Regulating the pore structure and heteroatom doping of soybean straw carbon based on a bifunctional template method for the high-performance carbon supercapacitor.

The previous research addressed the waste problem of agriculture and forestry residues by exploring the efficient utilization of liquefied soybean straw in supercapacitor. The structures of the liquefied soybean straw were controlled by coupling microwave hydrothermal treatment with carbonization under the influence of a C3N4 bifunctional template. What's more, C3N4 could effectively regulate the pore structures and provide an effective N active site of carbon materials C3N4. The obtained N-SLR Carbon-700 possess a specific surface area of up to 1593.7 m2 g-1, and the pore size is mainly concentrated in the range of 1.8-2.5 nm, providing efficient ions transmission channels and storage space. Its specific capacitance is up to 261.5F g-1 (current density of 0.5A g-1), and the capacity retention is 74.04% when the current density is expanded by 20 times. In the two-electrode system, the energy density of N-SLR Carbon-700 could reach to 31.3 W h kg-1 at a power density of 360 W kg-1, as well as the energy surface density is maintained at 69% when the power density is increased by a factor of 20. This work enhances effectively the charging and discharging stability and capacitance value of carbon-based supercapacitor.

Multi-Functional Repair and Long-Term Preservation of Paper Relics by Nano-MgO with Aminosilaned Bacterial Cellulose.

Paper relics, as carrieres of historical civilization's records and inheritance, could be severely acidic and brittle over time. In this study, the multi-functional dispersion of nanometer magnesium oxide (MgO) carried by 3-aminopropyl triethoxysilane-modified bacterial cellulose (KH550-BC) was applied in the impregnation process to repair aged paper, aiming at solving the key problems of anti-acid and strength recovery in the protection of ancient books. The KH550-BC/MgO treatment demonstrated enhanced functional efficacy in repairing aged paper, attributed to the homogeneous and stable distribution of MgO within the nanofibers of BC networks, with minimal impact on the paper's wettability and color. Furthermore, the treatment facilitated the formation of adequate alkali reserves and hydrogen bonding, resulting in superior anti-aging properties in the treated paper during prolonged preservation. Even after 30 days of hygrothermal aging tests, the paper repaired by KH550-BC/MgO was still in a gently alkaline environment (pH was about 7.56), alongside a 32.18% elevation compared to the untreated paper regarding the tear index. The results of this work indicate that KH550-BC/MgO is an effective reinforcement material for improving the long-term restoration of ancient books.

Anionic Hofmeister Effect Regulated Conductivity in Polyelectrolyte Hydrogels for High-Performance Supercapacitor.

The Hofmeister effect not only affects the stability and solubility of protein colloids but also has specific effects on the polymer molecules. Here, the impact of the Hofmeister effect on the electrochemical properties of polyelectrolyte hydrogels at room temperature and subzero temperature studied for the first time. Polyelectrolyte hydrogels exhibit an anti-polyelectrolyte effect in low concentrations of ammonium salt, while they exhibit an obvious Hofmeister effect in high concentrations of ammonium salt. Kosmotropic ions demonstrate strong interaction with water molecules or polymer chains, resulting in the reduction of conductivity of polyelectrolyte hydrogels. However, chaotropic ions exhibit weak interactions with water molecules or molecular chains, leading to an increase in conductivity. The Hofmeister effect has a more significant effect on the polyzwitterion electrolyte. The conductivity of polyzwitterion hydrogel soaked in chaotropic ion is up to 6.2 mS cm-1 at -40 °C. The supercapacitor assembled by polyzwitterion electrolytes maintains a capacitance retention rate of 85% and ≈100% coulomb efficiency after 15 000 cycles at -40 °C. This study elucidates the influence of the Hofmeister effect on conductivity in polyelectrolytes and expands the regulatory approach for improving the performance of energy storage devices.

Advances in the preparation and application of cellulose-based antimicrobial materials: A review.

The rise of polymer materials in modern life has drawn attention to renewable, easily biodegradable, environmentally-friendly bio-based polymers. Notably, significant research has been dedicated to creating green antimicrobial functional materials for the biomedical field using natural polymer materials. Cellulose is a rich natural biomass organic polymer material. Given its favorable attributes like film-forming capability, biodegradability, and biocompatibility, it is extensively employed to tackle a wide range of challenges confronting humanity today. However, its inherent drawbacks, such as insolubility in water and most organic solvents, hygroscopic nature, difficulty in melting, and limited antimicrobial properties, continue to pose challenges for realizing the high-value applications of cellulose. Achieving multifunctionality and more efficient application of cellulose still poses major challenges. In this regard, the current development status of cellulose materials was reviewed, covering the classification, preparation methods, and application status of cellulose-based antimicrobial materials. The application value of cellulose-based antimicrobial materials in biomedicine, textiles, food packaging, cosmetics and wastewater treatment was summarised. Finally, insights were provided into the developing prospects of cellulose-based antimicrobial materials were provided.

Improvement of interface bonding of bacterial cellulose reinforced aged paper by amino-silanization.

The aging of paper seriously threatens the service life of cultural heritage documents. Bacterial cellulose (BC), which has a good fiber aspect ratio and is rich in hydroxyl groups, is suitable for strengthening aged paper. However, a single BC added was not ideal for paper restoration, since only strengthening was not able to resist the persistent acidification of ancient book. In this work, BC was functionalized by 3-aminopropyltriethoxysilane (APTES) to develop the interface bonding with aged paper. Fourier transform infrared (FTIR), X-ray diffraction (XRD), nuclear magnetic resonance (NMR) and elemental analysis identified the successful amino-silanization of BC. The modification parameters were optimized as the concentration of APTES of 5 wt%, the reaction time of 4 h, and the reaction temperature of 80 °C based on a considerable improvement in the strength properties without obvious appearance impact on reinforced papers. Moreover, the pH value of the repaired paper was achieved at 8.03, ensuring the stability of the anti-aging effect. The results confirmed that APTES-BC had great potential applications in ancient books conservation.

Highly conductive, rapid self-healing, and anti-freezing poly(3,4-ethylenedioxythiophene)/lignosulfonate-cationic guar gum ionogels for multifunctional sensors.

Soft ionic conductors exhibit immense potential for applications in soft ionotronics, including ionic skin, human-machine interface, and soft luminescent device. Nevertheless, the majority of ionogel-based soft ionic conductors are plagued by issues such as freezing, evaporation, liquid leakage, and inadequate self-healing capabilities, thereby constraining their usability in complex environments. In this study, we present a novel strategy for fabricating conductive ionogels through the proportionally mixing cationic guar gum (CGG), water, 1-butyl-3-methylimidazolium chloride (BmimCl)/glycerol eutectic-based ionic liquid, and poly(3,4-ethylenedioxythiophene)/lignosulfonate (PEDOT/LS). The resultant benefits from strong hydrogen bonding and electrostatic interactions among its constituents, endowing it with an ultrafast self-healing capability (merely 30 s) while sustaining high electrical conductivity (~16.5 mS cm-1). Moreover, it demonstrates exceptional water retention (62 % over 10 days), wide temperature tolerance (-20 to 60 °C), and injectability. A wearable sensor fabricated from this ionogel displayed remarkable sensitivity (gauge factor = 17.75) and a rapid response to variations in strain, pressure, and temperature, coupled with both long-term stability and wide working temperature range. These attributes underscore its potential for applications in healthcare devices and flexible electronics.

Transparent, super stretchable, freezing-tolerant, self-healing ionic conductive cellulose based eutectogel for multi-functional sensors.

In this study, we propose a non - toxic and low-cost fabrication of cellulose-based eutectogel through the ZnCl2/H2O/H3PO4 deep eutectic solvent (DES) to dissolve cellulose followed by free-radical polymerization of acrylamide. Particularly, the introduction of cellulose enhances the mechanical properties of eutectogels while eliminating the environmental concerns of the traditional nanocellulose fabrication process. Owing to the dynamic transfer of ions in the eutectogel network, the prepared eutectogels exhibit adjustable conductivity (0.9- 1.37 Sm-1, 15 °C) and stretching sensitivity (Gauge factor = 5.4). The resulting DES - cellulose-based eutectogels (DCEs) exhibited ultra stretchability (4086 %), high toughness (261.3 MJ/m3), excellent ionic conductivity (1.64 Sm-1, 20 °C), high transparency (>85 %), outstanding antifreezing performance (<-80 °C), and other comprehensive characteristics. The DCEs had been proven to have multiple sensitivities to external stimuli, like temperature, strain, and pressure. As a result, the DCEs can be assembled into multifunctional sensors. Moreover, this work also demonstrated the satisfactory performance of DCEs in flexible electroluminescent devices. The low cost and high efficiency made the preparation method of this experiment an efficient strategy for developing high-performance cellulose-based eutectogels, which would greatly promote the application of such materials in areas such as artificial skin for soft robots and other wearable devices.

Preparation of Environmentally Friendly Oil- and Water-Resistant Paper Using Holo-Lignocellulosic Nanofibril (LCNF)-Based Composite Coating.

In the present study, an environmentally friendly oil- and water-resistant paper was developed using a holo-lignocellulosic nanofibril (LCNF)-based composite coating. The LCNF was prepared from wheat straw using a biomechanical method. Characterizations of oil- and water-resistant coated paper and the effect of LCNF content on the performance of the coated paper were confirmed by combining contact angle analysis, Cobb 300s, and mechanical performance tests. The results show that the barrier performance and mechanical strength of the coated paper were greatly improved with the increase of LCNF content. The contact angle of oil and water of coated paper containing 50% LCNF were 69° and 78°, respectively, while the contact angle of oil and water of the base paper were only 30° and 20°, respectively. Cobb 300s values reduced from 110 g/m2 to 30 g/m2 when the LCNF content increased from 50% to 90%. Moreover, under the coating amount of 20 g/m2, the tensile strength of the coating paper was 0.980 KN/m, an increase of 10.11% compared with the base paper. The bursting strength reached 701.930 KPa, which was 10.75% higher than the base paper. In short, it is feasible to prepare LCNF from wheat straw, and apply it to produce water-proof and oil-proof paper. The water-proof and oil-proof paper developed in this study not only offers a novel approach to addressing white pollution but also presents a new research avenue for exploring the potential applications of agricultural waste.

Biodegradable, Strong, and Hydrophobic Regenerated Cellulose Films Enriched with Esterified Lignin Nanoparticles.

The scientific community is pursuing significant efforts worldwide to develop environmentally viable film materials from biomass, particularly transparent, high-performance regenerated cellulose (RC) films, to replace traditional plastics. However, the inferior mechanical performance and hydrophilic nature of RC films are generally not suitable for use as a substitute for plastics in practical applications. Herein, lignin homogenization is used to synthesize high-performance composite films. The esterified lignin nanoparticles (ELNPs) with dispersible and binding advantages are prepared through esterification and nanometrization. In the presence of ELNPs, RC films exhibit a higher tensile strength (110.4 MPa), hydrophobic nature (103.6° water contact angle, 36.6% water absorption at 120 min, and 1.127 × 10-12 g cm cm-2 s-1 Pa-1 water vapor permeability), and exciting optical properties (high visible and low ultraviolet transmittance). The films further display antioxidant activity, oxygen barrier ability, and thermostability. The films completely biodegrade at 12 and 30% soil moisture. Overall, this study offers new insights into lignin valorization and regenerated cellulose composite films as novel bioplastic materials.

Characterization of microcrystalline cellulose prepared from long and short fibers and its application in ibuprofen tablets.

As a bio-based material, microcrystalline cellulose (MCC) has been applied in many fields including pharmaceuticals, foods, and cosmetics in recent years. However, traditional preparation methods of MCC are facing many challenges due to economic and eco-environmental issues. In this study, softwood dissolved pulp was sieved to long fiber (LF) and short fiber (SF), and subsequently to prepare LF-MCC and SF-MCC by hydrochloric acid hydrolysis at different acid dosages (3-7 wt%), reaction times (30-90 min), and temperatures (75-95 °C). The as-obtained MCC products were compared in terms of morphology, size, crystallinity, and chemical structure. The results indicated that the crystallinity and yield of LF-MCC were high, with maximum values of 78.41 % and 98.68 %, respectively. The particle size distribution of SF-MCC was more uniform in the range of 20-80 µm, with a maximum of 59.44 % at 20-80 µm occupancy proportion. Moreover, SF-MCC had a typical rod-like shape and larger surface area as well as better thermal behavior than LF-MCC. When LF-MCC and SF-MCC were used as fillers in the production of ibuprofen tablets, the tablets added with LF-MCC exhibited higher hardness, friability, dissolution rate, and shorter disintegration time. Therefore, this work is very beneficial for the preparation and application of MCC.

Production of Lignin-Derived Functional Material for Efficient Electromagnetic Wave Absorption with an Ultralow Filler Ratio.

Industrial lignin, a by-product of pulping for papermaking fibers or of second-generation ethanol production, is primarily served as a low-grade combustible energy source. The fabrication of high-value-added functional materials with industrial lignin is still a challenge. Herein, a three-dimensional hierarchical lignin-derived porous carbon (HLPC) was prepared with lignosulfonate as the carbon source and MgCO3 as the template. The uniform mixing of precursor and template agent resulted in the construction of a three-dimensional hierarchical porous structure. HLPC presented excellent electromagnetic wave (EMW) absorption performance. With a low filler content of 7 wt%, HLPC showed a minimum reflection loss (RL) value of -41.8 dB (1.7 mm, 13.8 GHz), and a maximum effective absorption bandwidth (EAB) of 4.53 GHz (1.6 mm). In addition, the enhancement mechanism of HLPC for EMW absorption was also explored through comparing the morphology and electromagnetic parameters of lignin-derived carbon (LC) and lignin-derived porous carbon (LPC). The three-dimensional hierarchical porous structure endowed the carbon with a high pore volume, resulting in an abundant gas-solid interface between air and carbon for interfacial polarization. This structure also provided conductive networks for conduction loss. This work offers a strategy to synthesize biomass-based carbon for high-performance EMW absorption.

Lignocellulosic biomass pretreatment with a lignin stabilization strategy and valorization toward multipurpose fractionation.

Lignocellulosic biomass has emerged as a promising alternative with sustainable advantages for the production of a wide range of renewable products and value-added chemicals. In this study, a pretreatment strategy that use a fully recyclable acid hydrotrope (p-TsOH aqueous solution) to extract lignin and employ glyoxylic acid (GA) to stabilize lignin was proposed for biomass valorization toward multipurpose fractionation. 83.0 % of lignin was dissolved out by p-TsOH hydrotrope (80 wt%) with GA addition to form GA-stabilized product at 80 o C for 15 min. The stabilized lignin was subsequently used as an additive in the preparation of lignin-based suncream. Notably, the incorporation of 4 wt% lignin nanospheres into an SPF15 sunscreen yielded a measured SPF of 59.94. Furthermore, the depolymerization of uncondensed lignin into aromatic monomers yielded a high lignin-oil yield of 84.2 %. Additionally, direct heating of the pretreatment liquor facilitated the conversion of monosaccharides into furfural, achieving a desired yield of 53.7 % without the addition of any acid catalyst. The pretreatment also enhanced the enzymatic hydrolysis of glucan, resulting in a saccharification yield of 98.4 %. Moreover, short-term ultrasonication of the pretreated substrate yielded pulp suitable for papermaking. Incorporating 15 wt% fibers into the produced paper sheets led to a 5.3 % increase in tear index and a 25.4 % increase in tensile index. This study presents a viable pretreatment strategy for the multipurpose fractionation of lignocellulosic biomass, offering potential avenues for biomass valorization.

Enhancing photocatalytic destruction of lignin via cellulose derived carbon quantum dots/g-C3N4 heterojunctions.

Lignocellulosic biomass exhibits a promising potential for production of carbon materials. Nitrogen and phosphorus co-doped carbon quantum dots (N,P-CQDs) were fabricated via (NH4)2HPO4 assisted hydrothermal treatment of cellulose pulp fibers. The as-prepared N,P-CQDs were characterized by HRTEM, FTIR, fluorescence and UV-vis, and then incorporated into g-C3N4 (CN) through sonication and liquid deposition, forming N,P-CQDs/sonication treated g-C3N4 (C-SCN) composites, which were then explored as photocatalysts. The photocatalytic ability of C-SCN towards model lignin was further analyzed. The results showed that, the fluorescence intensity and photoluminescence performance of N,P-CQDs were much higher than that of CQDs; the heterojunction was successfully constructed between the composites of N,P-CQDs and SCN; the incorporation of N,P-CQDs enhanced the visible light absorption, but reduced the band gap of the composite heterojunction; the resultant photocatalysts exhibited a good photocatalytic ability of model lignin via catalyze the fracture of ß-O-4' ether bond and CC bond, i.e., the photocatalytic degradation ratio reached up to 95.5 %; and the photocatalytic reaction generated some valuable organics such as phenyl formate, benzaldehyde, and benzoic acid. This study would promote the high value-added utilization of lignocellulosic resources especially in the transformation of lignin, conforming the concept of sustainable development.

Schiff base and coordinate bonds cross-linked chitosan-based eutectogels with ultrafast self-healing, self-adhesive, and anti-freezing capabilities for motion detection.

Ion conductors offer great potential for diverse electric applications. However, most of the ion conductors were fabricated from non - degradable petroleum-based polymers with non or low biodegradability, which inevitably leads to resource depletion and waste accumulation. Fabricating ion conductors based on renewable, and sustainable materials is highly desirable and valuable. Herein, a series of eutectogels were designed through dual-dynamic-bond cross-linking among ferric iron (Fe3+), protocatechualdehyde (PA), and chitosan (CS) in 1 - allyl-3 - methylimidazole chloride ionic liquid/urea (AmimCl/urea) eutectic-based ionic liquid. Due to the presence of AmimCl/urea eutectic-based ionic liquid, the obtained CS - PA@Fe eutectogels showed excellent ionic conductivity, superior anti-freezing properties that could maintain flexibility and high electrical properties at -20 °C. Dual-dynamic-bond cross-linking of catechol-Fe coordinate and dynamic Schiff base bonds equip CS - PA@Fe eutectogels with excellent injectable, and self-healing abilities. Additionally, due to the presence of phenolic hydroxyl groups of PA, the obtained CS - PA@Fe eutectogels present good adhesiveness. Based on the CS - PA@Fe eutectogels, multifunctional flexible strain sensors with high sensitivity, stability, as well as rapid response speed at wide operating temperature ranges were successfully fabricated. Thus, this study offers a promising strategy for fabricating naturally occurring biopolymers based eutectogels, which show great potential as high-performance flexible strain sensors for next-generation wearable electronic devices.

Recent advances in sustainable preparation of cellulose nanocrystals via solid acid hydrolysis: A mini-review.

As a green and renewable nanomaterial, cellulose nanocrystals (CNC) have received numerous attention due to the unique structural features and superior physicochemical properties. Conventionally, CNC was isolated from lignocellulosic biomass mostly depending on sulfuric or hydrochloric acid hydrolysis. Although this approach is effective, some critical issues such as severe equipment corrosion, excessive cellulose degradation, serious environmental pollution, and large water usage are inevitable. Fortunately, solid acid hydrolysis is emerging as an economical and sustainable CNC production technique and has achieved considerable progress in recent years. Herein, the preparation of CNC by solid acid hydrolysis was summarized systematically, including organic solid acids (citric, maleic, oxalic, tartaric, p-toluenesulfonic acid) and inorganic solid acids (phosphotungstic, phosphoric, and Lewis acid). The advantages and disadvantages of organic and inorganic solid acid hydrolysis methods were evaluated comprehensively. Finally, the challenges and opportunities in the later exploitation and application of solid acid hydrolysis to prepare CNC in the industrial context are discussed. Considering the future development of this technology in the large-scale CNC production, much more efforts should be made in lowering CNC processing cost, fabricating high-solid-content and re-dispersible CNC, developing value-added applications of CNC, and techno-economic analysis and life cycle assessment on the whole process.

Super-stretching and high-performance ionic thermoelectric hydrogels based on carboxylated bacterial cellulose coordination for self-powered sensors.

Self-powered sensors that do not require external power sources are crucial for next-generation wearable electronics. As environment-friendly ionic thermoelectric hydrogels can continuously convert the low-grade heat of human skin into electricity, they can be used in intelligent human-computer interaction applications. However, their low thermoelectric output power, cycling stability, and sensitivity limit their practical applications. This paper reports a 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-oxidized carboxylated bacterial cellulose (TOBC) coordination double-network ionic thermoelectric hydrogel with lithium bis(trifluoromethane) sulfonimide (LiTFSI) as an ion provider for thermodiffusion, as LiTFSI exhibits excellent thermoelectric properties with a maximum power output of up to 538 nW at a temperature difference of 20 K. The interactions between the ions and the hydrogel matrix promote the selective transport of conducting ionic ions, producing a high Seebeck coefficient of 11.53 mV K-1. Hydrogen bonding within the polyacrylamide (PAAm) network and interactions within the borate ester bond within the TOBC confer excellent mechanical properties to the hydrogel such that the stress value at a tensile deformation of 3100 % is reaches 0.85 MPa. The combination of the high ionic thermovoltage and excellent mechanical properties ionic thermoelectric hydrogels provides an effective solution for the design and application of self-powered sensors based on hydrogels.

Production of nanocellulose using acidic deep eutectic solvents based on choline chloride and carboxylic acids: A review.

Nowadays, nanocellulose production processes with numerous merits of green, eco-friendly, and cost-effective are in urgent need. Acidic deep eutectic solvent (ADES), as an emerging green solvent, has been widely applied in the preparation of nanocellulose over the past few years, owing to its unique advantages, including non-toxicity, low cost, easy synthesis, recyclability, and biodegradability. At present, several studies have explored the effectiveness of ADESs in nanocellulose production, particularly those based on choline chloride (ChCl) and carboxylic acids. Various acidic deep eutectic solvents have been employed, with representative ones such as ChCl-oxalic/lactic/formic/acetic/citric/maleic/levulinic/tartaric acid. Herein, we comprehensively reviewed the latest progress of these ADESs, focusing on the treatment procedures and key superiorities. In addition, the challenges and outlooks of ChCl/carboxylic acids-based DESs implementation in the fabrication of nanocellulose were discussed. Finally, some suggestions were proposed to advance the industrialization of nanocellulose, which would help for the roadmap of sustainable and large-scale production of nanocellulose.

Viscosity & SO2-sensitive dual colorimetric effect fluorescent sensor enabled imaging detection within plant onion and biological system.

The biological microenvironment includes important parameters such as viscosity, polarity, temperature, oxygen content and pH. In particular, abnormal cell viscosity is associated with the development of major diseases. Sulphur dioxide (SO2) serves not only as an essential atmospheric pollutant but also an influential signalling molecule in biological cells, predisposing individuals to increased respiratory disease. In this work, we designed and synthesized a novel fluorescent probe CouCN-V&S with dual response to micro environmental viscosity and SO2. The probe monitored viscosity and SO2 separately through dual emission channels with a difference of 135 nm. The probe responded sensitively to SO2 (<1s) and exhibited satisfactory immunity to interference and pH stability. The probe was successfully applied to imaging cellular, intra-zebrafish viscosity and SO2 changes. Interestingly, we took onion epidermal cells as model and explored the capability of probe CouCN-V&S to image SO2 in plant cells for the first time.

A morphology control engineered strategy of Ti3C2Tx/sulfated cellulose nanofibril composite film towards high-performance flexible supercapacitor electrode.

2D Ti3C2Tx MXene is an ideal material for fabricating supercapacitor electrodes due to its excellent physical-chemical properties. However, the inherent self-stacking, narrow interlayer spacing, and low general mechanical strength limit its application in flexible supercapacitors. Herein, facile structural engineering strategies by drying (vacuum drying, freeze drying, and spin drying) were proposed to fabricate 3D high-performance Ti3C2Tx/sulfated cellulose nanofibril (SCNF) self-supporting film supercapacitor electrodes. Compared with other composite films, the freeze-dried Ti3C2Tx/SCNF composite film exhibited a looser interlayer structure with more space which was conducive to charge storage and ion transport in the electrolyte. Therefore, the freeze-dried Ti3C2Tx/SCNF composite film exhibited a higher specific capacitance (220 F/g) compared to the vacuum-dried Ti3C2Tx/SCNF composite film (191 F/g) and the spin-dried Ti3C2Tx/SCNF composite film (211 F/g). After 5000 cycles, the capacitance retention rate of the freeze-dried Ti3C2Tx/SCNF film electrode was close to 100 %, showing excellent cycle performance. Meanwhile, the tensile strength of freeze-dried Ti3C2Tx/SCNF composite film (13.7 MPa) was much greater than that of the pure film (7.4 MPa). This work demonstrated a facile strategy for control of Ti3C2Tx/SCNF composite film interlayer structure by drying for fabricating well-designed structured flexible and free-standing supercapacitor electrodes.

Waterproof and ultrasensitive paper-based wearable strain/pressure sensor from carbon black/multilayer graphene/carboxymethyl cellulose composite.

Huge electronic wastes motivated the flourishing of biodegradable electrically conductive cellulosic paper-based functional materials as flexible wearable devices. However, the relatively low sensitivity and unstable output in combination with poor wet strength under high moisture circumstances impeded the practical application. Herein, a superhydrophobic cellulosic paper with ultrahigh sensitivity was proposed by innovatively employing ionic sodium carboxymethyl cellulose (CMC) as bridge to reinforce the interfacial interaction between carbon black (CB) and multilayer graphene (MG) and SiO2 nanoparticles as superhydrophobic layer. The resultant paper-based (PB) sensor displayed excellent strain sensing behaviors, wide working range (-1.0 %-1.0 %), ultrahigh sensitivity (gauge factor, GF = 70.2), and satisfied durability (>10,000 cycles). Moreover, the superhydrophobic surface offered well waterproof and self-cleaning properties, even stable running data without encapsulation under extremely high moisture conditions. Impressively, when the fabricated PB sensor was applied for electronic-skin (E-skin), the signal capture of spatial strain of E-skin upon bodily motion was breezily achieved. Thus, our work not only provides a new pathway for reinforcing the interfacial interaction of electrically conductive carbonaceous materials, but also promises a category of unprecedentedly superhydrophobic cellulosic paper-based strain sensors with ultra-sensitivity in human-machine interfaces field.