Application of the Island Blister Test for Thin Film Adhesion Measurement

The island blister test has recently been proposed as an adhesion test which allows the peel of thin, well-adhered films without exceeding the tensile strength of the film. The island blister test site is a modification of the standard blister test site, consisting of a suspended membrane of film with an “island” of substrate at the film center. The membrane support and island are secured to a rigid plate and the film is pressurized, peeling the film inward off the island. A model for this inward or “annular” peel indicates that even for systems of good adhesion, peel can be initiated at low enough pressures to prevent film failure by making the center island sufficiently small relative to the size of the film.

We have fabricated island blister test sites using micromachining techniques and have used them to measure the debond energy of polymer films on various substrates. The peel data obtained from these island sites match well to the behavior predicted by a simple fracture mechanics analysis. This paper reports the fabrication of the island test sites, the experimental verification of the test, and the results of application of the test to polyimide films on metallic and polymeric substrates.     

Analysis of Critical Debonding Pressures of Stressed Thin Films in the Blister Test

This paper reports a model for the relationship between critical debonding pressures and the work of adhesion of thin films in the blister test. Previous models have neglected the possible role of residual stresses in the film on the critical pressure. The model reported here shows that these stresses may have a large effect on the relation between the critical pressure and the work of adhesion. A similar model is developed for an alternative blister geometry, the annular or “island” blister. It is shown that films which cannot be peeled using the standard blister test (due to exceeding the tensile strength limit of the film before initiating a debond) can be peeled by varying the geometric parameters of the island blister.     

Changes in the adhesion strength between copper thin films and polyimide substrates after heat treatment

The adhesion strength between a copper (Cu) thin film and a polyimide [pyromellitic dianhydride-oxydianiline (PMDA-ODA)] substrate is reduced by heat treatment at 150°C in air. In this work, we determined the changes in adhesion strength between Cu films and polyimide substrates using Auger electron spectroscopy (AES), attenuated total reflection Fourier-transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). The analysis showed that the weak boundary layer (WBL) shifted towards the Cu interface as the heat treatment time was increased. To confirm this shift, we looked at two other polyimide substrates: biphenyl dianhydride-p-phenylene diamine (BPDA-PDA) and biphenyl dianhydride-oxydianiline (BPDA-ODA). Comparing the adhesion strength for the Cu thin film, the adhesion strength was high for the Cu/PMDA-ODA and Cu/BPDA-ODA laminates, but very low for the Cu/BPDA-PDA laminate. One of the possible reasons for this behavior could be that the ether moiety between the two benzene rings in ODA is related to the adhesion between a Cu film and an 0₂-plasma-treated polyimide (PI) substrate. The relationship between the adhesion strength and chemical bonding states is also discussed. We conclude that a Cu thin film sputtered onto a PI substrate is apt to peel at the oxidized interface, due to the heat treatment.     

Changes in the Peeled Surfaces of Copper Thin Films Deposited on Polyimide Substrates After Heat Treatment

Peel strength between a copper (Cu) thin film and a polyimide (pyromellitic dianhydride-oxydianiline, or PMDA-ODA) substrate is reduced by heat treatment at 150°C in air. In this work, we investigated the peel strength, the morphology of the interface between Cu films and polyimide substrates using optical microscopy and electron microscopy, and chemical change of the interface using Auger electron spectroscopy (AES) and micro X-ray photoelectron spectroscopy (XPS). The analysis showed that CuO “lumps” were present on the peeled surface of PMDA-ODA after heat treatment at 150°C in air. The peeled surfaces of other polyimide substrates were also analyzed: biphenyl dianhydride-para phenylene diamine (BPDA-PDA) and biphenyl dianhydride-oxydianiline (BPDA-ODA). CuO lumps were present on the peeled surface of BPDA-ODA after the heat treatment, but not that of BPDA-PDA. Compared with the adhesion strength for the Cu thin film, the adhesion strength was high for the Cu/PMDA-ODA and Cu/BPDA-ODA laminates, but the adhesion strength was very low for the Cu/BPDA-PDA laminate. This low strength is the reason that CuO lumps were not detected on the peeled surface of the BPDA-PDA substrate. These CuO lumps were related to the adhesion degradation of the Cu/polyimide laminates after the heat treatment.     

Temperature and humidity effects on adhesion of polyimide film to a silicon substrate

A 90° peel tester with substrate heating capability was built to evaluate the adhesion strength of polyimide films to a silicon substrate. The effects of polyimide film thickness and peel rate on polyimide adhesion to a silicon substrate under high or low humidity, and at elevated temperatures, have been evaluated. In a high humidity environment, a low peel strength was measured. The influence of moisture on the peel strength increases with decreasing peel rate. Peeling at elevated temperature reduces the moisture effect even under high humidity conditions. Using a low peel rate in a high humidity environment, the measured peel strength showed a maximum as the polyimide film thickness increased. No striations in peeled polyimide films were observed for peeling in a high humidity environment.     

Interlayer delamination and adhesion of coextruded films

Efforts to evaluate interlayer adhesion of coextruded films are often hampered by the inability to initiate delamination. On the other hand, interlayer delamination was often noticed at cut or trimmed edges of coextruded films. In this study, a test method was developed by first initiating delamination by uniaxial stretching and then measuring interlayer adhesion by peel test. Delamination was initiated by uniaxial stretching under controlled conditions for samples with double‐neck geometry. The double‐neck geometry was designed to create a specimen for the subsequent 180° peel test. Peel force was used to quantify interlayer adhesion of coextruded films based on polycarbonate and its copolymers. With this two‐step technique, coextruded films with peel force as high as 5300 N/m or 30 lb./in. were quantified. In addition, effects of copolymer composition and coextrusion processing condition on interlayer adhesion of these coextruded films were clearly demonstrated. A great deal of variation of interlayer adhesion across film surface was also revealed. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 92: 3901–3909, 2004     

Assessment of test methods for a cryogenic liquid containment system

This paper presents a study demonstrating the selection and use of adhesive joint test methods for the design and validation of an adhesively bonded, foam-composite membrane, cryogenic insulation system for the marine transportation of liquefied natural gas (LNG). The study considered the performance of epoxy and polyurethane adhesives under ambient and sub-zero operating temperatures. Double-lap, sandwich panel and double cantilever beam (DCB) joint tests, essential in “calibrating” the interpretation of finite element analysis (FEA), were performed along with FEA in order to assess the stress states (in-plane, peel and shear stress) in the adhesive layer that, under defined loads and extensions, are comparable with the stress levels in the LNG container under service conditions.The study reinforces the view that the presence of barrier film substrates has a major effect on performance, and that the critical state of stress for the integrity of the flexible composite barrier film (FSB) to rigid composite barrier film (RSB) bond in the cryogenic containment system is the tensile peel stress at the ends of the joint. Sandwich panel tests conducted using the two adhesives indicate that failure tends to occur when the peel stress exceeds the tensile strength of the bulk adhesive with the polyurethane adhesive exhibiting more robust adhesion properties than the epoxy with consequences for future design of LNG containers.     

The Mechanical Behaviour of Polyimide/Copper Laminates Part 2: Peel Energy Measurements

The mechanical peel behaviour of laminates consisting of polyimide films adhered to copper foil using a modified acrylic adhesive has been studied over a wide range of test rates and temperatures. The laminates were prepared from polyimide films which had been subjected to either a “high-thermal history” or a “low-thermal history” treatment during the production of the film. The measured peel energies of the laminates could be superimposed to give a master curve of peel energy versus the reduced rate of peel test, Ra_T , where R is the rate of peel test and a_T is the time-temperature shift factor. The appropriate shift factors were a function of the test temperature and were mainly deduced from tensile tests conducted on the bulk adhesive. The “high-thermal history” laminates gave higher peel energies and the locus of failure of the laminates was mainly by cohesive fracture through the adhesive layer. At low values of log₁₀ Ra_T , i.e. Low rates of peel and high test temperatures, the “low-thermal history” laminates also failed in the adhesive layer and possessed similar peel energies to those measured for the “high-thermal history” laminates. However, at high log₁₀ Ra_T values, the peel energies measured for the “low-thermal history” laminates were lower and showed a wider scatter. These arose from a different locus of failure occurring in these “low-thermal history” laminates when tested under these conditions. Namely, it was found that most of these laminates failed in a weak boundary layer in the outer regions of the “low-thermal history” polyimide film.     

Peeling of heterogeneous thin films: Effect of bending stiffness,adhesion energy,and level of heterogeneity

The peeling behaviour of a heterogeneous thin film bonded to a rigid substrate was investigated by using both experiments and finite element modeling. The enhancement in peel force was studied specifically for heterogeneous thin films with periodic stiff and compliant portions along the length. Peel tests with homogeneous thin films (uniform film thickness) showed that the maximum peel force can be observed before the onset of steady state peeling process. Moreover, this maximum peel force was observed to be a function of the bending stiffness of the film and adhesion energy at the film-substrate interface. For the heterogeneous thin films, maximum peel force can be observed either before the onset of steady state or when the peel front traverses from compliant to the stiff portion of the film. The three-dimensional finite element model, based on cohesive zone technique was developed, which provided further insight into the enhancement in peel force. The maximum force was shown to be dependent on the level of heterogeneity in addition to adhesion energy and bending stiffness as was observed with homogeneous films. The improvement in peel force was found to be prevalent at relatively low adhesion energy. This study may be helpful for the better design of homogeneous and heterogeneous thin film-substrate systems having improved bonding strength.     

Mechanical effects in peel adhesion test

—Mechanical effects in the peel strength of a thin film have been studied both experimentally and theoretically. It has been found that the adhesion strength measured by the peel test is a practical adhesion (an engineering strength per unit width) and does not represent the true interface adhesion strength. The measured value may represent a multiplication of the true interface adhesion and other work expended in the plastic deformation of the thin film. The contribution of the latter to the peel strength is found to be, sometimes, of the order of 100 times higher than the former. It is found that the major controlling factors in the peel strength are the thickness, Young's modulus, the yield strength, the strain hardening coefficient of the film, and the compliance of the substrate as well as the interface adhesion strength. Even though the true interface adhesion strength is the same, a higher peel strength is obtained if the film is thinner or more ductile under the test conditions reported in this paper. The same effect can be obtained if the substrate is thinner in the case where the substrate is a soft elastic material, or if the substrate is thicker in the case where the substrate is a rigid material.     

The effect of residual stresses on adhesion measurements

The adhesion of films and coatings is often measured by determining the load required to separate them from their substrate. If there are residual stresses that are relaxed upon delamination, then an additional contribution to the energy-release rate will affect the measurements. These residual stresses may also cause a shift in the mode-mixedness of the interface crack which, in turn, can affect the interfacial toughness. To ensure an accurate interpretation of adhesion measurements, therefore, the effects of these stresses must be considered. These effects are discussed with particular reference to two commonly used test geometries: the blister test and the peel test.     

Calorimetric Measurements of The Heat Generated by The Peel Adhesion Test

The peel test is a simple mechanical test commonly used to measure the adhesion of flexible films bonded to rigid substrates. When the film is deformed elastically during peeling, the peel force is a direct measure of the strength of the interface. However, when plastic deformation takes place, the work of detachment is much larger than the thermodynamic work of forming the fracture surfaces. Simultaneous mechanical and calorimetric measurements of the work of detachment and the heat generated during the peeling of polymeric films from metal substrates and metal films from polymeric substrates have been made. An energy balance for peeling has been proposed. Most of the work of peeling was consumed by plastic deformation. The peeled polymer dissipated approximately one half of the work of peeling as heat and most of the remainder was stored in the peeled material. The peeled metal dissipated most of the work of peeling as heat.     

Characterization of an evaporated Al/PET interface by TEM and correlation with adhesion measured by a peel test

Transmission electron microscopy (TEM) has been used to characterize thin Al films thermally evaporated (vacuum around 10^-4 Torr) onto polyethylene terephthalate (PET) (Mylar?). The morphology of the Al/PET system has been correlated with the adhesion as measured by a peel test of the Al films. A special cross-section preparation revealed the exact thickness of the thin Al film, the roughness of the interfaces (Al/PET and Al/vacuum), the presence of precipitates or the diffusion of Al in the PET, the morphology of the Al layer (small grains or rod-like structure), the size of the grains or the columns (also checked with plane section), and the structure (crystalline or amorphous) of the PET at the Al/PET interface. The results suggest that the grain size and the roughness of the Al/PET interface decrease as the adhesion of the Al increases. Some spherical precipitates and diffusion of Al into PET were also observed for the films which had a low adhesion strength.     

Adhesion of Pure and CaCO3 Filled Latex Films on Poly(ethylene terephthalate)

Adhesion to poly(ethylene terephthalate) of carboxylated styrene-butadiene latex films, filled with calcium carbonate particles, was studied in this work. The acid content (2, 4 or 6 wt%) the degree of crosslinking (25, 50 or 75 wt% of insoluble polymer) of the latex particles, and the percentage of filler (0, 20, 40, 60, 80 or 90wt%) were varied. A peel test at 180° was used.

It was shown that, for the lowest filler percentages (up to 60 wt%), the films were non-porous and adhesion decreased when the peel rate, the percentage of filler, the degree of crosslinking and the acid content increased. Failure was always localized at the film-support interface (except at very low peel rate). At low peel rate, stick-slip was observed. The adhesion lowering can be explained by a decrease of the energy dissipation during peeling due to a reduced mobility of the polymeric chains. At high filler percentage (80 or 90 wt%), the films became porous and the level of adhesion very low. Failure occurred in the bulk of the latex film. The peel rate dependence was reversed; adhesion increased at higher speed. Owing to its marked importance in this system, the mechanism of the stick-slip phenomenon is especially discussed.     

A peel adhesion study of electroless Cu layers on polymer substrates

The peel adhesion between two different electroless-plated Cu layers and polymer substrates was studied. Cu was electroless-plated onto polymer substrates using two different commercial solutions with different compositions. The adhesion strength between the electroless Cu layers and polymer substrates was measured with the 90° peel test. The adhesion was influenced by the coverage, grain size, and the thickness of the electroless Cu layer. Poor coverage of the electroless Cu layer increased the density of the pores at the interface between the Cu layer and the substrates, thereby degrading the adhesion strength because of a decrease in the contact area. In addition, the electroless Cu layers with larger nodules and larger grains were softer and had higher peel adhesion since the soft and ductile Cu layer promoted a greater amount of plastic deformation during the peel test. This led to enhanced peel adhesion. Finally, as the thickness of the electroless Cu layer increased, the peel adhesion decreased. The thicker Cu layers are not easily bent. Poor bending of the Cu layer induced less plastic deformation, causing a decrease in the peel adhesion. In conclusion, soft and thin electroless Cu layers with greater coverage are preferred in order to obtain good adhesion.     

The Contact Adhesion of Self-Adhesive Strain Gauges

Thin pieces of flexible polymers may be adhered to rigid substrates merely by pressing the two surfaces into intimate contact. The peel strength of the bond is poor, but the shear strength can be sufficiently high for strain gauge operation. This paper offers an explanation for the adhesion which can account quantitatively for the behaviour of various materials. Frictional phenomena, resulting from a normal force produced by the surface tension of a surface film, can explain why a gauge with a PVC body does not slip. With other polymers, other liquids or electrostatic effects may be of importance. Any surface “fluid” film of sufficiently high viscosity that viscous effects are important will behave as an integral part of the elastomer.     

Adhesion and interface studies between copper and polyimide

The adhesion and interface structure between copper and polyimide have been studied. Polyimide films were prepared by spinning a polyamic acid solution (Du Pont PMDA-ODA) in an NMP solvent onto a Cu foil, followed by thermal curing up to 400°C. The adhesion strength was measured by a 90° peel test. The peel strength of 25 μm thick Cu foil to 25 μm thick polyimide substrate was about 73 g/mm with the peel strength decreasing with increasing polyimide thickness. Cross-sectional TEM observation revealed very fine Cu-rich particles distributed in the polyimide. Particles were not found closer than 80-200 nm from Cu boundary. These Cu-rich particles were formed as a result of reaction of polyamic acid with Cu during thermal curing. We attribute the high peel strength to interfacial chemical bonding between Cu and polyimide. This behavior is in contrast to vacuum-deposited Cu onto fully cured polyimide.     

The use of stimulated boundary gas release for determination of the adhesion of thin films by the blister test

The processes of stimulated gas release and gas blister growth were investigated at the interface of 100 nm thick silver films on glass substrates after irradiation by hydrogen ions of 1 MeV energy to fluences of 1 x 10¹³-1 x 10¹⁵ ion cm^-2. An interference microscope was used to examine the gas blisters and to measure the blister parameters. The relationship of these processes to the adhesion of a thin film system was established. A method to determine the adhesion and to compute the adhesion characteristics in the film-substrate system is described. The calculated energy of the detachment ranges between 0.06 and 28 J m^-2. Based on the results of this study, a series of practical approaches are proposed to measure the adhesion of thin films to substrates with the method of stimulated gas release.     

Evaluation of the Constrained Blister Test for Measuring Adhesion

The constrained blister test (CBT) was evaluated as a method for measuring adhesion using a model system, electrical tape bonded to polystyrene. Pressure is applied through a circular inlet hole in the substrate, causing the adhesive to “blister” up and peel radially away from the substrate. A glass constraint, placed some distance above the adhesive, limits deformation of the adhesive in the vertical direction and promotes radial peel. By operating at low spacer height (the distance of the constraint above the adhesive) and very low growth rates, the energy spent for deformation of the adhesive and viscoelastic dissipation is minimized. Blister radial growth was linear with time, and growth rate increased linearly with the second power of the energy input. An intrinsic, rate-independent adhesion energy was obtained by extrapolation to zero crack growth rate. The CBT was compared with two peel tests. The dependence of the growth rate on energy input was different, but the extrapolation to zero growth rate gave the same value of the intrinsic adhesion energy.     

PEEL ADHESION PROPERTIES OF AIR-DRIED PHARMACEUTICAL PRESSURE SENSITIVE ADHESIVE

ABSTRACT

The performance of a pharmaceutical pressure sensitive adhesive, whose liquid formulation is based on a multicomponent mixture of solvents, has been examined during two peel adhesion types of tests (90° dynamic adhesive strength peel test and 180° release liner peel test). The experiments were carried out under various drying temperatures, initial coating thickness, and types of backing film and release liner. The results show that the peel force depends mainly on the dry film weight of the tested adhesive. The type of the backing film which is used to form the adhesive also affects its peel adhesion properties.