Remarkable Toughness Research Articles

Study on mechanical properties and curing properties of shear‐thickening gel toughened epoxy resin

AbstractThe shear‐thickening gel (STG) is introduced as a toughening agent into the epoxy resin (EP) to improve the toughness and impact resistance of the EP without significantly increasing its viscosity. By utilizing the unique BO dynamic bonds present in STG, the EP/STG composite exhibits remarkable toughness at low strain rates due to the gradual disentanglement of molecular chains. Conversely, at high strain rates, the disentanglement of molecular chains is hindered, resulting in a pronounced impact hardening effect and overall superior impact resistance. Our findings reveal that when STG is added at a concentration of 15%, the EP/STG composite material attains its peak mechanical performance. Specifically, it demonstrates a tensile strength of 31.8 MPa and a modulus of elasticity of 550.6 MPa. Furthermore, compared to pure EP, the EP/STG composite experiences an increase in elongation at break and impact strength by 40% and 8.1%, respectively. Additionally, the introduction of hydroxyl and B atoms in STG promotes the ring‐opening reaction of epoxy groups during the curing process of the EP, thus accelerating the curing reaction rate. These insights provide a solid theoretical foundation for optimizing the performance of EPs in engineering applications.Highlights The STG was actively utilized to enhance the toughness of EP. The modified EP system exhibits significant improvements in toughness and impact resistance without a notable increase in viscosity. The promotional effect of STG on the curing of EP systems was revealed through curing kinetics analysis and rheological analysis.

Development of Ultra-High-Performance Concrete Using GGBS and Alccofine

Abstract: Ultra-high-performance concrete, or UHPC, is a cementitious mixture that is distinguished by its exceptionally high compressive strength—more than 120 MPa as well as its remarkable toughness, tensile ductility, and longevity. Ground Granulated Blast Furnace Slag (GGBS) and Alccofine (AF) are commonly used in the matrix composition to increase the particle system's packing density and subsequently enhance the matrix's strength in order to guarantee that UHPC has the proper strength. To investigate the engineering properties of ternary blended UHPC with GGBS, AF, a comparative study was conducted. In comparison to the control UHPC mix, the ternary blended UHPC mix's mechanical and durability qualities were improved by the percentage variation of AF within specific bounds. In this study, the experimental work included mix proportioning and preparation of ternary blended UHPC specimens and various tests like Compressive Strength, Split Tensile Strength, Flexure Strength and RCPT (Rapid Chloride Penetration Test) were performed in the laboratory. The results show that under normal water curing conditions, the strength qualities of UHPC based on GGBS are considerable, up to a cement replacement level of 40%. In addition, compared to the binary counterpart, the mixture of 20 Percent AF and 40 Percent GGBS showed better mechanical and durability properties.

Understanding tool cutting-edge microstructure and deformation mechanism induced by adhesive wear in the turning of nickel-based superalloys

Nickel-based superalloy has great potential in the aerospace industry as key components. However, difficult-to-machine characteristics have further limited its application. Thermal-barrier coatings of the titanium-based family on carbide tools offer exceptional performance in cutting superalloys, combining high-temperature stability and remarkable toughness. This work primarily concentrates on understanding cutting-edge microstructure and deformation induced by tool adhesive wear in the turning of nickel-based superalloys with experiment and modelling. The dominant tool wear mechanisms are revealed to be adhesive wear and abrasive wear by SEM/EDS. The microstructure of the cutting-edge interface is qualitatively and quantitatively investigated by SEM/EDS and EBSD. The adhesive layer thickness at cutting edge is about 10–30 μm. The GND density of WC grains at cutting edge is 15-20 × 1014/m. The nanomechanics properties of the tool wear interface were quantitatively evaluated by nanoindentation. The average hardness of WC and Ni-superalloy at cutting-edge interface is evaluated to be 15–19 GPa and 6.2–6.5 GPa, respectively. Further, the underlying deformation mechanisms induced by tool wear behaviours are revealed through the transient heat conduction model and cutting-edge stress distribution model. This research offers a framework and mechanism for the cutting tool wear surface/interface characteristics targeted to the difficult-to-cut superalloy materials.

Fabrication of three-dimensional bicontinuous porous aluminum by vapor phase dealloying

The development of lightweight, high-specific-surface-area, and exceptionally tough porous aluminum (Al) through dealloying has been consistently captured the attention of the porous metal field. However, widely employed dealloying approaches such as electrochemical dealloying (ECD) and liquid metal dealloying (LMD) face limitations in constructing porous metals with high chemical reactivities. In this study, we employed an emerging vapor phase dealloying (VPD) method, utilizing the differences in saturated vapor pressures among alloy constituents to selectively remove elements with high vapor pressures under optimized temperature and vacuum conditions. The VPD process, characterized by its chemical-free nature and the application of high temperatures, rapidly produces porous Al with varying ligament sizes from the MgZnAl system. The resulting porous Al, distinguished by its crack-free structure and substantial ligament size, exhibits remarkable toughness. The successful fabrication of porous Al using the VPD method effectively bridges the existing gap in generating porous metals with low melting points and high chemical reactivity through ECD and LMD methods. This advancement holds significance for broadening the range of systems and application fields for porous metals.

One-step of ionic liquid-assisted stabilization and dispersion: Exfoliated graphene and its applications in stimuli-responsive conductive hydrogels based on chitosan

Conductive hydrogels, as novel flexible biosensors, have demonstrated significant potential in areas such as soft robotics, electronic devices, and wearable technology. Graphene is a promising conductive material, but its dispersibility in aqueous solutions exists difficulties. Here, we discover that untreated graphene, after exfoliation by different ionic liquids, can disperse well in aqueous solutions. We investigate the impact of four ionic liquids with varying alkyl chain lengths ([Bmim]Cl, [Omim]Cl, [Dmim]Cl, [Hmim]Cl) on the dispersibility of grapheme, and a dual physically cross-linked network hydrogel structure is designed using acrylamide (AM), acrylic acid (AA), methyl methacrylate octadecyl ester (SMA), ionic liquid@graphene (ILs@GN), and chitosan (CS). Notably, SMA, CS, AA and AM act as dynamic cross-linking points through hydrophobic interactions and hydrogen bonding, playing a crucial role in energy dissipation. The resulting hydrogel exhibits outstanding stretchability (2250 %), remarkable toughness (1.53 MJ/m3) in tensile deformation performance, high compressive strength (1.13 MPa), rapid electrical responsiveness (response time ∼ 50 ms), high electrical conductivity (12.11 mS/cm), and excellent strain sensing capability (GF = 12.31, strain = 1000 %). These advantages make our composite hydrogel demonstrate high stability in extensive deformations, offering repeatability in pressure and strain and making it a promising candidate for multifunctional sensors and flexible electrodes.

Mechanically Robust Photonic‐Ionic Skin Cross‐Linked by Metal–Imidazole Interactions

AbstractPhotonic‐ionic skins (PI‐skins) featuring multi‐signal synergistic outputs exhibit fascinating interactive sensing potential in flexible iononics. However, the existing ones are susceptible to irreversible damage in usage due to their poor toughness and deficiency in self‐healing. Herein, a novel tough mechanochromic PI‐skin is ingeniously constructed, from both molecular engineering and nanostructural engineering perspectives, via integrating the ordered photonic array and robust metal‐imidazole cross‐linked network. The PI‐skin displays synchronous structural color variation and sensitive electrical response under strain. Notably, the synergy of dense physical cross‐linking network and microphase‐separation structure achieved by strong metal‐imidazole coordination greatly promotes energy dissipation. PI‐skin possesses a combination of exceptional properties, including high fracture strength (8.22 MPa), remarkable toughness (10.23 MJ m−3), and robust adhesion behavior (2.30 MPa). Furthermore, favorable self‐healing capability at room temperature is realized thanks to the dynamic topological rearrangement of metal‐imidazole coordination. The PI‐skin demonstrates promising uses as a visually interactive wearable device for human motion monitoring and remote communication. This work not only broadens design considerations for the development of high‐performance artificial skins but also offers a general optical platform for high‐level interactive wearable devices.

Wet-spinning of reduced graphene oxide composite fiber by mechanical synergistic effect with graphene scrolling method

Carbon-based fibers have attracted attention in various field owing to their exceptional properties, including high tensile strength, thermal stability, and electrical conductivity. In particular, graphene-based high-strength fibers are promising materials in aerospace, automotive, and marine sectors. Recently, the hybrid fiber, consisting of carbon nanotubes (CNTs) and graphene with enhanced toughness was reported by deflecting cracks and enabling high deformation. However, complex synthesis and structural optimization of composite fiber with two different materials make challenge for mass production. Here, we introduce a novel graphene composite fiber, consisting of reduced graphene oxide (rGO) and scrolled rGO (SrGO), showing remarkable toughness. A multidimensional-state solution with 2D rGO and 1D SrGO was obtained by using a simple sonication technique. Mass production of high-toughness composite fibers was achieved via wet-spinning, with enhanced toughness attributed to microstructure optimization by controlling the SrGO ratio. Additionally, the use of poly(vinyl alcohol) (PVA) as the matrix facilitated high deformation, resulting in a remarkable 90.7 % increase in mechanical toughness without complex composite material synthesis.

Effect of comonomer loading on the thermal and mechanical properties of biobased copolyamides PA6/PA56

With bio-renewable and environmentally friendly nature, biobased polyamides have emerged as attractive alternatives to traditional petroleum-derived polymers. However, poor thermal and mechanical performance, high costs, and limited scalability significantly hinder their practical applications. Herein, a series of biobased copolyamides PA6/PA56 (CoPAs) were successfully synthesized from caprolactam, adipic acid, and the lysine-derived biobased monomers 1,5-pentanediamine. The copolyamides were characterized by gel permeation chromatography (GPC), nuclear magnetic resonance spectroscopy (1H NMR), wide-angle X-ray diffraction (WAXD), differential scanning calorimetry (DSC), dynamic mechanical analysis (DMA), thermogravimetric analysis (TGA), rheological analysis, mechanical testing, and scanning electron microscopy (SEM). The result shows the α to γ transition in the crystalline form of the copolyamides with comonomer loading. The melting temperature, crystallization temperature, and crystallinity gradually decrease due to the introduction of the odd-even structure, causing deviation in amide positions and reducing hydrogen bond formation between molecular chains. Furthermore, variable-temperature infrared (VTIR) analysis and density functional theory (DFT) calculations further confirm a decrease in intermolecular forces. Importantly, the mobility of the molecular chains in the amorphous region is significantly improved, endowing the copolyamides with sufficient degrees of freedom to cope with externally applied strains. Moreover, significant entanglement facilitates effective stress transfer during stretching. As a result, the synthesized copolyamides achieve a high strength of 51 MPa and a remarkable toughness of 199 MJ/m3, without sacrificing thermal stability and processing properties. These biobased CoPAs show great potential and prospects in the field of high-performance thermoplastic materials, films, and textiles.

A Healable Quasi-Solid Polymer Electrolyte with Balanced Toughness and Ionic Conductivity.

Solid polymer electrolytes (SPEs) have garnered extensive attention as potential alternatives to traditional liquid electrolytes, primarily due to their prowess in curbing lithium dendrite formation and preventing electrolyte leaks. The quest for SPEs that are both mechanically robust and exhibit superior ionic conductivity has been vigorous. However, achieving a harmonious balance between these two attributes remains a significant challenge. In this study, we introduce a novel quasi-solid electrolyte, ingeniously crafted from a poly(urethane-urea) network, enriched with lithium salts and plasticizers. This innovative composition not only boasts remarkable toughness but also ensures commendable ionic conductivity. Our post-gelation method yields gel polymer electrolytes that undergo rigorous evaluation, leading to an optimized version that stands out with its exceptional room-temperature ionic conductivity (2.94×10-4 S cm-1) and outstanding toughness (11.9 MJ m-3). Moreover, it demonstrates a broad electrochemical window (4.73 V), remarkable stability across a 600-hour cycle test, a high capacity retention exceeding 80 % after 100 cycles at 0.2 C, and a noteworthy self-healing capability. This quasi-solid polymer electrolyte emerges as a promising contender to replace current liquid electrolyte solutions.

Performance of Engineered Cementitious Composites (ECC) in shield tunnel segmental joints: A comparative study with ordinary reinforced concrete

Shield tunnel segmental joints are traditionally vulnerable, limited by their tensile capacity and susceptibility to cracking. Engineered Cementitious Composites (ECC) offer a promising solution due to their superior tensile strength, exceptional crack resistance, and remarkable toughness. However, the application of ECC in tunnel segment joints remains unexplored. To address this gap, this paper conducted comprehensive full-scale tests of ECC segmental joints versus ordinary reinforced concrete (RC) segmental joints. It investigated mechanical responses including material behavior, deflection, joint action, bolt strain, crack development, and failure modes. Results revealed that: (1) ECC joints provided a 33.97 % higher stable bearing capacity and a 50 % increase in initial cracking strength compared to RC joints. (2) ECC joints excelled in crack control, maintaining crack widths below 0.2 mm, while RC joints experienced significant cracking with widths exceeding 1 mm. (3) In terms of toughness, ECC joints surpassed RC by 66 % in the elastic stage and 123 % in the normal serviceability stage, with 96 % higher ductility. (4) ECC joints significantly outperformed RC joints in bolt stress uniformity and concentration, achieving a 43.21 % reduction in average bolt stress. (5) Regarding multi-scale mechanical effects, ECC joints increased the toughness and strength advantage over RC by more than 45 % in the elastic phase. These results reveal the potential of ECC in significantly enhancing the durability and resilience of shield tunnels, particularly in harsh environments subjected to high ground stress or seismic activities.

Impact of sand to aggregate ratio on mechanical properties and micro-structures of waste crumb rubber concrete

The replacement of natural river sand with crumb rubber (CR) in crumb rubber concrete (CRC) has attracted attention for its remarkable toughness and environmentally friendly properties. Sand to aggregate ratio (SAR) needs special attention as an important parameter in the mix proportions design of CRC as the CR volume fraction will vary with the SAR, affecting the particle packing within the CRC and therefore having a significant impact on the CRC properties, such as workability, mechanical properties and micro-structures. Thus, present study discusses the impact of SAR on both fresh and hardened properties of CRC. Relationship between SAR and workability, strength (including compressive and flexural-tensile), dynamic elastic modulus and damping ratio are analyzed. Cumulative pore size distribution and micro-morphology for each mixture were assessed using mercury intrusion porosimetry (MIP) and scanning electron microscopy (SEM) technology. Results show that the workability increases slightly and then decreases significantly with increasing SAR, and the best workability is demonstrated at a SAR of 40%. Wet packing density, compressive strength, and dynamic elastic modulus showed a monotonically decreasing trend with SAR from 30% to 70% due to the weaker bonding properties of the CR particles. Flexural-tensile strength and damping ratio exhibited an initial increase followed by a decrease with SAR, reaching peak values at 50%, measured at 9.75 MPa and 1.91%, respectively. Cumulative pore volume increased from 0.3244 to 0.4315 as SAR rose from 30% to 70%, potentially contributing to the decline in compressive strength and elastic modulus. Additionally, the micro morphology appeared to be more loose with the increase in SAR. Relationship between SAR and the above indicators is modelled. Radar charts were created to analyze the influence of SAR on the overall performance of CRC. The relative area shows a significant decrease when SAR exceeds 50%.

Digital Light Processing of Soft Robotic Gripper with High Toughness and Self‐Healing Capability Achieved by Deep Eutectic Solvents

AbstractInspired by nature's flexible and adaptable organisms, soft robotics are motorless robots made from highly compliant materials to work in confined environments and manipulate delicate objects. However, soft robots often suffer from early failure because of unexpected damage. At the same time, it is challenging to manufacture the geometrically complex structures of soft robots. This study introduces resins based on deep eutectic solvents (DES) to fabricate a pneumatically driven soft gripper using digital light processing (DLP). The resins consist of choline chloride (ChCl) as a hydrogen bond acceptor, glycerol (Gly), and acrylamide (AAm) as hydrogen bond donors. By utilizing the intense hydrogen bonding within DES, the resin can be rapidly cured by photopolymerization to form tough ionogels without chemical crosslinkers. The DES ionogels exhibit remarkable toughness and self‐healing performance compared to common hydrogels. Furthermore, the ionogels show not only efficient energy‐dissipating behavior but also achieve rapid self‐recovery. Finally, the DLP‐printed soft gripper from the DES‐based resin performs successful actuation and healing of macroscopic damages. This work presents a simple strategy to 3D print a soft robotic gripper with high toughness and self‐healing capability.

Piezoionic Elastomers by Phase and Interface Engineering for High-Performance Energy-Harvesting Ionotronics.

Piezoionic materials play a pivotal role in energy-harvesting ionotronics. However, a persistent challenge lies in balancing the structural requirements for voltage generation, current conduction, and mechanical adaptability. The conventional approach of employing crystalline heterostructures for stress concentration and localized charge separation, while effective for voltage generation, often compromises the stretchability and long-range charge transport found in homogeneous quasisolid states. Herein, phase and interface engineering strategy is introduced to address this dilemma and a piezoionic elastomer is presented that seamlessly integrates ionic liquids and ionic plastic crystals, forming a finely tuned microphase-separated structure with an intermediate phase. This approach promotes charge separation via stress concentration among hard phases while leveraging the high ionic charge mobility in soft and intermediate phases. Impressively, the elastomer achieves an extraordinary piezoionic coefficient of about 6.0mV kPa-1, a more than threefold improvement over current hydrogels and ionogels. The resulting power density of 1.3 µW cm-3 sets a new benchmark, exceeding that of state-of-the-art piezoionic gels. Notably, this elastomer combines outstanding stretchability, remarkable toughness, and rapid self-healing capability, underscoring its potential for real-world applications. This work may represent a stride toward mechanically robust energy harvesting systems and provide insights into ionotronic systems for human-machine interaction.

A multiscale fracture model to reveal the toughening mechanism in bioinspired Bouligand structures

The Bouligand structure has been observed in a variety of biological materials, such as lamellar bone and exoskeleton of lobsters. It is a hierarchical and non-homogeneous architecture that exhibits excellent damage-resistant performance. This paper presents a multiscale fracture model considering the material inhomogeneity, the multiscale property, and the anisotropy to reveal the toughening mechanisms in the Bouligand structure. Firstly, the macro and micro constitutive properties of this composite are derived. Then, a multiscale fracture model is developed to characterize the local stress intensity factors and the energy release rates at the crack front of twisted cracks. Our results demonstrate that the decrease in the local energy release rate can be attributed to two-step mechanisms. The first mechanism is that the multiscale structure and the material inhomogeneity cause a release of stress near the initial crack tip. The second mechanism is that the twisted crack leads to the transformation from single-mode loading to mixed-mode loading, which enhances the fracture toughness. These results can not only reveal the toughening mechanism of the Bouligand structure but also provide guidelines for the design of high-performance composites. Statement of significanceBiological materials in nature often possess excellent mechanical properties that have not been achieved by synthetic materials. Bioinspired Bouligand structures provide prototypes for designing high-performance materials. In this study, we propose a multiscale theoretical fracture model to investigate the fracture properties of Bouligand structures with twisted cracks. We systematically consider the roles of material inhomogeneity, anisotropy, and multiscale properties. Our analysis demonstrates that the remarkable toughness of Bouligand structures results from the combined effects of material inhomogeneity and twisted cracks. This research contributes to unveiling the secret behind the outstanding toughness of Bouligand structures and provides inspiration for the development of novel designs for man-made composites.

Performance analysis of twin-layer AlTiN and TiCN coated inserts during high speed turning of SS304 with synthetic coolant at 0°C

Industries are facing challenges to machine hard materials in economical ways and to improve the output machining characteristics. In pursuit of effective problem-solving, two distinct sets of AlTiN and TiCN coated inserts were meticulously prepared. Their respective performances were subsequently compared, using the output machining parameters as reference points. AlTiN inserts are fabricated by applying a twin layer consisting of Al50Ti40N (2 µm thickness) and Al60Ti50N (3 µm thickness) over the substrate. The insert obtained from this process has exceptional strength and remarkable toughness. Another substrate is coated with a 3 µm thick layer of TiCN, as TiCN coating offers excellent resistance against shock loads and impact stress. Previous research conducted by scholars has already established the efficacy of using synthetic coolant at 0°C for machining SS304. Hence, synthetic coolant was employed in combination with the aforementioned two types of inserts during their performance testing. A comprehensive analysis revealed that the performance of twin-layer AlTiN inserts surpassed that of TiCN inserts, showcasing superior tool life, reduced tool wear, and enhanced surface finish quality. The replacement of TiCN inserts with AlTiN inserts resulted in an impressive increase of around 70% in tool life and approximately 30% in surface finish quality.

Tailoring the cage and functionality of POSS for scalable low-dielectric and tough cyanate ester hybrid resin

2EGEP-POSS and 4EGEP-POSS with larger cage size and lower functionality were synthesised to copolymeize with cyanate ester (CE) resin. The CE/2(or 4)EGEP-POSS hybrid resins exhibit remarkable toughness and low-dielectric characteristics.

Towards sturdy and sensable pressure-sensitive adhesive through hierarchical supramolecular interaction

Endowing a robust pressure-sensitive adhesive (PSA) with sensable properties is of great significance for in-situ stress detection and information encryption in the fields of electronics, energy storage, flexible sensing, etc. However, it remains great challenge due to the difficulty in balancing interfacial wetting and cohesive strength. Herein, a microphase-separated strategy is proposed to construct an ionogel with a lower modulus of 1.96MPa, a strength of 728kPa as well as a remarkable toughness of 2258.9kJ/m3, which can be used as a sturdy PSA bonded to various substrates (metals, polar plastics, non-polar plastics) under gentle pressure. The comparable modulus and cohesive strength give it an excellent adhesion strength of 1340kPa, which far exceeds most of reported high-performance PSAs. Furthermore, due to the orientation of a large number of ionic groups, the adhesion strength increases by 31.3% once a voltage of 20V is applied. Finally, the sensitive force-resistance response of such PSA that can be used for encrypted messaging was demonstrated.

Tailoring the interfacial interaction of collagen fiber/waterborne polyurethane composite via plant polyphenol for mechanically robust and breathable wearable substrate

Collagen fiber-waterborne polyurethane composites possess great potential applications in flexible wearable devices owing to their excellent biocompatibility, flexibility, and biodegradability. However, the weak interfacial interactions which result in poor mechanical strength and breathability, have significantly hindered their practical application. Herein, high-performance collagen fiber-based wearable substrates prepares by constructing a hydrogen-bonded cross-linked network structure using bayberry tannin, a natural plant polyphenol, as a coupling bridge to bind collagen fibers and waterborne polyurethane (WPU). The dynamic rupture and reformation of sacrificial hydrogen bonds on the molecular scale effectively dissipate energy under mechanical stress, endowing these composites with remarkable toughness and ultrahigh water vapor permeability (WVP). The resultant composite’s tensile strength and WVP are 100% and 60 times higher than WPU, respectively. Additionally, this cost-effective strategy enables easy large-scale composite production. This method guides the development of high-performance, multifunctional collagen fiber-based wearable composites while advancing the tannery solid waste circular economy.

Advancing high-performance tailored dual-crosslinking network organo-hydrogel flexible device for wireless wearable sensing

Conductive hydrogels are essential for enabling long-term and reliable signal sensing in wearable electronics due to their tunable flexibility, stimulus responsiveness, and multimodal sensing integration. However, developing durable and dependable integrated hydrogel-based flexible devices has been challenging due to mismatched mechanical properties, limited water retention capability, and reduced flexibility. This work addresses these challenges by employing a tailored physical–chemical dual-crosslinking strategy to fabricate dynamically reversible organo-hydrogels with high performance. The resultant organo-hydrogels exhibit exceptional characteristics, including high stretchability (up to ∼495% strain), remarkable toughness (with tensile and compressive strengths of ∼1350 kPa and ∼9370 kPa, respectively), and outstanding transparency (∼90.3%). Moreover, they demonstrate excellent long-term water retention ability (>2424 h, >97%). Notably, the organo-hydrogel based sensor exhibits heightened sensitivity for monitoring physiological signals and motions. Furthermore, our integrated wireless wearable sensing system efficiently captures and transmits various human physiological signals and motion information in real-time. This research advances the development of customized devices utilizing functional organo-hydrogel materials, making contributions to fulfilling the increasing demand for high-performance wireless wearable sensing.

Development of robust and rapid self-healing polymers for the repair of microcracks in energetic composite materials

Adhesives with exceptional toughness and self-healing properties are vital for the practical application of energetic composite materials (ECMs). However, the majority of self-healing polymers used in ECMs lack sufficient toughness. In this study, we address this challenge by incorporating asymmetric alicyclic and bent biphenyl ring structures into the hard domain units of polymers. The synthesized PUDS-3 films exhibit a remarkable toughness of up to 20.93 MJ·m−3, recovering over 90% of this toughness within just 20 min after a complete fracture. This behavior results from the synergistic interaction between dynamic disulfide and hydrogen-bonding mechanisms during the restructuring process. Furthermore, elevated temperatures led to a rapid decrease in the relaxation modulus and characteristic relaxation time of the PUDS samples, effectively accelerating crack healing. Both experimental measurements and molecular dynamics simulations demonstrated that a higher hard segment content in the adhesive corresponded to increased strength in the interfacial interaction with 1,3,5-trinitro-2,4,6-triaminobenzene (TATB). Upon accidental mechanical damage, the cracked ECMs displayed significant and efficient self-healing capabilities within 24 h at 60 °C. The utilization of these self-healing and highly toughness adhesives hold promising prospects for enhancing the safety and longevity of ECMs.