Conductive hydrogels have been widely applied in human-computer interaction, tactile sensing, and sustainable green energy harvesting. Herein, a double cross-linked network composite hydrogel (MWCNTs/CNWs/PAM/SA) by constructing dual enhancers acting together with PAM/SA was constructed. By systematically optimizing the compositions, the hydrogel displayed features advantages of good mechanical adaptability, high conductivity sensitivity (GF = 5.65, 53 ms), low hysteresis (<11 %), and shape memory of water molecules and temperature. The nanocellulose crystals (CNWs) were bent and entangled with the backbone of the polyacrylamide/ sodium alginate (PAM/SA) hydrogel network, which effectively transferred the external mechanical forces to the entire physical and chemical cross-linking domains. Multi-walled carbon nanotubes (MWCNTs) were filled into the cross-linking network of the hydrogel to enhance the conductivity of the hydrogel effectively. Notably, hydrogels are designed as flexible tactile sensors that can accurately recognize and monitor electrical signals from different gesture movements and temperature changes. It was also assembled as a friction nanogenerator (TENG) that continuously generates a stable open circuit voltage (28 V) for self-powered small electronic devices. This research provides a new prospect for designing nanocellulose and MWCNTs reinforced conductive hydrogels via a facile method.

Hierarchical microstructures are widely recognized as one of the most effective components for enhancing the performance of flexible pressure sensors. However, the rapid and controllable fabrication of pressure sensing layers with hierarchical microstructures remains a significant challenge. In this study, we propose a method that utilizes laser-induced microscale shrinkage of shape memory polymers to enable rapid and controllable fabrication of hierarchical microstructures for high-performance pressure sensing. We systematically investigate the influence of UV laser fabrication parameters on the architecture and morphology of hierarchical microstructures. A flexible pressure sensor, equipped with optimized hierarchical microstructures, exhibits a high sensitivity larger than 15 kPa-1 and excellent linearity (R2 = 0.994) in a range from 0 to 200 kPa. It features response and recovery times of 57 and 62 ms, respectively, and maintains good stability, enduring over 5,000 cycles. The laser-induced shrinkage of shape memory polymers offers an effective method for the fabrication of hierarchical microstructures, holding great potential to boost the performance of flexible pressure sensors in applications within intelligent robotics and wearable healthcare.

Smart materials react to external triggers by changing size, color, mechanical properties, or permeability. The next generation of smart materials will be able to not only recognize and react to external triggers but also to their dynamics. The only existing example of such a material is heating rate-sensitive polymorphous cross-linked syndiotactic polypropylene. This study presents a new principle of a heating rate-sensitive material on the example of cross-linked and fully amorphous quenchable semi-crystalline polyethylene terephthalate (x-PET). The x-PET is stretched to high elongation above its melting temperature and constrained quenched to a fully amorphous state. Then the polymer is heated to 120-170 °C with different heating rates. Due to its heating-rate sensitivity, x-PET shrinks to different stabilized lengths dependent on the heating rate. The new length can be used to read out the heating rate and to specifically answer to this by mechanically switching a process. Detailed analytics of this process reveal that amorphous stretched x-PET is starting the retraction above Tg and simultaneously stopping it by crystallization. The different rates of these processes result in the heating rate sensitivity of x-PET.

In the field of tissue engineering, 3D printed shape memory polymers (SMPs) are drawing increased interest. Understanding how these 3D printed SMPs degrade is critical for their use in the clinic, as small changes in material properties can significantly change how they behave after in vivo implantation. Degradation of 3D printed acrylated poly(glycerol-dodecanedioate) (APGD) was examined via in vitro hydrolytic, enzymatic, and in vivo subcutaneous implantation assays. Three APGD manufacturing modalities were assessed to determine differences in degradation. Material extrusion samples showed significantly larger mass and volume loss at 2 months, compared to lasercut and vat photopolymerization samples, under both enzymatic and in vivo degradation. Critically, melt transition temperatures of degraded PGD increased over time in vitro, but not in vivo. Histology of tissue surrounding APGD implants showed no significant signs of inflammation compared to controls, providing a promising outlook for use of 3D printed APGD devices in the clinic.

Developing advanced engineering polymers that combine high strength and toughness represents not only a necessary path to excellence but also a major technical challenge. Here for the first time a rigid-flexible interlocking polymer (RFIP) is reported featuring remarkable mechanical properties, consisting of flexible polyurethane (PU) and rigid polyimide (PI) chains cleverly woven together around the copper(I) ions center. By rationally weaving PI, PU chains, and copper(I) ions, RFIP exhibits ultra-high strength (twice that of unwoven polymers, 91.4 ± 3.3 MPa), toughness (448.0 ± 14.2 MJ m-3), fatigue resistance (recoverable after 10 000 cyclic stretches), and shape memory properties. Simulation results and characterization analysis together support the correlation between microstructure and macroscopic features, confirming the greater cohesive energy of the interwoven network and providing insights into strengthening toughening mechanisms. The essence of weaving on the atomic and molecular levels is fused to obtain brilliant and valuable mechanical properties, opening new perspectives in designing robust and stable polymers.

Fluorescent 4D printing materials, as innovative materials that combine fluorescent characteristics with 4D printing technology, have attracted widespread interest and research. In this study, green lignin-derived carbon quantum dots (CQDs) were used as the fluorescent module, and renewable poly(propylene carbonate) polyurethane (PPCU) was used for toughening. A new low-cost fluorescent polylactic acid (PLA) composite filament for 4D printing was developed using a simple melt extrusion method. The strength of the prepared composite was maintained at 32 MPa, while the elongation at break increased 8-fold (34 % increase), demonstrating excellent shape fixed ratio (∼99 %), recovery ratio (∼92 %), and rapid shape memory recovery speed. The presence of PPCU prevented fluorescence quenching of the CQDs in the PLA matrix, allowing the composite to emit bright green fluorescence under 365 nm ultraviolet light. The composite exhibited shear thinning behavior and had an ideal melt viscosity for 3D printing. The results obtained demonstrated the versatility of these easy-to-manufacture and low-cost filaments, opening up a novel and convenient method for the preparation of strong, tough, and multifunctional PLA materials, increasing their potential application value.

Dynamic bonds can facilitate reversible formation and dissociation of connections in response to external stimuli, endowing materials with shape memory and self-healing capabilities. Temperature is an external stimulus that can be easily controlled through heat. Dynamic covalent bonds in response to temperature can reversibly connect, exchange, and convert chains in the polymer. In this review, we introduce dynamic covalent bonds that operate without catalysts in various temperature ranges. The basic bonding mechanism and the kinetics are examined to understand dynamic covalent chemistry reversibly performed by equilibrium control. Furthermore, a recent synthesis method that implements dynamic covalent coupling based on various polymers is introduced. Dynamic covalent bonds that operate depending on temperature can be applied and expand the use of polymers, providing predictions for the development of future smart materials.

Hydrogels endure various dynamic stresses, demanding robust mechanical properties. Despite significant advancements, matching hydrogels\' strength to biological tissues and plastics is often challenging without applying potentially harmful crosslinkers. Using hydrogen bonds as sacrificial bonds offers a promising strategy to produce tough, versatile hydrogels for biomedical and industrial applications. Poly(methacrylic acid) (PMA)/gelatin hydrogels were synthesized by thermally induced free-radical polymerization and crosslinked only by physical bonds, without adding any chemical crosslinker. The addition of gelatin increased the formation of hydrophobic domains in the structure of the hydrogels, which acted as permanent crosslinking points. The increase in PMA and gelatin contents generally led to a lower equilibrium water content (WC), higher thermal stability and better mechanical properties. The values of tensile strength and toughness reached up to 1.44 ± 0.17 MPa and 4.91 ± 0.51 MJ m-3, respectively, while the compressive modulus and strength reached up to 0.75 ± 0.06 MPa and 24.81 ± 5.85 MPa, respectively, with the WC being higher than 50 wt.%. The obtained values for compressive mechanical properties are comparable with super-strong hydrogels reported in the literature. In addition, hydrogels exhibited excellent fatigue resistance and biocompatibility, as well as great shape memory properties, which make them prominent candidates for a wide range of biomedical applications.

Irregular bone defects caused by trauma and bone diseases provide a complex implant environment for surgery. Traditional implants often fail to integrate well with the surrounding bone defect interface, therefore, developing an artificial bone scaffold that can adapt to irregular bone defect boundaries is of significant importance for bone defect repair. This study successfully utilized a shape memory ternary copolymer polylactic acid-trimethylene carbonate-hydroxyacetic acid (PLLA-TMC-GA) and dopamine-modified nano-hydroxyapatite (PHA) composite to construct a temperature-responsive bone repair scaffold (PTG/PHA), thereby enhancing the interface compatibility between the implant and the surrounding environment. The addition of PHA has effectively improved the hydrophilicity of the stent and significantly increased its mechanical strength. Furthermore, the Sodium alginate (SA) hydrogel loaded with Icariin (Ica) coated on the stent surface promotes the growth and differentiation of bone cells through the drug-scaffold synergistic effect. Both in vivo and in vitro experiments have shown that the synergistic effect of the composite stent with Icariin significantly enhances the repair of bone defects. This study provides a promising tissue engineering method for the repair of irregular bone defects.

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