On the evaluation of adhesion of coatings by automatic scratch testing

Automatic scratch testing is an expedient technique for comparatively evaluating the cohesive failure load and adhesion failure load of thin coatings on various substrates. In combination with SEM examination of the scratch track, this technique has been used herein to detect and evaluate various effects on coating strength and adhesion. For soft Triballoy T-800 and Stellite SF-6 cobalt-base coatings on 4340 low alloy steel, adhesion was found to be strong and failure was found to be cohesive in the coating. In the presence of a plated chromium interlayer, pre-existing cracks lowered substantially the cohesive failure load, which was also lowered by an increase in the coating deposition pressure. The spacing of transverse cracks within the coating was found in all cases to decrease with increasing applied normal load. In soft aluminum coatings on depleted uranium (DU)-0.75% Ti alloy specimens, alloying aluminum with magnesium or zinc enhanced the coating strength and adhesion. In (Al-Mg) coatings on this substrate, a smoother surface led to a lower friction coefficient and a higher adhesion failure load. In hard, thin TiN coatings on 17-4 PH steel, a lower bias voltage applied to the substrate yielded higher cohesive and adhesion failure loads. In hydrogenated amorphous SiC thin coatings on 4340 steel, loss of hydrogen by annealing converted the residual compressive stresses into tensile stresses and lowered both the cohesive and the adhesion failure loads. Finally, automatic scratch testing proved helpful in determining delamination loads in multilayer TiN/Ti/TiN coatings on DU-0.75% Ti alloy.     

Wetting behavior and interfacial interactions of molten Cu50Ti alloy with hexagonal BN and TiB2 ceramics

Wetting behavior of molten Cu50Ti alloy on hexagonal BN (h-BN) and TiB₂ ceramics has been studied under vacuum using a modified sessile drop method. Final contact angles of 8° and 3° are obtained at 1000 °C on h-BN and TiB₂, respectively. Interaction occurs at the interface between the molten alloy and BN, leading to the formation of a reaction layer containing TiB and Ti nitrides. Interfacial interaction of Cu50Ti with TiB₂ results in the formation of densely packed TiB layer about 60–100 μm thick and the detachment of TiB₂ grains. Spreading wetting of liquid Cu50Ti on h-BN is mainly controlled by the reactions between Ti and BN at the triple line. For Cu50Ti/TiB₂ system, spreading is mainly limited by the interfacial reaction in the first stage, and is possibly influenced by both the diffusion of boron atoms and viscous friction of the liquid in the second stage. Finally, brazing of graphite to CuCrZr alloy has been realized using Cu50TiH₂ with ceramic additives (including BN and TiB₂) as composite fillers. The joints exhibit favorable interfacial bonding between the filler layer and the substrates. The ceramic reinforcements in the filler layer could contribute to the improvement of the shear strength.     

Advanced characterization of laminated electrical steel structures under shear loading

ABSTRACT

The thermomechanical and mechanical behavior of electrical steel laminates was investigated by dynamic mechanical analysis (DMA) and a short beam test. These tests were implemented to evaluate the effect of various steel alloys on the adhesion properties of epoxy. DMA showed a dependency of curing state affected by the thermal conductivity of the steel alloy. Strain evaluation by digital image correlation showed that interlaminar shear failure occurred in a predominately cohesive manner in the epoxy layer at a shear angle of about 5°. This critical angle was not affected by the yield strength of the steel alloy used to create the laminate.     

Effect of heat treatment on microstructure and mechanical properties of cold sprayed Ti coatings with relatively large powder particles

In this study, the effect of post-spray heat treatment on the microstructure, microhardness, and adhesive strength of the cold-sprayed Ti coating was investigated. It was found that a thick and relatively porous Ti coating was deposited by cold spraying. The coating surface layer presented a more porous structure. The microhardness of the as-sprayed Ti coating was slightly higher compared to pure Ti bulk, owing to the work hardening effect during deposition. After annealing at 850°C for 4 h under vacuum condition, the Ti coating also presented a porous structure with more uniformly distributed small pores. A metallurgical bonding between the deposited particles was formed through annealing treatment. The adhesive strength of coating was significantly improved after annealing. The microhardness of the annealed Ti coating was also increased.     

Internal stresses and adhesion of thin silicon oxide coatings on poly(ethylene terephthalate)

The effect of internal stresses on the cohesion and adhesion of a thin silicon oxide (SiO_x) oxygen-barrier coating, evaporated on a poly(ethylene terephthalate) (PET) film substrate was studied. Internal stresses were generated during annealing in the temperature range for recrystallization of the PET,during calendering in a multilayer structure where two SiO_x /PET films were laminated together with a polypropylene film, and during long-term thermal aging below the glass transition temperature of the polymer. The cohesion of the coating and its adhesion to the polymer substrate were derived from fragmentation tests, in which the failure of the oxide coating was analyzed as a function of the applied stress during uniaxial tensile loading of the substrate. The intrinsic coating strength at critical length and the interfacial shear strength were found to be equal to 1350 MPa and 73 MPa, respectively. It was found that none of the thermal treatments investigated altered the interfacial interactions. Rather, these treatments induced shrinkage of the PET substrate, which increased the coating internal compressive stress and the SiO_x /PET interfacial shear strength. A linear relationship between the SiO_x /PET interfacial shear strength and the coating internal stress was determined from a stress transfer analysis. The coefficient of this linear relationship, equal to-1.34 · h _c/l _c, where h _c is coating thickness and l _c is the critical stress transfer length, reproduces the experimental data with good accuracy.     

Microstructure and mechanical property of SiC whisker coating modified C/C composite/Ti2AlNb alloy dissimilar joints prepared by transient liquid phase diffusion bonding

SiC whisker coating was prepared on the surface of C/C composite successfully by CVD, and transient liquid phase (TLP) diffusion bonding was employed to realize the joining of SiC whisker coating modified C/C composite and Ti₂AlNb alloy using Ti–Ni–Nb foils as interlayer. The microstructure, shear strength and fracture behavior were investigated by scanning electron microscopy (SEM) with energy dispersive X-ray spectrometer (EDS), X-ray diffraction (XRD) and universal testing machine. The results show that SiC has good compatibility with C/C composite, and gradient interface formed between SiC-modified C/C composite and Ti₂AlNb alloy. When the bonding experiment was carried out under bonding temperature of 1040 °C and holding time of 30min with 5 MPa pressure in vacuum, the joints formed well and no obvious defects can be observed. The typical microstructure of joints is C/C composite/SiC + TiC/Ti–Ni compounds + Ti–Ni–Nb solid solutions/residual Nb/diffusion reaction layer/Ti₂AlNb alloy. With the increasing of bonding temperature, the thickness of joining area increased due to sufficient element diffusion. However, when bonding temperature is elevated to 1060 °C, some defects such as cracks and slag inclusions exist in the interface layer between interlayer and Ti₂AlNb. The joints with maximum average shear strength of 32.06 MPa are bonded at 1040 °C for 30min. C, SiC and TiC can be found on the fracture surface of joints bonded at 1040 °C which indicated that fracture occurred at the interface layer adjacent SiC layer.     

Effects of moisture and temperature ageing on reliability of interfacial adhesion with black copper oxide substrate

The reliability of adhesion performance of bare Cu, as-deposited and surface-hardened black oxide coatings on Cu substrates was studied. The interfacial adhesion with a polyimide adhesive tape and an epoxy moulding compound was measured using the button shear and tape peel tests after hygrothermal ageing in an autoclave, high temperature ageing and thermal cycles. Moisture adsorption and desorption studies at different aging times suggested that the black oxide coating was effective in reducing the moisture adsorption. The bond strengths for all substrates remained almost unchanged after thermal ageing at 150°C for 8 h. Thermal cycling between ?50°C and 150°C for 500 cycles reduced by about 20% the button shear strength of the as-deposited black oxide substrate, but it did change much the bonding performance of the bare Cu substrate. Hygrothermal ageing at 121°C/100% RH in an autoclave was most detrimental to adhesion performance because of the combined effect of elevated temperature and high humidity. The reduction in button shear strength after the initial ageing for 48 h was 50–67%, depending on the type of coating. In all accelerated ageing tests, the residual interfacial bond strengths were consistently much higher for the black-oxide-coated substrates than the bare Cu surface, confirming a higher reliability of black oxide coating. Fracture surfaces analysis of tape-peeled bare copper substrates after 500 cycles of thermal loading revealed a transition in failure mechanism from interfacial to cohesive failure. In contrast, the failure mechanism remained unchanged for black-oxide-coated substrates. The observations made from the button shear and tape peel tests were generally different because of the different fracture modes involved.     

Evaluation of a structural epoxy adhesive for timber-glass bonds under shear loading and different environmental conditions

This article presents a study of timber-glass adhesive joints. It examines the shear specimen and shear tools preparation process and the evaluation of the results backed up with an overview of existing similar studies. The chosen adhesive was a cold-curing two-component structural bonding epoxy resin (Mapei Adesilex PG1). The shear tests were performed under different temperatures and the timber samples had different moisture contents. A simple shear test tool was designed and was clamped into a universal testing machine for the shear test. The force and crosshead displacement values from the universal testing machine were used for evaluating the results. The environmental conditions of 20 °C and 5% timber moisture content resulted in the highest average shear strength obtained from the shear tests of the analysed joints (9.89 MPa), whereas the environmental conditions of 50 °C and 20% timber moisture content resulted in the lowest average shear strength (3.42 MPa). It was found that the joint strength is dependent on the environmental temperature and timber moisture content. Moreover, the shear specimen load-displacement behaviour at the environmental temperature of 50 °C was linear and nonlinear – depending on the timber moisture content. The most frequent failure type was timber failure. Additionally, a nonlinear contact finite element analysis was performed to demonstrate the additional shear specimen rotation due to the clearance between the shear specimen and shear tools. This impact was evaluated regarding the stress distribution in the bond line. The evaluated epoxy resin adhesive was proved to be suitable for timber-glass bonds.     

Influence of epoxy resin on the microstructure and cavitation erosion of as-sprayed 8YSZ coating

The microstructures of materials are sensitive to shock waves and microjets induced by bubble collapse. The microstructure of coatings is thus closely related to their cavitation performance. Coating defects always act as the preferential sites for the bubble growth; thus, the materials around pores have been spalled preferentially under strong impact. In this study, epoxy resin (ER) was introduced into as-sprayed 8?wt% yttria-stabilized zirconia (8YSZ) coating by vacuum impregnation to prepare 8YSZ-ER coating. Results showed that the hardness, toughness, cohesive strength, and density of 8YSZ-ER coating are greatly improved. Cavitation performance is also improved; 8YSZ coating exhibited only a deceleration period whereas 8YSZ-ER coating showed a long steady-state period. This finding was mainly attributed to the enhanced compactness and cohesive strength of 8YSZ-ER coating, which caused the impact force to be evenly distributed on the specimen surface without accumulating in the pores. Cracks were also deflected, turned and terminated due to the presence of ER. Moreover, the relationship between ER aging and the damage mechanism of 8YSZ-ER coating under cavitation erosion was also examined.     

Improving the adhesive,mechanical, tribological properties and corrosion resistance of reactive sputtered tantalum oxide coating on Ti6Al4V alloy via introducing multiple interlayers

Tantalum oxide film has become an investigation focus for surface modification materials in the biomedical field owing to its outstanding biocompatibility, anti-corrosion, and anti-wear performances. However, tantalum oxide films exhibit poor adhesion because of the mismatch between the properties of the film and the substrate. In this study, a novel multilayer tantalum oxide coating of Ta_mO_n/Ta_mO_n-TiO₂/TiO₂/Ti (code M-Ta_mO_n) was deposited on Ti6Al4V by magnetron sputtering with Ta_mO_n single-layer coating as control. The purpose of this work is to evaluate the influence of the introduced Ta_mO_n-TiO₂/TiO₂/Ti multi-interlayer on the microstructure, adhesive, mechanical, and anti-corrosion properties of reactive sputtered tantalum oxide coatings. The outcomes show that the Ta_mO_n-TiO₂/TiO₂/Ti intermediate layer improves the bonding strength between the Ta_mO_n layer and Ti6Al4V matrix from 17.83 N to over 50 N and enables the Ta_mO_n coating to have an increased H/E and H³/E² ratio, decreased friction coefficient and wear rate, raised potential, and reduced corrosion current density. The improved properties of the multilayer system are attributed to the positive effects of the inserted multiple interlayers in reducing the residual stress in the coating, coupling the mechanical performance between the layer and the substrate, blocking the continuous growth of penetrating defects in a film with columnar structure. These experimental results provide a workable route for improving the properties of the tantalum oxide coating on Ti6Al4V alloy for medical applications.     

The Effect of Different Surface Pretreatment Methods on Nano-adhesive Application in High Strength Steel and Aluminum Bonding

Epoxy adhesives (single and two components) modified with SiO₂ nano-particles were used in this investigation to glue aluminum alloy and also two types of high strength steel (dip-galvanized steel DP 600 and micro-alloyed steel ZStE340). To improve the adhesion between metal surfaces and adhesives, the metal surfaces were pretreated with: a self-indicating pretreatment (SIP^*); corundum blasting; corundum blasting + a SIP coating; and a Pyrosil^® treatment + SurALink^® primer (PG 15 for epoxy adhesive). A single-lap shear tension test, done in accordance to DIN EN 1465, was used to determine the adhesive strength. Scanning Electron Microscopy (SEM) and Energy Dispersive X-ray spectroscopy (EDX) analysis were used to analyze fractures that took place in the samples. The results showed that the adhesion strength of glued samples, containing the nano-particles modified adhesive, had significantly higher strength than unmodified ones. Pretreatment of the metal surfaces affected the adhesion, using nano-adhesives, only slightly. The adhesive strength values for single component epoxy resins were higher than those for two component epoxy resins. It was found that steel samples fractured adhesively at the steel surfaces. Aluminum treated samples indicated after pretreatment an increase in adhesive strength and the fracture occurred adhesively at the aluminum surfaces. Aluminum glued with two-component adhesives and pretreated with corundum blasting plus a SIP coating showed a mixed fracture mode; adhesively at the aluminum surface and cohesively in the adhesive layer.     

Bonding properties between nitrile–butadiene rubber and aluminum alloy treated by anodizing methods

In this work, the bonding properties between the LD7 aluminum alloy anodized by sulfuric acid or phosphoric acid and nitrile–butadiene rubber (NBR) were investigated. The bonding properties between the anodized aluminum alloys and NBR were compared with those between aluminum alloys treated by burnishing or sandblasting and NBR. The results revealed that, in comparison with sulfuric acid anodized samples, samples anodized in phosphoric acid solutions showed higher 90° peel strength. Under the same conditions, an increase in the anodic film thickness in the studied range may improve the adhesion property between rubber and an aluminum alloy. In comparison with aluminum alloys treated by burnishing or sandblasting, the surface of the anodized aluminum alloy showed homogeneously dispersed pores, which resulted in better and homogeneous bonding properties. A vacuum‐drying process on the anodized aluminum alloys after they were coated with adhesives facilitated penetration of the adhesive molecules into the pores on the oxide layer, which considerably improved the bonding properties. In addition, rubber macromolecules could also penetrate the pores in the aluminum oxide layer, leading to a strong physical anchor–hold interaction after a long time of soaking and diffusion. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Microstructure and mechanical properties of C/C composite/Ti6Al4V joints with a Cu/TiCuZrNi composite brazing alloy

C/C composites and Ti₆Al₄V sheets were joined using a novel Cu/TiCuZrNi composite braze and the effect of Cu foil thickness on the microstructure and mechanical properties of the joints were investigated. A composite joining material, consisting of a TiC particle reinforced brazing alloy formed in situ during the brazing process was obtained. Before the joining process, the C/C composite surface was modified by solid state reaction with chromium to form a chromium carbide coating. This carbide reaction layer can react with the Ti-based brazing alloy and form evenly distributed TiC particles. The maximum apparent shear strength of as-received joint was 39±8.5 MPa obtained by using a 40 μm thick Cu foil together with the TiCuZrNi alloy; this value was 70% higher than the mechanical strength obtained for joints brazed with the TiCuZrNi alloy only.     

Joining of SiCf/SiC using a layered Ti3SiC2-SiCw and TiC gradient filler

A layered filler consisting of Ti₃SiC₂-SiC whiskers and TiC transition layer was used to join SiC_f/SiC. The effects of SiC_w reinforcement in Ti₃SiC₂ filler were examined after joining at 1400 or 1500 °C in terms of the microstructural evolution, joining strength, and oxidation/chemical resistances. The TiC transition layer formed by an in-situ reaction of Ti coating resulted in a decrease in thermal expansion mismatch between SiC_f/SiC and Ti₃SiC₂, revealing a sound joint without cracks formation. However, SiC_f/SiC joint without TiC layer showed formation of cracks and low joining strength. The incorporation of SiC_w in Ti₃SiC₂ filler showed an increase in joining strength, oxidation, and chemical etching resistance due to the strengthening effect. The Ti₃SiC₂ filler containing 10 wt.% SiC_w along with the formation of TiC was the optimal condition for joining of SiC_f/SiC at 1400 °C, showing the highest joining strength of 198 MPa as well as improved oxidation and chemical resistance.     

Effect of MWCNT filled epoxy adhesives on the quality of adhesively bonded joints

Most adhesively bonded joints exhibit adhesive or cohesive failure, i.e. failure at the adhesive/adherend interface or within the adhesive, respectively. The main objective of this study is to investigate the effect of surface modification of the metal substrate accompanied by modification of the adhesive properties on the strength and failure mechanism of bonded joints. A 5061 aluminium alloy has been used as the metal substrate onto which two types of surface treatments were applied; chemical surface modification and gritblasting. A standard epoxy resin was used as the adhesive medium, in which multi-wall carbon nanotubes (MWCNTs) were dispersed, with a range of weight fraction content (from 0.03% to 0.5%). The resin was fully characterised by mechanical testing in order to determine the optimum weight fraction to enhance its properties. Aluminium to aluminium and glass fibre reinforced polymer (GFRP) composite to aluminium single lap joints bonded with either pure epoxy resin or MWCNT reinforced epoxy resin were subsequently manufactured and tested. The tests show a moderate increase of the joint strength when MWCNTs are added into the adhesive with the failure mechanism changing from cohesive to adhesive. In addition, the comparison between different surface preparation methods shows that gritblasting results in considerably improved adhesive strength over chemical treatment.     

Effect of the microstructure of copper oxide on the adhesion behavior of epoxy/copper leadframe joints

The thermal oxidation of copper leadframe was carried out at 175°C and the adhesion behavior of the epoxy/copper leadframe joint was analyzed by investigating the microstructure changes of copper oxide with the thermal oxidation time of copper. The peel strength increased sharply at an early stage of oxidation (~20 min) followed by a slight increase. After further oxidation (120 min), the peel strength showed a slight decrease. The contact angles of water and diiodomethane decreased sharply at an early stage of oxidation with negligible change afterwards. As the oxidation time increased, X-ray photoelectron spectroscopy (XPS) results revealed that the chemical composition of copper oxide had changed (Cu/Cu₂O → Cu₂O → CuO); this change improved the wettability of the copper surface, which affected the peel strength. Increase of the surface roughness of copper oxide, investigated by scanning electron microscopy (SEM) and atomic force microscopy (AFM), causes the epoxy resin and copper oxide to undergo mechanical interlocking, which increases the peel strength. Failure analysis by SEM and XPS indicated that failure was largely in the copper oxide, and the amount of copper oxide on the peeled epoxy increased as the oxidation time increased, due to the weak mechanical strength of the oxide layer. However, a small portion of the epoxy resin was also fractured during the failure process, regardless of the oxidation time. Consequently, fracture proceeded mainly in the copper oxide close to the epoxy resin/copper oxide interface.     

Glass/epoxy composites and aluminium alloy joint using Kevlar® intermediate layer and nanoclay-reinforced epoxy adhesive

Adhesive lap joint between glass fibre/epoxy composites and aluminium alloy (2014 T4) was prepared by an in situ moulding process using a matched die mould. The surface of aluminium alloy was treated with chromic acid before adhesive bonding. Lap shear strength and fatigue life were evaluated in tensile mode and tension–compression mode (at 40% of lap shear load of adhesive joint), respectively. Knurling on the surface of aluminium alloy improved the lap shear strength of the adhesive joint but did not influence the fatigue life of the same. Lap shear strength and fatigue life of adhesive joint made with neat epoxy adhesive and reinforcement of an intermediate layer of Kevlar^® between glass/epoxy composite and aluminium alloy were observed to be 0.44?kg/mm² and 3.6?×?10⁵ cycles, respectively. In another case, lap shear strength and fatigue life of similar type of adhesive joint made from nanoclay (Cloisite 30B)-reinforced epoxy adhesive and without reinforcement of an intermediate layer of Kevlar^® were observed to be 0.38?kg/mm² and 2.3?×?10⁵ cycles, respectively. Whereas, lap shear strength and fatigue life of adhesive joint made from nanoclay-reinforced epoxy adhesive along with the reinforcement of an intermediate layer of Kevlar^® were 0.48?kg/mm² and 3.9?×?10⁵ cycles, respectively. Therefore, adhesive joint made from nanoclay-reinforced epoxy adhesive along with the reinforcement of an intermediate layer of Kevlar^® was the best.     

Brazing of Al2O3 to Ti-6Al-4V alloy with in situ synthesized TiB-whisker-reinforced active brazing alloy

65.9Cu-24.4Ti-9.7TiB₂ (wt.%) composite filler was used to join Al₂O₃ and Ti-6Al-4V alloy. 30 vol.% TiB whiskers were in situ synthesized as reinforcements in joints. Brazing temperature was 890 °C, 910 °C, 930 °C, 950 °C and 970 °C, and the holding time was 0, 5, 10, 20, and 30 min. The microstructure and mechanical properties of brazed joints were analyzed by scanning electron microscope equipped with energy dispersive spectrometer, shear test and nano-indentation test. Results show that reaction layer Ti₄(Cu,Al)₂O forms at Al₂O₃/brazing alloy interface. The reaction between TiB₂ powders and Ti atoms in brazing alloy brings on in situ synthesizing TiB whiskers in (Ti,Al)₂Cu and AlCu₂Ti intermetallics. Formation of TiB whiskers minimizes the mismatch of thermal expansion coefficient between Al₂O₃ and brazing alloy, and makes the ductile-rigid-ductile multiple layer present in joints, which reduces residual stress of joints. The maximum shear strength of joints can reach 143.3 MPa when the brazing temperature is 930 °C, and holding time is 10 min.     

Inorganic primers in bonded joints

An amorphous aluminium oxide coating, generated from aluminium chelate or alkoxide compounds, has been investigated as a primer for adhesively bonded phosphoric acid anodized 2024 aluminium adherends. Tensile lap shear and T-peel specimens were used to evaluate the effect of the alumina-coated surfaces on the mechanical properties of the bonded joints. Equivalent wet and dry tensile lap shear and T-peel bond strenghts were obtained when the inorganic coating was substituted for the normally used organic primer. Transmission and scanning electron microscopy of the alumina-primed surfaces showed that the oxide honeycomb/protrusion morphology resulting from phosphoric acid anodizing was infiltrated by the solution-deposited inorganic primer to produce a low profile bonding surface.     

Durability of Adhesive Bonds to Zinc-Coated Steels: Effects of Corrosive Environments on Lap Shear Strength

The effects of corrosive environments on adhesive bonds to electro-galvanized, zinc/aluminum alloy coated, coated electro-galvanized, and cold-rolled steels have been investigated. Bonds prepared using a rubber-modified dicyandiamide-cured epoxy adhesive, an epoxy-modified poly(vinyl chloride)-based adhesive, an acrylic-modified poly(vinyl chloride)-based adhesive a one-part urethane adhesive, and a two-component epoxy-modified acrylic adhesive were exposed under no-load conditions to constant high humidity or cyclic corrosion exposure for 50 days or 50 cycles (10 weeks) respectively.

Over the course of this study, exposure to constant high humidity had little effect on lap shear strength for any of the systems studied. Bond failures were initially cohesive, and with few exceptions remained so.

Bond strength retention under the cyclic corrosion exposure conditions employed was strongly dependent on adhesive composition and on substrate type. On galvanized substrates, lap shear strengths for the poly(vinyl chloride)-based adhesives were reduced by 90–100% during the course of the corrosion exposure, and a change in the mode of bond failure (from cohesive to interfacial) was observed. On the coated electro-galvanized steel substrate, the poly(vinyl chloride)-based adhesives showed about 50% retention in lap shear strength and a cohesive failure throughout most of the corrosion test. The dicyandiamide-cured epoxy adhesive used in this study generally showed the best lap shear strength retention to zinc-coated substrates; bonds to cold-rolled steel were severely degraded by corrosion exposure. The performance of the acrylic and urethane adhesives were intermediate to the dicyandiamide-cured epoxy and poly(vinyl chloride)-based adhesives in strength retention.