How do trees support their upright massive bodies? The support comes from the incredibly strong and stiff, and highly crystalline nanoscale fibrils of extended cellulose chains, called cellulose nanofibers. Cellulose nanofibers and their crystalline parts—cellulose nanocrystals, collectively nanocelluloses, are therefore the recent hot materials to incorporate in man‐made sustainable, environmentally sound, and mechanically strong materials. Nanocelluloses are generally obtained through a top‐down process, during or after which the original surface chemistry and interface interactions can be dramatically changed. Therefore, surface and interface engineering are extremely important when nanocellulosic materials with a bottom‐up process are fabricated. Herein, the main focus is on promising chemical modification and nonmodification approaches, aiming to prospect this hot topic from novel aspects, including nanocellulose‐, chemistry‐, and process‐oriented surface and interface engineering for advanced nanocellulosic materials. The reinforcement of nanocelluloses in some functional materials, such as structural materials, films, filaments, aerogels, and foams, is discussed, relating to tailored surface and/or interface engineering. Although some of the nanocellulosic products have already reached the industrial arena, it is hoped that more and more nanocellulose‐based products will become available in everyday life in the next few years.

A high-performance flexible supercapacitor electrode with a core–shell structure is successfully developed from cellulose nanocrystal (CNC)-stabilized carbon nanotubes (CNTs). By incorporating poly­(vinyl alcohol) (PVA) and poly­(acrylic acid) (PAA), a cross-linked nanofibrous membrane (CNT–CNC/PVA–PAA) is prepared as the core material via directional electrospinning, followed by a thermal treatment. The flexible supercapacitor electrodes are eventually fabricated via the in situ polymerization of polyaniline (PANI), which was used as the coating shell material, on the aligned electrospun nanofibers. By taking advantage of the thermally induced esterification cross-linking that occurs among PVA, PAA, and the CNT–CNC nanohybrids, the membranes present with enhanced water resistance, mechanical strength, and thermal stability. After the surface coating of the PANI shell, the optimized PANI@CNT–CNC/PVA–PAA nanofibrous membranes exhibit a large porosity, an enhanced specific surface area, a superior tensile strength of ∼54.8 MPa, and a favorable electroconductivity of ∼0.44 S m–1. As expected, the nanofibrous electrodes with a specific capacitance of 164.6 F g–1 can maintain 91% of the original capacitance after 2000 cycles. The symmetrical solid-state supercapacitor assembled by the nanofibrous electrodes shows an excellent capacitance of 155.5 F g–1 and a remarkable capacitance retention of 92, 90, and 89% after 2000 cycles under flat, bending, and twisting deformations, respectively.

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Recently, with the development of personal wearable electronic devices, the demand for portable power is miniaturization and flexibility. Electro-conductive hydrogels (ECHs) are considered to have great application prospects in portable energy-storage devices. However, the synergistic properties of self-healability, viscoelasticity, and ideal electrochemistry are key problems. Herein, a novel ECH was synthesized by combining polyvinyl alcohol-borax (PVA) hydrogel matrix and 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-cellulose nanofibers (TOCNFs), carbon nanotubes (CNTs), and polyaniline (PANI). Among them, CNTs provided excellent electrical conductivity; TOCNFs acted as a dispersant to help CNTs form a stable suspension; PANI enhanced electrochemical performance by forming a “core-shell” structural composite. The freeze-standing composite hydrogel with a hierarchical 3D-network structure possessed the compression stress (~152 kPa) and storage modulus (~18.2 kPa). The composite hydrogel also possessed low density (~1.2 g cm−3), high water-content (~95%), excellent flexibility, self-healing capability, electrical conductivity (15.3 S m−1), and specific capacitance of 226.8 F g−1 at 0.4 A g−1. The fabricated solid-state all-in-one supercapacitor device remained capacitance retention (~90%) after 10 cutting/healing cycles and capacitance retention (~85%) after 1000 bending cycles. The novel ECH had potential applications in advanced personalized wearable electronic devices.

With the rapid development of soft electronics, flexible and stretchable strain sensors are highly desirable. However, coupling of high sensitivity and stretchability in a single strain sensor remains a challenge. Herein, a kind of conductive elastomer is constructed with poly-(dimethylsiloxane) (PDMS) and silylated cellulose nanocrystal (SCNC)/ carbon nanotube (CNT) nanohybrids through a facile one-pot solutioncasting method. The hydrophobic SCNCs can effectively facilitate the dispersion of CNTs in PDMS and synergistically improve the interfacial compatibility between CNTs and the PDMS matrix, resulting in favorable stress and electron transfer in the polymer network. Due to the outstanding electrical conductivity of CNTs and the excellent dispersity and high mechanical performance of SCNCs, combined with the good compatibility between SCNC-mediated carbon nanotubes (SCNC-CNTs) and PDMS, the resulting composite elastomer (SCNC-CNT/PDMS) shows high electrical conductivity (∼2.77 S m −1 ), tensile strength (∼5.72 MPa), and fatigue resistance properties. The strain sensor assembled by SCNC-CNT/PDMS demonstrates a high strain range above 100%, appealing strain sensitivity with a gauge factor of 37.11 at 50−100% strain, and long-term stability and durability, which is capable of monitoring both real-time human motions and acoustic vibrations. This work paves a new way for the design and controllable preparation of flexible and stretchable conductive elastomers, demonstrating promising applications in wearable devices and intelligent electronics.

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In this study, cellulose nanofibrils (CNFs) were successfully isolated from coconut palm petiole residues falling off naturally with chemical pretreatments and mechanical treatments by a grinder and a homogenizor. FTIR spectra analysis showed that most of hemicellulose and lignin were removed from the fiber after chemical pretreatments. The compositions of CNFS indicated that high purity of nanofibrils with cellulose contain more than 95% was obtained. X-ray diffractogram demonstrated that chemical pretreatments significantly increased the crystallinity of CNFs from 38.00% to 70.36%; however, 10-15 times of grinding operation followed by homogenizing treatment after the chemical pretreatments did not significantly improve the crystallinity of CNFs. On the contrary, further grinding operation could destroy crystalline regions of the cellulose. SEM image indicated that high quality of CNFs could be isolated from coconut palm petiole residues with chemical treatments in combination of 15 times of grinding followed by 10 times of homogenization and the aspect ratio of the obtained CNFs ranged from 320 to 640. The result of TGA-DTG revealed that the chemical-mechanical treatments improved thermal stability of fiber samples, and the CNFs with 15 grinding passing times had the best thermal stability. This work suggests that the CNFs can be successfully extracted from coconut palm petiole residues and it may be a potential feedstock for nanofiber reinforced composites due to its high aspect ratio and crystallinity.

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