Polymerizable Deep Eutectic Solvents-Enabled High-Lignin-Density Networks for Rapid Multi-scale Fabrication of Multifunctional and Extreme Environment Adaptable Soft Devices

Polymerizable Deep Eutectic Solvents-Enabled High-Lignin-Density Networks for Rapid Multi-scale Fabrication of Multifunctional and Extreme Environment Adaptable Soft Devices | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article Polymerizable Deep Eutectic Solvents-Enabled High-Lignin-Density Networks for Rapid Multi-scale Fabrication of Multifunctional and Extreme Environment Adaptable Soft Devices Zhuang Xie, Xinlong Li This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7787557/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Skin-like soft electronics exploiting biomass-derived gel materials raise increasing research attentions, in which multifunctional lignin has been extensively explored. Nevertheless, elevating the lignin loading usually sacrifice the performance, limiting their application potentials. Herein we develop a unique polymerizable deep eutectic solvent (PDES) consisting of a quaternary ammonium monomer and lactic acid to incorporate with high-density lignosulfonate (LS) of > 20 wt% and address the performance trade-offs. The lignin-induced self-catalytic polymerization associated with electrostatic assembly enables room temperature gelation as fast as 1 MPa and versatile adhesion up to 160 kPa, meanwhile allowing self-healing and photothermal capabilities. Such LS-PDES eutectogels also permit intrinsic ion conduction (> 3 mS cm − 1 ) and superior environmental adaptivity over − 80°C to 100°C. Thus, employing the in-situ polymerization between electrodes, rapid prototyping of bend-/impact-resistant flexible supercapacitors is demonstrated to power wearable sensors. More importantly, it facilitates the production of miniaturized soft organic electrochemical transistor (OECT) arrays, whose performance can be well maintained under deformed and extreme temperature conditions. This high-lignin-density eutectogel platform paves a straightforward route towards printed soft ionotronics, bioelectronic interfaces, and brain-inspired computing. Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 1. Introduction The past decades have witnessed the boosting demand for bio-derived multifunctional materials and sustainable microdevices with broad applications in human-machine interfaces, soft robotics, and intelligent healthcare devices. [ 1 – 3 ] An ever-growing number of soft gel-based systems have been established to incorporate natural biomass resources into versatile devices with novel functionalities while enhancing biointerface compatibility and environmental benignity. [ 4 – 6 ] Hydrogels have garnered considerable attention to provide mobile ions within highly stretchable polymer networks, enabling a wide range of soft device applications including wearable ionic sensors/actuators, bioelectronic patches, energy harvesting and storage etc. [ 7 – 9 ] Moreover, ionogels [ 10 – 11 ] and the more biocompatible and eco-friendly organohydrogels and eutectogels, have been favored as alternative soft ion conductors to overcome the challenges associated with hydrogel dehydration and freezing in extreme environments. [ 4 – 5 , 12 – 18 ] Recently, lignin, the second-most abundant biopolymers from plants, has gained significant attention in the development of multifunctional materials due to its complex aromatic structure and unique chemical diversity derived from polyphenol groups. [ 19 – 20 ] In particular, research has shown that lignin can significantly accelerate the radical polymerization for various gel systems to achieve gelation within minutes through triggering the self-catalytic dynamic redox catechol chemistry. [ 20 – 28 ] This could alleviate the rigorous control conditions (e.g., UV/thermal initiation or inert atmosphere) in conventional free-radical polymerization, particularly benefiting the ambient printing of small-scale structures for on-skin or microdevice integration. [ 29 – 32 ] Besides, lignin is capable of enhancing mechanical toughness, interfacial adhesion, thermal stability, light absorption or antioxidant activity, [ 33 – 40 ] thereby broadening the versatility of soft gels. Nevertheless, in most reported lignin gels, the difficulty in achieving the lignin loading exceeding 2 wt% has greatly limited their application potentials, since various types of lignin display poor processibility in conventional solvents. [ 41 ] More critically, its catechol moieties as radical scavenger would inhibit the polymerization and induce gelation failure or lower the gel strength/adhesion with the increasing lignin loading. [ 22 – 26 ] So far, a lignin-incorporated soft gel has yet to demonstrate concurrent enhancement across diverse properties, including mechanical, interfacial, optical, etc., while allowing the rapid device manufacturing from macro- to micro-scales. Deep eutectic solvent (DES), featuring extensive hydrogen bonding interactions and high stability across wide temperature ranges (-80°C–150°C), represent a novel green solvent and electrolyte paradigm. [ 42 ] DES has been extensively employed to extract lignin from plants with high purity, low condensation, and high phenolic group content, and allows the efficient dissolution of lignin up to 50 wt%, [ 41 , 43 ] paving a sustainable route to biopolymers and eutectogels. [ 44 – 46 ] The eutectogels can not only enable remarkable mechanical compliance, self-bonded interface and electronic performance utilizing natural biomolecules, but also mitigate critical drawbacks of conventional hydrogel systems, namely, their short shelf life and vulnerability to huge environmental fluctuations, thereby promoting the practical potentials. [ 13 – 18 , 47 – 48 ] Exploiting the lignin-promoted polymerization, Yan group previously demonstrated fast formation of tough polyacrylic acid (PAA) eutectogels for supercapacitor and wearable sensors. [ 22 ] Sun and colleagues recently reported a lignin-reinforced healable and environmentally adaptable eutectogel with the working range over − 40 to 100°C. [ 17 ] Still, with the low lignin content, these eutectogels face limitations in balancing the gelation time, mechanical robustness, programmable adhesion, multi-functionality as well as scalable microfabrication and integration with UV/heat-sensitive components. Addressing these issues remains pivotal for advancing the real-world applicability of soft gel devices. Herein, we developed a fast-formed and versatile high-ligin-density eutectogel platform to resolve the above trade-offs via a polymerizable deep eutectic solvent (PDES) strategy (Fig. 1 ), where a quaternary ammonium deep eutectic monomer acts as both hydrogen-bond acceptor (HBA) and cationic polymer matrix, along with lactic acid (LA) as the hydrogen-bond donor (HBD), compatibilizing > 20 wt% anionic lignosulfonate (LS). In the presence of LS and small amount of Al 3+ , this LS-PDES system enables rapid room temperature (RT) gelation within minutes as well as open-air micropatterning, obtaining ion-conducting eutectogels with superior environmental adaptivity over the temperature range of -80°C to 100°C. Moreover, the incorporation of high-content LS also afforded multiple non-covalent interactions within the gel networks to improve the mechanical toughness and allow versatile adhesiveness, in addition to enabling self-healing and photothermal capabilities. We then demonstrated facile manufacturing of eutectogel-based soft devices across multi-scales, including bend/impact-resistant supercapacitors to power gel-based wearable strain sensors, and stretchable organic electrochemical transistor (OECT) arrays operated under extreme temperature conditions. Therefore, this multifunctional LS-PDES platform establishes a new paradigm for scalable, high-performance soft ionotronics and integrated microsystems. 2. Results and Discussion 2.1. Design of LS-PDES System for Rapid Gelation across Multi-scales We exploited a methacrylate monomer bearing quaternary ammonium, namely, ([2-(methacryloyloxy)ethyl]trimethylammonium chloride, METAC), in combination with the polar organic acid, typically METAC:LA, to form the PDES and realize LS solubility over 30 wt%. [ 41 ] As demonstrated in Figure S1a, the METAC aqueous solution formed highly viscos liquid as mixed with 20 wt% LS, while the as-prepared 20%LS-PDES solution displayed markedly reduced viscosity with the elevating LA ratio, benefiting further polymerization and a broad range of printing purpose. [ 39 ] Furthermore, for fast gelation, the amount of ammonium persulfate (APS) initiators is proportionally increased with the LS content, in which the APS is superior to react with LS and oxidize the methoxyl groups into semiquinone radicals and further adhesive catechol groups. [ 25 ] Thus, the sufficient amount of APS can ensure the initiation of METAC polymerization, which could be accelerated under the catalysis of Al 3+ . [ 24 , 27 , 49 ] The choice of METAC and LA as components of the PDES was also driven by several considerations. (1) The strong electrostatic attractions as well as non-covalent interactions between the METAC and the sulfonate/aromatic groups in LS would permit tough and dynamic interpenetrating polymer networks even though the radical polymerization may be interfered by LS, extending its elasticity and printability. [ 50 – 52 ] (2) METAC providing mobile chloride ions would endow the eutectogel with intrinsic ion conductivity, while the polyelectrolyte matrix could reduce the liquid leakage. [ 53 ] (3) LA contributes both hydroxyl and carboxyl groups to strengthen the dynamic and adhesive gel networks through plenty of hydrogen bonds. [ 17 ] (4) Both METAC and LA are highly hygroscopic and can adsorb moisture, while the METAC:LA DES retains its fluidity from − 20°C to 100°C (Figure S1b), ensuring the ion conduction and gel softness in long-term usage and extreme temperature ranges. In a typical experiment, a 75 wt% METAC aqueous solution was mixed with LA and AlCl 3 under a molar ratio of 3:1:0.1 to obtain a homogenous PDES, followed by dissolving LS sodium salt up to 20 wt%. The small amount of AlCl 3 (~ 1 wt%) was introduced into the LS-PDES system to promote LS dissolution and radical generation. As seen from Fig. 2 a, upon adding ~ 2 wt% APS together with N,N'-methylenebisacrylamide (MBA) crosslinkers to the polymerization precursor, the solution containing high-content LS (~ 20 wt%) formed black-colored gels in 5 minutes at RT, whereas the LS-free PDES solution showed no significant change even after several hours. This rapid exothermic reaction within minutes was also recorded through infrared thermography (Fig. 2 a), showing a temperature increase of ~ 10°C, in contrast to the LS-free mixture. The gelation time was revealed to correlate positively with the LS content, showing dramatic decrease from ~ 240 min to < 8 min when elevating the LS from 1 wt% to 5 wt%, and the highest gelation rate was observed at 15 wt% LS (Fig. 2 b). Additionally, through the incorporation of Al³⁺, the gelation time was reduced by approximately 3 folds at most under ~ 1 wt% AlCl 3 , which could be attributed to more semiquinone radicals produced as indicated by the electron paramagnetic resonance (EPR) analysis (Fig. 2 c). However, other ions including Li + , Mg 2+ , Zn 2+ and Fe 3+ did not induce such accelerated gelation, consistent with literature. [ 49 ] This may involve redox cycles among APS, Al 3+ and LS assisted by metal complexing with the catechol groups, promoting the radical generation. [ 26 , 49 , 54 ] Fourier transform infrared (FT-IR) spectroscopy (Fig. 2 d) further confirmed the conversion of methacrylate monomers into polymer networks. In order to gain more insights into the interactions between the LS and the PDES, molecular dynamics (MD) simulations were conducted utilizing a representative model containing the LS repeat unit, METAC, LA and H 2 O with the molar ratio of 1:6:2:25, corresponding to ~ 20 wt% LS. As seen from Fig. 2 e, the simulation suggested intense electrostatic attractions between METAC and LS under the polar DES environment, displaying the highest binding energy exceeding − 700 kJ mol − 1 . Other non-covalent interactions such as hydrogen bonding and cation-π interactions are also possible due to the excess METAC ratio. Interestingly, the simulation indicated an aggregation tendency of hydrophobic methacrylate terminals to the aromatic backbones of LS. Thus, these complicated interactions might reduce the stacking of LS chains in DES while drive the assembly into a 3D-interconnected structure, where the LS chains in affinity with METAC molecules may offer high-density non-covalent sites for interchain association, leading to viscosity increase. In addition, the LS chain might serve as a template to improve the probability of PMETAC chain growth and grafting onto the LS as well, facilitating the gelation. Besides, considering that the number of H 2 O molecules is far more than others, the LS-H 2 O binding (~ 400 kJ mol − 1 ) was obvious, with ~ 8 hydrogen bonds in average formed in one LS unit. Despite, LA was found to compete with H 2 O and allowed strong hydrogen bonds with the sulfonate and phenol groups in LS, showing the average hydrogen bond number of 1 per LS molecule but the binding energy close to 100 kJ mol − 1 . Such LS-LA interaction may weaken the long-range electrostatic attraction of LS-METAC and lower the viscosity, while improving chain flexibility in the gel networks. Owing to the high-density interchain connections, the as-prepared eutectogels exhibited excellent mechanical strength and softness to withstand various deformations, including bearing weight, curling, twisting, knotting, stretching (Fig. 2 f). For instance, the gel weighing approximately 1 g can support a 500 g weight, demonstrating its exceptional load-bearing capacity. It could also endure reversible stretching above 200% strain with fast recovery to its original shape. More importantly, the LS-PDES precursor solution allowed direct writing, painting or polymer pen microprinting [ 30 ] on arbitrary substrates immediately after adding the APS, and patterned gel microstructures as small as ~ 50 µm could still be generated in 30 min under ambient air in the presence of LS higher than 10 wt% (Fig. 2 g). Lower LS content of 3 h, in which LS might act as both gelators and anti-oxidants that prevent from oxygen inhibition during the radical polymerization of PMETAC. Moreover, as seen from Fig. 2 g, the patterned gel structures on elastic PDMS substrate, latex glove or porcine skin surface were capable of enduring large strains without cracking or delamination, displaying outstanding mechanical and interfacial robustness. Therefore, gel-based soft devices could be rapidly manufactured over macro- to micro-scales in a diverse variety of forms including 3D building blocks, thin film coatings and patterned microarrays. [ 39 , 55 – 56 ] 2.2. Mechanical and Adhesive Performances of LS-PDES Eutectogels Diverse non-covalent interactions among the chemically crosslinked PDES and the high-density LS could greatly enhance the mechanical performance of such eutectogels. [ 34 , 46 ] As shown in Fig. 3 a, under METAC:LA:AlCl 3 molar ratio of 3:1:0.1, elevating the LS content from 5 wt% to 20 wt% significantly increases the mechanical properties, in which the tensile strength was improved from ~ 0.1 MPa to ~ 0.57 MPa. Moreover, the Young’s modulus and toughness were enhanced by ~ 6 folds and ~ 4 folds, respectively, approaching ~ 120 kPa and ~ 1.2 MJ∙m − 3 at > 15 wt% LS. This could be attributed to the more rigid LS chains filling the gel networks and increasing the crosslinking density through the electrostatic interactions by -SO 3 − groups, as well as the hydrogen/Al 3+ -ligand bonding from polyphenolic groups. As a comparison, the PDES was also exploited to dissolve > 20 wt% alkaline lignin (AL), generating the AL-PDES eutectogels. Without the electrostatic assembly, such AL-PDES was obtained after 12-h RT polymerization and exhibited weaker mechanical strength of < 0.2 MPa and lower elongation strain (Figure S2a). More surprisingly, the LS-PDES without Al 3+ was discovered as much tougher than those including Al 3+ , allowing the tensile fracture stress of 1.4 MPa at 670% strain and Young’s modulus higher than 300 kPa under 20 wt% LS. The 3.7-fold elevated toughness of 4.5 MJ∙m − 3 in the absence of Al 3+ could suggest the considerable electrostatic screening effect of Al 3+ to diminish the interactions between LS and PMETAC chains and reduce physical crosslinking significantly, [ 57 ] which could also explain the increased gelation time under Al 3+ higher than 1 wt%. Such ion effect could be used to effectively tune the softness of the LS-PDES eutectogels over one order of magnitude. Besides, under a fixed concentration of 20 wt% LS, by tuning the METAC:LA:AlCl 3 molar ratio from 1:1:0.1 to 5:1:0.1, corresponding to 42 wt% to 56 wt% of PMETAC in the final networks, the stress and toughness of the LS-PDES gels gradually increased from 0.17 MPa and 0.35 MJ∙m − 3 to 0.64 MPa and 1.5 MJ∙m − 3 , respectively, indicating that a denser PMETAC network tightens the internal structure (Fig. 3 b). However, excessive LS or METAC may also increase the viscosity of the precursors and affect the polymerization degree, thus no further mechanical enhancement was acquired. Compared to previously reported low-lignin-loading (< 10 wt%) gels (Table S1), the high-density LS interconnected with the cationic PDES matrix demonstrated greater mechanical strength or modulus that was proportional to the elevating lignin loading. Because of the abundant non-covalent crosslinking, the LS-PDES networks could also manifest highly dynamic behavior, providing fast self-recovery as well as self-healing capabilities. As shown in Fig. 3 c and S2b, during continuous tensile loading-unloading tests, the 20%LS-PDES gels allowed dissipation of the mechanical energy by > 50% through disruption of the dynamic networks, while they could retain the shape and reduce the strain hysteresis within ~ 3 min, indicating the efficient network reconstruction. [ 51 , 57 ] Fig. 3 d further demonstrates that during the 30 cycles of continuous tests under 100% strain, the stress-strain curves maintained almost identical, displaying the adaptivity to repeated deformations. In addition to tension, the LS-reinforced PDES networks were also endowed excellent compression stability (Figure S2c). Again, in 100 consecutive compression tests (Figure S2d), the stress-strain curves of LS-PDES eutectogels nearly overlapped and the gel shape could be reversibly recovered undergoing 90% compressive strain, demonstrating superior toughness to resist compression over the LS-free PDES gels that cracked easily under pressure. These could be attributed to the double-network topology of LS-PDES, [ 12 , 34 ] with the chemically crosslinked PMETAC networks interpenetrated with LS chains in accompany with numerous physical crosslinking. Regarding the self-healing property, the damaged LS-PDES was discovered to recover ~ 80% of the mechanical stretchability and toughness after 8 h of contact at ambient conditions, possibly resulted from the mobile LS chains to reform the physical crosslinking joints (Fig. 3 e). Notably, gels with the deep black appearance were found to absorb > 90% light below 800 nm at > 10 wt% LS loading (Figure S3), providing a suitable platform for photothermal conversion. [ 38 , 58 ] Hence, the healing could be accelerated under IR illumination with the aid of local temperature raise. As demonstrated in Fig. 3 f, the LS-PDES gels under IR illumination (100 mW cm − 2 ) led to more rapid temperature increase than the PDES gels, reaching ~ 47.5°C within 1 min and ~ 70°C after 10 min. As a consequence, a 2-h illumination under humid air was demonstrated as sufficient to allow the welding of the fractured regions, regaining the stretchability (Fig. 3 g). Furthermore, the tough LS-PDES networks bearing high-density catechol and ionic moieties on the gel surface could permit versatile adhesion to a variety of materials, including glass, stain steel, plastics, rubber, polytetrafluoroethylene (PTFE), and biological tissues such as porcine skin and chicken heart (Fig. 4 a). To quantitatively assess the adhesion strength of the gel, lap shear tests were performed on a range of typical substrates. The test results show that the 20%LS-PDES eutectogel exhibited a maximum adhesion strength of up to 160 kPa on glass and polyacrylates, and 80–100 kPa on cellulose-based materials such as wood and paper, respectively (Fig. 4 b). Even for low-surface-energy PTFE and steel, it still achieved adhesion of approximately 50 kPa, demonstrating its good adaptability to polymer and metal surfaces. Additionally, the adhesion on wet porcine skin remained ~ 30 kPa, which was comparable to previous literatures. [ 20 , 25 , 35 ] In comparison with previous gel systems containing relatively low lignin loading (Fig. 4 c), it demonstrated dramatic enhancement in the shear adhesion strength of LS-PDES towards a broad range of substrates. Subsequently, we evaluated the on-skin adhesion of the LS-PDES with varied LS content through 180° peel tests on wet porcine skin (Fig. 4 d). The peeling strength of the LS-PDES showed a drastic increase as more LS was introduced, with the 10 wt% LS obtaining the maximum interfacial toughness of 430 J m − 2 . The remarkable adhesion may be attributed to the abundant catechol groups generated from the redox process between LS and APS, [ 25 , 49 ] which can form versatile anchoring points with the functional surface groups through hydrogen bonding, covalent attachment or hydrophobic interactions (Fig. 4 e). Furthermore, electrostatic interactions, ion-dipole interactions as well as metal complexation among different interfaces synergistically enhance the adhesion of LS-PDES. [ 17 , 49 ] Besides, the double-network topology rendered the gel toughness, promoting the establishment of intermolecular interactions and tough interfacial bonding. Hence, the improved mechanical stability upon elongation with increasing LS density led to notable enhancement in adhesion strength by the shear tests. Especially at higher LS concentrations where the gels’ cohesive strength increase, their resistance to peeling was thereby improved significantly as well. Thus, our LS-PDES strategy addresses the trade-off between the shear strength and the interfacial bonding in conventional gel systems with the increasing lignin loading, in which both the shear and peel adhesion performances were concurrently enhanced at up to 20 wt% LS. Additionally, as both quaternary ammonium groups and LS have been demonstrated outstanding antibacterial properties, [ 24 , 49 ] we also examined the bacterial culture of E.coli and MRSA on gel-contacted substrates. It turned out that the PDES gel did present certain anti-bacterial properties compared to control, and the LS-PDES added with > 1 wt% LS allowed exciting anti-bacterial capability to remove > 99% bacterial (Figure S4). Therefore, this multifunctional gel system demonstrated broad potential in the field of adhesives, medical dressing as well as bioelectronics. 2.3 Extreme Environment Adaptability of LS-PDES Eutectogels The high moisture affinity of the PDES as well as the LS molecules led to well-maintained gel properties in long-term usage. During the ambient storage (25°C, ~ 30% humidity) for 20 days, notable weight loss was observed on the first 3 days since the initial eutectogel contained ~ 22 wt% water ( Fig. 5 a ) . Despite, the gel weight loss gradually became constant at ~ 10 wt% in the following days, indicating more than half of the water could be eventually retained. The LS-PDES after storage for over 1 month still display high stretchability (Fig. 5 a insert). Additionally, the dehydration further improved the mechanical strength of the Al 3+ -incorporated LS-PDES eutectogel, reaching tensile fracture stress of ~ 1 MPa, Young’s modulus approaching 500 kPa and toughness exceeding 2.6 MJ∙m − 3 (Fig. 5 b). It is also worth noting that, while LS-PDES without chemical crosslinking failed to realize gelation at the > 20 wt% water content, the MBA-free gel after dehydration permitted > 50% elasticity and good toughness owing to the stronger electrostatic crosslinking and chain entanglement, as well as allowing entire degradation in water for recyclable devices (Fig. 5 b and S5). [ 4 , 12 ] Fig. 5 c further demonstrated that the dehydrated LS-PDES showed greater compressive capability to support the standing of a human volunteer of ~ 60 kg by columnar gels with 2-cm diameter and 1-cm height, enduring an estimated compressive stress of > 6 MPa. Besides, as the LS-PDES involves mobile Na + and Cl − from LS and METAC respectively, the ion conductivity was further investigated by varying the compositions. Notably, the as-prepared LS-PDES containing higher water content could reach an ion conductivity exceeding 10 mS∙cm − 1 at 5 wt% LS (Fig. 5 d). Increasing the LS from 5 wt% to 20 wt% was found to reduce the conductivity to 4 ± 1 mS∙cm − 1 , despite more Na + introduced into the gel, in which the restricted segmental mobility due to the rigid and dense LS chains may suppress ionic mobility by limiting ion diffusion pathways. With the reduced water content, the LS-PDES after long-term storage still preserved the conductivity of ~ 0.5 mS cm − 1 under 20 wt% LS (Fig. 5 e). Varying the METAC:LA:AlCl 3 molar ratio from 1:1:0.1 to 3:1:0.1 was found to slightly increase the conductivity, while more METAC induced significant drop in the conductivity resulted from the denser polymer networks. Remarkably, the LS-PDES eutectogels were also demonstrated performance retention under various extreme environment conditions. First, LS was found to increase the thermal stability of the eutectogels, as only ~ 5 wt% weight loss was observed at 150°C in the thermal gravimetric analysis (TGA) of the 15%LS-PDES eutectogel, in comparison to the ~ 10 wt% weight loss of the LS-free eutectogel (Figure S6). Moreover, owing to the inherent low melting point of the METAC:LA DES, excellent anti-freezing performance of the LS-PDES was demonstrated. As measured by differential scanning calorimetry (DSC, Fig. 5 f), the PMETAC hydrogel exhibited a notable exothermic peak at -62.5°C, corresponding to the freezing point of the hydrogel system. In contrast, the LS-free PDES as well as the LS-PDES eutectogels did not show a significant exothermic peak even at temperatures as low as -80°C, meanwhile the softness was maintained at such extremely low temperature as well (Fig. 5 f inset). In addition, taking advantage of the wide temperature tolerance, excellent ion conduction of the eutectogels could be enabled over the range of 100°C to -40°C, in which the conductivity could reach > 20 mS cm − 1 at high temperatures and maintained ~ 0.05 mS cm − 1 below − 40°C (Fig. 5 g). The linear log σ -1/ T relationship also indicated typical Arrhenius behavior of ion transport within the temperature range. Hence, LS-PDES eutectogels promised soft devices with wide environmental adaptivity. 2.4. Flexible Supercapacitors Based on In-situ Polymerized LS-PDES Electrolyte The rapid gelation of LS-PDES eutectogels without external heat or light could accelerate the fabrication of soft devices with outstanding mechanical toughness, interfacial adhesion and ion conductance. Leveraging these advantages, rapid prototyping of flexible supercapacitor was demonstrated through in-situ formed LS-PDES between electrodes, allowing intimate and robust electrode/electrolyte interface. As proof-of-concept, the LS-PDES precursor solution was sandwiched between two pieces of Ni foam loaded with active carbon (AC) electrode materials (Fig. 6 a), and the subsequent polymerization produced a conformal soft gel electrolyte layer. The as-assembled flexible supercapacitors utilizing LS-PDES gel electrolytes were characterized via cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and galvanostatic charge-discharge (GCD). With up to 20 wt% LS, the CV curves still maintained the quasi-rectangular shape as increasing the scan rate to 100 mV∙s -1 (Figs. 6 b), indicating satisfactory capacitive behavior. Compared to the physical attachment of the electrode onto the LS-PDES gel electrolyte, the in-situ gelation decreased the thickness of the entirely device to improve the mechanical flexibility, while the electrochemical capacitance was enhanced by ~ 5 folds as well owing to the improved interfacial contact and reduced resistance. In addition, as the eutectogel enabled excellent long-term stability, the device after 50 days of ambient storage demonstrated well-maintained capacitance of > 60%, proving its potential in practical applications. Moreover, the impact of LS content on supercapacitor performance was investigated. EIS characterizations indicated that, increasing the LS from 1 wt% to 5 wt% promoted both ionic transport and interfacial charge transfer, promising enhanced capacitance (Figure S7a). Further elevated LS content to 20 wt% lowered the internal ion conductivity, but the diffusion impedance was maintained comparable to the 5%LS-PDES. GCD measurements further verified that the LS loading of 5–20 wt% could allow supercapacitors with similar discharge times, which were at least 2 times higher than that with the 1%LS-PDES (Figure S7b). The 20%LS-PDES could achieve a specific capacity of ~ 40 mF∙cm -2 at 1.25 mA∙cm -2 , a value comparable to previous AC-based hydrogel supercapacitors. [ 51 , 59 ] Another interesting feature of the LS-PDES eutectogel electrolyte could be the numerous hydrogen bonds for tight binding with water molecules inside the networks, thus we hypothesized that it may allow high output voltage surpassing the water decomposition limitation in hydrogel-based supercapacitors. [ 60 ] The wider electrochemical window to 2.0 V was demonstrated using LiTFSI-doped PEDOT:PSS electrodes, which showed slight current increase above 1.7 V in the CV curve as seen from Fig. 6 c inset. GCD measurements in Fig. 6 c also verified the output voltage could reach 1.8 V at a current density down to 0.1 mA∙cm -2 . The specific capacity of the 1.8-V supercapacitor, calculated from GCD curves, was 13.5 mF∙cm -2 at the current density of 0.1 mA∙cm -2 . Mechanical stability of this gel-based flexible device was further evaluated. The CV curves were recorded under 90° and 180° bending, as well as under external pressure, and they retained good symmetry with slight variation to the flat device (Figure S7c), demonstrating excellent stability and resilience under forces. More impressively, the tough LS-PDES eutectogels also succeeded in impact protection tests, in which a glass slide covered with the LS-PDES thin film (~ 1 mm in thickness) effectively resisted impact by a 200 g weight from 20 cm height (Fig. 6 d), corresponding to an impact energy of 0.4 J and velocity of 2 m s -1 . In contrast, glass coated with PDES shattered severely upon impact. Hence, 100 cycles of mechanical impact testing were further applied on the flexible supercapacitor based on LS-PDES (Fig. 6 e), in which the CV profiles also exhibited negligible degradation. The abovementioned results highlight the role of the high-LS-density PDES tough networks in establishing mechanically robust soft devices to withstand diverse external forces in complicated real-world wearable scenarios. To prove the wearable potential of LS-PDES, a proof-of-concept integrated system was constructed with the flexible supercapacitor acting as the power source for an LS-PDES gel sensor (Fig. 6 f). The strain sensing performance of the LS-PDES was first examined under the strain range of 10%-300%, yielding increasing electric resistance with a nice linear correlation between the ΔR/R 0 and the strain (R 2 > 0.99, Fig. 6 g). Then the gel sensor was attached to a finger followed by recording the current response via chronoamperometry under the power supply of the charged supercapacitor attached to human body. The measurements showed current decrease of several to > 10 µA in response to various finger bending angles in real time, in accordance with the strain-induced elevation in the gel resistance. Therefore, the rapid and in-situ generation of LS-PDES ion conductors provides a straightforward approach to prototyping of self-powered soft sensing systems at low time and material cost, with promising potentials in further realizing closed-loop e-waste disposal. [ 61 ] 2.5 Printing LS-PDES for Miniaturized Stretchable OECT Arrays More importantly, since the in-air gelation of LS-PDES permits ambient writing of ion conductors, it also facilitates the production of miniaturized soft device arrays on stretchable substrates. Therefore, we demonstrated the fabrication of skin-like elastic OECT arrays based on the direct-write patterns of LS-PDES gel electrolyte in combination with PEDOT:PSS, which served as both the electrodes and active channels (Fig. 7 a). [ 62 ] First, LiTFSI-doped PEDOT:PSS and LS-PDES line arrays having 1–2 mm width were sequentially produced onto the PDMS surface via selective dewetting [ 62 ] or brush pen writing. To establish a crossbar configuration, the LS-PDES patterns were overlapped with the PEDOT:PSS/LiTFSI lines in a perpendicular manner to form a 3×3 array, in which the PEDOT:PSS regions in contact with the LS-PDES electrolyte constituted the active channels (Fig. 7 b). Subsequently, when a AgCl/Ag gate was in touch with the electrolyte to apply a positive bias to 1.5 V, the dedoping induced by cation insertion from the LS-PDES into the channel areas resulted in decreased PEDOT:PSS channel current. As seen from Fig. 7 c, the PEDOT:PSS line in the middle row of the array exhibited remarkably decline in the drain current (I D ) from > 0.2 mA to 10 − 2 − 10 − 3 mA levels via gating from three LS-PDES gel lines respectively, demonstrating the typical depletion-mode OECT characteristics with the ON/OFF ratio up to 100. All the 9 channels at the crossing areas of the 3×3 array succeeded in transistor switching performance, with the transconductance (Gm) ranging from ~ 0.4 to ~ 1 mS (Fig. 7 d). The highest normalized Gm was estimated as ~ 20 S∙cm − 1 , comparable to previously reported all-solid-state PEDOT:PSS OECTs. [ 63 ] The left column of the LS-PDES electrolyte contributed higher Gm than the others, possibly ascribed to the variation in ion conductance among the gel arrays. Furthermore, the OECT could be scaled down by exploiting a PEDOT:PSS microfiber with ~ 400-µm diameter [ 64 ] in contact with a Ag wire covered with a thin layer of LS-PDES electrolyte. As seen from Fig. 7 e, such fiber-type OECT also presented outstanding transfer characteristics with the ON/OFF ratio of > 100 and Gm value close to 0.35 mS. This simple strategy for producing ion conductor and transistor arrays at the microscale could further facilitate the high-throughput screening of ionic circuits, channel/electrolyte interfaces or artificial sensory networks. [ 29 , 65 – 66 ] Knowing that the LS-PDES could maintain its ion conduction in a wide strain and temperature ranges, we further demonstrated OECTs that could operate under deformed and extreme conditions. First, the transfer curves of one PEDOT:PSS/LS-PDES OECT were measured under tensile strains along the gel direction to 40% (Fig. 7 f). The stretched device maintained the electronic performance with slightly increased OFF current and reduced Gm from ~ 2 mS to ~ 1 mS, which could be resulted from the change in the channel dimensions as well as increased ion resistance upon elongation. Furthermore, the all-solid-state OECT was applied repeated strains of 30% for 100 cycles. Again, the device after cyclic deformation could still reserve its high ON/OFF ratio of close to 100, while maintaining ~ 50% of the Gm value (Fig. 7 g). OECT transfer characteristics were also examined by varying the temperature. From − 40°C to 40°C, both the initial I D at the ON state and the OFF current gradually increased with the temperature, as shown in Fig. 7 h. Hence the ON/OFF ratio was maintained as > 100, meanwhile higher Gm was found with the elevating temperature. At the temperature range above 40°C, the shift of the V G for the maximum Gm to higher bias indicated the diminished gating effect, and a significant drop in the ON/OFF ratio and Gm was seen at 80°C (Fig. 7 i), which may be attributed to higher ion injection barrier at the channel interface. Despite, these results suggested excellent temperature resilience of the LS-PDES-based all-solid-state OECTs as well as potential artificial synapse and neural network applications over a wide temperature window. [ 67 – 68 ] 3. Conclusion In summary, this work pioneers a rapid ambient-air polymerizable eutectogel platform integrating LS (up to 20 wt%) with quaternary ammonium-based deep eutectic monomers for producing soft devices across multi-scales. The resulting LS-PDES ion-conducting eutectogels exhibit exceptional environmental adaptability across broad temperature ranges, maintaining its mechanical softness down to -80°C and allowing the device performance from − 40°C to 80°C. The high-density LS interconnected with cationic PDES matrix are demonstrated to synergistically enhance the mechanical strength (> 1 MPa) and toughness (up to 4.5 MJ∙m − 3 ), and the interfacial adhesion as high as ~ 160 kPa towards diverse surfaces, while affording excellent ion conduction (> 3 mS cm − 1 ), photothermal conversion (ΔT > 20°C within 1 min) and self-healing efficacy. This platform further enables rapid prototyping of flexible supercapacitors with high durability towards bending and impact, along with self-powered motion monitoring. Miniaturized soft OECT arrays are also facilitated by ambient writing of LS-PDES patterns, achieving stable performance under deformation and extreme condition tolerance. Leveraging the tailored chemistry of lignin and PDES, this versatile system offers a sustainable pathway toward multifunctional bio-derived materials compatible with high-resolution additive manufacturing or high-throughput material screening for soft ionotronics, bioelectronic interfaces, and neuromorphic computing hardware. 4. Experimental Section Materials : [2-(methacryloyloxy)ethyl]trimethylammonium chloride (METAC, 75 wt.% in H 2 O), lactic acid (LA, 90%), aluminum chloride hexahydrate (AlCl 3 ∙6H 2 O, 99%), sodium lignosulfonate (LS), ammonium persulfate (APS, 98%), N,N′-methylenebisacrylamide (MBA, 98%), poly(3,4‑ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS, PH1000), lithium bis(trifluoromethyl)sulfonimide (LiTFSI, 99.9%) were purchased from Shanghai Aladdin Biochemical Technology Co., Ltd. All chemicals are used as received. Ni foams and Ni foams coated with activated carbon (AC) were purchased from Canrd Technology Co. Ltd. Preparation and Characterization of LS-PDES Eutectogels : METAC and LA were mixed at molar ratios of 1:1 to 5:1, followed by the addition of an appropriate amount of AlCl 3 ∙6H 2 O. The mixture was stirred in an oil bath at 80°C until a homogeneous and transparent polymerizable deep eutectic solvent (PDES) was obtained. Subsequently, LS (5–20 wt%) and MBA crosslinker (1 mol% to METAC) were added to the PDES and stirred at 70°C until completely dissolved. APS aqueous solution was then added and stirred rigorously to obtain a final APS concentration of > 2 wt%. The resulting mixture was immediately poured into a pre-designed PTFE mold to conduct free-radical polymerization. The tensile properties of the as-obtained LS-PDES were evaluated using the dumbbell-shaped gel samples (20 mm × 5 mm × 2 mm) at a speed of 10 mm∙min − 1 . Young’s modulus was calculated based on the slope of 5–25% strain range. Compression tests were conducted using cylindrical samples with a diameter of 25 mm and a height of 5 mm, at a testing rate of 2 mm∙min − 1 . Adhesion strength was measured using lap shear and 180° peeling tests. To test the shear stress, samples (25 mm × 25 mm × 2 mm) were adhered between two rectangular substrates, followed by stretching at a speed of 10 mm∙min − 1 . In the peeling test, samples (150 mm × 30 mm × 2 mm) were adhered to the substrate surface, with the reverse side bonded to a PET film using cyanoacrylate adhesive. The peeling was performed at a speed of 10 mm∙min − 1 . The interface toughness (J m − ²) was calculated as the ratio of the adhesion force to the sample width. The ion conductivity of the LS-PDES was evaluated using electrochemical impedance spectroscopy (EIS) with an electrochemical workstation (CHI660E, Shanghai Chenhua). The gel samples were encapsulated inside a coin cell, with the diameter of 15 mm and 1-mm thickness. EIS was conducted over a frequency range of 1 Hz to 10 6 Hz under varied temperature from − 40°C to 100°C. The ion conductivity was calculated using the following formula: σ= , where S and L are the cross-sectional area and thickness of the sample, and R is the serial resistance from EIS. Molecular Dynamics (MD) Simulation : 120 METAC, 20 LS, 40 LA, 40 Na⁺, 120 Cl⁻, and 500 water molecules were uniformly mixed. Force field parameters were assigned as follows: water molecules were modeled using the TIP3P model, [ 69 ] while all other molecular species were parameterized with the GAFF2 force field. [ 70 ] Topology and parameter files were generated using the Sobtop program. [ 71 ] All MD simulations were carried out using GROMACS version 2019.6 [ 72 ] with a time step of 1 fs. The initial configuration was first subjected to energy minimization to remove unfavorable contacts, followed by a 50 ns production simulation in the NPT ensemble at 298.15 K and 1 bar. Temperature was controlled using the V-rescale thermostat, and pressure was maintained with the Berendsen barostat. Electrostatic interactions were treated using the particle mesh Ewald method, and van der Waals interactions were modeled with the 12–6 Lennard–Jones potential truncated at 1.2 nm. Lorentz–Berthelot combining rules were applied for cross-interactions, and periodic boundary conditions were applied in all directions. Fabrication of Flexible Supercapacitors : 1 wt% PEDOT:PSS was mixed with 2 wt% LiTFSI aqueous solution with rigorous stirring to obtain the conducting polymer ink. The LS-PDES precursor solution was drop-cast onto a Ni foam electrode (20 mm × 20 mm) with an AC loading of ~ 10 mg∙cm -2 or PEDOT:PSS/LiTFSI loading of ~ 2 mg∙cm -2 , followed by uniform spreading across the surface. A second piece of electrode was then placed on top to form a sandwiched structure. The assembled device was left undisturbed for 10 min to complete the in-situ polymerization, yielding the flexible LS-PDES-based supercapacitor. Informed written consent was obtained from all participants in the wearable demonstrations prior to the research. Fabrication of Stretchable OECT Arrays : PDMS substrate was plasma treated with a polyimide mask, followed by dewetting of the PEDOT:PSS/LiTFSI ink and 130°C annealing to produce the electrode patterns. Then the LS-PDES precursor containing 20 wt% LS was direct written by a brush pen onto the PEDOT:PSS patterns in the perpendicular direction to form a crossbar array. Finally, AgCl/Ag paste was applied to the end of the LS-PDES lines, serving as the gate electrode to accomplish the OECT arrays. To produce the fiber-based OECT, PEDOT:PSS microfiber (~ 400 µm diameter) was prepared according to literature. [ 64 ] Then a silver wire was dip-coated with the LS-PDES thin layer, followed by contacting with the microfiber for OECT gating. Transfer characteristics of the OECTs were measured through sweeping the gate bias from − 0.5 V to 1.5 V. Declarations Conflict of Interest Zhuang Xie and Xinlong Li have filed a patent application on LS-PDES eutectogels. Funding: Natural Science Foundation of Guangdong Province (2024A1515010704), National Natural Science Foundation of China (Grant No. 22075325, 22475245) Keywords: extreme environment adaptivity, lignosulfonate, polymerizable deep eutectic solvents, soft electronics, organic electrochemical transistor arrays Acknowledgements The authors gratefully acknowledge the financial support from the Natural Science Foundation of Guangdong Province (2024A1515010704) and National Natural Science Foundation of China (Grant No. 22075325, 22475245). The authors would also like to thank Prof. Jiandong Yao at Sun Yat-sen University for assistance in infrared thermography and Prof. Yong Qian at South China University of Technology for helpful discussions. Data Availability Statement The data that support the findings of this study are available from the corresponding author upon reasonable request. 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06:30:28","extension":"png","order_by":18,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":170216,"visible":true,"origin":"","legend":"","description":"","filename":"Onlinefloatimage7.png","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/082ef7b92ee13f31b6f0ac98.png"},{"id":92919239,"identity":"2114a076-51f8-4585-8dea-3673b4f0e0da","added_by":"auto","created_at":"2025-10-07 06:30:28","extension":"png","order_by":19,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":403382,"visible":true,"origin":"","legend":"","description":"","filename":"Onlinefloatimage8.png","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/9fda0496fbf6e08e37bd98f4.png"},{"id":92919231,"identity":"d66374ed-40df-413c-b4f1-c3e6e9f5dd5b","added_by":"auto","created_at":"2025-10-07 06:30:27","extension":"png","order_by":20,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":430,"visible":true,"origin":"","legend":"","description":"","filename":"Onlineimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/4b5b878568bdb4e9c816e300.png"},{"id":92919667,"identity":"d5821589-acfe-493a-9c35-16a5de69f3ad","added_by":"auto","created_at":"2025-10-07 06:38:28","extension":"xml","order_by":21,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":172562,"visible":true,"origin":"","legend":"","description":"","filename":"rs77875570structuring.xml","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/3c84879449d7437b330ae78a.xml"},{"id":92919247,"identity":"51599b03-01bc-49ed-ba6c-b38437a42c4a","added_by":"auto","created_at":"2025-10-07 06:30:28","extension":"html","order_by":22,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":180139,"visible":true,"origin":"","legend":"","description":"","filename":"earlyproof.html","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/a287bad5b75ded1a73a655ec.html"},{"id":92919217,"identity":"4fe7cdbf-a7d4-4725-9df4-b9fe9c54fadb","added_by":"auto","created_at":"2025-10-07 06:30:27","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":2438204,"visible":true,"origin":"","legend":"\u003cp\u003eSchematic illustrations of the polymerizable deep eutectic solvent (PDES) of METAC:LA integrated with high-density lignosulfonate (LS) for rapid synthesis of multifunctional LS-PDES eutectogels and multi-scale production of soft devices with extreme environmental adaptivity.\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/3a9f98a611e8d3d8022ea056.png"},{"id":92919222,"identity":"9f42554d-12a5-48e6-844a-4585c3b7d637","added_by":"auto","created_at":"2025-10-07 06:30:27","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":3580189,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Digital photos and infrared thermal images of the self-exothermic free-radical polymerization process for rapid synthesis of the 20%LS-PDES eutectogels at room temperature (RT), in comparison with the METAC:LA PDES solution without LS. (b) Plot of the gelation time with LS concentrations added by 1 wt% AlCl\u003csub\u003e3\u003c/sub\u003e. Inset shows the gelation time under various AlCl\u003csub\u003e3 \u003c/sub\u003econtents. (c) Electron paramagnetic resonance (EPR) spectra capturing the presence of semiquinone radicals, with more radicals generated in the presence of AlCl\u003csub\u003e3\u003c/sub\u003e. (d) Fourier Transform infrared (FTIR) spectroscopy of LS, PDES, LS-METAC:LA precursor, and the as-prepared LS-PDES eutectogel. (e) Molecular dynamics (MD) simulation of the interactions among the LS repeat unit, METAC, LA and H\u003csub\u003e2\u003c/sub\u003eO with the molar ratio of 1:6:2:25 (~20 wt% LS), and the corresponding binding energy and average hydrogen bond numbers per mole of LS repeat unit. (f) Photos of the 20%LS-PDES under the conditions of bearing heavy objects, warping, knotting, and stretching. (g) Ambient-air writing of the 20%LS-PDES eutectogels on various elastic substrates including PDMS (i), latex glove (ii) and porcine skin (iii), as well as microdot arrays of LS-PDES gels printed on PDMS (iv). All scale bars are 1 cm.\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/bfd4e9369fde0aec9ec2045b.png"},{"id":92919219,"identity":"8ffceae4-2d23-4b7d-af0e-4da7352d1571","added_by":"auto","created_at":"2025-10-07 06:30:27","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":1338923,"visible":true,"origin":"","legend":"\u003cp\u003eMechanical performance of LS-PDES eutectogels. (a) Tensile stress-strain curves and the corresponding Young's modulus and toughness of the LS-PDES with varied LS contents and Al\u003csup\u003e3+\u003c/sup\u003e ratios. (b) Tensile stress-strain curves and the corresponding Young's modulus and toughness of the LS-PDES with 20 wt% LS and increasing METAC:LA:Al\u003csup\u003e3+\u003c/sup\u003e molar ratio from 1:1:0.1 to 5:1:0.1. (c) Cyclic loading-unloading curve of the 20%LS-PDES over the strain range of 100% to 500%. (d) Cyclic loading-unloading curve of the 20%LS-PDES at 100% strain, indicating self-recovery of the dynamic gel networks within an interval of ~3 min. (e) Comparison of the stress-strain curves between the original LS-PDES and the gel after healing at RT for 8 h, showing ~80% toughness recovery. (f) Temperature changes of LS-PDES with different LS concentrations under irradiation of a 780-nm IR laser. (g) Photos demonstrating the accelerated self-healing of the 20%LS-PDES via photothermal effect.\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/e5f6f0bafa058af603e9fc6a.png"},{"id":92919224,"identity":"0507a35a-f2bd-4d5b-ac4f-1ce49b00721d","added_by":"auto","created_at":"2025-10-07 06:30:27","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":1962599,"visible":true,"origin":"","legend":"\u003cp\u003eAdhesion performance of LS-PDES. (a) Photos of the LS-PDES eutectogels adhered to a wide variety of substrates. (b) The maximum adhesion strength of the LS-PDES to various substrates through lap shear test. (c) Comparison of the adhesion strength on different substrates among LS-PDES and previously reported lignin-based gels (lignin content \u0026gt;1 wt%). AL: alkaline lignin; DAL: demethylated AL. d) Peeling strength curves and the corresponding interfacial toughness of the LS-PDES towards porcine skin, in which the elevating LS content increased the interfacial bonding. (e) Schematic diagram illustrating the adhesion mechanism of LS-PDES. All scale bars are 1 cm.\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/3c29d03597bb25ceffc2b0d9.png"},{"id":92919225,"identity":"e35ff1ff-f551-4c06-8609-11a2b4900ea8","added_by":"auto","created_at":"2025-10-07 06:30:27","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":789664,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Weight change of the 20%LS-PDES eutectogel with initial water content of ~22 wt% during the storage under ambient air. Inset shows the printed eutectogel maintaining stretchability after 30 days of storage. (b) Tensile stress-strain curves of the dehydrated 20%LS-PDES on day 7 with and without the MBA crosslinker, respectively. (c) Photos of the dehydrated LS-PDES with high strength to support human standing and the corresponding compressive stress-strain curve. (d) Ion conductivity of the as-prepared LS-PDES eutectogels with varied LS contents. The METAC:LA:AlCl\u003csub\u003e3\u003c/sub\u003e\u003csup\u003e \u003c/sup\u003emolar ratio was 3:1:0.1. (e) Ion conductivity of the dehydrated 20%LS-PDES at different METAC:LA:AlCl\u003csub\u003e3\u003c/sub\u003e\u003csup\u003e \u003c/sup\u003emolar ratios. (f) Differential scanning calorimetry (DSC) curves of the PDES and LS-PDES eutectogels in comparison with PMETAC hydrogel. (g) Plot of the ion conductivity in the log form with 1000/T over the range of -40 °C to 100 °C.\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/80207544ecab8de6f2cacdc5.png"},{"id":92919240,"identity":"46ac51e5-1fb2-489f-9f2a-2d3a6a6861c3","added_by":"auto","created_at":"2025-10-07 06:30:28","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":1335605,"visible":true,"origin":"","legend":"\u003cp\u003eElectrochemical performance of LS-PDES-based flexible supercapacitors. (a) Schematic of the preparation of flexible supercapacitors via in-situ polymerized LS-PDES gel electrolyte between Ni foam electrodes. (b) Cyclic voltammetry (CV) curves of supercapacitors employing pasted LS-PDES and the in-situ polymerized LS-PDES and activated carbon (AC) electrodes, as well as the device with the in-situ generated electrolyte after ambient storage for 50 days. (c) Galvanostatic charge-discharge (GCD) and CV (inset, 10 mV∙s\u003csup\u003e-1\u003c/sup\u003e) curves of the supercapacitors with PEDOT:PSS/LiTFSI electrodes, demonstrating output voltage to 1.8 V. (d) Photos of glass slides coated with PDES and 20%LS-PDES against the impact (~0.4 J). (e) Retention of supercapacitor performance employing the 20%LS-PDES electrolyte to resist 100 cycles of successive impact tests. (f) Photo of the integrated supercapacitor power source with an on-finger LS-PDES sensor for motion monitoring. (g) Plots of resistance response of the LS-PDES sensor with the applied strain. (h) Real-time current response of the finger bending under the power supply of the flexible supercapacitor.\u003c/p\u003e","description":"","filename":"6.png","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/5683bcb6930880c3fad31afa.png"},{"id":92919241,"identity":"23f48e1d-86d3-4944-8491-0cf8b8313807","added_by":"auto","created_at":"2025-10-07 06:30:28","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":1365082,"visible":true,"origin":"","legend":"\u003cp\u003eDemonstration of stretchable OECT arrays. (a) Schematic illustration of the fabrication process of OECT arrays on elastic substrate based on LS-PDES electrolyte and PEDOT:PSS/LiTFSI electrode line arrays, and the photo of the as-obtained crossbar arrays. (b) Operation mechanism of the OECT arrays. (c) Transfer and corresponding transconductance (Gm) curves of 3 OECT devices exploiting the middle row of PEDOT:PSS/LiTFSI source/drain lines overlapped with three LS-PDES electrolyte respectively. (d) Statistics of the Gm across the 3×3 OECT arrays. (e) Transfer and corresponding Gm curves of an OECT based on a PEDOT:PSS microfiber channel in contact with a LS-PDES-coated Ag wire. (f) Transfer curves of one OECT in the 3×3 arrays under varied tensile strains, with the inset showing the stretching direction. (g) Plots of ON/OFF ratio and Gm of the OECT with stretching cycles at 30% strain. (h) Transfer curves of the OECT over the temperature range from -40 °C to 80 °C. (i) Plots of ON/OFF ratio and Gm of the OECT with the varying temperature.\u003c/p\u003e","description":"","filename":"7.png","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/88586b65ec1abaffba8373ba.png"},{"id":92920782,"identity":"23b07f06-c0b4-405d-af21-0c25529a4686","added_by":"auto","created_at":"2025-10-07 06:54:42","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":14258309,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/a77b7b3a-8295-4add-9893-87d33560cc06.pdf"},{"id":92919218,"identity":"86101358-19e1-4d3f-b1f8-1467c876b76a","added_by":"auto","created_at":"2025-10-07 06:30:27","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":207884,"visible":true,"origin":"","legend":"","description":"","filename":"TableofContents.docx","url":"https://assets-eu.researchsquare.com/files/rs-7787557/v1/bf5fe8e03e7f2d0fa072112e.docx"}],"financialInterests":"The authors declare no competing interests.","formattedTitle":"\u003cp\u003ePolymerizable Deep Eutectic Solvents-Enabled High-Lignin-Density Networks for Rapid Multi-scale Fabrication of Multifunctional and Extreme Environment Adaptable Soft Devices\u003c/p\u003e","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eThe past decades have witnessed the boosting demand for bio-derived multifunctional materials and sustainable microdevices with broad applications in human-machine interfaces, soft robotics, and intelligent healthcare devices.\u003csup\u003e[\u003cspan additionalcitationids=\"CR2\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e]\u003c/sup\u003e An ever-growing number of soft gel-based systems have been established to incorporate natural biomass resources into versatile devices with novel functionalities while enhancing biointerface compatibility and environmental benignity.\u003csup\u003e[\u003cspan additionalcitationids=\"CR5\" citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]\u003c/sup\u003e Hydrogels have garnered considerable attention to provide mobile ions within highly stretchable polymer networks, enabling a wide range of soft device applications including wearable ionic sensors/actuators, bioelectronic patches, energy harvesting and storage etc.\u003csup\u003e[\u003cspan additionalcitationids=\"CR8\" citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e]\u003c/sup\u003e Moreover, ionogels\u003csup\u003e[\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e]\u003c/sup\u003e and the more biocompatible and eco-friendly organohydrogels and eutectogels, have been favored as alternative soft ion conductors to overcome the challenges associated with hydrogel dehydration and freezing in extreme environments.\u003csup\u003e[\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e, \u003cspan additionalcitationids=\"CR13 CR14 CR15 CR16 CR17\" citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e]\u003c/sup\u003e\u003c/p\u003e\u003cp\u003eRecently, lignin, the second-most abundant biopolymers from plants, has gained significant attention in the development of multifunctional materials due to its complex aromatic structure and unique chemical diversity derived from polyphenol groups.\u003csup\u003e[\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e]\u003c/sup\u003e In particular, research has shown that lignin can significantly accelerate the radical polymerization for various gel systems to achieve gelation within minutes through triggering the self-catalytic dynamic redox catechol chemistry.\u003csup\u003e[\u003cspan additionalcitationids=\"CR21 CR22 CR23 CR24 CR25 CR26 CR27\" citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e]\u003c/sup\u003e This could alleviate the rigorous control conditions (e.g., UV/thermal initiation or inert atmosphere) in conventional free-radical polymerization, particularly benefiting the ambient printing of small-scale structures for on-skin or microdevice integration.\u003csup\u003e[\u003cspan additionalcitationids=\"CR30 CR31\" citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e]\u003c/sup\u003e Besides, lignin is capable of enhancing mechanical toughness, interfacial adhesion, thermal stability, light absorption or antioxidant activity,\u003csup\u003e[\u003cspan additionalcitationids=\"CR34 CR35 CR36 CR37 CR38 CR39\" citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e]\u003c/sup\u003e thereby broadening the versatility of soft gels. Nevertheless, in most reported lignin gels, the difficulty in achieving the lignin loading exceeding 2 wt% has greatly limited their application potentials, since various types of lignin display poor processibility in conventional solvents.\u003csup\u003e[\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e]\u003c/sup\u003e More critically, its catechol moieties as radical scavenger would inhibit the polymerization and induce gelation failure or lower the gel strength/adhesion with the increasing lignin loading.\u003csup\u003e[\u003cspan additionalcitationids=\"CR23 CR24 CR25\" citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e]\u003c/sup\u003e So far, a lignin-incorporated soft gel has yet to demonstrate concurrent enhancement across diverse properties, including mechanical, interfacial, optical, etc., while allowing the rapid device manufacturing from macro- to micro-scales.\u003c/p\u003e\u003cp\u003eDeep eutectic solvent (DES), featuring extensive hydrogen bonding interactions and high stability across wide temperature ranges (-80\u0026deg;C\u0026ndash;150\u0026deg;C), represent a novel green solvent and electrolyte paradigm.\u003csup\u003e[\u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e]\u003c/sup\u003e DES has been extensively employed to extract lignin from plants with high purity, low condensation, and high phenolic group content, and allows the efficient dissolution of lignin up to 50 wt%,\u003csup\u003e[\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e, \u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e]\u003c/sup\u003e paving a sustainable route to biopolymers and eutectogels.\u003csup\u003e[\u003cspan additionalcitationids=\"CR45\" citationid=\"CR44\" class=\"CitationRef\"\u003e44\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e]\u003c/sup\u003e The eutectogels can not only enable remarkable mechanical compliance, self-bonded interface and electronic performance utilizing natural biomolecules, but also mitigate critical drawbacks of conventional hydrogel systems, namely, their short shelf life and vulnerability to huge environmental fluctuations, thereby promoting the practical potentials.\u003csup\u003e[\u003cspan additionalcitationids=\"CR14 CR15 CR16 CR17\" citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e, \u003cspan citationid=\"CR47\" class=\"CitationRef\"\u003e47\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR48\" class=\"CitationRef\"\u003e48\u003c/span\u003e]\u003c/sup\u003e Exploiting the lignin-promoted polymerization, Yan group previously demonstrated fast formation of tough polyacrylic acid (PAA) eutectogels for supercapacitor and wearable sensors.\u003csup\u003e[\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e]\u003c/sup\u003e Sun and colleagues recently reported a lignin-reinforced healable and environmentally adaptable eutectogel with the working range over \u0026minus;\u0026thinsp;40 to 100\u0026deg;C.\u003csup\u003e[\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e]\u003c/sup\u003e Still, with the low lignin content, these eutectogels face limitations in balancing the gelation time, mechanical robustness, programmable adhesion, multi-functionality as well as scalable microfabrication and integration with UV/heat-sensitive components. Addressing these issues remains pivotal for advancing the real-world applicability of soft gel devices.\u003c/p\u003e\u003cp\u003eHerein, we developed a fast-formed and versatile high-ligin-density eutectogel platform to resolve the above trade-offs via a polymerizable deep eutectic solvent (PDES) strategy (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e), where a quaternary ammonium deep eutectic monomer acts as both hydrogen-bond acceptor (HBA) and cationic polymer matrix, along with lactic acid (LA) as the hydrogen-bond donor (HBD), compatibilizing\u0026thinsp;\u0026gt;\u0026thinsp;20 wt% anionic lignosulfonate (LS). In the presence of LS and small amount of Al\u003csup\u003e3+\u003c/sup\u003e, this LS-PDES system enables rapid room temperature (RT) gelation within minutes as well as open-air micropatterning, obtaining ion-conducting eutectogels with superior environmental adaptivity over the temperature range of -80\u0026deg;C to 100\u0026deg;C. Moreover, the incorporation of high-content LS also afforded multiple non-covalent interactions within the gel networks to improve the mechanical toughness and allow versatile adhesiveness, in addition to enabling self-healing and photothermal capabilities. We then demonstrated facile manufacturing of eutectogel-based soft devices across multi-scales, including bend/impact-resistant supercapacitors to power gel-based wearable strain sensors, and stretchable organic electrochemical transistor (OECT) arrays operated under extreme temperature conditions. Therefore, this multifunctional LS-PDES platform establishes a new paradigm for scalable, high-performance soft ionotronics and integrated microsystems.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e"},{"header":"2. Results and Discussion","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e\u003ch2\u003e2.1. Design of LS-PDES System for Rapid Gelation across Multi-scales\u003c/h2\u003e\u003cp\u003eWe exploited a methacrylate monomer bearing quaternary ammonium, namely, ([2-(methacryloyloxy)ethyl]trimethylammonium chloride, METAC), in combination with the polar organic acid, typically METAC:LA, to form the PDES and realize LS solubility over 30 wt%.\u003csup\u003e[\u003cspan citationid=\"CR41\" class=\"CitationRef\"\u003e41\u003c/span\u003e]\u003c/sup\u003e As demonstrated in Figure S1a, the METAC aqueous solution formed highly viscos liquid as mixed with 20 wt% LS, while the as-prepared 20%LS-PDES solution displayed markedly reduced viscosity with the elevating LA ratio, benefiting further polymerization and a broad range of printing purpose.\u003csup\u003e[\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e]\u003c/sup\u003e Furthermore, for fast gelation, the amount of ammonium persulfate (APS) initiators is proportionally increased with the LS content, in which the APS is superior to react with LS and oxidize the methoxyl groups into semiquinone radicals and further adhesive catechol groups.\u003csup\u003e[\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]\u003c/sup\u003e Thus, the sufficient amount of APS can ensure the initiation of METAC polymerization, which could be accelerated under the catalysis of Al\u003csup\u003e3+\u003c/sup\u003e.\u003csup\u003e[\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e, \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e, \u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e]\u003c/sup\u003e The choice of METAC and LA as components of the PDES was also driven by several considerations. (1) The strong electrostatic attractions as well as non-covalent interactions between the METAC and the sulfonate/aromatic groups in LS would permit tough and dynamic interpenetrating polymer networks even though the radical polymerization may be interfered by LS, extending its elasticity and printability.\u003csup\u003e[\u003cspan additionalcitationids=\"CR51\" citationid=\"CR50\" class=\"CitationRef\"\u003e50\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR52\" class=\"CitationRef\"\u003e52\u003c/span\u003e]\u003c/sup\u003e (2) METAC providing mobile chloride ions would endow the eutectogel with intrinsic ion conductivity, while the polyelectrolyte matrix could reduce the liquid leakage.\u003csup\u003e[\u003cspan citationid=\"CR53\" class=\"CitationRef\"\u003e53\u003c/span\u003e]\u003c/sup\u003e (3) LA contributes both hydroxyl and carboxyl groups to strengthen the dynamic and adhesive gel networks through plenty of hydrogen bonds.\u003csup\u003e[\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e]\u003c/sup\u003e (4) Both METAC and LA are highly hygroscopic and can adsorb moisture, while the METAC:LA DES retains its fluidity from \u0026minus;\u0026thinsp;20\u0026deg;C to 100\u0026deg;C (Figure S1b), ensuring the ion conduction and gel softness in long-term usage and extreme temperature ranges.\u003c/p\u003e\u003cp\u003eIn a typical experiment, a 75 wt% METAC aqueous solution was mixed with LA and AlCl\u003csub\u003e3\u003c/sub\u003e under a molar ratio of 3:1:0.1 to obtain a homogenous PDES, followed by dissolving LS sodium salt up to 20 wt%. The small amount of AlCl\u003csub\u003e3\u003c/sub\u003e (~\u0026thinsp;1 wt%) was introduced into the LS-PDES system to promote LS dissolution and radical generation. As seen from Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea, upon adding\u0026thinsp;~\u0026thinsp;2 wt% APS together with N,N'-methylenebisacrylamide (MBA) crosslinkers to the polymerization precursor, the solution containing high-content LS (~\u0026thinsp;20 wt%) formed black-colored gels in 5 minutes at RT, whereas the LS-free PDES solution showed no significant change even after several hours. This rapid exothermic reaction within minutes was also recorded through infrared thermography (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea), showing a temperature increase of ~\u0026thinsp;10\u0026deg;C, in contrast to the LS-free mixture. The gelation time was revealed to correlate positively with the LS content, showing dramatic decrease from ~\u0026thinsp;240 min to \u0026lt;\u0026thinsp;8 min when elevating the LS from 1 wt% to 5 wt%, and the highest gelation rate was observed at 15 wt% LS (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb). Additionally, through the incorporation of Al\u0026sup3;⁺, the gelation time was reduced by approximately 3 folds at most under ~\u0026thinsp;1 wt% AlCl\u003csub\u003e3\u003c/sub\u003e, which could be attributed to more semiquinone radicals produced as indicated by the electron paramagnetic resonance (EPR) analysis (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec). However, other ions including Li\u003csup\u003e+\u003c/sup\u003e, Mg\u003csup\u003e2+\u003c/sup\u003e, Zn\u003csup\u003e2+\u003c/sup\u003e and Fe\u003csup\u003e3+\u003c/sup\u003e did not induce such accelerated gelation, consistent with literature.\u003csup\u003e[\u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e]\u003c/sup\u003e This may involve redox cycles among APS, Al\u003csup\u003e3+\u003c/sup\u003e and LS assisted by metal complexing with the catechol groups, promoting the radical generation.\u003csup\u003e[\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e, \u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e, \u003cspan citationid=\"CR54\" class=\"CitationRef\"\u003e54\u003c/span\u003e]\u003c/sup\u003e Fourier transform infrared (FT-IR) spectroscopy (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed) further confirmed the conversion of methacrylate monomers into polymer networks.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eIn order to gain more insights into the interactions between the LS and the PDES, molecular dynamics (MD) simulations were conducted utilizing a representative model containing the LS repeat unit, METAC, LA and H\u003csub\u003e2\u003c/sub\u003eO with the molar ratio of 1:6:2:25, corresponding to ~\u0026thinsp;20 wt% LS. As seen from Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee, the simulation suggested intense electrostatic attractions between METAC and LS under the polar DES environment, displaying the highest binding energy exceeding \u0026minus;\u0026thinsp;700 kJ mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. Other non-covalent interactions such as hydrogen bonding and cation-π interactions are also possible due to the excess METAC ratio. Interestingly, the simulation indicated an aggregation tendency of hydrophobic methacrylate terminals to the aromatic backbones of LS. Thus, these complicated interactions might reduce the stacking of LS chains in DES while drive the assembly into a 3D-interconnected structure, where the LS chains in affinity with METAC molecules may offer high-density non-covalent sites for interchain association, leading to viscosity increase. In addition, the LS chain might serve as a template to improve the probability of PMETAC chain growth and grafting onto the LS as well, facilitating the gelation. Besides, considering that the number of H\u003csub\u003e2\u003c/sub\u003eO molecules is far more than others, the LS-H\u003csub\u003e2\u003c/sub\u003eO binding (~\u0026thinsp;400 kJ mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) was obvious, with ~\u0026thinsp;8 hydrogen bonds in average formed in one LS unit. Despite, LA was found to compete with H\u003csub\u003e2\u003c/sub\u003eO and allowed strong hydrogen bonds with the sulfonate and phenol groups in LS, showing the average hydrogen bond number of 1 per LS molecule but the binding energy close to 100 kJ mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. Such LS-LA interaction may weaken the long-range electrostatic attraction of LS-METAC and lower the viscosity, while improving chain flexibility in the gel networks. Owing to the high-density interchain connections, the as-prepared eutectogels exhibited excellent mechanical strength and softness to withstand various deformations, including bearing weight, curling, twisting, knotting, stretching (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ef). For instance, the gel weighing approximately 1 g can support a 500 g weight, demonstrating its exceptional load-bearing capacity. It could also endure reversible stretching above 200% strain with fast recovery to its original shape.\u003c/p\u003e\u003cp\u003eMore importantly, the LS-PDES precursor solution allowed direct writing, painting or polymer pen microprinting\u003csup\u003e[\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]\u003c/sup\u003e on arbitrary substrates immediately after adding the APS, and patterned gel microstructures as small as ~\u0026thinsp;50 \u0026micro;m could still be generated in 30 min under ambient air in the presence of LS higher than 10 wt% (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eg). Lower LS content of \u0026lt;\u0026thinsp;5 wt% led to much longer gelation time of \u0026gt;\u0026thinsp;3 h, in which LS might act as both gelators and anti-oxidants that prevent from oxygen inhibition during the radical polymerization of PMETAC. Moreover, as seen from Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eg, the patterned gel structures on elastic PDMS substrate, latex glove or porcine skin surface were capable of enduring large strains without cracking or delamination, displaying outstanding mechanical and interfacial robustness. Therefore, gel-based soft devices could be rapidly manufactured over macro- to micro-scales in a diverse variety of forms including 3D building blocks, thin film coatings and patterned microarrays.\u003csup\u003e[\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e, \u003cspan citationid=\"CR55\" class=\"CitationRef\"\u003e55\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR56\" class=\"CitationRef\"\u003e56\u003c/span\u003e]\u003c/sup\u003e\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec4\" class=\"Section2\"\u003e\u003ch2\u003e2.2. Mechanical and Adhesive Performances of LS-PDES Eutectogels\u003c/h2\u003e\u003cp\u003eDiverse non-covalent interactions among the chemically crosslinked PDES and the high-density LS could greatly enhance the mechanical performance of such eutectogels.\u003csup\u003e[\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e, \u003cspan citationid=\"CR46\" class=\"CitationRef\"\u003e46\u003c/span\u003e]\u003c/sup\u003e As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea, under METAC:LA:AlCl\u003csub\u003e3\u003c/sub\u003e molar ratio of 3:1:0.1, elevating the LS content from 5 wt% to 20 wt% significantly increases the mechanical properties, in which the tensile strength was improved from ~\u0026thinsp;0.1 MPa to ~\u0026thinsp;0.57 MPa. Moreover, the Young\u0026rsquo;s modulus and toughness were enhanced by ~\u0026thinsp;6 folds and ~\u0026thinsp;4 folds, respectively, approaching\u0026thinsp;~\u0026thinsp;120 kPa and ~\u0026thinsp;1.2 MJ∙m\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e at \u0026gt;\u0026thinsp;15 wt% LS. This could be attributed to the more rigid LS chains filling the gel networks and increasing the crosslinking density through the electrostatic interactions by -SO\u003csub\u003e3\u003c/sub\u003e\u003csup\u003e\u0026minus;\u003c/sup\u003e groups, as well as the hydrogen/Al\u003csup\u003e3+\u003c/sup\u003e-ligand bonding from polyphenolic groups. As a comparison, the PDES was also exploited to dissolve\u0026thinsp;\u0026gt;\u0026thinsp;20 wt% alkaline lignin (AL), generating the AL-PDES eutectogels. Without the electrostatic assembly, such AL-PDES was obtained after 12-h RT polymerization and exhibited weaker mechanical strength of \u0026lt;\u0026thinsp;0.2 MPa and lower elongation strain (Figure S2a). More surprisingly, the LS-PDES without Al\u003csup\u003e3+\u003c/sup\u003e was discovered as much tougher than those including Al\u003csup\u003e3+\u003c/sup\u003e, allowing the tensile fracture stress of 1.4 MPa at 670% strain and Young\u0026rsquo;s modulus higher than 300 kPa under 20 wt% LS. The 3.7-fold elevated toughness of 4.5 MJ∙m\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e in the absence of Al\u003csup\u003e3+\u003c/sup\u003e could suggest the considerable electrostatic screening effect of Al\u003csup\u003e3+\u003c/sup\u003e to diminish the interactions between LS and PMETAC chains and reduce physical crosslinking significantly,\u003csup\u003e[\u003cspan citationid=\"CR57\" class=\"CitationRef\"\u003e57\u003c/span\u003e]\u003c/sup\u003e which could also explain the increased gelation time under Al\u003csup\u003e3+\u003c/sup\u003e higher than 1 wt%. Such ion effect could be used to effectively tune the softness of the LS-PDES eutectogels over one order of magnitude.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eBesides, under a fixed concentration of 20 wt% LS, by tuning the METAC:LA:AlCl\u003csub\u003e3\u003c/sub\u003e molar ratio from 1:1:0.1 to 5:1:0.1, corresponding to 42 wt% to 56 wt% of PMETAC in the final networks, the stress and toughness of the LS-PDES gels gradually increased from 0.17 MPa and 0.35 MJ∙m\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e to 0.64 MPa and 1.5 MJ∙m\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e, respectively, indicating that a denser PMETAC network tightens the internal structure (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb). However, excessive LS or METAC may also increase the viscosity of the precursors and affect the polymerization degree, thus no further mechanical enhancement was acquired. Compared to previously reported low-lignin-loading (\u0026lt;\u0026thinsp;10 wt%) gels (Table S1), the high-density LS interconnected with the cationic PDES matrix demonstrated greater mechanical strength or modulus that was proportional to the elevating lignin loading.\u003c/p\u003e\u003cp\u003eBecause of the abundant non-covalent crosslinking, the LS-PDES networks could also manifest highly dynamic behavior, providing fast self-recovery as well as self-healing capabilities. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec and S2b, during continuous tensile loading-unloading tests, the 20%LS-PDES gels allowed dissipation of the mechanical energy by \u0026gt;\u0026thinsp;50% through disruption of the dynamic networks, while they could retain the shape and reduce the strain hysteresis within ~\u0026thinsp;3 min, indicating the efficient network reconstruction.\u003csup\u003e[\u003cspan citationid=\"CR51\" class=\"CitationRef\"\u003e51\u003c/span\u003e, \u003cspan citationid=\"CR57\" class=\"CitationRef\"\u003e57\u003c/span\u003e]\u003c/sup\u003e Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed further demonstrates that during the 30 cycles of continuous tests under 100% strain, the stress-strain curves maintained almost identical, displaying the adaptivity to repeated deformations. In addition to tension, the LS-reinforced PDES networks were also endowed excellent compression stability (Figure S2c). Again, in 100 consecutive compression tests (Figure S2d), the stress-strain curves of LS-PDES eutectogels nearly overlapped and the gel shape could be reversibly recovered undergoing 90% compressive strain, demonstrating superior toughness to resist compression over the LS-free PDES gels that cracked easily under pressure. These could be attributed to the double-network topology of LS-PDES,\u003csup\u003e[\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e, \u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]\u003c/sup\u003e with the chemically crosslinked PMETAC networks interpenetrated with LS chains in accompany with numerous physical crosslinking.\u003c/p\u003e\u003cp\u003eRegarding the self-healing property, the damaged LS-PDES was discovered to recover\u0026thinsp;~\u0026thinsp;80% of the mechanical stretchability and toughness after 8 h of contact at ambient conditions, possibly resulted from the mobile LS chains to reform the physical crosslinking joints (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ee). Notably, gels with the deep black appearance were found to absorb\u0026thinsp;\u0026gt;\u0026thinsp;90% light below 800 nm at \u0026gt;\u0026thinsp;10 wt% LS loading (Figure S3), providing a suitable platform for photothermal conversion.\u003csup\u003e[\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e, \u003cspan citationid=\"CR58\" class=\"CitationRef\"\u003e58\u003c/span\u003e]\u003c/sup\u003e Hence, the healing could be accelerated under IR illumination with the aid of local temperature raise. As demonstrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ef, the LS-PDES gels under IR illumination (100 mW cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e) led to more rapid temperature increase than the PDES gels, reaching\u0026thinsp;~\u0026thinsp;47.5\u0026deg;C within 1 min and ~\u0026thinsp;70\u0026deg;C after 10 min. As a consequence, a 2-h illumination under humid air was demonstrated as sufficient to allow the welding of the fractured regions, regaining the stretchability (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eg).\u003c/p\u003e\u003cp\u003eFurthermore, the tough LS-PDES networks bearing high-density catechol and ionic moieties on the gel surface could permit versatile adhesion to a variety of materials, including glass, stain steel, plastics, rubber, polytetrafluoroethylene (PTFE), and biological tissues such as porcine skin and chicken heart (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea). To quantitatively assess the adhesion strength of the gel, lap shear tests were performed on a range of typical substrates. The test results show that the 20%LS-PDES eutectogel exhibited a maximum adhesion strength of up to 160 kPa on glass and polyacrylates, and 80\u0026ndash;100 kPa on cellulose-based materials such as wood and paper, respectively (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb). Even for low-surface-energy PTFE and steel, it still achieved adhesion of approximately 50 kPa, demonstrating its good adaptability to polymer and metal surfaces. Additionally, the adhesion on wet porcine skin remained\u0026thinsp;~\u0026thinsp;30 kPa, which was comparable to previous literatures.\u003csup\u003e[\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e, \u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e, \u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e]\u003c/sup\u003e In comparison with previous gel systems containing relatively low lignin loading (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ec), it demonstrated dramatic enhancement in the shear adhesion strength of LS-PDES towards a broad range of substrates. Subsequently, we evaluated the on-skin adhesion of the LS-PDES with varied LS content through 180\u0026deg; peel tests on wet porcine skin (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed). The peeling strength of the LS-PDES showed a drastic increase as more LS was introduced, with the 10 wt% LS obtaining the maximum interfacial toughness of 430 J m\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe remarkable adhesion may be attributed to the abundant catechol groups generated from the redox process between LS and APS,\u003csup\u003e[\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e, \u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e]\u003c/sup\u003e which can form versatile anchoring points with the functional surface groups through hydrogen bonding, covalent attachment or hydrophobic interactions (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee). Furthermore, electrostatic interactions, ion-dipole interactions as well as metal complexation among different interfaces synergistically enhance the adhesion of LS-PDES.\u003csup\u003e[\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e, \u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e]\u003c/sup\u003e Besides, the double-network topology rendered the gel toughness, promoting the establishment of intermolecular interactions and tough interfacial bonding. Hence, the improved mechanical stability upon elongation with increasing LS density led to notable enhancement in adhesion strength by the shear tests. Especially at higher LS concentrations where the gels\u0026rsquo; cohesive strength increase, their resistance to peeling was thereby improved significantly as well. Thus, our LS-PDES strategy addresses the trade-off between the shear strength and the interfacial bonding in conventional gel systems with the increasing lignin loading, in which both the shear and peel adhesion performances were concurrently enhanced at up to 20 wt% LS.\u003c/p\u003e\u003cp\u003eAdditionally, as both quaternary ammonium groups and LS have been demonstrated outstanding antibacterial properties,\u003csup\u003e[\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e, \u003cspan citationid=\"CR49\" class=\"CitationRef\"\u003e49\u003c/span\u003e]\u003c/sup\u003e we also examined the bacterial culture of E.coli and MRSA on gel-contacted substrates. It turned out that the PDES gel did present certain anti-bacterial properties compared to control, and the LS-PDES added with \u0026gt;\u0026thinsp;1 wt% LS allowed exciting anti-bacterial capability to remove\u0026thinsp;\u0026gt;\u0026thinsp;99% bacterial (Figure S4). Therefore, this multifunctional gel system demonstrated broad potential in the field of adhesives, medical dressing as well as bioelectronics.\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec5\" class=\"Section2\"\u003e\u003ch2\u003e2.3 Extreme Environment Adaptability of LS-PDES Eutectogels\u003c/h2\u003e\u003cp\u003eThe high moisture affinity of the PDES as well as the LS molecules led to well-maintained gel properties in long-term usage. During the ambient storage (25\u0026deg;C, ~\u0026thinsp;30% humidity) for 20 days, notable weight loss was observed on the first 3 days since the initial eutectogel contained\u0026thinsp;~\u0026thinsp;22 wt% water \u003cb\u003e(\u003c/b\u003eFig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea\u003cb\u003e)\u003c/b\u003e. Despite, the gel weight loss gradually became constant at ~\u0026thinsp;10 wt% in the following days, indicating more than half of the water could be eventually retained. The LS-PDES after storage for over 1 month still display high stretchability (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea insert). Additionally, the dehydration further improved the mechanical strength of the Al\u003csup\u003e3+\u003c/sup\u003e-incorporated LS-PDES eutectogel, reaching tensile fracture stress of ~\u0026thinsp;1 MPa, Young\u0026rsquo;s modulus approaching 500 kPa and toughness exceeding 2.6 MJ∙m\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb). It is also worth noting that, while LS-PDES without chemical crosslinking failed to realize gelation at the \u0026gt;\u0026thinsp;20 wt% water content, the MBA-free gel after dehydration permitted\u0026thinsp;\u0026gt;\u0026thinsp;50% elasticity and good toughness owing to the stronger electrostatic crosslinking and chain entanglement, as well as allowing entire degradation in water for recyclable devices (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb and S5).\u003csup\u003e[\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e, \u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e]\u003c/sup\u003e Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ec further demonstrated that the dehydrated LS-PDES showed greater compressive capability to support the standing of a human volunteer of ~\u0026thinsp;60 kg by columnar gels with 2-cm diameter and 1-cm height, enduring an estimated compressive stress of \u0026gt;\u0026thinsp;6 MPa.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eBesides, as the LS-PDES involves mobile Na\u003csup\u003e+\u003c/sup\u003e and Cl\u003csup\u003e\u0026minus;\u003c/sup\u003e from LS and METAC respectively, the ion conductivity was further investigated by varying the compositions. Notably, the as-prepared LS-PDES containing higher water content could reach an ion conductivity exceeding 10 mS∙cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at 5 wt% LS (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed). Increasing the LS from 5 wt% to 20 wt% was found to reduce the conductivity to 4\u0026thinsp;\u0026plusmn;\u0026thinsp;1 mS∙cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, despite more Na\u003csup\u003e+\u003c/sup\u003e introduced into the gel, in which the restricted segmental mobility due to the rigid and dense LS chains may suppress ionic mobility by limiting ion diffusion pathways. With the reduced water content, the LS-PDES after long-term storage still preserved the conductivity of ~\u0026thinsp;0.5 mS cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e under 20 wt% LS (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ee). Varying the METAC:LA:AlCl\u003csub\u003e3\u003c/sub\u003e molar ratio from 1:1:0.1 to 3:1:0.1 was found to slightly increase the conductivity, while more METAC induced significant drop in the conductivity resulted from the denser polymer networks.\u003c/p\u003e\u003cp\u003eRemarkably, the LS-PDES eutectogels were also demonstrated performance retention under various extreme environment conditions. First, LS was found to increase the thermal stability of the eutectogels, as only\u0026thinsp;~\u0026thinsp;5 wt% weight loss was observed at 150\u0026deg;C in the thermal gravimetric analysis (TGA) of the 15%LS-PDES eutectogel, in comparison to the ~\u0026thinsp;10 wt% weight loss of the LS-free eutectogel (Figure S6). Moreover, owing to the inherent low melting point of the METAC:LA DES, excellent anti-freezing performance of the LS-PDES was demonstrated. As measured by differential scanning calorimetry (DSC, Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ef), the PMETAC hydrogel exhibited a notable exothermic peak at -62.5\u0026deg;C, corresponding to the freezing point of the hydrogel system. In contrast, the LS-free PDES as well as the LS-PDES eutectogels did not show a significant exothermic peak even at temperatures as low as -80\u0026deg;C, meanwhile the softness was maintained at such extremely low temperature as well (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ef inset). In addition, taking advantage of the wide temperature tolerance, excellent ion conduction of the eutectogels could be enabled over the range of 100\u0026deg;C to -40\u0026deg;C, in which the conductivity could reach\u0026thinsp;\u0026gt;\u0026thinsp;20 mS cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at high temperatures and maintained\u0026thinsp;~\u0026thinsp;0.05 mS cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e below \u0026minus;\u0026thinsp;40\u0026deg;C (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eg). The linear log\u003cem\u003eσ\u003c/em\u003e-1/\u003cem\u003eT\u003c/em\u003e relationship also indicated typical Arrhenius behavior of ion transport within the temperature range. Hence, LS-PDES eutectogels promised soft devices with wide environmental adaptivity.\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec6\" class=\"Section2\"\u003e\u003ch2\u003e2.4. Flexible Supercapacitors Based on In-situ Polymerized LS-PDES Electrolyte\u003c/h2\u003e\u003cp\u003eThe rapid gelation of LS-PDES eutectogels without external heat or light could accelerate the fabrication of soft devices with outstanding mechanical toughness, interfacial adhesion and ion conductance. Leveraging these advantages, rapid prototyping of flexible supercapacitor was demonstrated through in-situ formed LS-PDES between electrodes, allowing intimate and robust electrode/electrolyte interface. As proof-of-concept, the LS-PDES precursor solution was sandwiched between two pieces of Ni foam loaded with active carbon (AC) electrode materials (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ea), and the subsequent polymerization produced a conformal soft gel electrolyte layer. The as-assembled flexible supercapacitors utilizing LS-PDES gel electrolytes were characterized via cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and galvanostatic charge-discharge (GCD). With up to 20 wt% LS, the CV curves still maintained the quasi-rectangular shape as increasing the scan rate to 100 mV∙s\u003csup\u003e-1\u003c/sup\u003e (Figs.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003eb), indicating satisfactory capacitive behavior. Compared to the physical attachment of the electrode onto the LS-PDES gel electrolyte, the in-situ gelation decreased the thickness of the entirely device to improve the mechanical flexibility, while the electrochemical capacitance was enhanced by ~\u0026thinsp;5 folds as well owing to the improved interfacial contact and reduced resistance. In addition, as the eutectogel enabled excellent long-term stability, the device after 50 days of ambient storage demonstrated well-maintained capacitance of \u0026gt;\u0026thinsp;60%, proving its potential in practical applications.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eMoreover, the impact of LS content on supercapacitor performance was investigated. EIS characterizations indicated that, increasing the LS from 1 wt% to 5 wt% promoted both ionic transport and interfacial charge transfer, promising enhanced capacitance (Figure S7a). Further elevated LS content to 20 wt% lowered the internal ion conductivity, but the diffusion impedance was maintained comparable to the 5%LS-PDES. GCD measurements further verified that the LS loading of 5\u0026ndash;20 wt% could allow supercapacitors with similar discharge times, which were at least 2 times higher than that with the 1%LS-PDES (Figure S7b). The 20%LS-PDES could achieve a specific capacity of ~\u0026thinsp;40 mF∙cm\u003csup\u003e-2\u003c/sup\u003e at 1.25 mA∙cm\u003csup\u003e-2\u003c/sup\u003e, a value comparable to previous AC-based hydrogel supercapacitors.\u003csup\u003e[\u003cspan citationid=\"CR51\" class=\"CitationRef\"\u003e51\u003c/span\u003e, \u003cspan citationid=\"CR59\" class=\"CitationRef\"\u003e59\u003c/span\u003e]\u003c/sup\u003e\u003c/p\u003e\u003cp\u003eAnother interesting feature of the LS-PDES eutectogel electrolyte could be the numerous hydrogen bonds for tight binding with water molecules inside the networks, thus we hypothesized that it may allow high output voltage surpassing the water decomposition limitation in hydrogel-based supercapacitors.\u003csup\u003e[\u003cspan citationid=\"CR60\" class=\"CitationRef\"\u003e60\u003c/span\u003e]\u003c/sup\u003e The wider electrochemical window to 2.0 V was demonstrated using LiTFSI-doped PEDOT:PSS electrodes, which showed slight current increase above 1.7 V in the CV curve as seen from Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ec inset. GCD measurements in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ec also verified the output voltage could reach 1.8 V at a current density down to 0.1 mA∙cm\u003csup\u003e-2\u003c/sup\u003e. The specific capacity of the 1.8-V supercapacitor, calculated from GCD curves, was 13.5 mF∙cm\u003csup\u003e-2\u003c/sup\u003e at the current density of 0.1 mA∙cm\u003csup\u003e-2\u003c/sup\u003e.\u003c/p\u003e\u003cp\u003eMechanical stability of this gel-based flexible device was further evaluated. The CV curves were recorded under 90\u0026deg; and 180\u0026deg; bending, as well as under external pressure, and they retained good symmetry with slight variation to the flat device (Figure S7c), demonstrating excellent stability and resilience under forces. More impressively, the tough LS-PDES eutectogels also succeeded in impact protection tests, in which a glass slide covered with the LS-PDES thin film (~\u0026thinsp;1 mm in thickness) effectively resisted impact by a 200 g weight from 20 cm height (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ed), corresponding to an impact energy of 0.4 J and velocity of 2 m s\u003csup\u003e-1\u003c/sup\u003e. In contrast, glass coated with PDES shattered severely upon impact. Hence, 100 cycles of mechanical impact testing were further applied on the flexible supercapacitor based on LS-PDES (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ee), in which the CV profiles also exhibited negligible degradation. The abovementioned results highlight the role of the high-LS-density PDES tough networks in establishing mechanically robust soft devices to withstand diverse external forces in complicated real-world wearable scenarios.\u003c/p\u003e\u003cp\u003eTo prove the wearable potential of LS-PDES, a proof-of-concept integrated system was constructed with the flexible supercapacitor acting as the power source for an LS-PDES gel sensor (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ef). The strain sensing performance of the LS-PDES was first examined under the strain range of 10%-300%, yielding increasing electric resistance with a nice linear correlation between the ΔR/R\u003csub\u003e0\u003c/sub\u003e and the strain (R\u003csup\u003e2\u003c/sup\u003e\u0026thinsp;\u0026gt;\u0026thinsp;0.99, Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003eg). Then the gel sensor was attached to a finger followed by recording the current response via chronoamperometry under the power supply of the charged supercapacitor attached to human body. The measurements showed current decrease of several to \u0026gt;\u0026thinsp;10 \u0026micro;A in response to various finger bending angles in real time, in accordance with the strain-induced elevation in the gel resistance. Therefore, the rapid and in-situ generation of LS-PDES ion conductors provides a straightforward approach to prototyping of self-powered soft sensing systems at low time and material cost, with promising potentials in further realizing closed-loop e-waste disposal.\u003csup\u003e[\u003cspan citationid=\"CR61\" class=\"CitationRef\"\u003e61\u003c/span\u003e]\u003c/sup\u003e\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec7\" class=\"Section2\"\u003e\u003ch2\u003e2.5 Printing LS-PDES for Miniaturized Stretchable OECT Arrays\u003c/h2\u003e\u003cp\u003eMore importantly, since the in-air gelation of LS-PDES permits ambient writing of ion conductors, it also facilitates the production of miniaturized soft device arrays on stretchable substrates. Therefore, we demonstrated the fabrication of skin-like elastic OECT arrays based on the direct-write patterns of LS-PDES gel electrolyte in combination with PEDOT:PSS, which served as both the electrodes and active channels (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea).\u003csup\u003e[\u003cspan citationid=\"CR62\" class=\"CitationRef\"\u003e62\u003c/span\u003e]\u003c/sup\u003e First, LiTFSI-doped PEDOT:PSS and LS-PDES line arrays having 1\u0026ndash;2 mm width were sequentially produced onto the PDMS surface via selective dewetting\u003csup\u003e[\u003cspan citationid=\"CR62\" class=\"CitationRef\"\u003e62\u003c/span\u003e]\u003c/sup\u003e or brush pen writing. To establish a crossbar configuration, the LS-PDES patterns were overlapped with the PEDOT:PSS/LiTFSI lines in a perpendicular manner to form a 3\u0026times;3 array, in which the PEDOT:PSS regions in contact with the LS-PDES electrolyte constituted the active channels (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eb). Subsequently, when a AgCl/Ag gate was in touch with the electrolyte to apply a positive bias to 1.5 V, the dedoping induced by cation insertion from the LS-PDES into the channel areas resulted in decreased PEDOT:PSS channel current. As seen from Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ec, the PEDOT:PSS line in the middle row of the array exhibited remarkably decline in the drain current (I\u003csub\u003eD\u003c/sub\u003e) from \u0026gt;\u0026thinsp;0.2 mA to 10\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e \u0026minus;\u0026thinsp;10\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e mA levels via gating from three LS-PDES gel lines respectively, demonstrating the typical depletion-mode OECT characteristics with the ON/OFF ratio up to 100. All the 9 channels at the crossing areas of the 3\u0026times;3 array succeeded in transistor switching performance, with the transconductance (Gm) ranging from ~\u0026thinsp;0.4 to ~\u0026thinsp;1 mS (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ed). The highest normalized Gm was estimated as ~\u0026thinsp;20 S∙cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, comparable to previously reported all-solid-state PEDOT:PSS OECTs.\u003csup\u003e[\u003cspan citationid=\"CR63\" class=\"CitationRef\"\u003e63\u003c/span\u003e]\u003c/sup\u003e The left column of the LS-PDES electrolyte contributed higher Gm than the others, possibly ascribed to the variation in ion conductance among the gel arrays. Furthermore, the OECT could be scaled down by exploiting a PEDOT:PSS microfiber with ~\u0026thinsp;400-\u0026micro;m diameter\u003csup\u003e[\u003cspan citationid=\"CR64\" class=\"CitationRef\"\u003e64\u003c/span\u003e]\u003c/sup\u003e in contact with a Ag wire covered with a thin layer of LS-PDES electrolyte. As seen from Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ee, such fiber-type OECT also presented outstanding transfer characteristics with the ON/OFF ratio of \u0026gt;\u0026thinsp;100 and Gm value close to 0.35 mS. This simple strategy for producing ion conductor and transistor arrays at the microscale could further facilitate the high-throughput screening of ionic circuits, channel/electrolyte interfaces or artificial sensory networks.\u003csup\u003e[\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e, \u003cspan citationid=\"CR65\" class=\"CitationRef\"\u003e65\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR66\" class=\"CitationRef\"\u003e66\u003c/span\u003e]\u003c/sup\u003e\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eKnowing that the LS-PDES could maintain its ion conduction in a wide strain and temperature ranges, we further demonstrated OECTs that could operate under deformed and extreme conditions. First, the transfer curves of one PEDOT:PSS/LS-PDES OECT were measured under tensile strains along the gel direction to 40% (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ef). The stretched device maintained the electronic performance with slightly increased OFF current and reduced Gm from ~\u0026thinsp;2 mS to ~\u0026thinsp;1 mS, which could be resulted from the change in the channel dimensions as well as increased ion resistance upon elongation. Furthermore, the all-solid-state OECT was applied repeated strains of 30% for 100 cycles. Again, the device after cyclic deformation could still reserve its high ON/OFF ratio of close to 100, while maintaining\u0026thinsp;~\u0026thinsp;50% of the Gm value (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eg). OECT transfer characteristics were also examined by varying the temperature. From \u0026minus;\u0026thinsp;40\u0026deg;C to 40\u0026deg;C, both the initial I\u003csub\u003eD\u003c/sub\u003e at the ON state and the OFF current gradually increased with the temperature, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eh. Hence the ON/OFF ratio was maintained as \u0026gt;\u0026thinsp;100, meanwhile higher Gm was found with the elevating temperature. At the temperature range above 40\u0026deg;C, the shift of the V\u003csub\u003eG\u003c/sub\u003e for the maximum Gm to higher bias indicated the diminished gating effect, and a significant drop in the ON/OFF ratio and Gm was seen at 80\u0026deg;C (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ei), which may be attributed to higher ion injection barrier at the channel interface. Despite, these results suggested excellent temperature resilience of the LS-PDES-based all-solid-state OECTs as well as potential artificial synapse and neural network applications over a wide temperature window.\u003csup\u003e[\u003cspan citationid=\"CR67\" class=\"CitationRef\"\u003e67\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e]\u003c/sup\u003e\u003c/p\u003e\u003c/div\u003e"},{"header":"3. Conclusion","content":"\u003cp\u003eIn summary, this work pioneers a rapid ambient-air polymerizable eutectogel platform integrating LS (up to 20 wt%) with quaternary ammonium-based deep eutectic monomers for producing soft devices across multi-scales. The resulting LS-PDES ion-conducting eutectogels exhibit exceptional environmental adaptability across broad temperature ranges, maintaining its mechanical softness down to -80\u0026deg;C and allowing the device performance from \u0026minus;\u0026thinsp;40\u0026deg;C to 80\u0026deg;C. The high-density LS interconnected with cationic PDES matrix are demonstrated to synergistically enhance the mechanical strength (\u0026gt;\u0026thinsp;1 MPa) and toughness (up to 4.5 MJ∙m\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e), and the interfacial adhesion as high as ~\u0026thinsp;160 kPa towards diverse surfaces, while affording excellent ion conduction (\u0026gt;\u0026thinsp;3 mS cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), photothermal conversion (ΔT\u0026thinsp;\u0026gt;\u0026thinsp;20\u0026deg;C within 1 min) and self-healing efficacy. This platform further enables rapid prototyping of flexible supercapacitors with high durability towards bending and impact, along with self-powered motion monitoring. Miniaturized soft OECT arrays are also facilitated by ambient writing of LS-PDES patterns, achieving stable performance under deformation and extreme condition tolerance. Leveraging the tailored chemistry of lignin and PDES, this versatile system offers a sustainable pathway toward multifunctional bio-derived materials compatible with high-resolution additive manufacturing or high-throughput material screening for soft ionotronics, bioelectronic interfaces, and neuromorphic computing hardware.\u003c/p\u003e"},{"header":"4. Experimental Section","content":"\u003cp\u003e\u003cem\u003eMaterials\u003c/em\u003e: [2-(methacryloyloxy)ethyl]trimethylammonium chloride (METAC, 75 wt.% in H\u003csub\u003e2\u003c/sub\u003eO), lactic acid (LA, 90%), aluminum chloride hexahydrate (AlCl\u003csub\u003e3\u003c/sub\u003e∙6H\u003csub\u003e2\u003c/sub\u003eO, 99%), sodium lignosulfonate (LS), ammonium persulfate (APS, 98%), N,N\u0026prime;-methylenebisacrylamide (MBA, 98%), poly(3,4‑ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS, PH1000), lithium bis(trifluoromethyl)sulfonimide (LiTFSI, 99.9%) were purchased from Shanghai Aladdin Biochemical Technology Co., Ltd. All chemicals are used as received. Ni foams and Ni foams coated with activated carbon (AC) were purchased from Canrd Technology Co. Ltd.\u003c/p\u003e\n\u003cp\u003e\u003cem\u003ePreparation and Characterization of LS-PDES Eutectogels\u003c/em\u003e: METAC and LA were mixed at molar ratios of 1:1 to 5:1, followed by the addition of an appropriate amount of AlCl\u003csub\u003e3\u003c/sub\u003e∙6H\u003csub\u003e2\u003c/sub\u003eO. The mixture was stirred in an oil bath at 80\u0026deg;C until a homogeneous and transparent polymerizable deep eutectic solvent (PDES) was obtained. Subsequently, LS (5\u0026ndash;20 wt%) and MBA crosslinker (1 mol% to METAC) were added to the PDES and stirred at 70\u0026deg;C until completely dissolved. APS aqueous solution was then added and stirred rigorously to obtain a final APS concentration of \u0026gt;\u0026thinsp;2 wt%. The resulting mixture was immediately poured into a pre-designed PTFE mold to conduct free-radical polymerization. The tensile properties of the as-obtained LS-PDES were evaluated using the dumbbell-shaped gel samples (20 mm \u0026times; 5 mm \u0026times; 2 mm) at a speed of 10 mm∙min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. Young\u0026rsquo;s modulus was calculated based on the slope of 5\u0026ndash;25% strain range. Compression tests were conducted using cylindrical samples with a diameter of 25 mm and a height of 5 mm, at a testing rate of 2 mm∙min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. Adhesion strength was measured using lap shear and 180\u0026deg; peeling tests. To test the shear stress, samples (25 mm \u0026times; 25 mm \u0026times; 2 mm) were adhered between two rectangular substrates, followed by stretching at a speed of 10 mm∙min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. In the peeling test, samples (150 mm \u0026times; 30 mm \u0026times; 2 mm) were adhered to the substrate surface, with the reverse side bonded to a PET film using cyanoacrylate adhesive. The peeling was performed at a speed of 10 mm∙min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. The interface toughness (J m\u003csup\u003e\u0026minus;\u003c/sup\u003e\u0026sup2;) was calculated as the ratio of the adhesion force to the sample width. The ion conductivity of the LS-PDES was evaluated using electrochemical impedance spectroscopy (EIS) with an electrochemical workstation (CHI660E, Shanghai Chenhua). The gel samples were encapsulated inside a coin cell, with the diameter of 15 mm and 1-mm thickness. EIS was conducted over a frequency range of 1 Hz to 10\u003csup\u003e6\u003c/sup\u003e Hz under varied temperature from \u0026minus;\u0026thinsp;40\u0026deg;C to 100\u0026deg;C. The ion conductivity was calculated using the following formula: \u0026sigma;= \u003cimg src=\"data:image/png;base64,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\" style=\"width: 25px;\"\u003e, where S and L are the cross-sectional area and thickness of the sample, and R is the serial resistance from EIS.\u003c/p\u003e\n\u003cp\u003e\u003cem\u003eMolecular Dynamics (MD) Simulation\u003c/em\u003e: 120 METAC, 20 LS, 40 LA, 40 Na⁺, 120 Cl⁻, and 500 water molecules were uniformly mixed. Force field parameters were assigned as follows: water molecules were modeled using the TIP3P model,\u003csup\u003e[\u003cspan class=\"CitationRef\"\u003e69\u003c/span\u003e]\u003c/sup\u003e while all other molecular species were parameterized with the GAFF2 force field.\u003csup\u003e[\u003cspan class=\"CitationRef\"\u003e70\u003c/span\u003e]\u003c/sup\u003e Topology and parameter files were generated using the Sobtop program.\u003csup\u003e[\u003cspan class=\"CitationRef\"\u003e71\u003c/span\u003e]\u003c/sup\u003e All MD simulations were carried out using GROMACS version 2019.6\u003csup\u003e[\u003cspan class=\"CitationRef\"\u003e72\u003c/span\u003e]\u003c/sup\u003e with a time step of 1 fs. The initial configuration was first subjected to energy minimization to remove unfavorable contacts, followed by a 50 ns production simulation in the NPT ensemble at 298.15 K and 1 bar. Temperature was controlled using the V-rescale thermostat, and pressure was maintained with the Berendsen barostat. Electrostatic interactions were treated using the particle mesh Ewald method, and van der Waals interactions were modeled with the 12\u0026ndash;6 Lennard\u0026ndash;Jones potential truncated at 1.2 nm. Lorentz\u0026ndash;Berthelot combining rules were applied for cross-interactions, and periodic boundary conditions were applied in all directions.\u003c/p\u003e\n\u003cp\u003e\u003cem\u003eFabrication of Flexible Supercapacitors\u003c/em\u003e: 1 wt% PEDOT:PSS was mixed with 2 wt% LiTFSI aqueous solution with rigorous stirring to obtain the conducting polymer ink. The LS-PDES precursor solution was drop-cast onto a Ni foam electrode (20 mm \u0026times; 20 mm) with an AC loading of ~\u0026thinsp;10 mg∙cm\u003csup\u003e-2\u003c/sup\u003e or PEDOT:PSS/LiTFSI loading of ~\u0026thinsp;2 mg∙cm\u003csup\u003e-2\u003c/sup\u003e, followed by uniform spreading across the surface. A second piece of electrode was then placed on top to form a sandwiched structure. The assembled device was left undisturbed for 10 min to complete the in-situ polymerization, yielding the flexible LS-PDES-based supercapacitor. Informed written consent was obtained from all participants in the wearable demonstrations prior to the research.\u003c/p\u003e\n\u003cp\u003e\u003cem\u003eFabrication of Stretchable OECT Arrays\u003c/em\u003e: PDMS substrate was plasma treated with a polyimide mask, followed by dewetting of the PEDOT:PSS/LiTFSI ink and 130\u0026deg;C annealing to produce the electrode patterns. Then the LS-PDES precursor containing 20 wt% LS was direct written by a brush pen onto the PEDOT:PSS patterns in the perpendicular direction to form a crossbar array. Finally, AgCl/Ag paste was applied to the end of the LS-PDES lines, serving as the gate electrode to accomplish the OECT arrays. To produce the fiber-based OECT, PEDOT:PSS microfiber (~\u0026thinsp;400 \u0026micro;m diameter) was prepared according to literature.\u003csup\u003e[\u003cspan class=\"CitationRef\"\u003e64\u003c/span\u003e]\u003c/sup\u003e Then a silver wire was dip-coated with the LS-PDES thin layer, followed by contacting with the microfiber for OECT gating. Transfer characteristics of the OECTs were measured through sweeping the gate bias from \u0026minus;\u0026thinsp;0.5 V to 1.5 V.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003ch2\u003eConflict of Interest\u003c/h2\u003e\u003cp\u003eZhuang Xie and Xinlong Li have filed a patent application on LS-PDES eutectogels.\u003c/p\u003e\u003c/p\u003e\u003ch2\u003eFunding:\u003c/h2\u003e\u003cp\u003eNatural Science Foundation of Guangdong Province (2024A1515010704), National Natural Science Foundation of China (Grant No. 22075325, 22475245)\u003c/p\u003e\u003cp\u003eKeywords: extreme environment adaptivity, lignosulfonate, polymerizable deep eutectic solvents, soft electronics, organic electrochemical transistor arrays\u003c/p\u003e\u003ch2\u003eAcknowledgements\u003c/h2\u003e\u003cp\u003eThe authors gratefully acknowledge the financial support from the Natural Science Foundation of Guangdong Province (2024A1515010704) and National Natural Science Foundation of China (Grant No. 22075325, 22475245). The authors would also like to thank Prof. Jiandong Yao at Sun Yat-sen University for assistance in infrared thermography and Prof. Yong Qian at South China University of Technology for helpful discussions.\u003c/p\u003e\u003ch2\u003eData Availability Statement\u003c/h2\u003e\u003cp\u003eThe data that support the findings of this study are available from the corresponding author upon reasonable request.\u003c/p\u003e\u003cp\u003eReceived: ((will be filled in by the editorial staff))\u003c/p\u003e\u003cp\u003eRevised: ((will be filled in by the editorial staff))\u003c/p\u003e\u003cp\u003ePublished online: ((will be filled in by the editorial staff))\u003c/p\u003e\n\u003ch2\u003eSupporting Information\u003c/h2\u003e\n\u003cp\u003eSupporting Information is available from the Wiley Online Library or from the author\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eZhao C, Park J, Root SE, Bao Z (2024) Nat Rev Bioeng 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Nevertheless, elevating the lignin loading usually sacrifice the performance, limiting their application potentials. Herein we develop a unique polymerizable deep eutectic solvent (PDES) consisting of a quaternary ammonium monomer and lactic acid to incorporate with high-density lignosulfonate (LS) of \u0026gt;\u0026thinsp;20 wt% and address the performance trade-offs. The lignin-induced self-catalytic polymerization associated with electrostatic assembly enables room temperature gelation as fast as \u0026lt;\u0026thinsp;5 min and ambient-air micropatterning. Remarkably, the anionic LS and polycationic matrix affording multiple non-covalent interactions drastically enhance the mechanical strength to \u0026gt;\u0026thinsp;1 MPa and versatile adhesion up to 160 kPa, meanwhile allowing self-healing and photothermal capabilities. Such LS-PDES eutectogels also permit intrinsic ion conduction (\u0026gt;\u0026thinsp;3 mS cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) and superior environmental adaptivity over \u0026minus;\u0026thinsp;80\u0026deg;C to 100\u0026deg;C. Thus, employing the in-situ polymerization between electrodes, rapid prototyping of bend-/impact-resistant flexible supercapacitors is demonstrated to power wearable sensors. More importantly, it facilitates the production of miniaturized soft organic electrochemical transistor (OECT) arrays, whose performance can be well maintained under deformed and extreme temperature conditions. This high-lignin-density eutectogel platform paves a straightforward route towards printed soft ionotronics, bioelectronic interfaces, and brain-inspired computing.\u003c/p\u003e","manuscriptTitle":"Polymerizable Deep Eutectic Solvents-Enabled High-Lignin-Density Networks for Rapid Multi-scale Fabrication of Multifunctional and Extreme Environment Adaptable Soft Devices","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-10-07 06:30:22","doi":"10.21203/rs.3.rs-7787557/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"44b34982-2198-4c47-881c-aafb1daa232f","owner":[],"postedDate":"October 7th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2025-10-07T06:30:22+00:00","versionOfRecord":[],"versionCreatedAt":"2025-10-07 06:30:22","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-7787557","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7787557","identity":"rs-7787557","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}