rate and total heat release resulting from the formation of a protective char layer. This biomimetic design provides a feasible and efficient approach for developing sustainable starch-based adhesives with high bonding strength and multifunctionality.

Hydrophobic ionogels function as functional underwater materials, since their energy dissipation capability is crucial for ensuring structural stability. However, hydrogen bond-based energy dissipation mechanism is susceptible to water molecule interference, and conventional cellulose blend results in limited dissipative capacity. This study introduces a cellulose composite strategy to develop hydrophobic ionogel with a mitigated sea-island structure. Specifically, a novel composite interface was formed by incorporating alkylated cellulose with a high substitution degree (DS = 2.88) into the polymer matrix. The resulting structure enlarged the effective interfacial area, thereby strengthening interfacial friction and enhancing energy dissipation. Consequently, the hydrophobic ionogel exhibited ultrahigh adhesion, showing an interfacial toughness of 1.06 kJ/m2 upon debonding from stainless steel. Remarkably, it retained a high interfacial toughness of 0.68 kJ/m2 even for underwater adhesion. Furthermore, the ionogel demonstrated strong adhesion to substrates with different polarities, excellent reusability, remarkable acid/alkali resistance, and rapid wettability. Based on its excellent conductivity, it was used for underwater motion sensing, vital sign monitoring, and intelligent adhesion. These advances provide new insights for incorporating cellulose-mediated energy dissipation mechanisms in ionogels.

Adhesives with simultaneous strong cohesion and interfacial adhesion are highly desired but challenging to develop, especially for sustainable bio-based systems. Herein, a microphase-separated adhesive (NIPU/PAM) is reported, which bio-based non-isocyanate polyurethane (NIPU) embedded in an entangled polyacrylamide (PAM) network through hydrogen bond interactions. The dynamic hydrogen bonds act as sacrificial bonds for efficient energy dissipation, while the soft-hard phase synergy balances stiffness and ductility-endowing the adhesive with an exceptional fracture strain of 532.73 %, Young's modulus of 1041.51 kPa, and fracture energy of 13,817.27 Jm(-2). For interfacial adhesion, carbamate groups in NIPU form dense hydrogen bonds and covalent linkages with substrates, combined with topological entanglement from PAM chain penetration, achieving an interfacial toughness of 1082.56 Jm(-2). Benefiting from robust cohesion and strong interfacial adhesion, the dry/wet shear strengths of plywood bonded reach 3.71/2.69 MPa (far exceeding GB/T 9846-2015, Type II >= 0.7 MPa), while lap shear strengths on copper, aluminum, and steel reach 4.68, 7.62, and 6.59 MPa, respectively. Notably, it maintains robust adhesion (>3.21 MPa) under extreme conditions (strong acids/alkalis, -85-200 degrees C, organic solvents). This work provides a versatile strategy for balancing toughness, adhesion, and sustainability, offering a promising alternative to fossil-based adhesives.

The rapid development of flexible electronics resulted in a surge in the generation of e-waste, which stimulated a strong demand for environmentally friendly polymer substrates. Developing mechanically robust and recyclable polymer substrates is a promising approach, but remains an ongoing challenge due to the conflict in intrinsic mechanisms of that the weak noncovalent bonds required for recyclability resulting in poor mechanical strength. Herein, we design a dynamic hard domains strategy to develop a cellulose/castor oil-derived fully bio-based thermoset elastomer with excellent mechanical robustness, recyclability, and biodegradation performance for flexible electronic substrates. The construction of the phase separated structure realizes high strength (25.6 MPa), and toughness (43.5 MJ/m3), while the reconfigurability of the dynamic hard domains achieves excellent recyclability with a high mechanical strength retention rate of 88.2 %. Impressively, the bio-based thermoset elastomer can be completely degraded by being buried in the soil for 70 days. Given these features, the bio-based thermoset elastomers are employed as an environmentally friendly substrate for the preparation of printable capacitive sensors (PCSs). The PCSs exhibit robust capacitive sensing performance in both contact or non-contact modes for detecting multiple signals, including pressure, orientation, humidity, and respiration. This work promotes the development of environmentally friendly bio-based polymeric substrates for addressing the growing e-waste problem in flexible electronics.

The plant protein meal-based adhesives have shown promise as eco-friendly alternatives to replace formaldehyde-based resins because of their economics and sustainability. However, there are still challenges in achieving satisfactory water-resistant bonding strength and toughness of these adhesives, due to the high polysaccharide content of raw materials and irrational energy dissipation paths. This study leverages the chemical selectivity of borate towards polysaccharides to develop a robust and tough soybean meal (SM)-based adhesive with hierarchical structure by constructing a graphene oxide-supported dynamic covalent network, labeled SM/BGO/BCS. Benefitting from hierarchical structure and dynamic covalent network, the SM/BGO/BCS adhesive exhibited favorable mechanical strength (dry shear strength of 2.35 MPa), and the water-resistance bonding strength (63 degrees C) is 1.62 MPa, to our knowledge, surpassing most of the existing reported SM-based adhesives. The work of debonding of SM/BGO/BCS adhesive is 1148.2 N/m, an increase of 234% compared to the unmodified SM adhesive, which is toughened by stress transfer between the two phases (BGO and SM matrix), breaking the traditional approach of reinforcing polymers at the expense of toughness. In addition, the SM/BGO/BCS adhesive showed promising mildew resistance in both dry and wet states. According to the cost estimate, the cost of SM/BGO/BCS adhesive is comparable to that of commercially available urea-formaldehyde (UF) resin, making this strategy a viable insight for advancing the industrialization of plant protein adhesives.