Conductive hydrogels are promising interface materials utilized in bioelectronics for human-machine interactions. However, the low-temperature induced freezing problem and water evaporation-induced structural failures have significantly hindered their practical applications. To address these problems, herein, an elaborately designed nanocomposite organohydrogel is fabricated by introducing highly conductive MXene nanosheets into a tannic acid-decorated cellulose nanofibrils/polyacrylamide hybrid gel network infiltrated with glycerol (Gly)/water binary solvent. Owing to the introduction of Gly, the as-prepared organohydrogel demonstrates an outstanding flexibility and electrical conductivity under a wide temperature spectrum (from −36 to 60 °C), and exhibits long-term stability in an open environment (>7 days). Additionally, the dynamic catechol-borate ester bonds, along with the readily formed hydrogen bonds between the water and Gly molecules, further endow the organohydrogel with excellent stretchability (≈1500% strain), high tissue adhesiveness, and self-healing properties. The favorable environmental stability and broad working strain range (≈500% strain); together with high sensitivity (gauge factor of 8.21) make this organohydrogel a promising candidate for both large and subtle motion monitoring.

Flexible and highly sensitive humidity sensors are crucial for humidity detection. In this study, a flexible cellulose nanofiber/carbon nanotube (NFC/CNT) humidity sensor with high sensitivity performance was developed via fast vacuum filtration. CNTs were well dispersed in water by using 2,2,6,6-tetramethylpiperidinyl-1-oxyl (TEMPO)-oxidized NFC as a dispersant. More importantly, NFC also acted as a humidity sensitive material, achieving superior performance of NFC/CNT humidity sensors. The obtained NFC/CNT humidity sensor with 5 wt % CNT loading exhibits outstanding sensitive performance, and its response value reaches a maximum of 69.9% (ΔI/I 0) at 95% relative humidity (RH). It also displays good bending resistance and long-term stability. In addition, the NFC/CNT humidity sensor was employed to monitor human breath. Therefore, we believe that the flexible, highly sensitive, and simply designed NFC/CNT humidity sensor is a promising candidate for various applications in the field of humidity measurement.

A superelastic aerogel with fast shape recovery performance from large compressive strain is highly desired for numerous applications such as thermal insulation in clothing, high-sensitive sensors, and oil contaminant removal. Fabrication of superelastic cellulose nanofibrils (CNF) aerogels is challenging as the CNF can assemble into non-elastic sheet-like cell walls. Here, a dual ice-templating assembly (DITA) strategy is proposed that can control the assembly of CNF into sub-micrometer fibers by extremely low temperature freezing (-196 °C), which can further assemble into an elastic aerogel with interconnected sub-micron fibers by freezer freezing (−20 °C) and freeze drying. The CNF aerogel from the DITA process demonstrates isotropic superelastic behavior that can recover from over 80% compressive strain along both longitudinal and cross-sectional directions, even in an extremely cold liquid nitrogen environment. The elastic CNF aerogel can be easily modified by chemical vapor deposition of organosilane, demonstrating superhydrophobicity (164° water contact angle), high liquid absorption (489 g g −1 of chloroform absorption capacity), self-cleaning, thermal insulating (0.023 W (mK) −1 ), and infrared shielding properties. This new DITA strategy provides a facile design of superelastic aerogels from bio-based nanomaterials, and the derived high performance multifunctional elastic aerogel is expected to be useful for a wide-range of applications.

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