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Low-temperature self-healing polyurethane adhesives via dual synergetic crosslinking strategy

  • Yu Zhang , Jian Zheng , Xiao Zhang EMAIL logo and Yahao Liu
Published/Copyright: June 30, 2023
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e-Polymers
From the journal e-Polymers Volume 23 Issue 1

Abstract

Damage to polymer adhesives is one of the most common reasons for structural integrity damage of composite solid propellants. The introduction of self-repairing technology into the adhesive is expected to solve this problem. However, at low temperatures, the self-repairing and mechanical properties of the materials are greatly impaired, thereby limiting the application of self-repairing adhesives in composite solid propellants. In this study, based on the dual synergistic crosslinking strategy, a polyurethane adhesive exhibiting excellent self-healing and mechanical properties at low temperatures was successfully prepared. The adhesive exhibited high self-repairing efficiency and ultra-long elongation at break at low temperatures. Specifically, at a low temperature of −40°C, the self-repair efficiency was over 70% and the elongation at break was over 1,400%, which were much higher than the results of the control group. Moreover, the strength was comparable to that of the control group. This polyurethane adhesive shows excellent self-healing and mechanical properties at low temperatures and is expected to provide the strong self-healing ability and mechanical properties for composite solid propellants, alleviating the problem of structural integrity damage.

Graphical abstract

A self-healable HEPU-Zn polyurethane adhesive was prepared. Through the dual synergetic crosslinking strategy, HEPU-Zn was endowed with excellent mechanical and self-healing properties at low temperatures.

Keywords: composite solid propellants; adhesive; self-healing; mechanical performance; low temperature

1 Introduction

The composite solid propellant grain accounts for more than 90% of the total mass of a solid engine, and its performance is the key to determining the quality of a solid engine (1,2,3). However, the composite solid propellant is considered the weakest part of the whole propulsion system. It is a type of polymer energetic composite based on polymer binder and is filled with metal combustion agents, oxidizer powder, and other combustion auxiliaries (4,5,6), and its properties are highly dependent on the temperature. As a result, it shows weak mechanical properties at low temperatures (7). However, due to extreme conditions, such as temperature shock and complex loads, in the process of production, storage, transportation, and use, the propellant can easily suffer from micro-cracks and even structural damage (1), which pose a serious threat to the safety and service life of the system. At present, the occurrence of structural damage cannot be avoided, and once damage occurs, it is difficult to repair or replace it, which causes serious waste of resources and great security risks. The research and development of a composite solid propellant binder with a self-repairing function is expected to solve this problem.

Self-repair means that a material can repair its damage and maintain its structural integrity (8,9). Depending on their self-repairing performance, damaged materials can restore their original state and properties, improving their safety and durability thereby prolonging their life. Accordingly, in recent years, self-repair technology has been studied in various fields, especially in polymer materials (10,11,12). According to the repair mechanism, self-repairing materials can be divided into external (13,14,15,16,17) and intrinsic (18,19,20,21,22) self-repairing materials. White et al. (23) used a ruthenium catalyst to encapsulate a dicyclopentadiene (DCPD) repair agent in microcapsules and embedded them in an epoxy resin matrix; after the rupture of the microcapsule, the capillary diffuses the repair agent to the damaged area, polymerizes through contact with the embedded catalyst, and then repairs the crack. This method can achieve a repair efficiency of up to 75% but the number of repairs is very small. Mei et al. (24) combined dipyridine with the main chain of polydimethylsiloxane (PDMS). By exploiting the excellent fluidity of PDMS and the coordination ability of Pt2+ and dipyridine, they cross-linked each other to obtain self-repairing linear elastomers. Self-healing can be achieved by optimizing the strength of the cross-linking interaction; when the elastomer is damaged, it can heal at room temperature without any repair agent or external stimulation. Liu et al. (17) designed a new type of self-healing polyurea-carbamate by combining the adhesive protein structure of mussels with dynamic aromatic disulfide bonds. The dissociation energy of the aromatic disulfide bond is low and the free radical is stable, so the exchange reaction can be conducted under mild conditions. The results showed that the self-healing rate of the polyurea ester at room temperature was 98.4% after only 6 h and that after 30 min at 60°C was 90%. From the above results, compared with external self-repairing materials, intrinsic self-repairing materials do not need additional repairing agents and catalysts; rather, they rely on the movement and entanglement of molecular chains and dynamic reversible bonds to achieve self-repairing. As such, intrinsic self-repairing technology is more widely used.

However, some studies have shown that in intrinsic self-repairing materials, the introduction of self-repairing properties will lead to a decrease in mechanical properties because the strength of dynamic bonds is weaker than that of ordinary covalent bonds. For example, Tavakolizadeh et al. (25) designed a new type of hydrogel with high strength and rapid self-repair ability, which can self-repair in 15 min at room temperature, and the self-healing efficiency can reach 85%. However, its tensile strength is very low, and only 0.027 MPa. In addition, the mechanical and self-repairing properties of polymer materials will decrease significantly at lower temperatures. This is because the molecular chain of polymer materials is greatly hindered at low temperatures, and its migration ability is significantly reduced, which is very disadvantageous to the exchange reaction of dynamic reversible bonds, leading to a decrease or even loss of self-repair ability. For example, Li et al. (26) prepared a polymer with high stretchability and self-repair ability that can achieve healing at −20°C, but the repair efficiency is low (68 ± 2%) and the repair time is too long (72 h). Moreover, its tensile strength at −20°C is only 0.23 MPa. Sun et al. (27) synthesized a polyurea elastomer that can quickly repair surface scratches at room temperature within 100 s. However, when the temperature dropped to 0°C, the elastomer could only partially heal, even after 72 h. Moreover, its mechanical properties are poor at 0°C, and its tensile strength is only approximately 0.27 MPa. Therefore, the design of a self-repairing composite solid propellant adhesive must overcome the disadvantages of self-repair and weak mechanical properties at low temperatures, as well as the performance balance between them.

This article proposes an effective method for preparing polyurethane adhesives with excellent low-temperature self-repair and mechanical properties based on a double synergistic crosslinking strategy. Through copolymerization and double dynamic bond cross-linking, the molecular chain fluidity of polyurethane adhesive was improved, and disulfide bonds and highly dynamic reversible coordination bonds were introduced, providing the necessary conditions for low-temperature self-repairing properties and high extensibility. In this work, the self-repair and mechanical properties of the prepared polyurethane adhesive at low temperatures were characterized in many aspects.

2 Materials and methods

2.1 Materials

Hydroxyl-terminated polybutadiene (HTPB, hydroxyl value = 0.75 mmol·g−1, 99% purity), 1,4-butanediol (BDO), zinc chloride (ZnCl2), and N,N-dimethylformamide (DMF, ≥99.8% purity) were purchased from Jining Huakai Resin Co., Ltd. Hydroxyl-terminated polyethylene glycol-tetrahydrofuran copolyether (HTPE, hydroxyl value = 0.68 mmol·g−1, 99.5% purity) was purchased from Luoyang Liming Chemical Research and Design Institute Co., Ltd. Dibutyl phthalate (DBP, 99.5% purity) was provided by the Tianjin Damao Chemical Reagent Factory. Triphenylbismuth (TPB), 2-hydroxyethyl disulfide (HEDS, 90% purity), isophorone diisocyanate (IPDI, 99% purity), and tetrahydrofuran (THF) were obtained from Shanghai McLean Biochemical Technology Co., Ltd., China.

2.2 Synthesis of HEPU-Zn

First, 2.4 g of HTPB was added to a 100 mL three-necked flask and dried overnight at 60°C in a vacuum environment. Then, 1.8 mg of TPB (catalyst), 0.39 g of DBP (plasticizer), and 0.49 g of IPDI (curing agent) were thoroughly mixed, added to the flask, and stirred at 60°C under nitrogen protection for 2 h. Next, 0.6 g of HTPE was mixed well with 1 ml of DMF, and the mixture was added to the flask to conduct a copolymerization reaction for 1 h. Next, 0.27 g of HEDS (chain extender) was gradually added to the mixture, followed by stirring for 2 h to obtain the ligand. Finally, 58.6 mg of ZnCl2 was fully dissolved in 2 mL of THF and added to the mixture, reacted at 25°C for 12 h, poured into a polytetrafluoroethylene mold, and dried in a vacuum oven at 60°C for 24 h to evaporate the solvent and obtain the sample (labeled as HEPU-Zn). In addition, three control groups were fabricated, namely, the PU (HTPB was crosslinked with IPDI, and BDO was used as the chain extender instead of HEDS), EPU (without HEDS and ZnCl2, and BDO was used as the chain extender instead of HEDS), and HEPU (without ZnCl2) groups. In our experiments, the ratio of the isocyanate group to the hydroxyl group (R-value) of each group was 1.

2.3 Characterization

The structure of the coordination bonds was characterized using a Horiba Labram Raman spectrometer (Horiba Company) equipped with an Ar laser source (excitation wavelength = 633 nm, scanning range = 200–800 cm−1). The absorption spectra in the wavelength range of 400–4,000 cm−1 were analyzed using Fourier transform infrared spectroscopy (FTIR) with an infrared spectrometer (NICOLETiS10) at a resolution of 4 cm−1. In accordance with the GB/T528-92 standard, the tensile tests at −40°C and −20°C were performed at a speed of 100 mm·min−1 on an Instron 5982 material testing machine, and the results were averaged from at least three measured data. Optical microscopic images of the sample healing process were obtained using an AOSVI polarizing microscope (CM2000-3M100). For the self-healing experiments, the samples were cut into two pieces, contacted without an external force at each set temperature (−20°C or −40°C), and left to repair at this temperature for 12 h. Subsequently, they were tested on an Instron 5982 material testing machine. The tensile experiments were performed at each temperature at a speed of 100 mm·min−1, and the tensile strength ( σ b ) and elongation at break ( ε b ) values were recorded. The self-healing efficiency based on the strength and elongation at break ( η σ and η ε , respectively) was defined according to Eqs 1 and 2, respectively. In addition, frequency scanning tests of the original and repaired samples were conducted using a dynamic thermomechanical analyzer (DMA, Q800, TA Instruments) to further characterize the low-temperature self-healing performance of HEPU-Zn. The frequency scanning range was 0.1–100 Hz, and the temperature was set to −20°C or −40°C. In the stress relaxation experiments, the temperature was set to 25°C, −20°C, or −40°C, and the strain was set to 50%. The relaxation time (τ) of the polyurethane network was defined as the time required for the stress-relaxation modulus to reach 37% of its original value and was plotted on a curve:

(1) Healing efficiency ( η ε ) % = ε b of healing sample ε b of original sample %

(2) Healing efficiency ( η σ ) % = σ b of healing sample σ b of original sample %

3 Results and discussion

3.1 Material design and structural characterization

The main purpose of this study was to develop a polyurethane adhesive with superior self-healing and mechanical performances at low temperatures. To achieve this objective, dynamic bond crosslinking and copolymerization strategies were simultaneously applied to the polyurethane network (Figure 1). Initially, HTPB and IPDI were used as raw materials to synthesize long chains terminated with isocyanate groups. After the chains were copolymerized with HTPE, HEDS was added to form HEPU ligands. Finally, HEPU ligands were crosslinked with Zn2+ to obtain polyurethane (HEPU-Zn). The introduction of HTPE into HTPB effectively reduced the crosslinking density, which benefited the molecular chain mobility of polyurethane (28). In addition, HEDS can provide disulfide bonds to molecular chains. On the one hand, because the bond length of disulfide bonds is longer than that of C–C bond, the potential barrier of the molecular chain moving around the S–S axis is lower; on the other hand, the long molecular chain is decomposed into multiple-chain segments through the exchange reaction of disulfide bonds, which reduces the activation energy of the whole chain motion, thus improving the fluidity of the molecular chain and promoting the self-repair process. Moreover, the ZnCl2 formed Zn-coordination bonds with the ligands, where the zinc ions have an alternating configuration, and transformation between the tetrahedral and octahedral structure is possible. This endowed the zinc coordination bonds with high dynamic exchange characteristics and provided excellent self-repairing properties to polyurethane, especially at low temperatures (29).

Figure 1 Reaction process of HEPU-Zn samples.
Figure 1

Reaction process of HEPU-Zn samples.

Figure 2a shows the Raman spectra of HEPU-Zn, where the characteristic peaks at 245 and 319 cm−1 correspond to the stretching vibrations of Zn–N and Zn–O coordination bonds, respectively, indicating the presence of Zn–ligand bonds. The characteristic peak at approximately 626 cm−1 is due to the tensile vibration of the S–S covalent bond (30,31), suggesting the successful introduction of disulfide bonds into HEPU-Zn. Figure 2b shows the FTIR spectra of EPU, HEPU, and HEPU-Zn. Compared with the HEPU spectrum, new absorption peaks at 1,526 and 520 cm−1 are observed for HEPU-Zn, which are attributed to the stretching vibrations of Zn–N and Zn–O, respectively (29); this further indicates the presence of Zn–ligand bonds. In addition, the spectrum of EPU has a prominent absorption peak at 2,257 cm−1, which is due to the excess of –NCO groups. However, HEPU and HEPU-Zn show no characteristic –NCO peak, which indicates that –NCO is completely consumed and the disulfide bonds are successfully introduced. From the above characterization results, it is concluded that the HEPU-Zn polyurethane samples containing Zn-coordination and disulfide bonds were successfully synthesized.

Figure 2 (a) Raman spectra of HEPU-Zn and HEPU samples. (b) FTIR spectra of EPU, HEPU, and HEPU-Zn samples.
Figure 2

(a) Raman spectra of HEPU-Zn and HEPU samples. (b) FTIR spectra of EPU, HEPU, and HEPU-Zn samples.

3.2 Low-temperature self-healing performance

Figure 3 shows the tensile stress–strain curves of the original and repaired PU samples, HEPU and HEPU-Zn at −20°C and −40°C, respectively. The calculated η ε and η σ values of the HEPU-Zn polyurethane adhesive at −20°C and −40°C are shown in Figure 3c. The PU adhesive has no self-repairing ability at −20°C and −40°C, which is mainly due to its irreversible cross-linking network (32,33,34). After introducing copolymerization and disulfide bonds into the PU adhesive, the self-repair performance of HEPU at low temperatures is still very low because the disulfide bonds tend to be stable at low temperatures and its dynamic exchange capacity is essentially lost (12). Therefore, although the introduction of HTPE improves the fluidity of the molecular chain, self-repair cannot be realized without the reversible exchange reaction of dynamic bonds. After introducing Zn2+ into HEPU, the self-repairing property of the HEPU-Zn adhesive at low temperatures is significantly enhanced. Specifically, the η ε and η σ values of HEPU-Zn are as high as approximately 79.3% and 88.6% at −20°C and 72.6% and 87.8% at −40°C, respectively. This can be attributed to the following factors. First, the introduction of HTPE reduces the crystallization of the adhesive and improves the fluidity of the molecular chain. Second, although the disulfide bond cannot have a dynamic exchange reaction at low temperatures, its bond length is greater than that of C–C, which reduces the potential barrier of the molecular chain around the S–S axis (35,36,37,38), improving the dynamic characteristics of the adhesive network. Finally, although the dynamic characteristics of the Zn–urethane coordination bond are affected by low temperatures, its dynamic exchange ability is still strong and its dynamic exchange reaction helps reduce the energy barrier of the molecular chain slip, giving the adhesive network good low-temperature self-repair performance.

Figure 3 (a and b) Tensile stress–strain curves of pristine and the repaired samples of PU, HEPU, and HEPU-Zn at −20°C and −40°C. (c) The self-healing efficiency of HEPU-Zn samples at −20°C and −40°C.
Figure 3

(a and b) Tensile stress–strain curves of pristine and the repaired samples of PU, HEPU, and HEPU-Zn at −20°C and −40°C. (c) The self-healing efficiency of HEPU-Zn samples at −20°C and −40°C.

To further characterize the self-repairing performance of the HEPU-Zn adhesive at low temperatures, the original and repaired samples were tested by DMA frequency scanning, as shown in Figure 4a and b. It can be seen that the G′ and G″ values of the repaired HEPU-Zn samples at −20°C and −40°C are lower than those of the original samples, which is thought to be due to the incomplete healing of cracks. It also shows that HEPU-Zn has good self-repairing ability at −20°C and −40°C. Subsequently, stress relaxation experiments were conducted at a constant temperature and deformation rate to evaluate the recombination ability of the HEPU-Zn adhesive network to reflect its healing ability. A smaller τ value means that the recombination ability of the adhesive network is higher, which is beneficial to self-healing (39). Figure 4c shows the stress relaxation curves of the HEPU-Zn adhesive at 25°C, −20°C, and −40°C. Because the molecular chain movement is blocked at low temperatures, the recombination ability of the polyurethane network is weakened, and the value of τ increases with decreasing temperature. It is worth noting that the τ values of HEPU-Zn at 25°C and −20°C are similar, which indicates that HEPU-Zn has a strong network recombination ability at −20°C. Although the τ value of HEPU-Zn at −40°C is higher than that at 25°C, its internal stress decreased from 100% to 37% after only 22.46 min, which demonstrates the strong low-temperature recombination ability of the HEPU-Zn adhesive network. This is consistent with the above self-repairing performance test results.

Figure 4 (a and b) The DMA frequency scanning curves of pristine and the repaired samples of HEPU-Zn at −20°C and −40°C. (c) The stress relaxation curves of HEPU-Zn samples at 25°C, −20°C, and −40°C.
Figure 4

(a and b) The DMA frequency scanning curves of pristine and the repaired samples of HEPU-Zn at −20°C and −40°C. (c) The stress relaxation curves of HEPU-Zn samples at 25°C, −20°C, and −40°C.

To more intuitively characterize the self-repairing ability of the HEPU-Zn adhesive, its repair process at −20°C and −40°C was observed under an optical microscope, and the tensile condition of the damaged HEPU-Zn after repair at −20°C and −40°C was demonstrated by the manual tensile test, as shown in Figure 5a and b. It can be observed under the optical microscope that after the adhesive was repaired at −20°C and −40°C, the cracks became less noticeable, which demonstrates the excellent self-repairing ability of HEPU-Zn at low temperatures. And, in the manual tensile test, the repaired HEPU-Zn at low temperatures (−20°C and −40°C) still shows strong stretchability. Figure 5c shows the self-healing mechanism of the HEPU-Zn adhesive. When the adhesive is damaged, there will be many reversible active groups on the fracture surface, which is the key to self-repair. When the fracture surfaces are in contact with each other, with the help of excellent molecular chain fluidity, the active groups contact each other to form new coordination and disulfide bonds, leading to self-repair. In summary, the HEPU-Zn adhesive has excellent self-repairing properties at low temperatures.

Figure 5 (a) The repair process images of HEPU-Zn samples obtained under an optical microscope at −20°C and −40°C. (b) Photos of manual tensile test of damaged HEPU-Zn samples after repair at −20°C and −40°C. (c) The self-healing mechanism of HEPU-Zn.
Figure 5

(a) The repair process images of HEPU-Zn samples obtained under an optical microscope at −20°C and −40°C. (b) Photos of manual tensile test of damaged HEPU-Zn samples after repair at −20°C and −40°C. (c) The self-healing mechanism of HEPU-Zn.

3.3 Low-temperature mechanical properties

The tensile strength and elongation at break can be obtained from the stress–strain curves of the original samples of PU, HEPU, and HEPU-Zn adhesives in Figure 3 at −20°C and −40°C, as shown in Figure 6a and b. It can be seen that the PU adhesive shows higher tensile strength and lower elongation at break at −20°C and −40°C. After introducing copolymerization and disulfide bonds into the PU adhesive, the elongation at break of the HEPU adhesive increases significantly but its tensile strength decreases. This is because the introduction of HTPE reduces the crystallization of the adhesive and improves the fluidity of the molecular chain. Thus, the segmented action of the disulfide bond and its longer bond length will further reduce the activation energy of the molecular chain movement and improve the dynamic characteristics of the adhesive network, resulting in decreased strength and increased elongation at break. After introducing Zn2+ into HEPU, the elongation at break of the HEPU-Zn adhesive is further improved, and the elongation at break could still reach approximately 1,424.5% at −40°C. Moreover, its strength is also higher than that of HEPU. This can be attributed to the excellent dynamic exchange ability of the Zn–urethane coordination bond, which dissipates significant strain energy and increases the elongation at break. In addition, Zn2+ can act as a cross-linking point to increase the cross-linking density of the adhesive network, thus improving the tensile strength.

Figure 6 The elongation at break and tensile strengths of PU, HEPU, and HEPU-Zn samples at (a) −20°C and (b) −40°C, respectively.
Figure 6

The elongation at break and tensile strengths of PU, HEPU, and HEPU-Zn samples at (a) −20°C and (b) −40°C, respectively.

Figure 7 shows the DMA frequency scanning curves of the original samples of PU and HEPU-Zn binders at −20°C and −40°C, respectively. Generally, a higher G″/G′ ratio indicates better fluidity of polyurethane chains (40). In addition, the G″/G′ ratio of HEPU-Zn is significantly higher than that of PU at −20°C and −40°C, indicating that the molecular chain mobility of HEPU-Zn is higher at low temperatures, which is consistent with our previous conclusion. Based on the above analysis, the HEPU-Zn adhesive has excellent mechanical properties at low temperatures.

Figure 7 The DMA frequency scanning curves of PU and HEPU-Zn samples at (a) −20°C and (b) −40°C, respectively.
Figure 7

The DMA frequency scanning curves of PU and HEPU-Zn samples at (a) −20°C and (b) −40°C, respectively.

To further highlight the excellent self-repair and mechanical properties of the HEPU-Zn adhesive at low temperatures prepared in this study, the self-repairing temperature, repair time, self-repairing efficiency, elongation at break, and tensile strength of HEPU-Zn polyurethane are compared with those of other self-repairing materials, and the results are listed in Table 1. It can be seen that the properties of the HEPU-Zn polyurethane adhesive prepared in this study are comparably excellent. It can achieve self-repair at lower temperatures, and the self-repair efficiency can reach a higher level. Moreover, it has an ultra-long elongation at break and high tensile strength.

Table 1

Comparison of self-healing systems, self-healing temperature (T), self-healing time (t), and self-healing efficiency ( η ε , η ε ), as well as the tensile strength ( σ b ), and elongation at break ( ε b ) of the polymers reported in this work and others

References Dynamic bonds T (°C) t (h) η ε (%) η σ (%) ε b (%) σ b (MPa)
This work Quadruple hydrogen and disulfide bonds −40 12 ∼72.6 87.8 ∼1,425 7.5
−20 12 ∼79.3 88.6 ∼1,619 4.5
(41) Catechol−metal ion bonds 6 \ Partial healing ∼2,600 ∼0.015
(42) Carbonate bonds 5 1 68.7 88.9 16 5.4
(27) Hydrogen bonds 0 72 Partial healing 800 ∼0.27
(43) Fe-ligand and hydrogen bonds −15 24 \ ∼70 ∼474 0.15
(39) Zn–ligand and hydrogen bonds −20 48 Partial healing ∼230 1.1
(26) Fe-ligand and hydrogen bonds −20 72 68 ± 2 \ ∼1,825 ∼0.23
(29) Zn–ligand and hydrogen bonds −20 8 \ 97.0 ∼5,500 0.98
(44) Imine and hydrogen bonds −20 20 ∼82 \ ∼1,400 ∼0.17
(45) Boron linkages −25 30 ∼80 \ ∼175 ∼8.0
(46) Hydration of Li+ −80 0.5 68.6 \ >7,000 ∼0.02

4 Conclusions

Based on the double synergistic crosslinking strategy, a kind of HEPU-Zn adhesive with excellent self-repair and mechanical properties at low temperatures was successfully prepared by introducing zinc–carbamate coordination and dynamic disulfide bonds into the polyurethane adhesive. The adhesive has strong self-repairing ability at low temperatures, with self-repairing efficiencies as high as approximately 79.3% and 72.6% at −20°C and −40°C, respectively. In addition, HEPU-Zn has an ultra-long elongation at break, as high as approximately 1,424.5% at −40°C, which is approximately 359.5% higher than that of the PU adhesive. Moreover, its tensile strength is comparable to that of PU. The binder is expected to endow the composite solid propellant with the strong self-repairing ability and mechanical properties, alleviating the problem of structural integrity damage.

Acknowledgments

The authors would like to thank Conghua Qi from Shiyanjia Lab (www.shiyanjia.com) for the FTIR and Raman test.

  1. Funding information: This work was supported by the National Defense Pre-Research Projects (Grant No. LJ20212A031130), NSFC (Grant No. 11732012), and NSSFC (Grant No. 2020SKJJC108).

  2. Author contributions: Yu Zhang: writing – original draft, methodology, data curation, validation – verification; Jian Zheng: project administration, funding acquisition; Xiao Zhang: supervision, writing – review and editing; Yahao Liu: formal analysis.

  3. Conflict of interest: The authors state no conflict of interest.

  4. Data availability statement: All data generated or analyzed during this study are included in this published article.

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Received: 2022-09-06
Revised: 2022-10-21
Accepted: 2022-10-24
Published Online: 2023-06-30

© 2023 the author(s), published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

Articles in the same Issue

  1. Research Articles
  2. Chitosan nanocomposite film incorporating Nigella sativa oil, Azadirachta indica leaves’ extract, and silver nanoparticles
  3. Effect of Zr-doped CaCu3Ti3.95Zr0.05O12 ceramic on the microstructure, dielectric properties, and electric field distribution of the LDPE composites
  4. Effects of dry heating, acetylation, and acid pre-treatments on modification of potato starch with octenyl succinic anhydride (OSA)
  5. Loading conditions impact on the compression fatigue behavior of filled styrene butadiene rubber
  6. Characterization and compatibility of bio-based PA56/PET
  7. Study on the aging of three typical rubber materials under high- and low-temperature cyclic environment
  8. Numerical simulation and experimental research of electrospun polyacrylonitrile Taylor cone based on multiphysics coupling
  9. Experimental investigation of properties and aging behavior of pineapple and sisal leaf hybrid fiber-reinforced polymer composites
  10. Influence of temperature distribution on the foaming quality of foamed polypropylene composites
  11. Enzyme-catalyzed synthesis of 4-methylcatechol oligomer and preliminary evaluations as stabilizing agent in polypropylene
  12. Molecular dynamics simulation of the effect of the thermal and mechanical properties of addition liquid silicone rubber modified by carbon nanotubes with different radii
  13. Incorporation of poly(3-acrylamidopropyl trimethylammonium chloride-co-acrylic acid) branches for good sizing properties and easy desizing from sized cotton warps
  14. Effect of matrix composition on properties of polyamide 66/polyamide 6I-6T composites with high content of continuous glass fiber for optimizing surface performance
  15. Preparation and properties of epoxy-modified thermosetting phenolic fiber
  16. Thermal decomposition reaction kinetics and storage life prediction of polyacrylate pressure-sensitive adhesive
  17. Effect of different proportions of CNTs/Fe3O4 hybrid filler on the morphological, electrical and electromagnetic interference shielding properties of poly(lactic acid) nanocomposites
  18. Doping silver nanoparticles into reverse osmosis membranes for antibacterial properties
  19. Melt-blended PLA/curcumin-cross-linked polyurethane film for enhanced UV-shielding ability
  20. The affinity of bentonite and WO3 nanoparticles toward epoxy resin polymer for radiation shielding
  21. Prolonged action fertilizer encapsulated by CMC/humic acid
  22. Preparation and experimental estimation of radiation shielding properties of novel epoxy reinforced with Sb2O3 and PbO
  23. Fabrication of polylactic acid nanofibrous yarns for piezoelectric fabrics
  24. Copper phenyl phosphonate for epoxy resin and cyanate ester copolymer with improved flame retardancy and thermal properties
  25. Synergistic effect of thermal oxygen and UV aging on natural rubber
  26. Effect of zinc oxide suspension on the overall filler content of the PLA/ZnO composites and cPLA/ZnO composites
  27. The role of natural hybrid nanobentonite/nanocellulose in enhancing the water resistance properties of the biodegradable thermoplastic starch
  28. Performance optimization of geopolymer mortar blending in nano-SiO2 and PVA fiber based on set pair analysis
  29. Preparation of (La + Nb)-co-doped TiO2 and its polyvinylidene difluoride composites with high dielectric constants
  30. Effect of matrix composition on the performance of calcium carbonate filled poly(lactic acid)/poly(butylene adipate-co-terephthalate) composites
  31. Low-temperature self-healing polyurethane adhesives via dual synergetic crosslinking strategy
  32. Leucaena leucocephala oil-based poly malate-amide nanocomposite coating material for anticorrosive applications
  33. Preparation and properties of modified ammonium polyphosphate synergistic with tris(2-hydroxyethyl) isocynurate for flame-retardant LDPE
  34. Thermal response of double network hydrogels with varied composition
  35. The effect of coated calcium carbonate using stearic acid on the recovered carbon black masterbatch in low-density polyethylene composites
  36. Investigation of MXene-modified agar/polyurethane hydrogel elastomeric repair materials with tunable water absorption
  37. Damping performance analysis of carbon black/lead magnesium niobite/epoxy resin composites
  38. Molecular dynamics simulations of dihydroxylammonium 5,5′-bistetrazole-1,1′-diolate (TKX-50) and TKX-50-based PBXs with four energetic binders
  39. Preparation and characterization of sisal fibre reinforced sodium alginate gum composites for non-structural engineering applications
  40. Study on by-products synthesis of powder coating polyester resin catalyzed by organotin
  41. Ab initio molecular dynamics of insulating paper: Mechanism of insulating paper cellobiose cracking at transient high temperature
  42. Effect of different tin neodecanoate and calcium–zinc heat stabilizers on the thermal stability of PVC
  43. High-strength polyvinyl alcohol-based hydrogel by vermiculite and lignocellulosic nanofibrils for electronic sensing
  44. Impacts of micro-size PbO on the gamma-ray shielding performance of polyepoxide resin
  45. Influence of the molecular structure of phenylamine antioxidants on anti-migration and anti-aging behavior of high-performance nitrile rubber composites
  46. Fiber-reinforced polyvinyl alcohol hydrogel via in situ fiber formation
  47. Preparation and performance of homogenous braids-reinforced poly (p-phenylene terephthamide) hollow fiber membranes
  48. Synthesis of cadmium(ii) ion-imprinted composite membrane with a pyridine functional monomer and characterization of its adsorption performance
  49. Impact of WO3 and BaO nanoparticles on the radiation shielding characteristics of polydimethylsiloxane composites
  50. Comprehensive study of the radiation shielding feature of polyester polymers impregnated with iron filings
  51. Preparation and characterization of polymeric cross-linked hydrogel patch for topical delivery of gentamicin
  52. Mechanical properties of rCB-pigment masterbatch in rLDPE: The effect of processing aids and water absorption test
  53. Pineapple fruit residue-based nanofibre composites: Preparation and characterizations
  54. Effect of natural Indocalamus leaf addition on the mechanical properties of epoxy and epoxy-carbon fiber composites
  55. Utilization of biosilica for energy-saving tire compounds: Enhancing performance and efficiency
  56. Effect of capillary arrays on the profile of multi-layer micro-capillary films
  57. A numerical study on thermal bonding with preheating technique for polypropylene microfluidic device
  58. Development of modified h-BN/UPE resin for insulation varnish applications
  59. High strength, anti-static, thermal conductive glass fiber/epoxy composites for medical devices: A strategy of modifying fibers with functionalized carbon nanotubes
  60. Effects of mechanical recycling on the properties of glass fiber–reinforced polyamide 66 composites in automotive components
  61. Bentonite/hydroxyethylcellulose as eco-dielectrics with potential utilization in energy storage
  62. Study on wall-slipping mechanism of nano-injection polymer under the constant temperature fields
  63. Synthesis of low-VOC unsaturated polyester coatings for electrical insulation
  64. Enhanced apoptotic activity of Pluronic F127 polymer-encapsulated chlorogenic acid nanoparticles through the PI3K/Akt/mTOR signaling pathway in liver cancer cells and in vivo toxicity studies in zebrafish
  65. Preparation and performance of silicone-modified 3D printing photosensitive materials
  66. A novel fabrication method of slippery lubricant-infused porous surface by thiol-ene click chemistry reaction for anti-fouling and anti-corrosion applications
  67. Development of polymeric IPN hydrogels by free radical polymerization technique for extended release of letrozole: Characterization and toxicity evaluation
  68. Tribological characterization of sponge gourd outer skin fiber-reinforced epoxy composite with Tamarindus indica seed filler addition using the Box–Behnken method
  69. Stereocomplex PLLA–PBAT copolymer and its composites with multi-walled carbon nanotubes for electrostatic dissipative application
  70. Enhancing the therapeutic efficacy of Krestin–chitosan nanocomplex for cancer medication via activation of the mitochondrial intrinsic pathway
  71. Variation in tungsten(vi) oxide particle size for enhancing the radiation shielding ability of silicone rubber composites
  72. Damage accumulation and failure mechanism of glass/epoxy composite laminates subjected to repeated low velocity impacts
  73. Gamma-ray shielding analysis using the experimental measurements for copper(ii) sulfate-doped polyepoxide resins
  74. Numerical simulation into influence of airflow channel quantities on melt-blowing airflow field in processing of polymer fiber
  75. Cellulose acetate oleate-reinforced poly(butylene adipate-co-terephthalate) composite materials
  76. Radiation shielding capability and exposure buildup factor of cerium(iv) oxide-reinforced polyester resins
  77. Recyclable polytriazole resins with high performance based on Diels-Alder dynamic covalent crosslinking
  78. Adsorption and recovery of Cr(vi) from wastewater by Chitosan–Urushiol composite nanofiber membrane
  79. Comprehensive performance evaluation based on electromagnetic shielding properties of the weft-knitted fabrics made by stainless steel/cotton blended yarn
  80. Review Articles
  81. Preparation and application of natural protein polymer-based Pickering emulsions
  82. Wood-derived high-performance cellulose structural materials
  83. Flammability properties of polymers and polymer composites combined with ionic liquids
  84. Polymer-based nanocarriers for biomedical and environmental applications
  85. A review on semi-crystalline polymer bead foams from stirring autoclave: Processing and properties
  86. Rapid Communication
  87. Preparation and characterization of magnetic microgels with linear thermosensitivity over a wide temperature range
  88. Special Issue: Biodegradable and bio-based polymers: Green approaches (Guest Editors: Kumaran Subramanian, A. Wilson Santhosh Kumar, and Venkatajothi Ramarao)
  89. Synthesis and characterization of proton-conducting membranes based on bacterial cellulose and human nail keratin
  90. Fatigue behaviour of Kevlar/carbon/basalt fibre-reinforced SiC nanofiller particulate hybrid epoxy composite
  91. Effect of citric acid on thermal, phase morphological, and mechanical properties of poly(l-lactide)-b-poly(ethylene glycol)-b-poly(l-lactide)/thermoplastic starch blends
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https://doi.org/10.1515/epoly-2022-0083
Keywords for this article
composite solid propellants; adhesive; self-healing; mechanical performance; low temperature
Creative Commons
BY 4.0

Articles in the same Issue

  1. Research Articles
  2. Chitosan nanocomposite film incorporating Nigella sativa oil, Azadirachta indica leaves’ extract, and silver nanoparticles
  3. Effect of Zr-doped CaCu3Ti3.95Zr0.05O12 ceramic on the microstructure, dielectric properties, and electric field distribution of the LDPE composites
  4. Effects of dry heating, acetylation, and acid pre-treatments on modification of potato starch with octenyl succinic anhydride (OSA)
  5. Loading conditions impact on the compression fatigue behavior of filled styrene butadiene rubber
  6. Characterization and compatibility of bio-based PA56/PET
  7. Study on the aging of three typical rubber materials under high- and low-temperature cyclic environment
  8. Numerical simulation and experimental research of electrospun polyacrylonitrile Taylor cone based on multiphysics coupling
  9. Experimental investigation of properties and aging behavior of pineapple and sisal leaf hybrid fiber-reinforced polymer composites
  10. Influence of temperature distribution on the foaming quality of foamed polypropylene composites
  11. Enzyme-catalyzed synthesis of 4-methylcatechol oligomer and preliminary evaluations as stabilizing agent in polypropylene
  12. Molecular dynamics simulation of the effect of the thermal and mechanical properties of addition liquid silicone rubber modified by carbon nanotubes with different radii
  13. Incorporation of poly(3-acrylamidopropyl trimethylammonium chloride-co-acrylic acid) branches for good sizing properties and easy desizing from sized cotton warps
  14. Effect of matrix composition on properties of polyamide 66/polyamide 6I-6T composites with high content of continuous glass fiber for optimizing surface performance
  15. Preparation and properties of epoxy-modified thermosetting phenolic fiber
  16. Thermal decomposition reaction kinetics and storage life prediction of polyacrylate pressure-sensitive adhesive
  17. Effect of different proportions of CNTs/Fe3O4 hybrid filler on the morphological, electrical and electromagnetic interference shielding properties of poly(lactic acid) nanocomposites
  18. Doping silver nanoparticles into reverse osmosis membranes for antibacterial properties
  19. Melt-blended PLA/curcumin-cross-linked polyurethane film for enhanced UV-shielding ability
  20. The affinity of bentonite and WO3 nanoparticles toward epoxy resin polymer for radiation shielding
  21. Prolonged action fertilizer encapsulated by CMC/humic acid
  22. Preparation and experimental estimation of radiation shielding properties of novel epoxy reinforced with Sb2O3 and PbO
  23. Fabrication of polylactic acid nanofibrous yarns for piezoelectric fabrics
  24. Copper phenyl phosphonate for epoxy resin and cyanate ester copolymer with improved flame retardancy and thermal properties
  25. Synergistic effect of thermal oxygen and UV aging on natural rubber
  26. Effect of zinc oxide suspension on the overall filler content of the PLA/ZnO composites and cPLA/ZnO composites
  27. The role of natural hybrid nanobentonite/nanocellulose in enhancing the water resistance properties of the biodegradable thermoplastic starch
  28. Performance optimization of geopolymer mortar blending in nano-SiO2 and PVA fiber based on set pair analysis
  29. Preparation of (La + Nb)-co-doped TiO2 and its polyvinylidene difluoride composites with high dielectric constants
  30. Effect of matrix composition on the performance of calcium carbonate filled poly(lactic acid)/poly(butylene adipate-co-terephthalate) composites
  31. Low-temperature self-healing polyurethane adhesives via dual synergetic crosslinking strategy
  32. Leucaena leucocephala oil-based poly malate-amide nanocomposite coating material for anticorrosive applications
  33. Preparation and properties of modified ammonium polyphosphate synergistic with tris(2-hydroxyethyl) isocynurate for flame-retardant LDPE
  34. Thermal response of double network hydrogels with varied composition
  35. The effect of coated calcium carbonate using stearic acid on the recovered carbon black masterbatch in low-density polyethylene composites
  36. Investigation of MXene-modified agar/polyurethane hydrogel elastomeric repair materials with tunable water absorption
  37. Damping performance analysis of carbon black/lead magnesium niobite/epoxy resin composites
  38. Molecular dynamics simulations of dihydroxylammonium 5,5′-bistetrazole-1,1′-diolate (TKX-50) and TKX-50-based PBXs with four energetic binders
  39. Preparation and characterization of sisal fibre reinforced sodium alginate gum composites for non-structural engineering applications
  40. Study on by-products synthesis of powder coating polyester resin catalyzed by organotin
  41. Ab initio molecular dynamics of insulating paper: Mechanism of insulating paper cellobiose cracking at transient high temperature
  42. Effect of different tin neodecanoate and calcium–zinc heat stabilizers on the thermal stability of PVC
  43. High-strength polyvinyl alcohol-based hydrogel by vermiculite and lignocellulosic nanofibrils for electronic sensing
  44. Impacts of micro-size PbO on the gamma-ray shielding performance of polyepoxide resin
  45. Influence of the molecular structure of phenylamine antioxidants on anti-migration and anti-aging behavior of high-performance nitrile rubber composites
  46. Fiber-reinforced polyvinyl alcohol hydrogel via in situ fiber formation
  47. Preparation and performance of homogenous braids-reinforced poly (p-phenylene terephthamide) hollow fiber membranes
  48. Synthesis of cadmium(ii) ion-imprinted composite membrane with a pyridine functional monomer and characterization of its adsorption performance
  49. Impact of WO3 and BaO nanoparticles on the radiation shielding characteristics of polydimethylsiloxane composites
  50. Comprehensive study of the radiation shielding feature of polyester polymers impregnated with iron filings
  51. Preparation and characterization of polymeric cross-linked hydrogel patch for topical delivery of gentamicin
  52. Mechanical properties of rCB-pigment masterbatch in rLDPE: The effect of processing aids and water absorption test
  53. Pineapple fruit residue-based nanofibre composites: Preparation and characterizations
  54. Effect of natural Indocalamus leaf addition on the mechanical properties of epoxy and epoxy-carbon fiber composites
  55. Utilization of biosilica for energy-saving tire compounds: Enhancing performance and efficiency
  56. Effect of capillary arrays on the profile of multi-layer micro-capillary films
  57. A numerical study on thermal bonding with preheating technique for polypropylene microfluidic device
  58. Development of modified h-BN/UPE resin for insulation varnish applications
  59. High strength, anti-static, thermal conductive glass fiber/epoxy composites for medical devices: A strategy of modifying fibers with functionalized carbon nanotubes
  60. Effects of mechanical recycling on the properties of glass fiber–reinforced polyamide 66 composites in automotive components
  61. Bentonite/hydroxyethylcellulose as eco-dielectrics with potential utilization in energy storage
  62. Study on wall-slipping mechanism of nano-injection polymer under the constant temperature fields
  63. Synthesis of low-VOC unsaturated polyester coatings for electrical insulation
  64. Enhanced apoptotic activity of Pluronic F127 polymer-encapsulated chlorogenic acid nanoparticles through the PI3K/Akt/mTOR signaling pathway in liver cancer cells and in vivo toxicity studies in zebrafish
  65. Preparation and performance of silicone-modified 3D printing photosensitive materials
  66. A novel fabrication method of slippery lubricant-infused porous surface by thiol-ene click chemistry reaction for anti-fouling and anti-corrosion applications
  67. Development of polymeric IPN hydrogels by free radical polymerization technique for extended release of letrozole: Characterization and toxicity evaluation
  68. Tribological characterization of sponge gourd outer skin fiber-reinforced epoxy composite with Tamarindus indica seed filler addition using the Box–Behnken method
  69. Stereocomplex PLLA–PBAT copolymer and its composites with multi-walled carbon nanotubes for electrostatic dissipative application
  70. Enhancing the therapeutic efficacy of Krestin–chitosan nanocomplex for cancer medication via activation of the mitochondrial intrinsic pathway
  71. Variation in tungsten(vi) oxide particle size for enhancing the radiation shielding ability of silicone rubber composites
  72. Damage accumulation and failure mechanism of glass/epoxy composite laminates subjected to repeated low velocity impacts
  73. Gamma-ray shielding analysis using the experimental measurements for copper(ii) sulfate-doped polyepoxide resins
  74. Numerical simulation into influence of airflow channel quantities on melt-blowing airflow field in processing of polymer fiber
  75. Cellulose acetate oleate-reinforced poly(butylene adipate-co-terephthalate) composite materials
  76. Radiation shielding capability and exposure buildup factor of cerium(iv) oxide-reinforced polyester resins
  77. Recyclable polytriazole resins with high performance based on Diels-Alder dynamic covalent crosslinking
  78. Adsorption and recovery of Cr(vi) from wastewater by Chitosan–Urushiol composite nanofiber membrane
  79. Comprehensive performance evaluation based on electromagnetic shielding properties of the weft-knitted fabrics made by stainless steel/cotton blended yarn
  80. Review Articles
  81. Preparation and application of natural protein polymer-based Pickering emulsions
  82. Wood-derived high-performance cellulose structural materials
  83. Flammability properties of polymers and polymer composites combined with ionic liquids
  84. Polymer-based nanocarriers for biomedical and environmental applications
  85. A review on semi-crystalline polymer bead foams from stirring autoclave: Processing and properties
  86. Rapid Communication
  87. Preparation and characterization of magnetic microgels with linear thermosensitivity over a wide temperature range
  88. Special Issue: Biodegradable and bio-based polymers: Green approaches (Guest Editors: Kumaran Subramanian, A. Wilson Santhosh Kumar, and Venkatajothi Ramarao)
  89. Synthesis and characterization of proton-conducting membranes based on bacterial cellulose and human nail keratin
  90. Fatigue behaviour of Kevlar/carbon/basalt fibre-reinforced SiC nanofiller particulate hybrid epoxy composite
  91. Effect of citric acid on thermal, phase morphological, and mechanical properties of poly(l-lactide)-b-poly(ethylene glycol)-b-poly(l-lactide)/thermoplastic starch blends
  92. Dose-dependent cytotoxicity against lung cancer cells via green synthesized ZnFe2O4/cellulose nanocomposites
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