Hydrogen Bonds-Pinned Entanglement Blunting the Interfacial Crack of Hydrogel-Elastomer Hybrids.

Anchoring a layer of amorphous hydrogel on an antagonistic elastomer holds potential applications in surface aqueous lubrication. However, the interfacial crack propagation usually occurs under continuous loads for amorphous hydrogel, leading to the failure of hydrogel interface. This work presents a universal strategy to passivate the interfacial cracks by designing a hydrogen bonds-pinned entanglement (Hb-En) structure of amorphous hydrogel on engineering elastomers. The unique Hb-En structure is created by pinning well-tailored entanglements via covalent-like hydrogen bonds, which can amplify the delocalization of interfacial stress concentration and elevate the necessary fracture energy barrier within hydrogel interface. Therefore, the interfacial crack propagation can be suppressed under single and cyclic loads, resulting in a high interfacial toughness over 1650 J m-2 and an excellent interfacial fatigue threshold of 423 J m-2. Such a strategy universally works on blunting the interfacial crack between hydrogel coating and various elastomer materials with arbitrary shapes. The superb fatigue-crack insensitivity at the interface allows for durable aqueous lubrication of hydrogel coating with low friction.

Tough adhesion enhancing strategies for injectable hydrogel adhesives in biomedical applications.

Injectable hydrogel adhesives have gained widespread attention due to their ease of use, fast application time, and suitability for minimally invasive procedures. Several biomedical applications depend on tough adhesion between hydrogel adhesives and tissues, including wound closure and healing, hemostasis, tissue regeneration, drug delivery, and wearable electronic devices. Compared with bulk hydrogel adhesives formed ex situ, injectable hydrogel adhesives are more difficult to achieve strong adhesion strength due to a further balance of cohesion and adhesion while maintaining their flowability. In this review, the critical principles in designing tough adhesion of injectable hydrogel adhesives are summarized, including simultaneously enhancing their intrinsic interfacial toughness (Γ0inter) and mechanical dissipation (ΓDinter). Thereafter, various design strategies to enhance the Γ0inter and ΓDinter are discussed and evaluated respectively, involving multiple noncovalent/covalent interactions, topological connections, and polymer network structures. Furthermore, targeted biomedical applications of injectable hydrogel adhesives for specific tissue needs are systematically highlighted. In the end, this review outlines the challenges and trends in producing next-generation multifunctional injectable hydrogels for both practical and translational applications.

Predictive model of ice adhesion on non-elastomeric materials.

HYPOTHESIS: When ice accumulates on a surface, it can adversely impact functionality and safety of a platform in infrastructure, transportation, and energy sectors. Despite several attempts to model the ice adhesion strength on ice-shedding materials, none have been able to justify variation in the ice adhesion strength measured by various laboratories on a simple bare substrate. This is primarily due to the fact that the effect of underlying substrate of an ice-shedding material has been entirely neglected. EXPERIMENTS: Here, we establish a comprehensive predictive model for ice adhesion using the shear force method on a multi-layered material. The model considers both shear resistance of the material and shear stress transfer to the underlying substrate. We conducted experiments to validate the model predictions on the effect of coating and substrate properties on the ice adhesion. FINDINGS: The model reveals the importance of the underlying substrate of a coating on ice adhesion. Most importantly, the correlation between the ice adhesion and the coating thickness are entirely different for elastomeric and non-elastomeric materials. This model justifies different measured ice adhesion across various laboratories on the same material and elucidates how one could achieve both low ice adhesion and high mechanical durability. Such predictive model and understanding provides a rich platform to guide the future material innovation with minimal adhesion to the ice.

Robust, anti-freezing and conductive bonding of chitosan-based double-network hydrogels for stable-performance flexible electronic.

Unstable hydrogel-substrate interfaces and defunctionalization at low temperature severely restrict versatile applications of hydrogel-based systems. Herein, various chitosan-polyacrylamide double-network (CS-PAM DN) ionic hydrogels were chemically linked with diverse substrates to construct robust and anti-freezing hydrogel-substrate combination, wherein the destructible CS physical network rendered effective energy dissipation mechanism to significantly enhanced the cohesion of hydrogels and the covalent linkage between PAM network with substrate surface strongly improved the interfacial adhesion. The synergistic effects enabled the CS-PAM DN hydrogels to be tightly bonded on diverse metals and inorganics. Impressively, the hydrogel-substrate combinations were freezing tolerant to well-maintain high interfacial toughness at low temperature. Notably, due to the high toughness and conductivity of hydrogel-metal interface, the hydrogel-metal combination can be utilized as a multi-model flexible sensor to detect strain and pressure within broad temperature range. This work may provide a platform for construction and emerging application of robust, anti-freezing and stable-performance hydrogel-based systems.

Effect of Doping SiO2 Nanoparticles and Phenylmethyl Silicone Oil on the Large-Scale Deicing Property of PDMS Coatings.

Recently, low interfacial toughness (LIT) materials have been developed to solve large-scale deicing problems. According to the theory of interfacial fracture, ice detachment is dominated by strength-controlled or toughness-controlled regimes, which are characterized by adhesive strength or constant shear force. Here, a new strategy is introduced to regulate the interfacial toughness of poly(dimethylsiloxane) (PDMS) coatings using silicon dioxide nanoparticles (SiO2 NPs) and phenylmethyl silicone oil (PMSO). By systematically adjusting the doping proportion of SiO2 NPs and PMSO, it is found that a lower interfacial toughness can be achieved with a lower constant shear force. The synergistic effect of the two dopants on the adhesive strength and interfacial toughness is analyzed. Meanwhile, finite element method (FEM) analysis of ice detachment is conducted to show the cracking process intuitively and explicate the mechanism of lowering the interfacial toughness of PDMS by doping SiO2 NPs and PMSO. It can be concluded that the cohesive zone material (CZM) model is effective for simulating the deicing process of PDMS coatings and provides a comprehensive understanding of the modulation of interfacial toughness.

Quasicrystalline Coatings Exhibit Durable Low Interfacial Toughness with Ice.

Ice accretion can adversely impact many engineering structures in commercial and residential sectors. Although there are many reports of low-ice-adhesion-strength materials, a scalable and durable deicing solution remains elusive, as ice detachment is dominated by interfacial toughness for large interfaces. In this work, durable metallic coatings based on Al-rich quasicrystalline alloys were prepared and applied on aluminum substrates using high-velocity oxyfuel thermal spray. X-ray diffraction patterns confirmed the quasicrystalline phases of the coating, and its large-scale deicing capability was studied by evaluating the coating's ice detachment mechanics using long lengths of ice. A toughness-controlled regime of interfacial fracture was observed for ice lengths longer than ∼2 cm, and a low shear strength of ∼30 kPa was achieved for a 20 cm ice length. The metallic coatings exhibited excellent ice repellency even after being abraded, scratched, heated, UV-irradiated, and exposed to chemical contaminations, demonstrating promising durability for real-world, large-scale ice removal.

Enhanced Interfacial Toughness of Thermoplastic-Epoxy Interfaces Using ALD Surface Treatments.

Interfacial fracture and delamination of polymer interfaces can play a critical role in a wide range of applications, including fiber-reinforced composites, flexible electronics, and encapsulation layers for photovoltaics. However, owing to the low surface energy of many thermoplastics, adhesion to dissimilar material surfaces remains a critical challenge. In this work, we demonstrate that surface treatments using atomic layer deposition (ALD) on poly(methyl methacrylate) (PMMA) and fluorinated ethylene propylene (FEP) lead to significant increases in surface energy, without affecting the bulk mechanical response of the thermoplastic. After ALD film growth, the interfacial toughness of the PMMA-epoxy and FEP-epoxy interfaces increased by factors of up to 7 and 60, respectively. These results demonstrate the ability of ALD to engineer the adhesive properties of chemically inert surfaces. However, in the present case, the interfacial toughness was observed to decrease significantly with an increase in humidity. This was attributed to the phenomenon of stress-corrosion cracking associated with the reaction between Al2O3 and water and might have a significant implication for the design of these tailored interfaces.

Bonding measurement -Strength and fracture mechanics approaches.

This study investigated the effect of cross-sectional areas on interfacial fracture toughness and bond strength of bilayered dental ceramics. Zirconia core ceramics were veneered and cut to produce specimens with three different cross-sectional areas. Additionally, monolithic specimens of glass veneer were also prepared. The specimens were tested in tension until fracture at the interface and reported as bond strength. Fracture surfaces were observed, and the apparent interfacial toughness was determined from critical crack size and failure stress. The results showed that cross-sectional area had no effect on the interfacial toughness whereas such factor had a significant effect on interfacial bond strength. The study revealed that cross-sectional area had no effect on the interfacial toughness, but had a significant effect on interfacial bond strength. The interfacial toughness may be a more reliable indicator for interfacial bond quality than interfacial bond strength.

Shear Strength and Interfacial Toughness Characterization of Sapphire-Epoxy Interfaces for Nacre-Inspired Composites.

The common tensile lap-shear test for adhesive joints is inappropriate for brittle substrates such as glasses or ceramics where stress intensifications due to clamping and additional bending moments invalidate results. Nevertheless, bonding of glasses and ceramics is still important in display applications for electronics, in safety glass and ballistic armor, for dental braces and restoratives, or in recently developed bioinspired composites. To mechanically characterize adhesive bondings in these fields nonetheless, a novel approach based on the so-called Schwickerath test for dental sintered joints is used. This new method not only matches data from conventional analysis but also uniquely combines the accurate determination of interfacial shear strength and toughness in one simple test. The approach is verified for sapphire-epoxy joints that are of interest for bioinspired composites. For these, the procedure not only provides quantitative interfacial properties for the first time, it also exemplarily suggests annealing of sapphire at 1000 °C for 10 h for mechanically and economically effective improvements of the interfacial bond strength and toughness. With increases of strength and toughness from approximately 8 to 29 MPa and from 2.6 to 35 J/m2, respectively, this thermal modification drastically enhances the properties of unmodified sapphire-epoxy interfaces. At the same time, it is much more convenient than wet-chemical approaches such as silanization. Hence, besides the introduction of a new testing procedure for adhesive joints of brittle or expensive substrates, a new and facile annealing process for improvements of the adhesive properties of sapphire is suggested and quantitative data for the mechanical properties of sapphire-epoxy interfaces that are common in synthetic nacre-inspired composites are provided for the first time.

Effect of zirconia surface treatment on zirconia/veneer interfacial toughness evaluated by fracture mechanics method.

OBJECTIVES: The aim of this study was to evaluate the effect of the airborne-particle abrasion and liner application on the interfacial toughness between veneering porcelain and zirconia core by means of a fracture mechanics test. METHODS: Beam-shaped zirconia specimens were sectioned and divided into 4 groups according to different surface treatments as follows: Group C (control): no treatment; Group L: application of liner; Group A: airborne-particle abrasion with Al2O3 (sandblasting); and Group AL: airborne-particle abrasion and application of liner. The zirconia surfaces before and after sandblasting were observed and analyzed by SEM and white light interferometer. Specimens of each pretreated group were veneered with 3 core/veneer thickness ratios of 2:3, 1:1, and 3:2, corresponding to 3 phase angles respectively. Fracture mechanics test was performed on each specimen, the energy release rate G and phase angle ψ were calculated to characterize interfacial toughness. The experimental data were analyzed statistically using three-way ANOVA and the Tukey's HSD test. The surfaces of fractured specimens were examined by SEM and EDX. RESULTS: At each phase angle, the interfaces with no treatment had higher mean G values than that of other groups. All the specimens showed mixed failure mode with residual veneer or liner on the zirconia surfaces. CONCLUSIONS: The toughness of zirconia/veneer interface with no treatment is significantly higher than that of interfaces subjected to liner application and airborne-particle abrasion. CLINICAL SIGNIFICANCE: Liner application and airborne-particle abrasion seem to reduce zirconia/veneer interfacial toughness. Therefore, the two surface treatment methods should be applied with caution.