- Abstract：Currently, the enhancement in electromagnetic interference (EMI) performance of polymeric composite generally relies on either improving electrical conductivity (σ) for stronger electromagnetic (EM) reflections or tailoring structure for higher EM resonances. Herein, we proposed a novel technique called cyclic pulsating pressure enhanced segregating structuration (CPP-SS), which can reinforce these two factors simultaneously. The structural information was supplied by optical microscopy (OM) and scanning electron microscopy (SEM), both of which confirmed the formation and evolution of segregate structured ultra-high molecular weight polyethylene (UHMWPE)/graphene composites. Then, the result showed that CPP-SS can significantly improve the σ of samples. Ultimately, advanced specific EMI shielding efficiency of 31.1 dB/mm was achieved for UHMWPE/graphene composite at 1-mm thickness and a low graphene loading of 5 wt%. Meanwhile, it also confirmed that the intrinsic disadvantage of poor mechanical properties of conventional segregated structure composites can be surpassed. This work is believed to provide a fundamental understanding of the structural and performance evolutions of segregated structured composites prepared under CPP-SS, and to bring us a simple and efficient approach for fabricating high-performance, strong and light-weight polymeric EMI shields.Keywords：Cyclic pulsating pressure;Segregated structure;Ultra-high molecular weight polyethylene;Graphene;Electromagnetic interface
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Published：2024-04-25 - Abstract：In this work, aramid nanoparticles (ANPs) were prepared in dimethyl formamide (DMF) solution containing high impact polystyrene (HIPS) via a bottom-up approach. Transmission electron microscopy (TEM) images showed that the obtained ANPs were evenly distributed in the HIPS matrix without any agglomeration. Chemical composition of the ANPs, i.e., poly(p-phenyl-p-phenylenediamine) (PPTA), was confirmed by Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) and X-ray diffractometer (XRD). The ANP/HIPS composites, obtained after ethanol precipitation, were added to neat HIPS as fillers to fabricate ANP/HIPS composite sheets. The surface roughness and the glass transition temperature (Tg) of the sheets were characterized by atomic force microscope (AFM) and differential scanning calorimetry (DSC), respectively. Compared with neat HIPS, the mechanical properties of the composite sheet were significantly improved, and the Young's modulus increased from 246.55 MPa to 2025.12 MPa, the tensile strength increased from 3.07 MPa to 29.76 MPa, and the toughness increased from 0.32 N/mm2 to 3.92 N/mm2, with an increase rate of 721%, 869% and 1125%, respectively. Moreover, the thermal stability of the composites improved with the increase in ANP content.Keywords：High impact polystyrene;PPTA nanoparticle;Reinforce;Mechanical property
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Published：2024-04-25 - Abstract：The antioxidant N-isopropyl-N'-phenyl-p-phenylenediamine (4010NA) was dissolved in ethanol and impregnated into silica aerogel (SAG) via vacuum-pressure cycles, yielding composite particles (A-N) with enhanced sustained-release and reinforcing capabilities. The effect of A-N on the mechanical properties and thermal-oxidative aging resistance of styrene-butadiene rubber (SBR) vulcanizates was investigated. TGA and BET assessments indicated that the loading efficiency of 4010NA in SAG reached 14.26% within ethanol's solubility limit. Incorporating A-N into SBR vulcanizates significantly elevated tensile strength by 17.5% and elongation at break by 41.9% over those with fumed silica and free 4010NA. Furthermore, A-N notably enhanced the thermal-oxidative aging resistance of SBR. After aging for 96 h at 100 °C, the tensile strength and elongation at break of SBR with A-N sustained 70.09% and 58.61% of their initial values, respectively, with the retention rate of elongation at break being 62.8% higher than that of SBR with fumed silica and free antioxidant. The study revealed that A-N composite particles significantly inhibited the crosslinking in SBR's molecular chains, reducing hardening and embrittlement during later thermal-oxidative aging stages.Keywords：Styrene-butadiene rubber;Silica aerogel;Loading modification;Thermal-oxidative aging
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Published：2024-04-25 - Abstract：Due to their excellent biocompatibility and biodegradability, aliphatic polyesters are widely used in the biomedical, packaging and agricultural fields, which are usually accessed by the ring-opening polymerization (ROP) of lactones and the catalysts particularly play an important role. Herein a series of quinolinyl-urea catalysts have been synthesized via the reaction between isocyanate and aminoquinoline with an amino group at different substitution positions and characterized. In combination with 7-methyl-1, 5, 7-triazabicyclo[4,4,0]dec-5-ene (MTBD) as a cocatalyst and benzyl alcohol (BnOH) as an initiator, 1-(3,5-bis(trifluoromethyl)phenyl)-3-(quinolin-3-yl)urea (3-QU) was observed to be most active for the ROP of δ-valerolactone (δ-VL). The polymerization conditions were optimized by varying the type of organic base, catalyst concentration and reaction temperature. By changing the ratio of [M]0/[I], linear polyvalerolactones (PVLs) with different molecular weights and narrow molecular weight distribution were prepared. The kinetic and chain extension experiments were carried out to prove the “living”/controllable feature. And the NMR experiments were used to support the proposal of possible mechanism.Keywords：Quinolinyl-urea;Ring-opening polymerization;PVL
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Published：2024-04-25 - Abstract：Conjugated homopolymers based on six-member rings, e.g., polyfluorene, always exhibit blue emission and conjugated homopolymers based on five-member rings, e.g., polythiophene, can give red emission with low efficiency. In this work, we report a series of new conjugated homopolymers based on six-member rings with high-efficiency deep-red emission. The repeating units of the red light emitting homopolymers are double B←N bridged bipyridine (BNBP) with the boron atoms functionalized with diphenyl, borafluorene, and 2,7-di-tert-butyl-borafluorene groups, respectively. The relationship between the chemical structures and the opto-electronic properties of the monomers and the homopolymers has been systematically studied. The three polymers emit pure red light (λmax=656 nm) or deep red light (λmax=693 nm) with fluorescence quantum efficiency in solution higher than 60%. The polymers can be used as the emitters in solution-processed organic light-emitting diodes with red emission and decent device performance. This work indicates a new strategy to design highly efficient light emitting conjugated polymers.Keywords：Conjugated homopolymers;Double B←N bridged bipyridine (BNBP);Deep-red emission;High fluorescent efficiency
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Published：2024-04-25 - Abstract：Polyelectrolytes are charged polymers comprising macromolecules in which substantial portions of the constituent units contain cationic (e.g., pyridinium, ammonium) or anionic (e.g., sulfonate, carboxylate) groups, which possess special functions from the features of counterions, such as dissociation to charged species, mechanical stability, phase behavior, etc. Therefore, functional polyelectrolytes have been widely applied in many fields. In this perspective, we present some progresses in the studies of poly(polyoxometalate)s, denoted as poly(POM)s, as a kind of new charged polymers/polyelectrolytes, by covalent bonding between the inorganic polyoxometalate (POM) clusters and the organic polymer chains. According to the distinct positions of POMs in polymer chain and functions of poly(POM)s, they are divided into the following four categories: crosslinked poly(POM); side-chain poly(POM); backbone poly(POM), including poly(POM)-conjugated polymer hybrid and block poly(POM)-polymer; and POM-based covalent organic framework (PCOF). This perspective introduces the synthesis methods of poly(POM) polyelectrolytes and their macromolecular and aggregate structural characteristics, while also focusing on their properties and functions. Their application areas include catalysis, thermal resistance, optical functions, fuel cells and batteries, etc.Keywords：Charged polymer;Polyelectrolyte;Polyoxometalate;Poly(polyoxometalate);Covalent organic framework
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Published：2024-04-20 - Abstract：Non-aromatic fluorescent and multi-responsive materials, exhibiting inherent fluorescence emission and controlled phase change, have garnered significant attention in recent years. However, the underlying interaction between their fluorescent properties and phase transition remains unclear. In this study, we synthesized a series of catalyst-free aza-Michael addition-based polyethyleneimine (RFPEI) materials by reacting polyethyleneimine (PEI) with N-isopropyl acrylamide (NIPAM). The resulting RFPEI was comprehensively characterized, and demonstrated dual-phase transition behavior (LCST and UCST) in water, which could be finely tuned by adjusting its composition or external factors such as pH. Notably, upon UV irradiation (365 nm), RFPEI exhibited strong fluorescence emission. We further investigated the effects of NIPAM grafting percentage to PEI, polymer concentration, and pH on the LCST/UCST and fluorescent properties of RFPEI aqueous solutions. Moreover, we showcased the great potential of RFPEI as a versatile tool for physiological cell imaging, trace detection, and controlled release of doxorubicin. Our study presents a novel class of stimuli-responsive fluorescent materials with promising applications in the field of biomedicine.Keywords：Polyethyleneimine;Multi-responsiveness;Intrinsic fluorescence emission;Cell imaging;Controlled drug release
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Published：2024-04-16 - Abstract：In this work, poly(3-hexylthiophene) (P3HT) ultrathin films (P3HT-T) were prepared by spin-coating a dilute P3HT solution (in a toluene: o-dichlorobenzene (Tol:ODCB) blend with a volume ratio of 80:20) with ultrasonication and the addition of the nucleating agent bicycle [2.2.1] heptane-2,3-dicarboxylic acid disodium salt (HPN-68L) on glass, Si wafers and indium tin oxide (ITO) substrates. The electrical and mechanical properties of the P3HT-T ultrathin films were investigated, and it was found that the conductivity and crack onset strain (COS) were simultaneously improved in comparison with those of the corresponding pristine P3HT film (P3HT-0, without ultrasonication and nucleating agent) on the same substrate, regardless of what substrate was used. Moreover, the conductivity of P3HT-T ultrathin films on different substrates was similar (varying from 3.7 S·cm−1 to 4.4 S·cm−1), yet the COS increased from 97% to 138% by varying the substrate from a Si wafer to ITO. Combining grazing-incidence wide-angle X-ray diffraction (GIXRD), UV-visible (UV-Vis) spectroscopy and atomic force microscopy (AFM), we found that the solid order and crystallinity of the P3HT-T ultrathin film on the Si wafer are highest, followed by those on glass, and much lower on ITO. Finally, the surface energy and roughness of three substrates were investigated, and it was found that the polar component of the surface energy γp plays a critical role in determining the crystalline microstructures of P3HT ultrathin films on different substrates. Our work indicates that the P3HT ultrathin film can obviously improve the stretchability and simultaneously retain similar electrical performance when a suitable substrate is chosen. These findings offer a new direction for research on stretchable CP ultrathin films to facilitate future practical applications.Keywords：P3HT ultrathin film;Substrate;Crystalline microstructures;Polar component of the surface energy;Electrical and stretchable performances
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Published：2024-04-16 - Abstract：In this study, a series of hindered urea bond (HUB) containing polyurethane-urea methacrylate prepolymers and a none HUB containing polyurethane methacrylate prepolymer were prepared using isobornyl methacrylate as the reactive diluent via one-pot procedure. The prepolymers were characterized fully by various techniques. Then, their thermosets were fabricated via UV curing in presence of a photo initiator, and their mechanical property and thermal behavior were investigated and compared. Different from the none HUB containing thermoset, the HUB containing thermosets (defined as PUT) could be recycled and reprocessed by hot press under relatively mild conditions with high recovery ratio of mechanical property. Furthermore, zinc oxide (ZnO) nanoparticles were modified with 3-(trimethoxysilyl) propyl methacrylate and the modified ZnO (defined as ZnO-TPM) was dispersed and polymerized into PUT matrix to prepare their nanocomposites. The influence of ZnO-TPM on the mechanical performance of the composites was evaluated, which indicated that the Young’s modulus and tensile strength increased gradually to the maximum values at ZnO-TPM content of 1 wt% and then decreased. The composites also displayed good reprocessability with improved recovery ratio compared to the pure PUT sample. In addition, the composite materials exhibited strong UV absorption capacity, implying their potential application in the circumstance where UV-shielding was required.Keywords：Polyurethane-urea methacrylate;Hindered urea bond;ZnO nanoparticles;Reprocessing;UV curing
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Published：2024-04-16 - Abstract：To enhance the mechanical properties of polypropylene random copolymer (PPR), polystyrene (PS) with four different contents were added to the PPR matrix through melt blending. Subsequently, using the Multi-Flow Vibration Injection Molding (MFVIM) technology, PPR/PS in situ microfiber composites (MFC) with different blending ratios were prepared. The results indicated that blending ratio had a great impact on the phase morphology and crystal structure of MFVIM samples, which was different from those of conventional injection molding (CIM) samples. PS ultrafine fibers could be formed under the shear field and could absorb the PPR molecular chains to form hybrid shish-kebab structures. Meanwhile, the PPR matrix could also form shish-kebab structures under the effect of strong shear. When the PS content reached 20%, under the combined action of PS in situ microfibers and highly oriented crystal structure, the tensile strength and Young's modulus of the sample were obviously improved and the impact strength remained at a relatively high level. So a strong and tough balanced PPR based material was obtained. These results provide valuable insights for expanding the industrial and daily-life applications of PPR and show promising development prospects.Keywords：PPR;MFVIM;In situ microfibers;Shear field;Hybrid shish-kebab structures
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Published：2024-04-16 - Abstract：Efforts to develop innovative water harvesting strategies offer powerful solutions to alleviate the water crisis, especially in remote and arid areas. Inspired by the hydrophobic/hydrophilic pattern of desert beetles and water self-propulsion property of spider silks, a double-strand hydrophobic PVDF-HFP/hydrophilic PAN nanofibers yarn is proposed by electrospinning and twisting techniques. The double-strand cooperation approach allows for water deposition on hydrophobic PVDF-HFP segment and transport under the asymmetric capillary driving force of hydrophilic PAN segment, thus speeded up the aggregation and growth of droplets. The effects of the composition and the diameter ratio of the two primary yarns were studied and optimized for boosting fog collection performance. The double-strand anisotropic yarn not only provide an effective method for water harvesting, but also hold the potential to inspire innovative design concepts for fog collection materials in challenging environments.Keywords：Fog collection;Wettability;Electrospinning;Nanofibers;Spider silk
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Published：2024-04-16 - Abstract：Holographic optical elements (HOEs) based on polymer composites have become a research hot spot in recent years for augmented reality (AR) due to the significant improvement of optical performance, dynamic range, ease of processing and high yield rate. Nevertheless, it remains a formidable challenge to obtain a large field of view (FOV) and brightness due to the limited refractive index modulation. Herein, we report an effective method to tackle the challenge by doping an epoxy liquid crystal termed E6M, which enables a large refractive index modulation of 0.050 @ 633 nm and low haze of 5.0% at a doping concentration of 5 wt%. This achievement may be ascribed to the improved molecular ordering of liquid crystals within the holographic polymer composites. The high refractive index modulation can endow transmission-type holographic polymer composites with a high diffraction efficiency of 96.2% at a small thickness of 5 μm, which would promise the design of thin and lightweight AR devices.Keywords：Polymer nanocomposites;Holography;AR/VR;Refractive index modulation;Liquid crystal
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Published：2024-04-16 - Abstract：Since electromagnetic pollution is detrimental to human health and the environment, numerous efforts have been successively made to achieve excellent electromagnetic interference shielding effectiveness (EMI SE) via designing the hierarchical structures for electromagnetic interference (EMI) shielding polymer composites. Among the plentiful structures, the asymmetric structures are currently a hot spot, principally categorizing into multi-layered, porous, fibrous, and segregated asymmetric structures, which endows the high EMI shielding performance for polymer composites incorporated with magnetic, conductive, and/or dielectric micro/nano-fillers, due to the “absorption-reflection-reabsorption” shielding mechanism. Therefore, this review provides the retrospection and summary of the efforts with respect to abundant asymmetric structures and multifunctional micro/nano-fillers for enhancing EMI shielding properties, which is conducive to the booming development of polymeric EMI shielding materials for the promising prospect in modern electronics and 5-generation (5G) technology.Keywords：Asymmetric structure;Micro/nano functional filler;Polymer composite;Electromagnetic interference shielding
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Published：2024-04-16 - Abstract：We utilize molecular dynamics simulations to investigate the microstructures of ions and polyelectrolytes in aqueous solutions under external electric fields. By focusing on the multi-body interactions between ionic components and H2O molecules, as well as their responses to the external electric fields, we clarify several nontrivial molecular features of the ionic and polyelectrolyte solutions, such as the solvations of cations and anions, clustering of the ions, and dispersions/aggregations of polyelectrolyte chains, as well as the corresponding responses of H2O molecules in these contexts. Our simulations illustrate the variations in structures of ionic solutions caused by reversing the charge sign of the ions, and elucidate the disparity in structures between anionic and cationic polyelectrolyte solutions in the presence of the external electric fields. This work clarifies the mechanism for the alternations in complex multi-body interactions in aqueous solutions caused by the application electric field, which can contribute to the fundamental understanding of the physical and chemical natures of ion-containing and charged polymeric systems.Keywords：Polyelectrolyte;Ions;Aqueous solutions;External electric fields;Asymmetric dipole
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Published：2024-04-08 - Abstract：In order to achieve efficient and durable oil-water emulsion separation, the membranes possessing high separation efficiency and mechanical strength attract extensive attention and are in great demand. In present study, a kind of polytetrafluoroethylene (PTFE)-based bilayer membrane was fabricated by electrospinning fibrous PTFE (fPTFE) on an expanded PTFE (ePTFE) substrate. The morphological observation revealed that the fibrous structure of the fPTFE layer could be tailored by controlling the formulation of spinning solution. The addition of appropriate polyoxyethylene (PEO) would make the fibers in the fPTFE layer finer and more uniform. As a result, the compounded membrane exhibited a small pore size of approximately 1.25 μm and a substantial porosity nearing 80%. This led to super-hydrophobicity, characterized by a high water contact angle (WCA) of 149.8°, and facilitated rapid oil permeation. The water-in-oil emulsion separation experiment further confirmed that the compounded membrane not only had a high separation efficiency closing 100%, but such an outstanding separation capacity could be largely retained, either through multiple cycles of use or through strong acid (pH=1), strong alkali (pH=12), or high-temperature (100 °C) treatment. Additionally, the mechanical behavior of the bilayer membrane was basically contributed by that of each layer in terms of their volume ratio. More significantly, the poor creep resistance of fPTFE layer was suppressed by compounding with ePTFE substrate. Hence, this study has laid the groundwork for a novel approach to create PTFE-based compounded membranes with exceptional overall characteristics, showing promise for applications in the realm of emulsion separation.Keywords：ePTFE;Electrospinning membrane;Bilayer compounding;Emulsion separation
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Published：2024-04-03 - Abstract：In this study, flexible and highly conductive composite rubber at low filler content was successfully prepared through polydopamine-assisted electroless silver plating plus mechanical mixing. Firstly, carbon fibers (CF) were activated by polydopamine (PDA) to improve the surface activity by self-polymerization reaction. Next, because of the metal chelating ability of PDA, silver layer was firmly deposited on the surface of CF through a facile electroless silver plating method. Finally, flexible silver-plated carbon fibers (Ag/pCF) silicone rubber composites prepared by mechanical mixing. By using X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD), the chemical composition and crystal structure of Ag/pCF were examined, and scanning electron microscopy (SEM) was used to assess the surface morphology of the Ag/pCF. The results showed that a uniform and dense silver layer was formed on the surface of the CF, and the conductivity of the Ag/pCF could reach 7885 S/cm. It was noteworthy that the composite rubber filled with only 45 phr Ag/pCF had a high electromagnetic interference shielding effectiveness (100 dB) due to the low density and high aspect ratio of Ag/pCF. The composite rubber has excellent potential for application in the field of electromagnetic interference shielding.Keywords：Carbon fibers;Polydopamine;Electroless plating;Silver;Electromagnetic interference shielding
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Published：2024-04-03 - Abstract：Against the backdrop of a global paper resource shortage, there is a growing need to identify fast-growing tree species capable of producing long-lasting paper. Three plant species namely Broussonetia kazinoki, Broussonetia papyrifera and hybrid paper mulberry, belong to the Broussonetia genus, were collected from China to study their white bark suitability for pulp and papermaking. Their chemical composition revealed that the holocellulose content in Broussonetia kazinoki and Broussonetia papyrifera was more than 80%. The molecular weight distribution of several holocellulose/α-cellulose is observed by GPC, which allows us to better observe the changes of various components on the molecular weight. The yield, lignin, whiteness, and molecular weight of the pulps obtained by NaOH treatment were determined. Optical microscope was used to characterize the fiber length-width ratio and rigidity. Finally, the improvement of the fiber rigidity method based on the Kratky-Porod chain model makes it more theoretical and further reveals the influencing factors of fiber rigidity. This study demonstrates the high potentiality of these three species for papermaking applications.Keywords：Broussonetia genus;Cellulose;Alkaline pulping;Kratky-Porod chain model;Fiber rigidity
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Published：2024-04-03 - Abstract：Inkjet 3D printing has potential in the additive manufacturing of electronic circuits and devices. However, inks that can be used for printing layers with T5%>300 °C or hardness>200 MPa have been rarely reported. Cyanate ester (CE) polymers have excellent thermal stability, high strength, and low shrinkage compared to other common dielectric inks for inkjet 3D printing, but cannot be quickly shaped by ultraviolet (UV) irradiation or thermal treatment. Combining CEs with UV-curable monomers may be a possible way to accelerate crosslinking, but there are challenges from the adverse effects of the dilution of both monomers. In this study, dielectric inks with acrylate and cyanate moieties were developed. The low viscosity and surface tension of the CE precursor (Bisphenol E cyanate ester) were combined with photocurable acrylate diluent monomers and cross-linker to realize an ink suitable for inkjet 3D printing. An internal dual three-dimensional cross-linked network structure resin was prepared by a combination of photocuring and thermal curing with T5% up to 326.69 °C, hardness up to 431.84 MPa, dielectric constant of 2.70 at 8 GHz, and shrinkage of 1.64%. The developed dielectric inks can be applied to the 3D printing of printed circuit boards and other electronic devices that require dielectric properties.Keywords：Inkjet printing;Cyanate ester resin;3D doubly cross-linked network;Good thermal stability
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Published：2024-03-29 - Abstract：Polyampholyte gels, which have hierarchical structures, exhibit excellent self-healing properties and have great promise for biomaterials and bioengineering. We investigated the relationship between microscopic structures and macroscopic viscoelastic properties of polyampholyte gels and found three factors influencing their viscoelastic properties, including the chemical crosslinking bonds, topological entanglements controlled by monomer concentration, and the ionic bonds. Ionic strength plays a major role on the strength of ionic bonds. A crossover point of elastic modulus and loss modulus was observed in the dynamic frequency sweeps at low monomer concentration or low chemical crosslinking density for gels with intermediate strength of ionic bonds. The solid-liquid transition signaled by the crossover point is a typical feature of dynamic associated gels, representing the dynamical association-dissociation of the ionic bonds and full relaxation of the topological entanglements in the gel network. While the crossover point disappears when the ionic bonds are too weak or too strong to form “permanent” bonds. Consistently, in the non-linear yielding measurement, gels with intermediate strength of the ionic bonds are ductile and yield at very large shear strain due to the self-healing properties and the dynamic association-dissociation of the ionic bonds. But the self-healing properties disappear when the ionic bond strength is too weak or too strong. Our work reveals the mechanism of how the dynamic association-dissociation of ionic bonds influences both the linear and non-linear viscoelastic properties of the polyampholyte gels.Keywords：Polyampholyte gel;Ionic bond;Topological entanglement;Self-healing;Hierarchical structure
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Published：2024-03-29 - Abstract：Wood, a readily available and sustainable natural resource, has found widespread use in construction and furniture. However, its inherent flammability poses a potential fire risk. Although intumescent fire-retardant coatings effectively mitigate this risk, achieving high transparency in such coatings presents a significant challenge. In our approach, we employed a cross-linked network of phytic acid anion and N-[3-(trimethoxysilyl) propyl]-N,N,N-trimethylammonium cation to create a transparent "three-in-one" intumescent coating. The collaborative P/N/Si flame-retardant effect markedly improved the intumescent char-forming capability, preventing the wood from rapid decomposition. This resulted in a substantial reduction in heat release (13.9% decrease in THR) and an increased limiting oxygen index (LOI) value of 35.5%. Crucially, the high transparency of the coating ensured minimal impact on the wood's appearance, allowing the natural wood grains to remain clearly visible. This innovative approach provides a straightforward method for developing transparent intumescent flame-retardant coatings suitable for wooden substrates. The potential applications extend to preserving ancient buildings and heritage conservation efforts.Keywords：Fire-resistant coating;Flame retardancy;Wood;Transparency
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Published：2024-03-29
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