POLYMER DEGRADATION AND STABILITY
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2025
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IF 7.4
Jiaqi Wang,Yin Lu,Ruiyu Yuan,Kan Zhang
The increasing frequent occurrence of fire accidents alone with the desirable sustainable development have accelerated searching for more resilient and safer flame-retardant polymers derived from natural renewable resources. Here we have successfully designed and synthesized bio-based benzoxazine monomers ( PH-fa-[ 2 -ph, 4 -DEP] and PH-fa-[ 2 - o OHph, 4 -DEP] ) with oxazine ring substituted by diethyl phosphite (DEP) via hydrophosphonylation for the first time, thereby achieving non-flammable green thermoset materials. Specifically, PH-fa-[ 2 - o OHph, 4 -DEP] with phenolic -OH group also shows a latent catalytic feature through its in-built intramolecular hydrogen bonding. As a result, we chose this newly synthesized monomer as both latent catalyst and flame retardant for enhancing the comprehensive properties of the well-commercialized benzoxazine resin (BA-a). The peak curing temperature of BA-a thermosetting system was decreased 23.3°C and the glass transition temperature of resulting thermoset increased by 61.7% with only adding 3 mol% of PH-fa-[ 2 - o OHph, 4 -DEP] . Finally, the mechanistic insights into both advantages including low curing temperature and excellent flame retardancy have been discussed. With this work we demonstrate the possibilities for achieving bio-based non-flammable thermosets using benzoxazine chemistry, and offer molecular level insights into the functions, paving the way for new applications of green thermosetting resins for high-performance non-flammable composite materials.
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高影响因子
JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
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2025
·Vol. 40
·期 4
·946-952
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IF 1.1
Guo Jiahua,Wei Tao,Huagn Zhixiong,Deng Zongyi,Shi Minxian
We aimed to enhance the flame retardancy of epoxy resin (EP) by synthesizing a novel, halogen-free flame retardant through a one-pot method. The synthesis utilized 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO), furfurylamine (FA), and benzene propionaldehyde (BPA) as raw materials. We conducted differential scanning calorimetry (DSC) analysis to investigate the effects of FPD on the curing process and thermal properties of EP. Our findings reveal that incorporating FPD into EP can facilitate a faster curing process and increase the carbon residue post-combustion. Specifically, the FPD/EP-7 composite demonstrates a limiting oxygen index (LOI) of 34.9% and achieves a UL-94V-0 rating with a phosphorus content of 0.91wt%. These results indicate that FPD significantly enhances the thermal stability and charring rate of EP, thereby improving its flame retardancy. Although the addition of FPD slightly reduces the mechanical properties of EP, the composite material maintains excellent performance.
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ACS Applied Polymer Materials
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2025
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IF 4.7
Wenlin Zhang,Jiahua Meng,Yongjin Zou,Chuanguo Ma,Yuqi Liu
Simultaneously achieving high performance and green benzoxazine resins is challenging yet highly significant. In this work, a bifunctional benzoxazine monomer, HT-fa, was successfully synthesized using a green strategy with hydroxytyrosol as the phenol source and furylamine as the amine source, and the monomer demonstrated excellent processability. Cured HT-fa resin, poly(HT-fa), exhibited a high glass transition temperature (Tg) of 297 °C and an initial decomposition temperature (Tdi) of 354 °C. Additionally, it demonstrated exceptional flame retardancy, with a limiting oxygen index (LOI) of 44.1%, a heat release capacity (HRC) of 21.3 J/g·K, a total heat release (THR) value of 2.9 kJ/g, and a flame-retardant rating of UL-94 V-0. Notably, its LOI, HRC, and THR were superior to those of all benzoxazines synthesized using biomass-derived amine and phenolic sources and a solvent-free method. The excellent properties of HT-fa and poly(HT-fa) are due to their unique rigid-flexible molecular structures. In addition, HT-fa can be used as a modifier for the commercially available bisphenol A/aniline based benzoxazine (BA-a). The addition of HT-fa not only significantly reduces the curing temperature of BA-a but also enhances the heat-resistance and flame-retardant properties of the cured resins. Poly(HT-fa) and these copolymers have potential applications in the field of halogen- and phosphorus-free flame-retardant materials.
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POLYMER BULLETIN
·
2025
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IF 4
Gorar Athar Ali Khan,Zhiyi Guo,Zhicheng Wang,Daham Abbas,wang Xudong,Wang Jun,Liu Wen-Bin
Using agricultural waste as biocarbon material is a recent development with many potential applications. Nutshells can be utilized to produce biocarbon, enhancing the electrical properties of thermoset composites. In this research, Walnut shells (WSs) were carbonized at 750 °C, and activated carbon filler was thoroughly examined. Isothermal compression molding was used, and composites were produced by incorporating 1–2.5 wt.% of carbonized bio-filler (CW) into Vanillin-furfuryl amine-derived bio-benzoxazine. The composites showed improved thermal stability, increasing from 293 to 321 °C; Char yield enhanced from 53.3% to 60.4%. The flexural modulus and flexural strength exhibited enhancements of 41.3% and 20%, respectively, while toughness significantly increased from 0.87 to 0.94 N-mm compared to the neat matrix. Heat deflection temperature tests showed improved thermomechanical properties in composites. Flammability tests indicated that they are flame-resistant and fire-safe due to the CW filler. Thermal conductivity enhanced by 6%, and dielectric characteristics increased by 56.7% with 2.5 wt.% filler reinforcement. With the above findings, these composites can be utilized in designing parts exposed to fire, high temperatures, efficient energy storage, enhanced functionality in electronic devices, and improved insulation efficiency.
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EUROPEAN POLYMER JOURNAL
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2024
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IF 5.8
Bowen Yang,Xin Chen,Yuqi Li,Hong Ruan
Improving the mechanical properties, self-healing capabilities, and recyclability of friction layer materials is crucial for the advancement of high-performance triboelectric nanogenerators (TENG). In this study, self-healing cross-linked polyurethanes were synthesized through the prepolymer technique, employing the Diels-Alder (D-A) reaction between the furan ring and Bismaleimide (BMI). The tensile strength of PU film with 10 wt% MBI is 54 MPa, and the shape recovery rate is 96.99 %. Moreover, it exhibits excellent self-healing and recyclable characteristics. Surface cracks can be healing within 10 min under heat, reshaped through hot pressing, while retaining 93.3 % of its mechanical properties. Additionally, the 2 cm × 2 cm area PU-based TENG can generate a short-circuit current, open-circuit voltage, transferred charge, and power density of 3.6 μA, 89 V, 29 nC, and 2.5 W/m 2 , respectively, at a frequency of 1 Hz. Futhermore, the self-healing efficiency of mechanical properties and the triboelectric output performances were found to reach 93.3 % and 98 %, respectively, after reprocessing. This study introduces a promising method for enhancing self-healing, shape memory characteristics, and the design of wearable TENG devices.
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COMPOSITES PART B-ENGINEERING
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2024
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IF 12.7
Xinbei Zhu,Jingkai Liu,Kerong Yang,Liyue Zhang,Shuaipeng Wang,Xiaoqing Liu
Micro-nano encapsulation strategy combining three-dimensional (3D) porous carriers and phase change materials (PCMs) has been widely investigated due to its structure stability, high efficiency, and designability. However, the current 3D scaffolds suffering from structure regularity are hard to meet the urgent requirements of high energy conversion efficiency and versatile applications. Herein, a 3D porous graphene scaffold (2LrGO@LIG), which is fabricated from polybenzoxazine/graphene oxide (GO) composite using laser irradiation that structurally engineers a gully-shaped surface and a 3D overlapped graphene networks, was employed for PCMs encapsulation. The addition of GO is proved to enhance the quality of produced laser induced graphene (LIG), which could also be reduced into laser-reduced graphene oxide (LrGO) and connect the adjacent LIGs as thermal bridges. As a consequence, the obtained phase change composite (2LrGO@LIG/MA) showed photo-thermal and electro-thermal conversion efficiency of 94.1 % and 99.1 %, respectively. In addition, benefiting from the surface hydrophobicity (135°), high energy storage density (167.7 J/g) and electrical conductivity (307.9 S/m), 2LrGO@LIG/MA also demonstrated great potential in smart building materials and wearable electronic devices. This study provides a facile method for designing advanced PCM composites with multi-energy conversion capacity and application versatility.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Danbin Zhu,Chenyang Guo,Haocheng Liu,Jiaofeng Ye,Haoran Chen,Jianbin Zhang,Yanhua Liu,Libang Feng
Thermal reversible Diels-Alder reaction (DA) is widely used to prolong the lifespan of polyurethane and cut down maintenance costs. However, it requires high temperature to repair damages with limited repair efficiency. In this study, a novel dual dynamic covalent bonds-based self-healing polyurethane (SPU-DA) with remarkable room temperature repair capability is fabricated by incorporating a custom-made chain extender containing disulfide bonds into DA bonds-based polyurethane. The resultant SPU-DA exhibits good comprehensive mechanical properties, and the tensile strength and elongation at break can reach 9.87 MPa and 636 %, respectively. Meanwhile, cracks emerged in SPU-DA can be repaired efficiently by the synergetic actions of the exchange of disulfide bonds, dissociation of hydrogen bonds, and the thermal reversible DA reaction. Furthermore, SPU-DA can be repaired multiply and the self-repair efficiency reaches 90.1 % at 120 °C and maintains a considerable 71 % even after three damage-repair cycles. More importantly, the as-prepared SPU-DA demonstrates the ability to heal at lower and room temperature. The repair efficiency of 41.3 % is achieved even at room temperature for 24 h without any additional treatment. Therefore, this research offers an ideal method to balance the rigidity provided by Diels-Alder bonds and the self-healing efficiency offered by the disulfide bonds. SPU-DA will be a potential functional material to be utilized in a wide range of engineering applications.
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ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Yuqi Liu,Li Yuan,Guozheng Liang,Aijuan Gu
Developing biomass resins with high thermal resistance and mechanical performance through a green strategy is an interesting challenge. Increasing the functionality of oxazine ring is favorable to improve the thermal resistance and mechanical strength of resins; however, no tri- or more functional benzoxazine monomers synthesized using the green strategy have been reported. Herein, two novel trifunctional benzoxazine monomers (coded as DPTA-f and DPTR-f) with very low melting points (61, 49 °C) were synthesized using biomass raw materials (diphenolic acid, tyramine, tyrosol, and furfurylamine) and green solvents (ethanol and water). The cured resins of DPTA-f and DPTR-f, designed as P(DPTA-f) and P(DPTR-f), not only exhibit high storage moduli (3600 and 3080 MPa) and high tensile strength (65.0 and 55.1 MPa) but also have high glass transition temperature (Tg = 328, 302 °C) and initial degradation temperature (351 and 350 °C), especially P(DPTA-f) exhibits bigger Tg than all benzoxazine resins prepared using the green strategy (SCI database). They also have good flame retardancy. The above excellent processing nature of DPTA-f and DPTR-f together with competitive thermal resistance and mechanical strength of two cured resins benefits from the unique chemical and aggregate state structures of the biobased benzoxazines.
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Advanced Healthcare Materials
·
2025
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IF 9.6
Linying Yan,Masoumeh Kianfar,Yuqian Liu,Yang Huang,Huining Xiao,Farzad Seidi
The development of injectable hydrogel wound dressings with inherent antibacterial and antioxidant properties for treating full-thickness skin injuries represents one of the most promising solutions in clinical care. In this study, a series of injectable hydrogels with tunable gelation times is designed and prepared through the Diels-Alder (DA) reaction between diene-functionalized quaternary cellulose and maleimide-grafted quaternary chitosan. The high degree of substitution of diene and maleimide groups on these polysaccharides enables the formation of highly crosslinked hydrogels. By fine-tuning the structure of the dienes, the gelation time can be reduced to 4 min at 37 ° C. Both precursors and hydrogels showed strong antibacterial activity with killing efficacies >98% against E. coli and S. aureus . Meanwhile, the encapsulation of epigallocatechin gallate (EGCG, a green tea derivative) endowed the hydrogel with strong antioxidant performance. Moreover, the hydrogel exhibited good biocompatibility with 100% cell viability for NIH3T3 cells. In vivo wound healing assessment in a mouse full-thickness skin defect model revealed that the optimum hydrogel exhibited significant collagen deposition and vascularization, as well as remarkable regenerative wound healing performance, demonstrating its great potential as a bio-based wound dressing for improving wound healing.
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PubMed
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Kuiling Wei,Xuejuan Cao,Yan Wu,Xiaoyu Yang,Boming Tang,Tianqiang Jiang
Recycling thermosets is essential for environmental protection and the sustainable development of a circular economy. Among various approaches, dynamic chemistry has proven to be an effective solution for recycling thermosetting polymers. To improve the sustainability of thermosetting polyurethanes and investigate their thermoreversible behavior with different combinations of disulfide bonds and Diels–Alder bonds, this study developed castor oil-based polyurethane vitrimer (Co-PUV 1/Co-PUV 2/Co-PUV 3) with varying dynamic covalent networks. The chemical structure, dynamic reversible reactions, rheological characteristics, and thermal-responsive self-healing were analyzed. The results revealed that disulfide bonds, combined with Diels–Alder bonds, can significantly enhance the thermoreversible response of the crosslinked networks. The first-rank combination was found in Co-PUV 2, which contained Diels–Alder bonds and 4.22 mol% disulfide bonds. This sample exhibited the shortest stress relaxation time and the largest creep range between 60°C and 100°C. Additionally, Co-PUV 2 achieved an 84.4% recovery rate of mechanical properties at 85°C and 0.3 MPa and regained its melt-recyclability at 135°C. In general, this work provides insights into the influence of disulfide and Diels–Alder bonds on the thermoreversible behavior of castor oil-based polyurethane vitrimer, enlightening a foundation for the design of recyclable polyurethane using a multi-dynamic bond strategy.
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Surfaces and Interfaces
·
2025
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IF 6.3
Hengrui Hu,Junying Chen,Xia Huang,Jiachang Chen
Limited research exists on the temporary protection of unearthed bronzes during transportation to museum environments. An eco-friendly protective coating for bronzes featuring corrosion inhibition, reinforcement, and nondestructive peeling was developed. The HV-PA+ L -Arg composite microgel was prepared by mixing polyvinyl alcohol/polyethylene glycol diacrylate microgel (PA) with l -arginine-containing pre-crosslinking solution (HV) followed by centrifugation. Results from colorimetric analysis showed that the composite microgel did not alter the appearance of bronzes. Electrochemical impedance spectroscopy revealed a corrosion inhibition efficiency of up to 95.72 %. The corrosion inhibition mechanism was analyzed using X-ray photoelectron spectroscopy, Raman spectroscopy, density functional theory, and molecular dynamics simulation. Compression and tensile tests quantified the reinforcement of HV-PA-based composite microgels before and after cross-linking, demonstrating that compressive strength increased by approximately 2.70-fold and tensile strength by 2.27-fold. Reinforcement mechanisms were analyzed using rheological tests and scanning electron microscopy (SEM). The nondestructive stripping performance of the HV-PA+ L -Arg composite microgel was characterized by scanning electron microscopy/energy dispersive X-ray spectroscopy and Raman. Nondestructive stripping, achievable via ethanol spraying and ultraviolet (UV) irradiation, offers dual options for flexible removal of the protective coating, ensuring subsequent restoration or reprocessing of bronze relics.
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POLYMER BULLETIN
·
2025
·
IF 4
Jing Yichen,Lu Yin,Zhang Kan
It is well-established that the oxazine ring in benzoxazine resin generally exhibits good stability at ambient temperature, but undergoes ring-opening polymerization reactions at relatively higher temperatures. To make benzoxazine resin more practical for application, it is crucial to lower its curing temperature. In this study, novel thermosetting systems were prepared by using bio-based benzoxazine derived from daidzein (Dz-fa) blending with commercialized novolac resin. Novolac resin, which contains rich phenolic hydroxyl groups, was utilized as the curing accelerator for Dz-fa. The curing behavior of the thermosetting blends as well as the properties of the resulting thermosets was systematically investigated. The curing kinetics of the bio-based benzoxazine with novolac resin were monitored using differential scanning calorimetry and in situ FTIR spectroscopy. The thermal properties of the cured resins were assessed by thermogravimetric analysis and dynamic mechanical analysis. The flexural strength of materials is tested by universal material testing machine. These results demonstrated that employing the novolac resin effectively reduced the curing temperature of the bio-based benzoxazine without sacrificing too much in terms of the thermal stability and mechanical property. Specifically, the char yield of cured resin (Yc), the glass transition temperature ( T g ) and flexural strength of Dz-fa and novolac resin blends in the ratio of 9:1 were found to be 65.0%, 314 °C and 84.05 MPa, respectively. This study provides a practical approach to lowering the curing temperature of benzoxazine resins. The thermosets with relatively high thermal stability can be achieved through implementable process, thereby potentially reducing overall costs during the production of benzoxazine-based materials.
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