Properties Of Elastomers Research Articles

Study on the influence of carbon nanotube modification on the mechanical and magnetic properties of chloroprene rubber‐based magnetorheological elastomers

AbstractThis study explores the mechanical and magnetic properties of magnetorheological elastomers (MREs) based on chloroprene rubber, enhanced with carbonyl iron powder (CIP) as the primary filler. Carbon black serves as the primary reinforcing filler, with multi‐walled carbon nanotubes (CNTs) used as a secondary filler to strengthen the rubber matrix. The primary objective of this research is to examine the effects of the mixture of iron powder with reinforcing fillers and the interaction of these fillers with the rubber matrix on the mechanical and magnetomechanical performance of MREs. CNTs, tubular nanoscale carbon molecules, significantly enhance the tensile strength and fatigue resistance when combined with the MRE matrix. During mixing, CNTs form a network structure within the MRE matrix, promoting the dissipation of accumulated heat and reducing thermal fatigue loss. The addition of 20 parts of CNTs to the CR matrix significantly improved the tensile mechanical properties, with the 100% set elongation stress increasing by up to 260% and the magnetic responsiveness increasing by 30.6%. The addition of 10 parts of carboxylated CNTs most notably enhanced the magnetorheological effect, increasing the magnetic stress relaxation rate by 78%. These enhanced properties enable MREs to provide better vibration control and comfort in automotive suspension systems, improve energy absorption and damping effects in industrial damping systems, and enhance durability and sealing performance in sealant applications.Highlights Carbonyl iron powder, carbon black, and carbon nanotubes (CNTs) were used as fillers to strengthen the chloroprene (CR) matrix magnetorheological elastomers (MREs). CNTs formed a network structure, promoting the dissipation of accumulated heat and reducing thermal fatigue loss. The tensile mechanical property of MRE with 20 parts of CNTs has been significantly improved, with an increasing magnetic responsiveness of 30.6%. Magnetorheological effect of MRE with 10 parts of CNTs has notably enhanced, with the magnetic stress relaxation rate of 78%.

An Adaptive Elastic Support Seat-Based Magnetorheological Elastomer for Human Body Vibration Reduction.

This paper introduces an electromagnetic structure utilizing the controllable mechanical properties of magnetorheological elastomer (MRE) materials through magnetic flux. An adaptive elastic foundation composed of these materials is explored for vibration reduction and frequency modulation. This study investigates these effects using both a single-mass model and a coupled human-seat model. For objects supported by the adaptive elastic foundation, increasing the magnetic flux enhances the stiffness and damping, thereby significantly reducing the peak response while slightly increasing the resonance frequency. Strategies such as increasing the magnetic flux, reducing the object mass, and minimizing the system's degrees of freedom and internal damping contribute to enhancing the vibration reduction and frequency modulation in the adaptive elastic foundation. The simulation results indicate that for a seated human (weighing between 72.4 kg and 88.4 kg), the adaptive elastic foundation reduces the head peak response by approximately 15.7% and increases the resonance frequency by approximately 3.4% at a magnetic flux of 138 mT.

CO2 derived ABA triblock all-polycarbonate thermoplastic elastomer with ultra-high elastic recovery

Although triblock polycarbonate thermoplastic elastomers (TPEs) have recently attracted great interests due to their biodegradability, insufficient attentions have been paid to improving the elastomeric properties. Through a tandem reaction strategy involving CO2 / allyl glycidyl ether (AGE) / cyclohexene oxide (CHO), poly(cyclohexene carbonate)-b-poly(allyl glycidyl ether carbonate)-b-poly(cyclohexene carbonate) (PCAC) is successfully synthesized using a metal-free Lewis acid-base pair catalyst. The synthesized PCACs are pure well-defined ABA triblock all-polycarbonate, which is supported by 1H NMR, gel permeation chromatography (GPC), and diffusion-ordered spectroscopy (DOSY). A simple modification by grafting alkylthiol chains to PCAC results in excellent TPEs named PCAC-g-S-CaH2a+1 (PCASaC). The synthesized TPEs are characterized by atomic force microscopy (AFM), thermogravimetric analysis (TG), differential scanning calorimetry (DSC), and mechanical test. They demonstrate a semi-network and semi-domain phase separation structure, wide service temperature range, good strength, high elongation, and extremely high elastic recovery properties. This low-cost, biodegradable, high-performance TPE shows great potential for applications in biomedical, wearable products, sports equipment, and other fields.

Vat photopolymerization of olefinic elastomers from sulfonated ethylene-propylene-diene monomer (EPDM) latexes

Ethylene-Propylene-Diene Monomer (EPDM) rubber is recognized for elasticity over a wide temperature range and exceptional resistance to UV light and oxidative degradation. In this study, sulfonated EPDM (sEPDM) latex serves as an innovative platform for 3D printing olefinic elastomers through vat photopolymerization (VPP). The sulfonation of EPDM and subsequent neutralization with potassium hydroxide enabled the production of water-dispersible sEPDM (K-sEPDM), yielding a stable latex with an average particle diameter of 125 nm. The inherent low viscosity of the latexes allowed the direct application of elastomeric polymers during the VPP process. The photopolymerization of a scaffold precursor composition, which consisted of n-vinylpyrrolidone (NVP) and poly(ethylene glycol) diacrylate (PEGDA) in the aqueous phase of K-sEPDM latex, solidified the latex as a particle embedded hydrogel. Post-processing for removing water from the 3D printed green body facilitated coalescence of the K-sEPDM particles throughout the scaffold network, generating a second ionically crosslinked network together with scaffold as an interpenetrating polymer network (IPN). Tensile testing demonstrated tunable elastomeric properties with an ultimate strain from 315±11–453±37 % and ultimate stress from 7.6±0.5–8.2±0.3 MPa with excellent thermal recoverability. VPP of photocurable K-sEPDM with a commercial printer showcased high-resolution printing capabilities with controllable isotropic shrinkage for the printing of olefinic elastomers.

Experimental study and mechanism analysis on the effect of pre-curing time on the microstructure and mechanical properties of magnetorheological elastomers under compression

The effects of the pre-curing time before exposing the carbonyl iron particles (CIPs) filled liquid polydimethylsiloxane (PDMS) mixture to a preparatory magnetic field on the magnetorheological (MR) effects of the magnetorheological elastomers (MREs) were experimentally and theoretically investigated. The anisotropic MRE samples with different pre-curing time were firstly fabricated and their compressive MR effects were tested. The results showed that the longer pre-curing time induces the shorter and more irregular particle chains formed in the MREs, and the sample pre-cured for 20 min showed the maximum MR effect. Then based on the rheological characterization, a rheological model was proposed to predict the rheological property evolution of CIPs/PDMS mixture with respect to the pre-curing time, and a modified three-dimensional (3D) particle dynamics (PD) model was developed to simulate the particle structure evolution in the MRE mixtures under a preparatory magnetic field. The simulation results showed that short chains were first formed owing to the magnetic attraction between the adjacent particles. Then these short chains approached each other to form long chains and even thick chain-like clusters. The later process can be restrained by increasing the pre-curing time, thus more short and incompact particle chains are formed in the MREs. Lastly, simplified microstructure models representing the wavy chains were used to explore the effect of particle arrangement on the MR effect of the MREs under compression. It is found that the wavy chains with incompactly packed particles are beneficial for improving the MR effect owing to the strong transverse magnetic attraction between the neighboring particles. This work demonstrates that PD simulation is an efficiency method to predict the particle arrangement evolution in the MRE mixture, and the possibility to tailoring the microstructures of the MREs by adjusting the viscosity of MRE mixtures to improve their MR effects, while keeping a high zero-field modulus simultaneously.

Preparation and properties of high electrical conductivity elastomer from alcoholysis product of waste plastic

Preparation and properties of high electrical conductivity elastomer from alcoholysis product of waste plastic

A poly(L-lactic Acid)-based flexible piezoelectric energy harvester with micro-zigzag structures

Piezoelectric energy harvester (PEH) holds great potential for flexible electronics and wearable devices. However, the power conversion efficiency of flexible PEH (fPEH) has often been a limiting factor, especially under variable excitation. Herein, we propose a practical solution: a poly(L-lactic acid)-based fPEH with 3D-printed micro-zigzag structures. This design not only broadens the operational bandwidth and enhances low-frequency response but also offers a tangible improvement in the power conversion efficiency of fPEH. The micro-zigzag structure was designed and fabricated using a digital light processing 3D printing technique with acrylates, a method that is readily accessible to researchers and engineers in the field. Mechanical properties of the 3D-printed acrylic elastomers with different compositions were investigated to obtain the material parameters, and then fPEH with the sandwich structure was fabricated via sputtering and packaging. Subsequently, numerical simulation was conducted on the micro-zigzag structures to determine the structure sizes and oscillation frequencies of fPEH. Finally, four micro-zigzag structures with 3-, 4-, 5- and 6 mm lengths were tested to obtain oscillation frequencies of 51, 37, 22, and 21 Hz consistent with the simulation. The output voltages of fPEH are 11–30 mV with the load ranges of 60–100 MΩ. Stability evaluation showed that the fPEH can work under low frequency (<100 Hz) and broadband conditions. The micro-zigzag structure provided new insights for the design of fPEH, paving the way for more efficient and practical energy harvesting solutions in the future.

2-Cyanopropan-2-yl versus 1-Cyanocyclohex-1-yl Leaving Group: Comparing Reactivities of Symmetrical Trithiocarbonates in RAFT Polymerization.

This study introduces bis(1-cyanocyclohex-1-yl)trithiocarbonate (TTC-bCCH) as a novel trithiocarbonate chain transfer agent and compares its reactivity with the previously described bis(2-cyanopropan-2-yl)trithiocarbonate (TTC-bCP) for the reversible addition-fragmentation chain transfer (RAFT) polymerization of styrene (St), n-butyl acrylate (nBA), and methyl methacrylate (MMA). Significant findings include the effective control of Mn and low dispersities from the onset of polymerization of St and nBA showing swift addition-fragmentation kinetics, leading to similar behaviors between the two RAFT agents. In contrast, a fourfold decrease of the chain transfer constant to MMA is established for TTC-bCCH over TTC-bCP. This trend is confirmed through density functional theory (DFT) calculations. Finally, the study compares thermoplastic elastomer properties of all-(meth)acrylic ABA block copolymers produced with both RAFT agents. The impact of dispersity of PMMA blocks on thermomechanical properties evaluated via rheological analysis reveals a more pronounced temperature dependence of the storage modulus (G') for the triblock copolymer synthesized with TTC-bCCH, indicating potential alteration of the phase separation.

Humidity effect on electromechanical breakdown of dielectric elastomers subject to a ramp voltage

As is known, the external excitations, material parameters, and ambient environment may affect the electromechanical properties of dielectric elastomers (DEs), which directly induce the occurrence of electrical breakdown. In this paper, we experimentally and theoretically studied the effects of voltage ramp rate, ambient humidity, electrode material, and pre-stretch on electromechanical deformation and electrical breakdown of DEs. By coupling the above four factors, the nonlinear constitutive model and electrical breakdown model of the viscoelastic DE are developed, which are shown to be consistent with the experimental observations. Firstly, when the ramp voltages with different rate are loaded to the same value, a larger voltage ramp rate leads to a smaller stretch and a higher electrical breakdown field strength of the elastomer. Besides, as the humidity increases, the electromechanical deformation increases and the electrical breakdown field decreases. In addition, it is found that different electrode materials show diverse sensitivity to the electromechanical deformation and breakdown field. Finally, with the increase of the pre-stretch from 2 to 4, the deformation and breakdown field both show an upward trend.

Experimental and theoretical investigation of the effect of physical and chemical compatibilization on the properties of thermoplastic elastomers derived from natural rubber and polypropylene blends

The objective of this research was to improve the compatibility between Natural Rubber/Polypropylene NR/PP blends through physical and chemical compatibilization methods. The physical compatibilization involved the use of epoxidized natural rubber/maleic anhydride-grafted polypropylene (ENR50/PP-g-MA) as a dual compatibilizing agent (CA50), while the process of reactive compatibilization entailed chemically modifying NR and PP phases through the grafting maleic anhydride (MA). Several formulations were prepared by melt mixing using a Brabender plasti-corder. The effects of physical and chemical compatibilization on the technical properties were investigated. FTIR analysis revealed the emergence of two distinctive peaks corresponding to the CO group of MA grafted onto PP and NR chains. FTIR analysis has also confirmed the taking place of reactions between the polar functional groups of PP-g-MA and ENR50. The rheological properties indicated that the viscosity of the NR-g-MA/PP-g-MA is lower than those of the control blend and CA50-based NR/PP system. The mechanical and dynamic mechanical findings corroborated the improvement of interfacial adhesion between NR/PP phases, especially for the NR/PP/CA50 system. SEM examination demonstrated a more uniform dispersion of the PP phase in the CA50-based NR/PP, compared to the control blend and NR-g-MA/PP-MA. NR-g-MA/PP-g-MA exhibits greater miscibility and interaction potential compared to the control NR/PP, and less than NR/(ENR50/PP-g-MA)/PP system. DFT calculations further validate the effect of compatibilization methods on TPE blends. Specifically, Quantum molecular descriptors revealed the role of ENR50/PP-g-MA as an intermediary in facilitating compatibility between NR/PP. These findings indicate that the physical compatibilization method approach using ENR50/PP-g-MA as a dual compatibilizer is a potential compatibilizer for NR/PP.

In situ study of the effect of endogenous and exogenous agents on color stability, hardness, and surface roughness of an elastomer for facial prostheses.

To evaluate in situ the influence of sweat, oil, sunscreen, and disinfectant solution on the color stability, hardness, and roughness of elastomer for facial prostheses. Standardized and intrinsically pigmented specimens remained in contact with human skin from the same person for 30days, considering exposures (n=36 per group), absent of exposition (Control, C); sweat and oiliness contact (SO); sweat and oiliness associated with sunscreen (SOS); 0.12% chlorhexidine digluconate immersion (CD0.12%); and all agents exposed (SOSCD). The main variables were color change (CIELab and National Standard Bureau system, NBS), Shore A hardness, and surface roughness, measured at baseline and 30days. Qualitative analyses were performed by atomic force microscopy (AFM) and scanning electron microscopy (SEM). The data were analyzed by Kruskal-Wallis tests (color) and two-way ANOVA (hardness and roughness) with Sidak post-test (α=0.05). CD0.12% (1.54±0.49) and SOSCD (2.10±1.03) had similar effects and caused the smallest color changes, considered mild and noticeable (NBS), respectively. SOS promoted the greatest color change (6.99±1.43, NBS: large) and hardness (17.97±0.56); SOS promoted intermediate roughness (3.48±1.05) between SOSCD (2.25±0.53), and two similar groups: C (4.46±0.95), and CD0.12% (4.39±1.26). The qualitative analysis showed an irregular, dense, dry, and whitish layer on the surface of the specimens exposed to sunscreen, which was reduced when in contact with 0.12% chlorhexidine digluconate. Endogenous and exogenous factors are capable of altering elastomer properties. The 0.12% chlorhexidine digluconate minimized the changes caused by sweat, oil, and sunscreen.

Experimental and theoretical investigation on magnetorheological elastomers containing carbonyl iron particles coated with silane coupling agent

Magnetorheological (MR) elastomer composites, comprising soft silicone rubber, various additives, and different weight fractions of carbonyl iron particles (CIPs) coated with silane coupling agent, are produced via a novel manufacturing process in an anisotropic state. This study encompasses both experimental and modeling investigations into the dynamic viscoelastic properties of magnetorheological elastomer (MREs) in shear mode under varying magnetic fields, displacement amplitudes, and frequencies. Two MRE vibration mitigation devices are fabricated to experimentally assess the shear storage modulus and the loss factor of MREs. The experimental findings reveal a pronounced MR effect in the MRE devices, where both the shear storage modulus and the loss factor increase with rising magnetic fields, frequencies, and particle weight fractions, yet decrease with higher displacement amplitudes. A modified fractional-derivative equivalent parametric model, grounded in a magnetic field- and frequency-dependent shear modulus model along with internal variable theory, is proposed to describe the effects of these key influencing factors on the MREs’ dynamic viscoelastic properties. Comparative analysis of experimental and numerical data demonstrates that this refined mathematical model can accurately represent the dynamic viscoelastic properties of MREs.

Fundamental Principles and Emerging Opportunities for Selectively‐Solvated Block Copolymer Networks in Nonpolar Media: A Perspective

AbstractBlock polymers remain an extensively studied class of macromolecules due to their ability to self‐organize spontaneously as a result of microphase separation into a variety of ordered nanostructures, depending on the number of contiguous sequences (“blocks”) present and their sequential arrangement. These polymers are classified as multifunctional since they exhibit two or more different property sets during application. In this work, the focus is on bicomponent block copolymers composed of soft and hard segments arranged as linear triblock or higher‐order multiblock copolymers and possessing the properties of a thermoplastic elastomer (TPE). Of particular interest are selectively‐solvated TPEs, designated as TPE gels (TPEGs), with precisely‐ and composition‐tunable properties. An important aspect of TPEs and their TPEG analogs is their elasticity, which reflects the ability of the soft block(s) to form a contiguous molecular network connected by dispersed microdomains composed of the hard block. Here, the origins of microphase separation and network formation in styrenic TPEs and TPEGs are explored, and experimental, theoretical, and simulation results are examined to elucidate chemistry‐structure‐property‐processing (CSPP) relationships in these self‐networking materials. Once such relationships are established, several unconventional technologies that can directly benefit from TPEGs, along with TPEGs fabricated from TPEs possessing different chemical moieties, are likewise considered.

Filled Elastomers: Mechanistic and Physics-Driven Modeling and Applications as Smart Materials.

Elastomers are made of chain-like molecules to form networks that can sustain large deformation. Rubbers are thermosetting elastomers that are obtained from irreversible curing reactions. Curing reactions create permanent bonds between the molecular chains. On the other hand, thermoplastic elastomers do not need curing reactions. Incorporation of appropriated filler particles, as has been practiced for decades, can significantly enhance mechanical properties of elastomers. However, there are fundamental questions about polymer matrix composites (PMCs) that still elude complete understanding. This is because the macroscopic properties of PMCs depend not only on the overall volume fraction (ϕ) of the filler particles, but also on their spatial distribution (i.e., primary, secondary, and tertiary structure). This work aims at reviewing how the mechanical properties of PMCs are related to the microstructure of filler particles and to the interaction between filler particles and polymer matrices. Overall, soft rubbery matrices dictate the elasticity/hyperelasticity of the PMCs while the reinforcement involves polymer-particle interactions that can significantly influence the mechanical properties of the polymer matrix interface. For ϕ values higher than a threshold, percolation of the filler particles can lead to significant reinforcement. While viscoelastic behavior may be attributed to the soft rubbery component, inelastic behaviors like the Mullins and Payne effects are highly correlated to the microstructures of the polymer matrix and the filler particles, as well as that of the polymer-particle interface. Additionally, the incorporation of specific filler particles within intelligently designed polymer systems has been shown to yield a variety of functional and responsive materials, commonly termed smart materials. We review three types of smart PMCs, i.e., magnetoelastic (M-), shape-memory (SM-), and self-healing (SH-) PMCs, and discuss the constitutive models for these smart materials.

A physics-guided deep learning model for predicting the magneto-induced mechanical properties of magnetorheological elastomer: Small experimental data-driven

Magnetorheological elastomer (MRE) is a novel intelligent material, which shows excellent potential in vibration control applications. Previous researches have fully demonstrated that the magneto-induced shear storage modulus of MRE largely determines the vibration control effect. However, both existing theoretical and experimental ways to measure the magneto-induced shear storage modulus of MRE face their own shortage. Therefore, a novel physics-guided deep learning model is proposed to efficient predict the magneto-induced mechanical properties of MRE based on Magnetic Dipole theory and data-driven methods. A small database is built by collecting the magneto-induced shear storage modulus of MRE with different material ratios tested on a special shear rheometer. The proposed model trained with small training samples and its prediction results fit well with experimental values (average R2 of 0.99) which is superior to existing constitutive models. The training only takes 25 s, which significantly shortens the time compared to the experiment. Furthermore, the proposed model effectively predicts the magneto-induced storage modulus of MRE and has good generalization and superior transfer performance.

Ti3C2Tx MXene‐Reinforced Natural Rubber Nanocomposites with Tailored Mechanical and Antiaging Properties

Recently, MXene has been identified as a novel reinforcing material for elastomers. Also, the free‐radical scavenging ability of MXene can be used to improve the antiaging properties of unsaturated elastomers, such as natural rubber (NR). Herein, Ti3C2Tx MXene is incorporated into NR at 0–0.8 wt% to investigate the mechanical and antiaging properties of NR/MXene nanocomposites (NRMX). The resultant nanocomposites with increasing MXene content show improved tensile properties and storage modulus due to the homogeneous distribution of MXene in the nanocomposite, interfacial interaction between MXene and NR molecules, and immobilization of NR polymer chains by MXene. Also, the reduced permanent deformation and hysteresis indicate a lowered heat build‐up with increasing MXene concentration. Finally, the improved mechanical properties retention, increased glass transition temperature, reduced free radical, and –OH and CO formation upon accelerated aging confirm the enhancement of the antiaging properties of NRMX nanocomposites.

Recyclable elastomers with high mechanical performance and vibration-damping property via triple dynamic bonds

Enhancing the mechanical properties of vibration-damping elastomers with dynamic bonds is crucial for practical applications. Herein, we synthesize recyclable damping elastomers with superior mechanical strength through the incorporation of triple dynamic bonds. Firstly, linear polymers with carboxyl and imidazole groups are fabricated by random copolymerization, which consist of dual dynamic bonds (hydrogen bonds and ionic bonds). Then, 1,4-phenylenediboronic acid is introduced by solution blending and can form boron/nitrogen coordination bonds with imidazole groups, thereby converting dual dynamic bonds into triple dynamic bonds. Therefore, the resulting elastomer exhibits remarkable tensile strength of 16.29 MPa, toughness of 73.53 MJ/m3, and damping properties (maintaining tan δ > 0.3 over a temperature range of 75 °C). Furthermore, owning to the triple dynamic bonds, the elastomer retains exceptional mechanical and vibration-damping properties even after three times of recycling. This work provides a simple strategy to fabricate recyclable elastomers with high mechanical performance and vibration-damping property, which have promising and sustainable potential for practical damping applications.

Dynamic healing-assembly for biocompatible, biodegradable, stretchable and self-healing triboelectric nanogenerators

Triboelectric nanogenerators (TENGs) have great potential as power sources for on-skin and implantable electronics. However, most existing TENGs are not suitable for the above applications due to limited material choices, often characterized by rigidity, susceptibility to damage, biological incompatibility, and non-biodegradability. Herein, we developed a simple self-healing assembly strategy based on introducing dynamic Cu(II)-dimethylglyoxime-urethane groups into a biocompatible and biodegradable polyurethane elastomer, to simultaneously address the above obstacles. The coordination of Cu2+ with dynamic bonds significantly enhanced the mechanical properties of elastomer, resulting in a modulus of 9.4 MPa and toughness of 40.2 MJ/m3. These bonds also gave the elastomer skin-like self-healing capabilities, achieving a healing efficiency of 77.5 % at 80 °C. Subsequently, a highly stretchable and integrated triboelectric nanogenerator (Cu-POU TENG) with self-healing capabilities was developed. The Cu-POU TENG with an effective area of 1.5 × 1.5 cm2 produced an open-circuit voltage of 38 V in single-electrode mode. The Cu-POU TENG could restore its original electrical properties through self-healing after mechanical damage. Furthermore, the Cu-POU TENG exhibited biocompatibility and biodegradability, making it suitable for on-skin and implantable electronics. Notably, the Cu-POU TENG maintained a stable voltage output throughout the degradation process. The integration of self-healing feature enabled a sophisticated structure, allowing the Cu-POU TENG to function effectively as a motion sensor for tracking body movement. This Cu-POU TENG holds great potential for applications in on-skin and implantable electronics.

Physical, magnetic, morphological, and optical properties of isotropic magnetorheological elastomers with cobalt as fillers for assistive sensor devices applications

Physical, magnetic, morphological, and optical properties of isotropic magnetorheological elastomers with cobalt as fillers for assistive sensor devices applications

Interpenetrating polymer networks of polyurethane and polytriazole: Effect of the composition and number average molecular weight of glycidyl azide polymer on the mechanical properties and morphology

AbstractOn account of some special advantages of interpenetrating polymer networks (IPNs), the preparation of IPNs with excellent properties may be a promising way to strengthen the polyurethanes (PUs) and toughen the glycidyl azide polymer (GAP) based polytriazoles (PTAs). This work provides the effect of composition and number average molecular weight (Mn) of GAP on the mechanical properties and morphology of full‐IPNs. A series of IPNs based on the crosslinked Ace‐terminated GAP (Ace‐GAP) as polytriazole phase and crosslinked hydroxy‐terminated liquid fluorinated polymer (HTLF‐1500) as polyurethane phase (namely, GAP‐HTLF‐X full‐IPNs) were successfully fabricated via in situ polymerization without any catalysts at 80°C by azide–alkynyl click chemistry and hydroxyl‐isocyanate urethane reaction. These IPNs were characterized using attenuated total reflectance/Fourier‐transform infrared spectroscopy (ATR/FTIR), uniaxial tensile testing, swelling measurement, and scanning electron microscopy (SEM). The tensile strength of GAP‐HTLF full‐IPNs gradually increased by increasing the weight ratio of Ace‐GAP, but the breaking elongation dramatically decreased compared with elongation at break of HTLF polyurethane. In addition, a small Mn of GAP is beneficial in enhancing the tensile strength, elongation at break and toughness of the IPNs. However, a small Mn of GAP corresponds to increased difficulty of preparing GAP‐HTLF full‐IPNs. GAP1k‐HTLF full‐IPN was not successfully prepared. When the Mn of GAP was 2000 g/mol, the GAP2k‐HTLF‐80 full‐IPN exhibited prominent mechanical performance with a tensile strength of 83.1 MPa, elongation at break of 28.5% and fracture energy of 99.1 kJ/m3. Swelling measurement showed that when the weight ratio of GAP with larger Mn (5, 3, and 2 k) increased to more than 70%, the molecular interpenetration existed in the IPNs, demonstrating the presence of additional physical crosslinks and entanglement for full‐IPNs. SEM studies revealed that highly formed interpenetration and few microphase separations can be observed on the fracture surface of the IPNs with optimal mechanical properties. Combined with the results of mechanical properties, swelling measurement, and SEM studies, the degree of molecular interpenetration and microphase separation were beneficial to improve the mechanical properties of elastomers. This work can provide a certain guiding significance for the preparation of IPN with excellent properties.