Thermal Fluctuations Limit the Adhesive Strength of Compliant Solids

For compliant solids, the stress required to separate an interface (its adhesive strength) appears to be much lower than that calculated by computing intersurface interactions. We explore the hypothesis that the adhesive strength is limited in value by thermal fluctuations. In a simple model of an interface, molecules bridging the two surfaces are represented by linear entropic springs. Asymptotic and numerical analyses are carried out to evaluate the adhesive strength and effective work of adhesion. For stiff materials, adhesive strength is found to be equal to the intrinsic strength—the maximum value of intersurface stress computed ignoring fluctuations. For compliant materials, adhesive strength is significantly reduced and is on the order of the elastic modulus. The effective work of adhesion agrees with the intrinsic work of adhesion for stiff materials and can decay slowly with increasing compliance.     

Adhesion of polymer coils to a solid surface: influence of the depletion effect

The specific properties of polymer coils are often disregarded in theories of adhesion, but polymer properties are essential for the strength of the adhesive bond. Polymer coils are repelled entropically from impenetrable surfaces. This causes the depletion effect and creates a layer of reduced concentration right at the interface. To bond a polymer coil to a substrate, it must be forced actively towards the interface, driven by the gaining of adsorption energy. The adsorption of specific groups in the (co)polymer, which interact with 'polar' sites on the substrate, must be used to suppress the depletion. Adsorption diminishes the effective distance between the surface and the adhesive polymer. The balance between adsorption and depletion (rather than the effect of polar groups or pretreatments on the work of adhesion as such) is the most important chemical possibility of affecting adhesion. The strength of the bond between polymeric materials and solid surfaces varies as H^-3, with the effective distance H between the polymer and substrate. Therefore, it changes by an order of magnitude when the polymer adhesive is pulled towards the substrate by adsorption.     

Cracks at adhesive interfaces

The application of Griffith's energy balance argument to cracks at adhesive interfaces is studied. Adhesive interfaces are generally brittle, representing the simplest form of fracture mechanics geometry because cracks are constrained to travel along the interface, giving a defined crack path which eases analysis. Experimentally, such cracks may be propagated along the interface between optically smooth rubber pieces, and measured through the transparent material. The development of adhesive fracture test-pieces since Griffith's time reveals difficulties in his reasoning, and allows improved understanding of the energy balance method. The most important conclusion is that stress does not normally enter the cracking criterion. It is demonstrated experimentally that stress may remain constant while the crack criterion changes. The strength of an adhesive interface is shown to be a meaningless parameter; instead, the work of adhesion, or adhesive energy, which is the work of adhesion together with energy losses, should be used to define the behaviour of cracks at interfaces.     

The Strength of Adhesive Joints

The main rules pertaining to the strength of adhesive joints are: (1) This strength is a mechanical (or rheological) property. The local stress which causes the extension of a pre-existing crack can be determined only if the stress pattern in the whole adhint is known and the intensification of stress at flaws is taken into account. (2) The rupture occurs in a material, not between two materials. Consequently, the molecular forces across the adhesive-adherend interface are irrelevant, and the “adhesion tension” does not determine the adhint strength.     

CALENDAR OF EVENTS

The main rules pertaining to the strength of adhesive joints are: (1) This strength is a mechanical (or rheological) property. The local stress which causes the extension of a pre-existing crack can be determined only if the stress pattern in the whole adhint is known and the intensification of stress at flaws is taken into account. (2) The rupture occurs in a material, not between two materials. Consequently, the molecular forces across the adhesive-adherend interface are irrelevant, and the “adhesion tension” does not determine the adhint strength.     

A three-dimensional finite-element stress analysis and strength evaluation of stepped-lap adhesive joints subjected to static tensile loadings

Stress distributions in stepped-lap adhesive joints subjected to static tensile loadings are analyzed using three-dimensional finite-element calculations. For establishing an optimum design method of the joints, the effects of the adhesive Young's modulus, adhesive thickness and number of steps on the interface stress distributions are examined. The results show that the maximum value of the maximum principal stress σ₁ occurs at the edge of the adhesive interfaces. The maximum value of the stress σ₁ decreases as the adhesive Young's modulus and number of steps increase and as the adhesive thickness decreases under static loadings. A method for estimating the joint strength under static loadings is proposed using interface stress distributions. For verification of the finite-element method calculations, experiments were carried out to measure the strains and the joint strengths under static loadings. Fairly good agreements were found between the numerical and the experimental results.     

Stress Transfer Function for Interface Assessment in Composites with Plasma Copolymer Functionalized Carbon Fibres

Radio-frequency-induced plasma copolymerization of acrylic acid/1,7-octadiene was used to produce a range of functionalized plasma copolymer coatings with controlled degree of adhesion. The single-fibre fragmentation test was used to characterize the adhesion of plasma copolymer coated fibres to epoxy resin. The cumulative stress transfer function (CSTF) and Kelly-Tyson approaches were used to evaluate the degree of adhesion. By continuous monitoring of the fragmentation process, it was found that the mechanical performance of a composite material could be evaluated using the CSTF methodology at strain well below saturation. The degree of debonding was a good measure of relative interface/interphase adhesive strength. The trend in the CSTF is consistent with the propagation of interfacial debonds during the test. For a completely debonded fibre a normalized CSTF value, referred as stress transfer efficiency (STE), was found to provide a more consistent analysis that was able to differentiate between fibres with similar degrees of debonding. The calculated values of interfacial shear strength (IFSS) were only valid for a fully debonded fibre (1,7-octadiene plasma homopolymer coating) where the assumption of a constant shear stress, as in the Kelly-Tyson model, applied. However, IFSS did not provide the same ranking. Where debonding does not occur, the stress transfer efficiency also provides a sensitive measure of the interface/interphase performance. Improved adhesion over the untreated-unsized carbon fibre was observed for both of the plasma copolymer-coated and commercially treated carbon fibres. Since there is a concentration dependence of carboxyl groups on adhesion, the mechanism appears to relate to covalent bond formation with the epoxy group. Plasma copolymer coatings on carbon fibres also causes an increased tensile strength and Weibull modulus.     

Stress Transfer Function for Interface Assessment in Composites with Plasma Copolymer Functionalized Carbon Fibres

Radio-frequency-induced plasma copolymerization of acrylic acid/1,7-octadiene was used to produce a range of functionalized plasma copolymer coatings with controlled degree of adhesion. The single-fibre fragmentation test was used to characterize the adhesion of plasma copolymer coated fibres to epoxy resin. The cumulative stress transfer function (CSTF) and Kelly-Tyson approaches were used to evaluate the degree of adhesion. By continuous monitoring of the fragmentation process, it was found that the mechanical performance of a composite material could be evaluated using the CSTF methodology at strain well below saturation. The degree of debonding was a good measure of relative interface/interphase adhesive strength. The trend in the CSTF is consistent with the propagation of interfacial debonds during the test. For a completely debonded fibre a normalized CSTF value, referred as stress transfer efficiency (STE), was found to provide a more consistent analysis that was able to differentiate between fibres with similar degrees of debonding. The calculated values of interfacial shear strength (IFSS) were only valid for a fully debonded fibre (1,7-octadiene plasma homopolymer coating) where the assumption of a constant shear stress, as in the Kelly-Tyson model, applied. However, IFSS did not provide the same ranking. Where debonding does not occur, the stress transfer efficiency also provides a sensitive measure of the interface/interphase performance. Improved adhesion over the untreated-unsized carbon fibre was observed for both of the plasma copolymer-coated and commercially treated carbon fibres. Since there is a concentration dependence of carboxyl groups on adhesion, the mechanism appears to relate to covalent bond formation with the epoxy group. Plasma copolymer coatings on carbon fibres also causes an increased tensile strength and Weibull modulus.     

Effect of Flaws in the Adhering Interface on the Strength of Adhesive-bonded Butt Joints

This paper presents the strength of metal-to-metal bonded joints with a flaw in the interface between the adhesive layer and the adhering surface of adherend. The test specimens of butt joints are prepared by bonding two thin-wall metal tubes. The materials are carbon steel, aluminum alloy, brass and copper. The adhesive is epoxy resin. The tensile and shear strength of the joints are experimentally determined by subjecting the specimens to axial load and torsion for various flaw sizes and thickness of adhesive layers. Linear elastic fracture mechanics is applied to the experimental results. The stress intensity factors for a layered composite with a flaw in the interface are numerically calculated in terms of flaw size and loading by using Erdogan's formulas. The fracture stresses of joints with a flaw are predicted at the critical values of the stress intensity factors. The strength of joints without a flaw is also correlated with the stress intensity factors by use of a concept of “effective flaw size”.     

Estimation of dynamic adhesion from static test results in the model cord–RFL–rubber system

Generally, nylon and polyester cords are used to reinforce rubber compounds. These composites are used in many sectors, such as tire and belt manufacturing. To increase adhesion performance a resorcinol–formaldehyde–latex (RFL) adhesive is applied on the cord, which bonds chemically to both cord and rubber and, thus, it improves both the thermodynamic work of adhesion and the loss function at the cord/rubber interface. Adhesion strength between the cord and rubber determines the performance of the system. So to study the performance of the cord–rubber system, adhesion strength must be evaluated. Cord–rubber adhesion strength can be evaluated in static and dynamic modes. The H-Pull (H-adhesion) test method is a static and relatively simple method that is usually employed to control raw material quality. Fatigue test is one of dynamic adhesion test methods that are used to determine the performance of cord–rubber interface. Some important factors such as cyclic stress and heat buildup are involved in this test procedure. To investigate the accuracy of the H-Pull test results, the cord–rubber samples were prepared using poly(ethylene terephthalate) (PET) cord and NR/SBR rubber. Then H-adhesion was determined at elevated temperatures. The adhesion strength was also evaluated in dynamic (fatigue) mode at different temperatures. Authors have proposed an equation to estimate dynamic adhesion from H-Pull test results.     

A simplified approach to achieve gecko-mimic nano-structural adhesives by a simple polymer

In this work, we graft polyacrylate with 3,4-dihydroxyphenylalanine, a functionality alike adhesive protein in mussels, to obtain a mussel-mimic polyacrylate with good adhesive property and interesting nano-patterns during adhesion. The chemical structure of the product is confirmed by ¹H NMR that dopamine is grafted onto the polymer. The analysis of the tensile strength test reveals that the adhesive is improved more than 2 times, from 53 to 124 KPa, when polyacrylate grafted by dopamine. The analysis of the static water contact angle suggests that the hydrophilic of the as-synthesized final polymer is enhanced. It is very interesting to observe that such an adhesive material can form nano-patterns on the adhesion interface during bonding, at about 100 nm in diameter each contact point, which something look like the gecko foot structure. This structural feature maybe related to the increasing adhesive properties of such materials.     

Effects of wood-surface roughness,adhesive viscosity and processing pressure on adhesion strength of protein adhesive

The objective of this research was to study the effects of wood-surface roughness, adhesive viscosity and processing pressure on adhesion strength between soybean protein adhesive and wood, and to seek the relative importance of the individual factors in determining adhesion strength. Processing pressure was found to be the most important factor in determining adhesion strength. An optimum pressure, which was about 4.55 MPa in this research, is needed for development of a strong bond. A higher pressure resulted in reduced adhesion strength, possibly due to damage to the wood surface; a lower pressure also resulted in decreased adhesion strength because of the lack of bond formation. Adhesive viscosity had greater effect on adhesion strength than surface roughness. Contact angle, which was found to be mainly determined by adhesive viscosity and surface roughness, was a major factor controlling adhesive penetration. A smaller contact angle, resulting from lower viscosity and rougher surface, produced deeper penetration, while a larger contact angle, resulting from higher viscosity and smoother surface, produced shallower penetration. An optimum penetration is needed to enhance adhesion strength by developing a three-dimensional interactive zone at the interface. Too deep or too much penetration would result in 'dry-out' at the interface; less penetration would limit the formation of the three-dimensional zone at the interface. Both cases resulted in reduced adhesion strength. Contact angles ranging from 35 to 47° provided the optimum penetration needed for good adhesion. The results of this research could be used as reference to determine optimum process parameters in plywood manufacturing when an aqueous based adhesive is used.     

Estimating work of adhesion using spherical contact between a glass lens and a PDMS block

This study proposes a method of estimating the thermodynamic work of adhesion using the spherical contact between a glass lens and a polydimethylsiloxane (PDMS) block. An equivalent stiffness of the measurement system is determined prior to the experimental measurements. Parameters such as force, contact radius, and displacement are measured during the contact processes that consist of a loading process and an unloading process. The elastic modulus of the PDMS is determined from the measured parameters. Hysteresis is observed in the contact process, showing that the process is in a non-equilibrium state. However, an equilibrium instant exists when the contact area attained a maximum value. The work of adhesion can be determined from the strain energy release rate using the parameters of the instant. The estimated work of adhesion is in the range estimated by another method. The limitation of the conventional method is also presented. The proposed method is suggested to be applicable to interface characterization in a practical adhesive contact with soft materials.     

Strength and bonding characteristics of adhesive joints with surface-treated titanium-alloy substrates

This paper presents a study on the effect of surface treatments on the mechanical behavior of adhesively bonded titanium alloy joints. Several different treatments were selected for the preparation of Ti-6Al-4V alloy faying surfaces, and bonded joints were fabricated using surface-treated titanium alloy substrates and a film adhesive. Tensile tests were performed on single-lap specimens to evaluate the joint strength and to assess the failure mode, i.e. cohesive failure, adhesive (interfacial) failure or a mix of both. Contact angle measurements were also carried out, and the surface free energies of titanium alloys and the thermodynamic works of adhesion for the adhesive/titanium alloy interfaces were obtained. A three-dimensional finite element analysis was used to predict the strength of the specimens exhibiting cohesive failure. In addition, an expression of the relationship between the joint strength corresponding to interfacial failure and the thermodynamic work of adhesion was introduced based on the cohesive zone model (CZM) concept. It is shown that two surface treatments, Itro treatment and Laseridge, lead to cohesive failure and a significant increase in the joint strength, and the numerically predicted strength values are fairly close to the experimental values. These surface treatments are possible replacements for the traditional surface treatment processes. For degreasing, emery paper abrasion, atmospheric plasma treatment, sulfuric acid anodizing, nano adhesion technology and high-power lasershot, the specimens fail at the adhesive/substrate interface and the joint strength increases linearly with the thermodynamic work of adhesion as expected from our CZM-based expression.     

Effects of solvent exposure on the adhesion of grafted PE to EVOH copolymer

Multilayer polymers are gaining popularity in many industrial applications, where the combination of various advantages of the individual materials may be exploited (e.g. mechanical strength and chemical resistance). Such materials rely heavily on the quality of interfacial adhesion and this in turn may alter with solvent exposure. Here, we study the ageing of a multilayer high density polyethylene, grafted polyethylene (PEg), ethylene/vinyl alcohol copolymer (EVOH) assembly in organic solvents, and its effect on the T-peel resistance of the EVOH/PEg interface (interphase). Apolar solvents absorb essentially in the polyethylenic materials leading to reduced peel strength due to modification of polymer bulk properties, rather than to changes in intrinsic adhesion strength. Ethanol diffuses readily into the EVOH leading to an intrinsic drop in energy of adhesion. In the cases studied, reduction of interfacial, peel strength was found to be largely reversible on drying the polymer assembly.     

Studies on tack of pressure-sensitive adhesive tapes: On the relationship between pressure-sensitive adhesion and surface energy of adherends

The relationship between wetting and pressure-sensitive adhesion was studied using an adhesive composed of poly(butyl acrylate) and various adherends of different surface tension. The amount of adhesive deposit was determined quantitatively by tracer technique although the unbonding process was apparently observed as interface failure. The adhesive force and amount of deposit were both dependent on the critical surface tension of the adherends. Maximum tack value and contamination were observed with adherends whose critical surface tension was close to that but a little higher than that of the adhesive. The adhesive force obtained was lower than cohesive strength of adhesive. From this evidence, a mechanism for pressure-sensitive adhesion was discussed: the bond breaks in the addesive mass around the very minute spots where interaction is at work between adhesive and adherend. Inasmuch as the density of the minute spots per unit area depends on the surface tension, the adhesive force also depends on the surface tension.     

Influence of Acrylic Adhesive Viscosity and Surface Roughness on the Properties of Adhesive Joint

In adhesion, the wetting process depends on three fundamental factors: the surface topography of the adherend, the viscosity of the adhesive, and the surface energy of both. The aim of this paper is to study the influence of viscosity and surface roughness on the wetting and their effect on the bond strength. For this purpose, an acrylic adhesive with different viscosities was synthesized and some properties, such as viscosity and surface tension, were studied before adhesive curing took place. Furthermore, the contact angle and the lap-shear strength were analyzed using aluminum adherends with two different roughnesses. Scanning electron microscopy was used to determine the effect of the viscosity and the roughness on the joint interface. The results showed that the adhesive exhibits an optimal value of viscosity. Below this value, at low viscosities, the low neoprene content produces poor bond strength due to the reduced toughness of the adhesive. Additionally, it also produces a high shrinkage during curing, which leads to the apparition of residual stresses that weakens the interfacial strength. However, once the optimum value, an increase in the viscosity produces a negative effect on the joint strength as a result of an important decrease in the wettability.     

A Stress Analysis of Adhesive Butt Joints of Dissimilar Materials Subjected to Cleavage Loads

Stress distributions are examined when an adhesive butt joint, in which two thin plates made of dissimilar materials are joined, is subjected to cleavage loads. General representations of the stress and displacement fields are given using the two-dimensional theory of elasticity. The effects of the ratios of young's modulus among two adherends and an adhesive and the thickness of the adhesive on the stress distributions of the joints are clarified by numerical calculations. In addition, the stress singularity near the edge of the interface in the load application side is evaluated. For verification, the strain distributions near the interface of each adherend were measured. The analytical results are closely consistent with the experimental ones.     

Butt joint tensile strength: interface corner stress intensity factor prediction

The asymptotic form of the interface corner stress field in a butt joint is discussed, and a failure analysis based on the stress intensity factor defining the magnitude of this asymptotic stress field is validated. A stress singularity of type Kr^δ(δ < 0) exists at an interface corner in a butt joint (i.e. where an interface intersects a stress-free edge). A simple relation defines the stress intensity factor K for an idealized butt joint composed of a thin elastic adhesive layer bonded between rigid adherends and subjected to transverse tension and uniform adhesive shrinkage. This stress intensity factor, referred to here as the free-edge stress intensity factor K_f, is applicable to both plane strain and axisymmetric geometries. The way that uniform adhesive shrinkage (thermal contraction) during cure alters interface corner stress fields is also discussed. When adhesive shrinkage is present, both constant and singular terms must be included in the asymptotic solution to attain good agreement with full field finite element results over a reasonably large interface corner region. Experiments have been carried out to investigate the applicability of a K_f-based failure criterion to butt joints. Butt joints were fabricated by bonding two stainless steel rods together with an epoxy adhesive (Epon 828/T-403). The measured joint strength increased by a factor of 2 as the bond thickness was reduced from 2.0 to 0.25 mm. The observed bond thickness effect is accurately predicted when failure is presumed to occur at a critical K_f value. This fracture criterion suggests that the butt joint tensile strength varies roughly as the reciprocal of the cube root of bond thickness when the adhesive's Poisson's ratio is between 0.3 and 0.4, residual stress levels at the interface corner are negligible, the adherends are essentially rigid relative to the adhesive, and small-scale yielding conditions hold at the interface corner.     

Adhesion of two elastic conforming solids with a single interface gap

The adhesive contact between a half-space with a single surface micro-groove and a flat half-space is investigated. Surface interaction is described by the Maugis–Dugdale adhesion model. The contact problem is reduced to a singular integral equation for a height of the interface gap, which is solved analytically. For evaluating widths of the gap and the adhesion zone, a system of two transcendental equations is obtained, which is solved numerically. Three stable equilibrium states are found. The gap width-applied pressure curves are characterized by discontinuities and hysteresis. The effects of the maximum groove height and the adhesive stress on the adhesive contact are studied. It is shown that the adhesion hysteresis is greater for smaller grooves and larger adhesive stresses.