High Toughness Research Articles

Self-Healing Polyurethane-Urea Elastomers with High Strength and Toughness Based on Dynamic Hindered Urea Bonds and Hydrogen Bonds

Self-Healing Polyurethane-Urea Elastomers with High Strength and Toughness Based on Dynamic Hindered Urea Bonds and Hydrogen Bonds

Strong, Spontaneous, and Self-Healing Poly(Ionic Liquid) Elastomer Underwater Adhesive with Borate Ester Dynamic Crosslinking.

Adhesion in aqueous environments is often hindered by the water layer on the surface of the substrate due to the water sensitivity of the adhesive, greatly limiting the application environment. Here, a borate ester dynamically crosslinked poly(ionic liquid) elastomer adhesive (PIEA) with high strength, toughness, self-healing abilities, and ionic conductivity is synthesized by copolymerizing hydrophobic ionic liquid monomer ([HPVIm][TFSI]) and 2-methoxyethyl acrylate (MEA). The adhesion strength of PIEA can increase spontaneously from almost no adhesion to 314 kPa after 12 h without any external preloading due to the dissociation of the borate ester in water, leading to noncovalent interactions between the hydroxyl groups of PIEA and the substrate. Additionally, PIEA can be developed for soft sensors or ion electrodes to enable underwater detection and communication. This strategy offers broad application potential for the development of novel underwater smart adhesives.

Mechanically Adaptable High‐Performance p(SBMA‐MMA) Copolymer Hydrogel with Iron (II/III) Perchlorate for Wearable Thermocell Applications

AbstractQuasi‐solid‐state thermocells (QTECs) show promise as a power source for wearable devices by converting body heat into electricity. While significant progress has been made with p‐type elements for QTECs, challenges remain with their n‐type counterparts. Here, a high‐performance n‐type QTEC element is presented, using a copolymer hydrogel that outperforms conventional p‐type elements. This copolymer hydrogel combines hydrophilic zwitterionic sulfobetaine methacrylate (SBMA) for ionic conduction and hydrophobic methyl methacrylate (MMA) for structural stability. By increasing the MMA content from 35 to 100 wt.%, versatile control is achieved over the hydrogel's elastic modulus (72 kPa to 127.7 MPa) and tensile strength (54 kPa to 6.7 MPa). A high mechanical toughness of 7.2 MJ m−3 is also achieved at 68 wt.% MMA. The mechanically robust and high toughness p(SBMA‐MMA) hydrogel is then immersed in Fe(ClO4)2/3 solutions of different concentrations to evaluate its performance as an n‐type QTEC element. The hydrogel with 0.8 M Fe(ClO4)2/3 exhibits a high ionic Seebeck coefficient of −1.7 mV K−1, a power density of 1.1 mW m−2 K−2, and an elastic modulus of 1.6 MPa, which is similar to that of human skin. Finally, the optimized n‐type p(SBMA‐MMA) hydrogels demonstrate the potential application for wearable devices.

An Investigation of the Effects of Flame Straightening Heating on the High-Strength Structural Steels Microstructure

AbstractIn this research, the effects of heating cycles that are performed correctly and excessively—well above the limitations given by the steel manufacturer—on flame straightening are assessed and analyzed. The paper focuses on the microstructural changes caused by the overheating during the flame straightening process. To create geometrical changes in a metal construction, a tiny section of the element or structure is heated to the straightening temperature during the flame straightening process. Strenx® 960 is typically produced through a combination of thermomechanical rolling and quenching and tempering, resulting in a fine-grained martensitic or bainitic microstructure. These processes are designed to achieve a balance of high strength and good toughness. The microstructural changes associated with different working conditions in the case of welding include HAZ softening and grain growth. The study aimed to highlight the influence of flame hardening on the microstructure of the material.

Preparation and Sensing Applications of PAMgA/GL Conductive Hydrogels with Antifreezing, High Toughness and High Adhesion

Preparation and Sensing Applications of PAMgA/GL Conductive Hydrogels with Antifreezing, High Toughness and High Adhesion

Data-driven predictions of retained austenite content and yield strength and elucidation of the sliding wear performance of carbide-free bainitic steels

Carbide-free bainitic (CFB) steels have drawn much attention due to their high strength and toughness. The present work aims to build machine learning (ML) based surrogate models to predict retained austenite (RA) content and yield strength (YS) of isothermal transformed CFB steels and study the sliding wear performance. The input data for ML prediction were related to compositions, heat treatment process, and phases. The Random Forest regression and Gaussian process regression were respectively selected to build the predictive models for RA content and YS. Result shows that the predicted RA content agrees well with the experimentally determined ones in steel with high stability of untransformed austenite. For YS prediction, the present surrogate model can predict YS of CFB steels even without additional microstructural information such as dislocation and effective substructure size. Steels with different YS and RA content were designed to study the sliding wear performance. Result shows that the dominant wear mechanism of the tested steels is abrasive wear and the weight loss is inversely proportional to hardness when the load and wear distance are constant. Increasing YS and RA content can increase the initial hardness and work hardening ability at the worn surface, thereby enhancing wear resistance.

Designing Novel All-Polymer Nanocomposites with Pearl Necklace Chain Structure with High Strength, High Toughness, and Low Hysteresis

Designing Novel All-Polymer Nanocomposites with Pearl Necklace Chain Structure with High Strength, High Toughness, and Low Hysteresis

Super Strong and Tough PVA Hydrogel Fibers Based on an Ordered‐to‐Disordered Structural Construction Strategy Targeting Artificial Ligaments

AbstractHydrogels with high strength, high modulus, and high toughness have great application potential in the field of artificial human load‐bearing tissues, but the preparation of materials with the above high performance is still a huge challenge. In this paper, a structural construction strategy of ordered‐to‐disordered (OTD) transition is proposed to obtain hydrogel fibers with high strength, high modulus, and high toughness. The structural construction strategy of OTD refers to the ordered‐to‐disordered transition of molecular segments in PVA polymer fibers through swelling and subsequent salting‐out treatment, while still maintaining the general order of the entire polymer chain. PVA molecular chain crystallites provide physical crosslinking to stabilize the structure. The results show that the elongation at break of the hydrogel fiber can reach 257%). The strength reaches 190.04 MPa, which is more than 4 times higher than that of human ligaments. The modulus reaches 137.31 MPa, which perfectly matches the human ligaments, and the toughness can reach 100.61 MJ m−3. In addition, it has stable mechanical properties in liquid environment and excellent biocompatibility, which has great application potential in the field of artificial ligaments. This OTD structural construction strategy provides a facile approach to achieving hydrogel fibers with desired mechanical properties.

Highly Stretchable Sensitive Multiscale Hydrogel Inspired by Biological Muscles for Wearing Sensors.

Hydrogels have attracted substantial research interest for application in wearable electronics due to their stretchability, elasticity, and compliance. However, most hydrogels could not satisfy the application requirements for high-performance wearable sensors due to their poor sensitivity, low mechanical properties, and sensing detection range until this day. Inspired by the fascia in biological muscles, we propose a strategy to form entangled "clusters" through the dense entanglement between highly cross-linked elastic hydrogel microspheres and polymer segments, and prepared a multiscale hydrogel with high sensitivity and mechanical toughness. This strategy embedded highly swollen hydrogel microspheres (with different pore sizes) to act as the microregions of dense entanglement in the soft matrix to adjust the microstructure of multiscale gel. When pressure was applied, this structure could provide a fast response due to the stack layer formed by microspheres and soft matrix produced effective stress distribution, resulting in the outstanding sensitivity of the multiscale hydrogel (S = 1.1 kPa-1) in the pressure range of 0-50 kPa. The distinct microspheres functioning as microscale joint areas significantly augment energy dissipation, culminating in exceptional mechanical stability, ultrastretchability (≈1050%), and high strength of the multiscale hydrogel. The most notable progress was that the synthesized multiscale hydrogel not only combined the above advantages but also simultaneously solved multiple dilemmas of tedious synthesis steps, high cost, and poor durability. Besides, the multiscale hydrogel also had excellent antibacterial properties and biocompatibility, which enabled them to have large-scale application potential in wearable and implantable electronic devices. Our research could provide a universal approach to the creation of robust, flexible, wearable, and sensitive sensors, significantly increasing the uses of stress sensors in wearable technology.

Controlling the rheology of cellulose dissolved in 4–methylmorpholine N–oxide and tensile properties of precipitated cellulose films via mixture design

AbstractProperties which control the mechanical performance of regenerated or precipitated cellulose films are currently not well-known and a mechanistic understanding of the underlying phenomena should be established. Solution rheology is a crucial property for casting films and spinning fibres in terms of process runnability, and it can have a considerable effect on the mechanical properties of the prepared cellulose products. We hypothesized that the viscosity of cellulose dissolved in 4-methylmorpholine N-oxide (NMMO) and the mechanical properties of precipitated cellulose films could potentially be improved by controlling the molecular weight distribution of cellulose pulp, taking inspiration from traditional plastic industry. We evaluated the effects of pulp blends on the viscoelastic properties of dissolved cellulose-NMMO dopes and used the dopes to prepare cellulose films and determined their mechanical properties. Lastly, we employed the determined dope and film characteristics to build linear regression models for predicting dope rheology and mechanical performance of films. Mixture films with 2:1 and 1:2 ratios of pulps with both medium and high degree of polymerization showed in average 36% and 46% higher toughness than their unimodal versions. The model results demonstrated that film performance could be tailored by changing the pulp composition. These findings play an important role in optimizing the future processability of dissolved cellulose dopes for producing bio-based cellulose materials and could bring us a step closer to traditional plastic polymer disciplines by tailoring their performance based on pulp properties. Graphic abstract

Nanoscale Structures of Tough Microparticle-Based Films Investigated by Synchrotron X-Ray Scattering and All-Atom Molecular-Dynamics Simulation.

In this study, the nanoscale structures of microparticle-based films are revealed by synchrotron small-angle X-ray scattering (SAXS) and all-atom molecular-dynamics (AA-MD) simulations. The microparticle-based films consisting of the simplest acrylate polymer microparticles are applied as a model because the films are formed without additives and organic solvents and exhibit high toughness properties. The characteristic interfacial thickness (tinter) obtained from the SAXS analysis reflects the mixing degree of polymer chains on the microparticle surface in the film. The cross-linking density of inner microparticles is found to be strongly correlated to not only several properties of individual microparticles, such as swelling ratio and radius of gyration, but also the tinter and toughness of the corresponding films. Therefore, the tinter and toughness values follow a linear relationship because the cross-linking restricts the mixing of polymer chains between their surfaces in the film, which is a unique feature of microparticle-based films. This characteristic also affects their deformation behavior observed by in situ SAXS during tensile testing and their density profiles calculated by AA-MD simulations. This work provides a general strategy for material design to control the physical properties and structures of their films for advanced applications, including volatile organic compound-free sustainable coatings and adhesives.

Boosting the Strength and Toughness of Polymer Blends via Ligand-Modulated MOFs.

Mechanically robust and tough polymeric materials are in high demand for applications ranging from flexible electronics to aerospace. However, achieving both high toughness and strength in polymers remains a significant challenge due to their inherently contradictory nature. Here, a universal strategy for enhancing the toughness and strength of polymer blends using ligand-modulated metal-organic framework (MOF) nanoparticles is presented, which are engineered to have adjustable hydrophilicity and lipophilicity by varying the types and ratios of ligands. Molecular dynamics (MD) simulations demonstrate that these nanoparticles can effectively regulate the interfaces between chemically distinct polymers based on their amphiphilicity. Remarkably, a mere 0.1wt.% of MOF nanoparticles with optimized amphiphilicity (ML-MOF(5:5)) delivered ≈3.4- and ≈34.1-fold increase in strength and toughness of poly (lactic acid) (PLA)/poly (butylene succinate) (PBS) blend, respectively. Moreover, these amphiphilicity-tailorable MOF nanoparticles universally enhance the mechanical properties of various polymer blends, such as polypropylene (PP)/polyethylene (PE), PP/polystyrene (PS), PLA/poly (butylene adipate-co-terephthalate) (PBAT), and PLA/polycaprolactone (PCL)/PBS. This simple universal method offers significant potential for strengthening and toughening various polymer blends.

High-Strength PVA/Cellulosic hydrogels with Acid/Base and thermo dual-responsive fluorescence

Fluorescent polymer hydrogels (FPHs) with tunable luminous features have attracted immense interest. Nevertheless, until now, the development of most FPHs had been hindered by their poor mechanical properties and limited application range. This study presents a novel strategy to fabricate high-strength, multi-application cellulosic fluorescent hydrogels using polyvinyl alcohol (PVA) and fluorescent nanocellulose (containing pyrene tetracarboxylic acid) through a salting-out process. Such strategy enables cellulosic hydrogels with high tensile strength and toughness (26.45 MPa and 201.27 MJ/m3), compressive strength (165.58 MPa), dual-responsive fluorescence (acid/base and temperature), and multiple applications. Specifically, cellulosic hydrogels exhibit fluorescence switching through the utilization of lanthanide metals (Eu3+/Tb3+), acid/base, and temperature, owing to the presence of perylene tetracarboxylic acid as a fluorescent moiety with an aggregation-caused quenching (ACQ) effect. Based on this, the resulting hydrogels were utilized in rewritable display systems, temperature monitoring, and encrypted QR codes. This study envisions opening new possibilities for the development of high-strength fluorescent hydrogels with multiple applications.

Effect of fiber orientation of adjacent plies on the mode I delamination fracture of carbon fiber reinforced polymer multidirectional laminates

AbstractThe extensive use of multidirectional composite laminates requires to understand the delamination behavior at interfaces between plies with different fiber orientations. In this study, double cantilever beam testing was performed to investigate the mode I interlaminar fracture of carbon fiber reinforced polymer laminates with different central interfaces (0//0, 0//+45 and +45//−45). X‐ray microtomography revealed the curved crack front shape that was incorporated to calculate fracture toughness. The fracture toughness varies with the crack length in a typical delamination resistance curve, which can be quantified by an empirical equation. Incorporation of variable fracture toughness into a cohesive zone model can better predict the delamination fracture of the laminate, compared to constant toughness. It was found that the delamination mechanism is independent of central interfaces. However, compared to unidirectional laminates, multidirectional laminates are less resistant to crack initiation, but more resistant to propagation with higher toughness and shorter fiber bridging zone.Highlights Mode I interlaminar fracture of CFRP laminates with different central interfaces was investigated experimentally and numerically. Curved crack front shape was incorporated to calculate fracture toughness. Incorporation of variable fracture toughness into a cohesive zone model can better predict the delamination fracture of the laminate. Multidirectional laminates are less resistant to crack initiation but more resistant to propagation with higher toughness and shorter fiber bridging zone.

Ultra-Stretchable, Adhesive, Conductive, and Antifreezing Multinetwork Borate Ester-Based Hydrogel for Wearable Strain Sensor and VOC Absorption.

Hydrogels based on borate ester bonds exhibit remarkable tensile strength and self-healing ability, which make them a promising material for various biological research and strain sensor applications. However, in order to meet the practical application of hydrogel strain sensors, they must also show high conductivity, frost resistance, and proper adhesion, which is still a continuous challenge. Herein, a triple network hydrogel was prepared using poly(vinyl alcohol) (PVA) as the first network, ethylene imine polymer (PEI) as the second network, and poly(acrylamide-co-acrylic acid) copolymer (denoted as P(AM-Co-AA)) as the third network. 3-Carboxy-4-fluorophenylboronic acid (CFBS) was used as the cross-linking agent, glycerol (GL) was added to improve low-temperature resistance, and sodium chloride (NaCl) was incorporated to enhance electrical conductivity. The resulting PVA-CFBS@PEI@P(AM-Co-AA) triple network hydrogel exhibited impressive mechanical properties, including ultra tensile strength (4100%, 266.8 kPa), high toughness (6.5 MJ/m3), and low-temperature resistance (-60 °C). Additionally, it demonstrated high conductivity (σ = 1.83 mS/cm). The incorporation of CFBS endowed the hydrogel with excellent self-healing ability, while GL improved low-temperature resistance and strain sensing sensitivity (gauge factor (GF) = 2.8 (0-300%), GF = 5.6 (300-600%), GF = 8.7 (600-1000%)). The prepared hydrogel sensor can repetitively detect and differentiate between a wide range of human activities such as joint movements, frowning, and smiling. Additionally, the hydrogel demonstrated favorable mechanical properties at -20 °C (good adhesion, tensile strength: 1169.8%, 1.2 MPa; conductivity: 0.71 mS/cm, and strain sensing coefficient: GF = 1.3), making it suitable for applications in low-temperature environments. Furthermore, it also functions as an exceptional adsorbent, capable of selectively absorbing volatile organic compounds at high capacity (e.g., methanol: 1.80 g/g; acetone: 1.50 g/g).

Energy Dissipation and Toughening of Covalent Networks via a Sacrificial Conformation Approach.

Covalent polymer networks find wide utility in diverse engineering applications owing to their desirable stiffness and resilience. However, the rigid covalent chemical structure between crosslinking points imposes limitations on enhancing their toughness. Although the incorporation of sacrificial chemical bonds has shown promise in improving toughness through energy dissipation, composite networks struggle to maintain both rapid recovery and stiffness. Consequently, a significant challenge persists in achieving a covalent network that combines high strength, stiffness, toughness, and fast recovery performance. To address this challenge, we propose a novel sacrificial structure termed "sacrificial conformation." In this approach, β-cyclodextrin is covalently embedded into the network skeleton as the sacrificial conformation element. Compared to traditional covalent networks (LCN), well-designed cyclodextrin-embedded covalent network (CCN) exhibit a 100-fold increase in Young's modulus and a 60-fold increase in toughness. Importantly, CCN maintains excellent elasticity, ensuring swift recovery after deformation. This sacrificial conformational strategy enables efficient energy dissipation without necessitating the rupture of chemical bonds, thereby overcoming the limitations of traditional approaches. This advancement holds great promise for the design and fabrication of advanced elastomers and hydrogels with superior mechanical properties and dynamic behavior.

Energy Dissipation and Toughening of Covalent Networks via a Sacrificial Conformation Approach

Covalent polymer networks find wide utility in diverse engineering applications owing to their desirable stiffness and resilience. However, the rigid covalent chemical structure between crosslinking points imposes limitations on enhancing their toughness. Although the incorporation of sacrificial chemical bonds has shown promise in improving toughness through energy dissipation, composite networks struggle to maintain both rapid recovery and stiffness. Consequently, a significant challenge persists in achieving a covalent network that combines high strength, stiffness, toughness, and fast recovery performance. To address this challenge, we propose a novel sacrificial structure termed "sacrificial conformation." In this approach, β‐cyclodextrin is covalently embedded into the network skeleton as the sacrificial conformation element. Compared to traditional covalent networks (LCN), well‐designed cyclodextrin‐embedded covalent network (CCN) exhibit a 100‐fold increase in Young's modulus and a 60‐fold increase in toughness. Importantly, CCN maintains excellent elasticity, ensuring swift recovery after deformation. This sacrificial conformational strategy enables efficient energy dissipation without necessitating the rupture of chemical bonds, thereby overcoming the limitations of traditional approaches. This advancement holds great promise for the design and fabrication of advanced elastomers and hydrogels with superior mechanical properties and dynamic behavior.

Ultra-Tough, yet Rigid and Healable Supramolecular Polymers with Variable Stiffness for Multimodal Actuators.

Variable stiffness materials have shown considerable application in soft robotics. However, previously reported materials often struggle to reconcile high stiffness, stretchability, toughness, and self-healing ability, because of the inherently conflicting requisite of these properties in molecular design. Herein, we propose a novel strategy that involves incorporating acid-base ionic pairs capable of from strong crosslinking sites into a dense and robust hydrogen-bonding network to construct rigid self-healing polymers with tunable stiffness and excellent toughness. To demonstrate these distinct features, the polymer was employed to serve as the strain-regulation layers within a fiber-reinforced pneumatic actuator (FPA). The exceptional synergy between the configuration versatility of FPA and the dynamic molecular behavior of the supramolecular polymers equips the actuator with simultaneous improvement in motion dexterity, multimodality, loading capacity, robustness, and durability. Additionally, the concept of integrating high dexterity at both macro- and micro-scale is prospective to inspire the design of intelligent yet robust devices across various domains.

Enabling High Strength and Toughness Polyurethane through Disordered-Hydrogen Bonds for Printable, Recyclable, Ultra-Fast Responsive Capacitive Sensors.

The rapid advancement of smart, flexible electronic devices has paralleled a surge in electronic waste (e-waste), exacerbating massive resource depletion and serious environmental pollution. Recyclable materials are extensively investigated to address these challenges. Herein, this study designs a unique polyurethane (SPPUs) with ultra-high strength up to 60MPa and toughness of 360MJ m-3. This synthetic SPPUs can be fully recycled at room temperature by using green solvents of ethanol. Accordingly, the resultant SPPU-Ni composites, created by mixing the ethanol-dissolved SPPUs solution with nickel (Ni) powder, effectively combine the flexibility and recyclability of SPPUs with the electrical conductivity of the nickel filler. Notably, this work develops the printable capacitive sensors (PCBS) through transcribing the paste of SPPUs-Ni slurry onto PET film and paper using screen-printing technology. The devised PCBS have fast response time ≈50ms, high resolution, and multiple signal recognition capabilities. Remarkably, SPPUs and Ni powder can be fully recycled by only dissolving the waste PCBS in ethanol. This work offers a sustainable solution to the growing e-waste problem in recyclable flexible electronics.

Effect of Coarse Aggregate Type on the Fracture Toughness of Ordinary Concrete

This research work aims to compare the strength and fracture mechanics properties of plain concretes, obtained from different coarse aggregates. During the study, mechanical parameters including compressive strength (fcm) and splitting tensile strength (fctm), as well as fracture parameters involving critical stress intensity factor (KIcS) and critical crack tip opening displacement (CTODc) were evaluated. The effect of the aggregates used on the brittleness of the concretes was also analyzed. For better understanding of the crack initiation and propagation in concretes with different coarse aggregates, a macroscopic failure surfaces examination of the tested beams is also presented. Crushed aggregates covered were basalt (BA), granite (GT), and limestone (LM), and natural peeble gravel aggregate (GL) were used in the concrete mixtures. Fracture toughness tests were performed on an MTS 810 testing machine. Due to the high strength of the rock material, the rough surface of the aggregate grains, and good bonding in the ITZ area between the aggregate and the paste, the concretes with crushed aggregates exhibited high fracture toughness. Both of the analyzed fracture mechanics parameters, i.e., KIcS and CTODc, increased significantly in the case of concretes which were manufactured with crushed aggregates. They amounted, in comparison to concrete based on gravel aggregate, to levels ranging from 20% for concrete with limestone aggregate to over 30% for concrete with a granite aggregate, and to as much as over 70% for concrete with basalt aggregate. On the other hand, the concrete with gravel aggregate showed the lowest fracture toughness because of the smooth surface of the aggregate grains and poor bonding between the aggregate and the cement paste. However, the fracture process in each series of concrete was quasi-plastic in the case of gravel concrete, semi-brittle in the case of limestone concrete, and clearly brittle in the case of the concretes based on granite and basalt aggregates. The results obtained help to explain how the coarse aggregate type affects the strength parameters and fracture toughness at bending.