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Direct 3D printing of liquid metal is difficult to form and easy to destroy. In this paper, we developed a 3D printed composite material consisting of a thermoplastic polyurethane (TPU) matrix and liquid metal (LM) dispersed droplets, and introduced the method for realizing 3D printed devices with this composite material: First, the LM is added to 10~50wt %TPU at 190~200 °C through ultrasonic blending to prepare blended ink. After solid cooling, the LM-TPU composite fiber with a diameter of 600 µm was prepared by Wellzoom desktop extruder at 190 °C at an extrusion speed of 400 mm/min. It has excellent elasticity, with a tensile limit of 0.637 N/m2, and the TPU could evenly wrap LM droplets. Finally, the LM-TPU fiber is 3D printed at 240 °C by using a 3D printer, and 2D/3D flexible electronic devices with heating and conductive functions could be prepared. The microcircuit has good electrical conductivity; after adding voltage, the circuit has heat release; it could be used as heating equipment to keep warm and used in various flexible wearable electronic products.

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Numerous endeavors have been dedicated to the development of composite polymer electrolyte (CPE) membranes for all-solid-state batteries (SSBs). However, insufficient ionic conductivity and mechanical properties still pose great challenges in practical applications. In this study, a flexible composite electrolyte membrane (FCPE) with fast ion transport channels was prepared using a phase conversion process combined with in situ polymerization. The polyvinylidene fluoride-hexafluoro propylene (PVDF-HFP) polymer matrix incorporated with lithium lanthanum zirconate (LLZTO) formed a 3D net-like structure, and the in situ polymerized polyvinyl ethylene carbonate (PVEC) enhanced the interface connection. This 3D network, with multiple rapid pathways for Li+ that effectively control Li+ flux, led to uniform lithium deposition. Moreover, the symmetrical lithium cells that used FCPE exhibited high stability after 1200 h of cycling at 0.1 mA cm-2. Specifically, all-solid-state lithium batteries coupled with LiFePO4 cathodes can stably cycle for over 100 cycles at room temperature with high Coulombic efficiencies. Furthermore, after 100 cycles, the infrared spectrum shows that the structure of FCPE remains stable. This work demonstrates a novel insight for designing a flexible composite electrolyte for highly safe SSBs.

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Viologen and Prussian blue (PB) exhibit good electrochromic properties, but certain limitations still exist. To improve the electrochromic properties of viologen, a viologen derivative 1,1'-bis(4-(bromomethyl)benzyl)-[4,4'-bipyridine]-1,1'-diium hexafluorophosphate (BBDV) was synthesized, and its electrochromic properties were investigated. Additionally, a flexible composite electrochromic device (FC-ECD) was prepared by using BBDV and PB as active materials. The structure of the FC-ECD was PET-ITO/gel electrolyte-BBDV/PB/PET-ITO. The applied voltage required for the FC-ECD was found to be lower than that of the ECD based on BBDV(FBBDV-ECD). Compared to FBBDV-ECD, FC-ECD exhibited a higher optical contrast (71.42%) and cyclic stability (89.51%). The FC-ECD exhibited multicolor changes under different applied voltages (ranging from -2.0 to +1.6 V). Especially, the color of the FC-ECD remained stable for 14 h after the removal of the applied voltage.

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Piezoelectric poly(vinylidene fluoride) (PVDF) and its copolymers have been widely investigated for applications in wearable electric devices and sensing systems, owing to their intrinsic piezoelectricity and superior flexibility. However, their weak piezoelectricity poses major challenges for practical applications. To overcome these challenges, we propose a two-step synthesis approach to fabricate sandwich-structured piezoelectric films (BaTiO3@PDA/PVDF/BaTiO3@PDA) with significantly enhanced ferroelectric and piezoelectric properties. As compared to pristine PVDF films or conventional 0-3 composite films, a maximum polarization (Pmax) of 11.24 µC/cm2, a remanent polarization (Pr) of 5.83 µC/cm2, and an enhanced piezoelectric coefficient (d33 ∼ 14.6 pC/N) were achieved. Simulation and experimental results have demonstrated that the sandwich structure enhances the ability of composite films to withstand higher poling electric fields in comparison with 0-3 composites. The sandwich-structured piezoelectric films are further integrated into a wireless sensor system with a high force sensitivity of 288 mV/N, demonstrating great potential for movement monitoring applications. This facile approach shows great promise for the large-scale production of composite films with remarkable flexibility, ferroelectricity, and piezoelectricity for wearable sensing devices.

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As the rapid development of advanced foldable electronic devices, flexible and insulating composite films with ultra-high in-plane thermal conductivity have received increasing attention as thermal management materials. Silicon nitride nanowires (Si3N4NWs) have been considered as promising fillers for preparing anisotropic thermally conductive composite films due to their extremely high thermal conductivity, low dielectric properties, and excellent mechanical properties. However, an efficient approach to synthesize Si3N4NWs in a large scale still need to be explored. In this work, large quantities of Si3N4NWs were successfully prepared using a modified CRN method, presenting the advantages of high aspect ratio, high purity, and easy collection. On the basis, the super-flexible PVA/Si3N4NWs composite films were further prepared with the assistance of vacuum filtration method. Due to the highly oriented Si3N4NWs interconnected to form a complete phonon transport network in the horizontal direction, the composite films exhibited a high in-plane thermal conductivity of 15.4 W·m-1·K-1. The enhancement effect of Si3N4NWs on the composite thermal conductivity was further demonstrated by the actual heat transfer process and finite element simulations. More significantly, the Si3N4NWs enabled the composite film presenting good thermal stability, high electrical insulation, and excellent mechanical strength, which was beneficial for thermal management applications in modern electronic devices.

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P-type multiwalled carbon nanotubes (MWCNTs), as well as heterostructures fabricated by direct deposition of inorganic thermoelectric materials as antimony and bismuth chalcogenides on MWCNT networks are known as perspective materials for application in flexible thermoelectric polymer-based composites. In this work, the electrical response of three types of Sb2Te3-MWCNT heterostructures-based flexible films-free standing on a flexible substrate, encapsulated in polydimethylsiloxane (PDMS), and mixed in polyvinyl alcohol (PVA) is studied in comparison with the flexible films prepared by the same methods using bare MWCNTs. The electrical conductance of these films when each side of it was subsequently subjected to compressive and tensile stress during the film bending down to a 3 mm radius is investigated in relation to the distribution gradient of Sb2Te3-MWCNT heterostructures or bare MWCNTs within the film. It is found that all investigated Sb2Te3-MWCNT films exhibit a reversible increase in the conductance in response to the compressive stress of the film side with the highest filler concentration and its decrease in response to the tensile stress. In contrast, free-standing and encapsulated bare MWCNT networks with uniform distribution of nanotubes showed a decrease in the conductance irrelevant to the bending direction. In turn, the samples with the gradient distribution of the MWCNTs, prepared by mixing the MWCNTs with PVA, revealed behavior that is similar to the Sb2Te3-MWCNT heterostructures-based films. The analysis of the processes impacting the changes in the conductance of the Sb2Te3-MWCNT heterostructures and bare MWCNTs is performed. The proposed in this work bending method can be applied for the control of the uniformity of distribution of components in heterostructures and fillers in polymer-based composites.

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The construction of ballistic-resistant body armor is experiencing an increasing use of flexible unidirectional (UD) composite laminates that comprise multiple layers. Each UD layer contains hexagonally packed high-performance fibers with a very low modulus matrix (sometimes referred to as binder resins). Laminates are then made from orthogonal stacks of these layers, and these laminate-based armor packages offer significant performance advantages over standard woven materials. When designing any armor system, the long-term reliability of the armor materials is critical, particularly with regard to stability with exposure to temperature and humidity, as these are known causes of degradation in commonly used body armor materials. To better inform future armor designers, this work investigates the tensile behavior of an ultra-high molar mass polyethylene (UHMMPE) flexible UD laminate that was aged for at least 350 d at two accelerated conditions: 70 °C at 76% relative humidity (RH) and 70 °C in a desiccator. Tensile tests were performed at two different loading rates. The mechanical properties of the material after ageing demonstrated less than 10% degradation in tensile strength, indicating high reliability for armor made from this material.

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The number of scrap wind turbines is expanding globally as the wind power industry develops rapidly. Zero-waste recycling of scrap wind turbine blades (WTB) is the key for wind power firms to achieve green and sustainable development on the premise of satisfying environmental protection criteria. In this work, the pyrolysis of fiber/epoxy composites obtained from scrap WTB in oxidizing inert atmospheres was investigated. Various characterization methods were employed to characterize the microstructure and chemical characteristics of the heat-treated fiber/epoxy and to reveal the pyrolysis mechanism. In addition, the heat-treated fibers/epoxy were used as reinforcing agents to investigate their impact on the elastic deformation of butadiene styrene rubber-based flexible composites, and the reinforcing mechanism was revealed. The results revealed that the constituents of fiber/epoxy composites were mostly fiberglass (SiO2, CaCO3) and cured epoxy resin, with covalent bonding being the interaction between the fiberglass and epoxy resin. The total weight of the epoxy resin in the fiber/epoxy composites was 22%, and the 11% weight loss was achieved at around 350 °C, regardless of the presence of oxygen; however, the features of heat-treated fibers/epoxy were associated with the pyrolysis atmosphere at a higher temperature. The pyrolysis products in inert atmospheres, with water contact angles of 58.8°, can considerably improve the tensile properties of flexible composites at the elastic stage. Furthermore, the flexible composite granules were prepared to plug large channels in sand-filled pipes, and the plugging rate had the potential to reach 81.1% with an injection volume of 5.0 PV. The plugging performance was essentially unaffected by water salinity, owing to the high stability of flexible composite granules in mineralized water. The findings of this study present a realistic route to the industrial application of fiber/epoxy, as well as a novel approach for encouraging the efficient use of scrap wind turbines on a large scale.

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Next-generation wearable electronics requires mechanical robustness. In addition to the previously reported eco-friendliness, low cost, and light weight of molecular perovskites, flexibility is also a desired merit for their practical use. Here we design a flexible X-ray detector based on a novel molecular perovskite, DABCO-CsBr3 (DABCO = N-N'-diazabicyclo[2.2.2]octonium), which is the missing link between metal-free molecular perovskites A(NH4)X3 (A = divalent organic ammoniums) and conventional metal halide based ABX3 (B = divalent metal cations) perovskites. DABCO-CsBr3 inherits its band nature from A(NH4)X3, while it exhibits a stronger stopping power. DABCO-CsBr3 shows potential for high-performance ionizing radiation detectors due to low dark current, low ion migration, and an efficient mobility-lifetime (µτ) product. Finally, a molecular-perovskite-based flexible X-ray detector is demonstrated on the basis of the DABCO-CsBr3/poly(vinylidene fluoride) composite, with a sensitivity of 106.7 µC Gyair-1 cm-2. This work enriches the molecular perovskite family and highlights the promise of molecular perovskites for the next-generation eco-friendly and wearable optoelectronic devices.

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Studies that aim to produce flexible films of composite materials based on ionomers-PZT, and volume fractions lower than 10% PZT, in order to monitor damage in aeronautical structures are seldom investigated. The growing emphasis on the use of polymers capable of self-healing after damage or activation by heating has motivated the application of self-healing ionomers as polymeric matrices in composites with piezoelectric particles aiming to monitor damage. Flexible composite films were developed based on the self-healing polymer matrix Surlyn® 8940 ionomer (DuPontTM-Wilmington, DE, USA) and PZT particles (connectivity 2-3) in volume fractions of 1, 3, 5 and 7%, with thickness around 50-100 µm. The choice of PZT volume fractions followed the preliminary requirement that establishes a final density, which is lower or at least close to the density of the materials used in aeronautical structures. Since the application of composites based on epoxy resin/carbon fibers has been increasing in the aeronautical segment, this material (with density lower than 1500 kg/m3) was chosen as a reference for the present work. Thus, due to self-healing (a characteristic of the matrix Surlyn® 8940) combined with recyclability, high flexibility and low thickness, the flexible composite films showed advantages to be applied on aeronautical structures, which present complex geometries and low-density materials. The manufactured films were characterized by SEM, XRD, DMA and mechanical tensile tests. The results were discussed mainly in terms of the volume fraction of PZT. X-ray diffraction patterns showed coexistent rhombohedral and tetragonal phases in the PZT particles-dispersed composite, which can potentialize the alignment of ferroelectric domains during polarization under strong electrical field, enhancing dielectric and piezoelectric properties toward sensing applications. DMA and tensile testing results demonstrated that the addition of PZT particles did not impair either dynamic or quasi-static mechanical performance of the flexible composite films. It was concluded that the PZT volume fraction should be lower than 3% because, for higher values, the molecular mobility of the polymer would suffer significant reductions. These findings, combined with the high flexibility and low density of the ceramic particle-filled thermoplastic polymer, render the developed flexible composite film a very promising candidate for strain and damage sensing in aeronautical structures.

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With the rapid advance of electronics, the light, flexible, and multifunctional composite films with high electromagnetic interference (EMI) shielding effectiveness and excellent thermal management are highly desirable for next-generation portable and wearable electronic devices. Herein, a series of flexible and ultrathin natural rubber/MXene/carbon nanotubes (NR/MXene/CNTs) composite films with sandwich structure are constructed layer by layer through a facile vacuum-assisted filtration method for EMI shielding and Joule heating application. The fabricated NR/MXene/CNTs-50 composite film, with NR/MXene as inner layer and NR/CNTs as out layers, not only has high EMI shielding efficiency, but also has excellent comprehensive mechanical properties at the thickness of only 200 µm. In addition, the superior environmental durability, high electrothermal conversion efficiency, hydrophobicity, and fine performance stability after periodic cyclic bending make the film possess more value in practical application.

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Replacing liquid electrolytes with solid polymer electrolytes (SPEs) is considered as a vital approach to developing sulfur (S)-based cathodes. However, the polysulfides shuttle and the growth of lithium (Li) dendrites are still the major challenges in polyethylene oxide (PEO)-based electrolyte. Here, an all-solid-state Li metal battery with flexible PEO-Li10 Si0.3 PS6.7 Cl1.8 (LSPSCl)-C-lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) composite cathode (FCC) and PEO-LSPSCl-LiTFSI composite electrolyte (S-CPE) is designed. The initial capacity of the Li|S-CPE|FCC battery is 414 mAh g-1 with 97.8% capacity retention after 100 cycles at 0.1 A g-1 . Moreover, the battery displays remarkable capacity retention of 80% after 500 cycles at 0.4 A g-1 . Cryo-transmission electron microscopy (Cryo-TEM) reveals rich large-sized Li2 CO3 particles at the Li/PEO interface blocking the Li+ transport, but the layer with rich Li2 O nanocrystals, amorphous LiF and Li2 S at the Li/S-CPE interface suppresses the growth of lithium dendrite and stabilizes the interface. In situ optical microscopy demonstrates that the excellent cyclic stability of FCC is ascribed to the reversible shuttle of P-S-P species, resulting from the movement of ether backbone in PEO. This study provides strategies to mitigate the polysulfide shuttle effect and Li dendrite formation in designing high energy density solid-state Li-S-based batteries.

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The role of Ag addition on the structural, dielectric, and mechanical harvesting response of 20%(xAg - (1 - x)BaTiO3) - 80%PVDF (x = 0, 2, 5, 7 and 27 vol.%) flexible composites is investigated. The inorganic fillers were realized by precipitating fine (~3 nm) silver nanoparticles onto BaTiO3 nanoparticles (~60 nm average size). The hybrid admixtures with a total filling factor of 20 vol.% were embedded into the PVDF matrix. The presence of filler enhances the amount of ß-PVDF polar phase and the BaTiO3 filler induces an increase of the permittivity from 11 to 18 (1 kHz) in the flexible composites. The addition of increasing amounts of Ag is further beneficial for permittivity increase; with the maximum amount (x = 27 vol.%), permittivity is three times larger than in pure PVDF (εr ~ 33 at 1 kHz) with a similar level of tangent losses. This result is due to the local field enhancement in the regions close to the filler-PVDF interfaces which are additionally intensified by the presence of silver nanoparticles. The metallic addition is also beneficial for the mechanical harvesting ability of such composites: the amplitude of the maximum piezoelectric-triboelectric combined output collected in open circuit conditions increases from 0.2 V/cm2 (PVDF) to 30 V/cm2 for x = 27 vol.% Ag in a capacitive configuration. The role of ferroelectric and metallic nanoparticles on the increasing mechanical-electric conversion response is also been explained.

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Flexible N-doped carbon fibers decorated with Cu/Cu2O particles (NCF-Cu/Cu2O) are synthesized through electrospinning, preoxidation and carbonization processes in this work. The characterization results indicate that HKUST-1 is embedded in polyacrylonitrile (PAN) fibers, and a special structure in which Cu/Cu2O particles are strung together by carbon fibers is formed after preoxidation and carbonization. NCF-Cu/Cu2O is mixed with paraffin in different mass ratios (5%, 10%, 15%, 20% and 25%) to study electromagnetic (EM) wave absorption performance at frequencies from 2.0 GHz to 18.0 GHz. When the filling ratio is 10%, the maximum reflection loss (RL) value is -50.54 dB at 14.16 GHz with a thickness of 2.4 mm, and the maximum effective absorption bandwidth (EAB) value reaches 7.2 GHz (10.8 âˆ¼ 18.0 GHz) with a thickness of 2.6 mm. The NCF-Cu/Cu2O composite fibers exhibit strong absorption, broad bandwidth, low filling ratio and thin thickness, and the corresponding absorption mechanism is analyzed in detail. The excellent EM wave absorption performance is attributed to a suitable attenuation ability, good impedance matching, conductive loss, interfacial polarization, dipole polarization, multiple reflections and scattering. This work provides a research reference for the application of flexible carbon-based composite fibers in the field of EM wave absorption.

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Flexible electromagnetic shielding composites have a great potential for wide range applications. In this study, two flexible composites were produced by plating Ni nanoparticles on carbon nanotubes (CNTs) or infiltrating carbon nanofibers/polydimethylsiloxane (CNF/PDMS) polymer into CNT/sodium alginate (CNT/SA) sponge skeleton (CNT/SA/CNF/PDMS composites). The composites are tested under the X band in the frequency range of 8.2 - 12.4 GHz, the electromagnetic interference shielding effectiveness (EMI-SE) values of the above two composites are almost as twice as that of CNT/SA/PDMS composite at a same CNT loading. Introducing nano-sized Ni particles on CNT improved the microwave absorption capacity of the composite, while adding CNF on the PDMS matrix enhanced the conductivity of these composites. Under 10% strain, both flexible composites show stable conductivity. Simulation and calculation results shown that increasing the cladding rate of Ni nanoparticles on the surface of CNT, reducing the average size of Ni particles, and increasing the loading of CNF in PDMS matrix can significantly improve conductivity and then EMI performance of the materials. All of these could benefit for the design of flexible electromagnetic shielding composites.

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Although wearable antennas have made great progress in recent years, how to design high-performance antennas suitable for most wireless communication systems has always been the direction of RF workers. In this paper, a new approach for the design and manufacture of a compact, low-profile, broadband, omni-directional and conformal antenna is presented, including the use of a customized flexible dielectric substrate with high permittivity and low loss tangent to realize the compact sensing antenna. Poly-di-methyl-siloxane (PDMS) is doped a certain proportion of aluminum trioxide (Al2O3) and Poly-tetra-fluoro-ethylene (PTFE) to investigate the effect of dielectric constant and loss tangent. Through a large number of comparative experiments, data on different doping ratios show that the new doped materials are flexible enough to increase dielectric constant, reduce loss tangent and significantly improve the load resistance capacity. The antenna is configured with a multisection microstrip stepped impedance resonator structure (SIR) to expand the bandwidth. The measured reflection return loss (S11) showed an operating frequency band from 0.99 to 9.41 GHz, with a band ratio of 146%. The antenna covers two important frequency bands, 1.71-2.484 GHz (personal communication system and wireless body area network (WBAN) systems) and 5.15-5.825 GHz (wireless local area network-WLAN)]. It also passed the SAR test for human safety. Therefore, the proposed antenna offers a good chance for full coverage of WLAN and large-scale development of wearable products. It also has potential applications in communication systems, wireless energy acquisition systems and other wireless systems.

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This work presents the morphological, structural and photocatalytic properties of flexible graphene composites decorated with Ni@TiO2:W nanoparticles (TiNiW NPs) with an average size of 27 ± 2 nm. The TiNiW NPs were immobilized on the surface of a flexible graphene composite using a PVA-based slurry-paste (FG/TiNiW composite). The SEM study showed that the TiNiW NPs remained exposed on the surface of the FG/TiNiW composite, which benefited its photocatalytic activity. The photocatalytic performance for the degradation of acetaminophen (ACT) was evaluated using both the TiNiW powders and the FG/TiNiW composite, obtaining maximum degradation efficiencies of 100 and 86%, respectively, after 3 h under natural solar irradiation. The degradation of ACT was caused mainly by the reactive oxygen species such as OH radicals and h+, which was confirmed by scavenger experiments. Photoluminescence, XPS and absorbance experiments revealed that oxygen vacancy defects were created by i) doping the TiNiW NPs with W and by ii) introducing graphene into the composites. These defects enhanced the absorbance of light in the range of 400-800 nm, which in turn, promoted the photocatalytic degradation of ACT. Moreover, the reuse experiments confirmed that both the TiNiW NPs and FG/TiNiW composite were very stable for the degradation of ACT, since degradation efficiencies >82% were obtained after 4 reuse cycles for both photocatalysts. The experimental findings of this work demonstrate that the flexible TiO2/graphene composites are a feasible option for the removal of pharmaceutical contaminants from water using natural solar irradiation.

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The focus of this research is to quantify the effect of load-coupling mechanisms in anisotropic composites with distinct flexibility. In this context, the study aims to realize a novel testing device to investigate tension-twist coupling effects. This test setup includes a modified gripping system to handle composites with stiff fibers but hyperelastic elastomeric matrices. The verification was done with a special test plan considering a glass textile as reinforcing with different lay-ups to analyze the number of layers and the influence of various fiber orientations onto the load-coupled properties. The results demonstrated that the tension-twist coupling effect strongly depends on both the fiber orientation and the considered reinforcing structure. This enables twisting angles up to 25° with corresponding torque of about 82.3 Nmm, which is even achievable for small lay-ups with 30°/60° oriented composites with distinct asymmetric deformation. For lay-ups with ±45° oriented composites revealing a symmetric deformation lead, as expected, no tension-twist coupling effect was seen. Overall, these findings reveal that the described novel test device provides the basis for an adequate and reliable determination of the load-coupled material properties between stiff fibers and hyperelastic matrices.

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Flexible Unidirectional (UD) composite laminates are commonly being used for ballistic-resistant body armor. These laminates comprise UD layers, each constructed by laminating thin layers of high-performance fibers held in place using very low modulus binder resins, with the fibers in each layer oriented parallel to each other. As these materials are used in body armor, it is important to investigate their long-term reliability, particularly with regards to exposure to temperature and humidity as these are known causes of degradation in other commonly used body armor materials. This work investigates the tensile behavior of a poly(p-phenylene terephthalamide), or PPTA flexible UD laminate aged for up to 150 d at accelerated conditions of 70 °C and 76 % relative humidity (RH). Tests were performed at three different crosshead displacement rates and three different gauge lengths. The effect of ageing on the mechanical properties of the material resulted in less than 10 % degradation in tensile strength, with a more significant reduction in longer specimens when tested at slower rates.

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The aim of this work was to analyze the influence of fibers on the mechanical behavior of fiber-reinforced elastomers under cyclic loading. Thus, the focus was on the characterization of structure-property interactions, in particular the dynamic mechanical and viscoelastic behavior. Endless twill-woven glass fibers were chosen as the reinforcement, along with silicone as the matrix material. For the characterization of the flexible composites, a novel testing device was developed. Apart from the conventional dynamic mechanical analysis, in which the effect of the fiber orientation was also considered, modified step cycle tests were conducted under tensile loading. The material viscoelastic behavior was studied, evaluating both the stress relaxation response and the capability of the material to dissipate energy under straining. The effects of the displacement rate of the strain level, the amplitude of the strain applied in the loading-unloading step cycle test, and the number of the applied cycles were evaluated. The results revealed that an optimized fiber orientation leads to 30-fold enhanced stiffness, along with 10 times higher bearable stress. The findings demonstrated that tailored reinforced elastomers with endless fibers have a strong influence on the mechanical performance, affecting the structural properties significantly.