Highly Tribo-Positive Nylon-11 Film Fabricated by Multiscale Structural Regulation through a Roll-to-Roll Processing.

Triboelectric polymers have attracted extensive attention due to their great electron-accepting and electron-donating properties in contact electrification as well as their flexible and low-cost merits and have become promising electrode materials in triboelectric nanogenerators (TENGs). However, most research has exclusively focused on improving the electron capture capability of the triboelectric layer, neglecting to enhance the electron-donating capability, which leads to a low output performance of TENG and limits its practical application. In this study, we developed a method to fabricate highly tribo-positive Nylon-11 film through roll-to-roll processing. Paired with the poly(tetrafluoroethylene) triboelectric layer, the transferred charge density of contact-separation TENG based on Nylon-11 film prepared by this method reaches 291.1 µC/m2, which has been improved by 12.4% compared with the conventional compression molding sample. The novel fabricating method can regulate the surface functional groups to achieve higher surface potential and obtain a favorable pseudohexagonal crystal phase, leading to an increasing transferred charge density in triboelectrification. Additionally, it has been analyzed that higher chemical potential of materials can facilitate the transfer of electrons from the triboelectric polymer surface. This study provides a nonadditive, simple, and effective strategy to fabricate excellent tribo-positive material, which can significantly enhance the performance of TENG.

Acid-Doped Pyridine-Based Polybenzimidazole as a Positive Triboelectric Material with Superior Charge Retention Capability.

The energy conversion efficiency of a triboelectric nanogenerator (TENG) is severely limited by the charge density of triboelectric materials, while drastic and unavoidable charge decay happens during contact due to the insufficient charge retention capacity of positive triboelectric materials. Here, elaborately synthesized acid-ion-doped pyridine-based polybenzimidazole processing with strong charge retention capability is demonstrated to couple with negatively corona-polarized electrets. As illustrated by thermal stimulation and an ion mass spectrometer, the formation of acid-ion chimerism processes high activation energy for stored charges, and the selective anion migration can compensate the escape of polarized charge. Accordingly, the charge density can reach up to 596 µC m-2 and the charge retention rate reaches 49.7%, which is so far the highest intrinsic charge density obtained in the open air. Thus, the ionic chimerism strategy provides an effective way to suppress the charge escaping in the open air and gives a great expandable avenue for the material challenges of TENG's practical deployment.

Self-poled piezoelectric polymer composites via melt-state energy implantation.

Lightweight flexible piezoelectric polymers are demanded for various applications. However, the low instinctively piezoelectric coefficient (i.e. d33) and complex poling process greatly resist their applications. Herein, we show that introducing dynamic pressure during fabrication is capable for poling polyvinylidene difluoride/barium titanate (PVDF/BTO) composites with d33 of ~51.20 pC/N at low density of ~0.64 g/cm3. The melt-state dynamic pressure driven energy implantation induces structure evolutions of both PVDF and BTO are demonstrated as reasons for self-poling. Then, the porous material is employed as pressure sensor with a high output of ~20.0 V and sensitivity of ~132.87 mV/kPa. Besides, the energy harvesting experiment suggests power density of ~58.7 mW/m2 can be achieved for 10 N pressure with a long-term durability. In summary, we not only provide a high performance lightweight, flexible piezoelectric polymer composite towards sustainable self-powered sensing and energy harvesting, but also pave an avenue for electrical-free fabrication of piezoelectric polymers.

Strengthening-toughening pure poly(lactic acid) with ultra-transparency through increasing mesophase promoted by elongational flow field.

Poly(lactic acid) (PLA), as a biodegradable material, finds wide applications in packaging, automotive, and biological industries. However, achieving high strength, toughness, ultra-transparency, and heat resistance simultaneously in pure PLA through continuous one-step manufacturing remains a significant challenge. In this study, we addressed this challenge by utilizing the eccentric rotor extruder (ERE) in combination with cooling rolls to manufacture PLA sheets with outstanding mechanical performance. The ERE's elongational flow field combined with the cooling roller's weak stretching action induced orientation in the PLA molecular chains and promoted the formation of more mesophase, significantly improving mechanical properties. When the extrusion-stretch ratio (λ) value was 3.5, the tensile yield strength, Young's modulus, and elongation at break of ERE-fabricated samples ER-3.5 reached 86.2 MPa, 1777 MPa, and 57.9 %, respectively. Compared to the SE-3.5 samples manufactured with traditional methods, the increases were 38.8 %, 25.8 %, and 9.4 times, respectively. Additionally, the ERE manufactured samples maintained ultra-transparency and high heat resistance, making them suitable for food packaging, biomedicine, and other related fields. This methodology provides an efficient industrial-scale approach for manufacturing neat, biodegradable PLA with outstanding mechanical performance and ultra-transparency.

Water evaporation induced in-situ interfacial compatibilization for all-natural and high-strength straw-fiber/starch composites.

In this paper, we proposed a novel and green strategy based on water evaporation induced in-situ interfacial compatibilization (WEIC) mechanism for fabricating high-strength and all-natural lignocellulose/starch composites. This mechanism exploits the natural compatibility of the lignocellulose and starch and was tested through an internal mixing process with regulated water evaporation. Specifically, we revealed that a restrained layer was in-situ formed at the interface of the lignocellulose and starch during the internal mixing process; a faster water evaporation rate thickens this restrained layer, restricts the starch's molecular movement and significantly increases the composite's mechanical properties. The highest tensile strength and Young's modulus of the composites achieved are 21.7 ± 0.8 MPa and 2.2 ± 0.1 GPa, respectively, superior to many existing starch/lignocellulose composites. Thus, this work provides new insight into the compatibilization of various hydrophilic polysaccharides and paves new avenues for developing greener and more facile methods to fabricate all-polysaccharide composites.

Efficient fabrication of tilt micro/nanopillars on polypropylene surface with robust superhydrophobicity for directional water droplet rebound.

The directional rebound and transport of water droplets plays an important role in microfluidic devices, anti-fogging, and water harvesting. Herein, an extrusion compression molding and directional stretch demolding method was used to prepare a polypropylene (PP) surface with tilt micro/nanopillars with a contact angle of 157 ± 3°. The rolling angle is the highest (9 ± 4°) when the direction of rotation is opposite the tilt direction of the micro/nanopillars, showing excellent water repellency and anisotropy of the surface. Compared with the position of the first collision of the water droplet, the position of the second collision shifted ∼1.5 mm along the tilt direction of the micro/nanopillars, driven by the surface tension component during the collision. The directional rebound behavior is controlled by the droplet energy and the tilt angle. The micro/nanopillars demonstrate excellent self-cleaning property and mechanical durability, which shows the possibility of their practical engineering applications.

Fabrication of triboelectric polymer films via repeated rheological forging for ultrahigh surface charge density.

Triboelectric polymer with high charge density is the foundation to promote the wide range of applications of triboelectric nanogenerators. This work develops a method to produce triboelectric polymer based on repeated rheological forging. The fluorinated ethylene propylene film fabricated by repeated forging method not only has excellent mechanical properties and good transmittance, but also can maintain an ultrahigh tribo-charge density. Based on the film with a thickness of 30 µm, the output charge density from contact-separation nanogenerator reaches 352 µC·m-2. Then, the same film is applied for the nanogenerator with air-breakdown mode and a charge density of 510 µC·m-2 is further achieved. The repeated forging method can effectively regulate the composition of surface functional groups, the crystallinity, and the dielectric constants of the fluorinated ethylene propylene, leading to the superior capability of triboelectrification. Finally, we summarize the key parameters for elevating the electrification performance on the basis of molecular structure and related fabrication crafts, which can guide the further development of triboelectric polymers.

Layer-by-Layer Assembly of Multifunctional NR/MXene/CNTs Composite Films with Exceptional Electromagnetic Interference Shielding Performances and Excellent Mechanical Properties.

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.

One-step laser etching of a bionic hierarchical structure on a silicone rubber surface with thermal and acid/alkali resistance and tunable wettability.

Superhydrophobic silicone rubbers with robust physical and chemical stability have promising application potential in the field of flexible electronics. A one-step laser etching strategy is proposed for successfully fabricating superhydrophobic silicone rubbers with bioinspired hierarchical micro/nanostructures. Regular and dense micro/nano spheres gradually accumulate on the modified silicone rubber surface with the increase of laser etching cycles. Owing to the bioinspired hierarchical micro/nano spheres, a 5 µL water droplet on the modified silicone rubber surface exhibits a contact angle of 158 ± 3° and a sliding angle of 5 ± 1°. Moreover, the modified silicone rubber can maintain a stable superhydrophobic state in acid/alkali (pH = 2, 4, 6, 8, and 10) and thermal environments (50-90 °C). Importantly, the contact angle and sliding angle are adjustable depending on the number of laser etching cycles, which is beneficial for the different application requirements. The proposed method for the fast fabrication of superhydrophobic silicone rubbers with tunable wettability can provide an excellent candidate for the protection of flexible electronics in rainy and acid/alkali environments.

Cost-Effective Fabrication of Micro-Nanostructured Superhydrophobic Polyethylene/Graphene Foam with Self-Floating, Optical Trapping, Acid-/Alkali Resistance for Efficient Photothermal Deicing and Interfacial Evaporation.

Solar evaporation is one of the most attractive and sustainable approaches to address worldwide freshwater scarcity. Unfortunately, it is still a crucial challenge that needs to be confronted when the solar evaporator faces harsh application environments. Herein, a promising polymer molding method that combines melt blending and compression molding, namely micro extrusion compression molding, is proposed for the cost-effective fabrication of lightweight polyethylene/graphene nanosheets (PE/GNs) foam with interconnected vapor escape channels and surface micro-nanostructures. A contact angle of 155 ± 2°, a rolling angle of 5 ± 1° and reflectance of ≈1.6% in the wavelength range of 300-2500 nm appears on the micro-nanostructured PE/GNs foam surface. More interestingly, the micro-nanostructured PE/GNs foam surface can maintain a robust superhydrophobic state under dynamic impacting, high temperature and acid-/alkali solutions. These results mean that the micro-nanostructured PE/GNs foam surface possesses self-cleaning, anti-icing and photothermal deicing properties at the same time. Importantly, the foam exhibits an evaporation rate of 1.83 kg m-2 h-1 under 1 Sun illumination and excellent salt rejecting performance when it is used as a self-floating solar evaporator. The proposed method provides an ideal and industrialized approach for the mass production of solar evaporators suitable for practical application environments.

Ultrafast Fabrication of Graphene-Reinforced Nanocomposites via Synergy of Steam Explosion and Alternating Convergent-Divergent Flow.

Producing high-quality graphene and polymer/graphene nanocomposite is facing the problems of complex procedure, low efficiency, and serious resource waste. To explore a new fabrication approach with high efficiency and low cost is crucial for solving these technical issues, which becomes a current research hotspot and also a great challenge. Herein, a one-step melt mixing strategy based on the synergy of steam explosion and alternating convergent-divergent flow, is innovatively developed to fabricate high-density polyethylene (HDPE)/graphene nanocomposites using industrial-grade expanded graphite (EG) without chemical agents and complex procedures. The co-action of the external force derived from elongational melts and the internal force generated by steam explosion make EG ultrafastly exfoliate into few-layer graphene nanosheets (GNS) and simultaneously disperse in melts within 4 min. The as-produced GNS have a lateral size of over 5 µm and a minimum thickness of 1.4 nm, can introduce super heterogeneous nucleation to HDPE macromolecules and greatly increases nanocomposite crystallinity up to 86.5%. Moreover, plentiful HDPE crystallites and well-dispersed GNS jointly form an improved thermally-conductive network, making nanocomposites with a rapid-respond ability in solar-to-thermal conversion and heat dissipation. This facile strategy will facilitate the development of scalable production and wide application of high-performance graphene and highly-filled nanocomposites.

Constructing Bone-Mimicking High-Performance Structured Poly(lactic acid) by an Elongational Flow Field and Facile Annealing Process.

Poly(lactic acid) (PLA) as one of the most promising biodegradable polymers is being tremendously restricted in large-scale applications by the notorious toughness, ductility, and heat distortion resistance. Manufacturing PLA with excellent toughness, considerable ductility, balanced strength, and great heat distortion resistance simultaneously is still a great challenge. Natural structural materials usually possess excellent strength and toughness by elaborately constructed sophisticated hierarchical architectures, however, completely reproducing natural structural materials' architecture have evidenced to be difficult. Inspired by the hierarchical construction of the compact bone, an innovational method with an intensive and continuous elongational flow field and facile annealing process was developed to create bone-mimicking structured PLA at an industrial scale. The bone-mimicking structured PLA with unique and novel hierarchical architectures of interlocked 3D network lamellae and large extended-chain lamellae connecting the regular lamellae was constructed by in situ formed oriented thermoplastic poly(ether)urethane nanofibers (TNFs) acting as "collagen fibers", orderly staggered PLA lamellae behaving as "hydroxyapatite (HA) nanocrystals", and the tenacious interface functioning as a "soft protein" adhesive layer. Attributed to the unique structure, it possesses super toughness (90.3 KJ/m2), high stiffness (2.15 GPa), balanced strength (52.6 MPa), and notable heat distortion resistance (holding at 163 °C for 1 h) simultaneously. These excellent performances of the structured PLA provide it with immense potential applications in both structural and bio-engineering materials fields such as artificial bones and tissue scaffolds.

Phase Morphology and Performance of Supertough PLA/EMA-GMA/ZrP Nanocomposites Prepared through Reactive Melt-Blending.

Nanofiller zirconium phosphate (ZrP) and ethylene-methyl acrylate-glycidyl methacrylate copolymer (EMA-GMA) were introduced into poly(lactic acid) (PLA) through reactive melt-blending method to improve its toughness. The impact strength of PLA/EMA-GMA/ZrP (82/15/3) nanocomposites was improved about 22 times that of pure PLA to 65.5 kJ/m2. Fourier transform infrared spectroscopy (FTIR) analysis indicated there were compatibilization reactions between the components. The miscibility and thermal behavior of the blends were investigated by dynamic mechanical analysis (DMA), differential scanning calorimetric (DSC), and thermogravimetric analysis (TGA). Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) were applied to observe the fractured surface and phase morphology to study the toughness mechanism. A typical core-shell morphology, ZrP wrapped by EMA-GMA phase, was observed in the nanocomposites, which can cause plastic deformations. The supertough effect of the compound was mainly confirmed by effective interfacial compatibilization and massive shear-yielding deformation achieved by the synergy of EMA-GMA with ZrP in the PLA matrix.

Super-Toughened Poly(lactic Acid) with Poly(ε-caprolactone) and Ethylene-Methyl Acrylate-Glycidyl Methacrylate by Reactive Melt Blending.

In recent years, poly(lactic acid) (PLA) has attracted more and more attention as one of the most promising biobased and biodegradable polymers. However, the inherent brittleness significantly limits its wide application. Here, ternary blends of PLA, poly(ε-caprolactone) (PCL) with various amounts of ethylene-methyl acrylate-glycidyl methacrylate (EMA-GMA) terpolymer were fabricated through reactive melt blending in order to improve the toughness of PLA. The effect of different addition amounts of EMA-GMA on the mechanical properties, interfacial compatibility and phase morphology of PLA/PCL blends were studied. The reactions between the epoxy groups of EMA-GMA and carboxyl and hydroxyl end groups of PLA and PCL were investigated thorough a Fourier transform infrared (FT-IR). The miscibility and thermal behavior of the blends were studied through a dynamic mechanical analysis (DMA), differential scanning calorimetric (DSC) and X-ray diffraction (XRD). The phase morphology and impact fracture surface of the blends were also investigated through a scanning electron microscope (SEM). With the addition of 8 phr EMA-GMA, a PLA/PCL (90 wt %:10 wt %)/EMA-GMA ternary blend presenting a suitable multiple stacked phase structure with an optimum interfacial adhesion exhibited an elongation at break of 500.94% and a notched impact strength of 64.31 kJ/m2 with a partial break impact behavior. Finally, the toughening mechanism of the supertough PLA based polymers have been established based on the above analysis.

An Effective On-line Polymer Characterization Technique by Using SALS Image Processing Software and Wavelet Analysis.

This paper describes an effective on-line polymer characterization technique by using small-angle light-scattering (SALS) image processing software and wavelet analysis. The phenomenon of small-angle light scattering has been applied to give information about transparent structures on morphology. Real-time visualization of various scattered light image and light intensity matrices is performed by the optical image real-time processing software for SALS. The software can measure the signal intensity of light scattering images, draw the frequency-intensity curves and the amplitude-intensity curves to indicate the variation of the intensity of scattered light in different processing conditions, and estimate the parameters. The current study utilizes a one-dimensional wavelet to delete noise from the original SALS signal and estimate the variation trend of maximum intensity area of the scattered light. So, the system brought the qualitative analysis of the structural information of transparent film success.