Keywords: Adhesively bonded joint, laminates, CFRP, stacking sequence

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THE 19 TH INTERNATIONAL CONFERENCE ON COMPOSITE MATERIALS GLOBAL AND LOCAL INFLUENCE OF STACKING SEQUENCE ON THE STRENGTH OF ADHESIVELY BONDED JOINTS OF CFRP LAMINATES J. Rousseau*, P. Satthamnuwong DRIVE, Institut Supérieur de l Automobile et des Transports, Université de Bourgogne, 49 rue Mademoiselle Bourgeois, 58000 Nevers, France * Corresponding author (jerome.rousseau@u-bourgogne.fr) Keywords: Adhesively bonded joint, laminates, CFRP, stacking sequence 1 Introduction Although adhesive bonding of composite materials has undeniable advantages compared to other joining techniques, the difficulties encountered in predicting the failure of such joints prevent the generalization of their use. In the case of CFRP laminates, the failure strength can be affected by the ply orientation near the adhesive layer. But the assessment of the influence of this local parameter is difficult because changing local ply orientations results often in changing also the global elastic properties of the laminates. Matthews and Tester [1] studied the influence of the stacking sequence on the failure of single lap joints (SLJ) of laminates with different configurations of 0, 45 and -45 layers. The highest strengths were obtained when the 0 layers were placed on the outer surfaces of the laminates. In this case, the bending stiffness was also increased, making it difficult to attribute the strength to the local orientation or to the global stiffness. Johnson and Mall [2] studied 0/0, 45/45 and 90/90 interfaces in SLJ of composite laminates. The higher strength was attained with 45/45, followed by 0/0 and 90/90 was the worst case. Kairouz and Matthews [] investigated the behavior of cross ply adherends with 0 or 90 surface layer. They noticed that the joint strength increased when the bending stiffness increased in the first case and increased when the bending stiffness decreased in the second case. The failure mechanisms were also different. Song et al. [4], in a more recent study, compared the behavior of SLJ made from laminates with three different sequences and concluded that the larger in plane moduli led to higher strength. These various studies show that the assessment of the effect of the stacking sequence is a difficult task, and the explanations provided are sometimes linked to the global laminate properties, and sometimes to local fracture effects. This study presents a method to separate these effects. Local effects are evaluated using a special quasi isotropic quasi homogeneous (QIQH) laminate stacking sequence, allowing variation of the ply orientations without changing the elastic properties of the adherends [5]. For comparison purpose, tests are performed on a well-known quasi isotropic stacking sequence which actually possesses isotropic membrane properties but anisotropic bending properties. The same local orientations are studied, but their influence on the joint strength is somewhat masked by the effect of the varying overall stiffness of the joint. It is nevertheless possible to explain the observed results by superposing local effects and global effects computed from a simple closed form analysis. 2 Specimens and testing The adherends were manufactured from a 100g/m2 carbon/epoxy unidirectional prepreg (Hexcel NHCM 676/4%/106/M40J with properties as indicated in Table 1). After curing (120 min at 175 C under 700 kpa pressure), the final thickness of the 24 ply laminates was 2.4 mm. Table 1. Elastic properties of the unidirectional ply

In order to study the local ply distribution effect, the chosen stacking sequences must possess the same [0/45/90/-45] local sequence near the adhesive. Hence the two selected stacking sequences: - Seq A: [0/45/90/-45/90/-45/45/-45/0/90/0/45/ 0/45/-45/45/90/0/90/-45/90/-45/0/45] T - Seq B: [0/45/90/-45] S Sequence A is called a quasi-isotropic, quasi homogeneous (QIQH) sequence. These laminates are uncoupled and isotropic with identical bending and membrane elastic properties. It means that all the terms of the coupling matrix [B] are equal to zero and that the membrane and bending reduced stiffness matrices are identical. 1 h A 12 D (1) h With such a choice, no change occurs in the overall elastic behavior of the laminate when changing the loading direction. Sequence B is the well-known quasi-isotropic symmetrical sequence involving [0/45/90/45] group of plies. This sequence actually presents isotropic elastic membrane properties, but marked anisotropic properties when considering its bending behavior. near the adhesive, according to the loading direction. One can note that the bending stiffness of the sequence A adherends remains the same (79 MPa) regardless of the orientation. In the case of sequence B and for the selected orientations, this stiffness changes from a minimum of 61 MPa at -45 to a maximum of 97 MPa at 0. The single lap joint adherends were cut from the laminate plates manufactured at four directions rotated by 45 steps. The regions to be bonded were abraded with fine abrasive paper. This operation was followed by a solvent wipe. The laminates plates were then clamped in a special jig and a bond thickness of 0.4 mm was obtained using calibrated wire. The adhesive is a single part epoxy with aluminum filler (Permabond ESP110). An example of a tensile test performed on a bulk specimen of this adhesive is presented Fig. 2. The boundaries of the bonded area were covered with a non-stick adhesive tape, so as to avoid the formation of a spew fillet at both ends of the overlap. The curing cycle was 1 h at 120 C. After curing, the specimens were cut at 20 mm width with a diamond saw. The wires ensuring the bond thickness were removed during this sawing operation. The specimen geometry is presented Fig.. Fig. 2. Stress-strain curve of the Permabond ESP110 adhesive Fig. 1. Polar diagram of the bending moduli Fig. 1 shows the polar plots of the bending moduli of the two sequences, along with the ply distribution All specimens are made of two identical adherends, which means from the geometry of the single-lap joints that the plies orientations on each side of the adhesive layer are not symmetrical. For example, two opposite plies oriented at 0 or 90 are aligned,

Failure load (N) 20 mm GLOBAL AND LOCAL INFLUENCE OF STACKING SEQUENCE ON THE STRENGTH OF ADHESIVELY BONDED JOINTS OF CFRP LAMINATES whereas two opposite plies oriented at 45 are orthogonal. 100 mm 180 mm 20 mm Fig.. Specimen geometry 0 mm For each lay-up and each orientation, five specimens were tested until failure in a MTS screw-driven tensile testing machine at a rate of 0. mm/min. Acoustic emission was constantly monitored during the test using two micro-0 wide band piezoelectric transducers (100-600 khz) attached on each adherend (Fig. 4). An acquisition threshold of 40 db EA was chosen in order to filter background noise. The signal was amplified and processed by a PCI-2 system from EuroPhysical Acoustics. Using two transducers allowed us to only take into consideration the AE events coming from the loaded specimen, and to eliminate noises coming from the grips. It also allowed locating the position of the event sources. average value since the sound propagates through two different materials and two interfaces. A sound velocity value of 5000 m/s was measured using Hsu- Nielsen pencil lead fractures. Results Failure loads measured for both sequences are presented fig 5. The results are ordered according to the position of the 0 layer among the first four plies near the adhesive. 5000 4000 000 2000 1000 0 Seq A Seq B 1 2 4 Fig. 5. Failure loads with respect to the local ply distribution (1: [0/45/90/-45/ ; 2: [-45/0/45/90/ ; : [90/-45/0/45/ ; 4: [45/90/-45/0/ ) The standard deviation of the failure load values is in the order of 200 MPa for each set of specimens. The highest values of standard deviation are observed for the specimens with a 0 ply near the adhesive. Fig. 4. Specimen with attached acoustic emission transducers The accuracy of this event location computation depends on the precision of the sound velocity measurement in the material. In the case of an adhesively bonded joint, the sound velocity is an The strength of the SLJ made from Seq A adherends seems to increase when the position of the 0 layer is farther from the adhesive layer. This is not the case for Seq B, which gives better results than Seq A for the first orientation, similar results for the second and lower results for the third and fourth orientations. These observations cannot be straightaway explained with local or global analyses and need further investigation. Fracture examination Close examination of the specimens after failure shows that the fracture mechanisms are identical for

the two sequences A and B when considering the same set of first four plies near the adhesive layer. The fracture initiates at the end of the overlap, where the peel and shear stresses are the highest, and then propagates inside the first plies until the adherend breaks. No adhesive fracture has ever been observed at any time. A typical lateral view of a broken joint is presented in Fig. 6: the adhesive layer is intact; the lower adherend has failed while the upper one is only partially fractured. triangular shapes and some of these remain unbroken. Case [45/90/-45/0 (Fig. 7-d) The crack initiates in the 45 layer and propagates in a triangular zone. The 90 layer under this first layer is easily crossed and the fibers of this layer in front of the crack path are totally expelled during the failure. The next layer is composed of -45 fibers. It separates also in two triangular shapes. The post failure examination does not allow determining if the failure of this -45 layer appears at the same time or after the failure of the 45 layer. As in the previous cases, the crack crosses some fibers of the 0 layer and propagates in this layer until total joint separation. Fig. 6. Typical fracture The different fracture mechanisms can be reconstructed from the examination of broken specimens presented in Fig. 7. Case [0/45/90/-45 (Fig. 7-a) The 0 layer fibers are fractured at the end of the overlap under the action of the peel stress (or under a combination of bending and peel stresses). Once the crack has crossed a small fraction of the thickness of this layer, it propagates very easily along the fibers and across the matrix in an intralaminar mode. Only this 0 layer is affected by the fracture mechanism. Case [-45/0/45/90 (Fig. 7-b) The crack initiates in the -45 layer and propagates in an intralaminar fashion. It cannot lead to the total failure of the joint because only a triangular zone is delaminated. The crack then crosses some fibers of the 0 layer and propagates in this layer until failure. Case [90/-45/0/45 (Fig. 7-c) The first 90 layer is easily crossed since no fibers need to be broken. Once this layer is crossed, the apparent failure mechanism becomes very similar to the [-45/0/45/90 case. The only difference is that the -45 fibers are less neatly separated in two a - 0 layer in first position [0/45/90/-45 b - 0 layer in second position [-45/0/45/90 c - 0 layer in third position [90/-45/0/45 d - 0 layer in fourth position [45/90/-45/0 Fig. 7. Crack paths for the four configurations of the first four plies

GLOBAL AND LOCAL INFLUENCE OF STACKING SEQUENCE ON THE STRENGTH OF ADHESIVELY BONDED JOINTS OF CFRP LAMINATES The main conclusion that can be drawn from these observations it that the crack always goes through the first layers until it reaches the 0 layer which then fails in an intralaminar mode. In the case of sequence A, the number of crossed layers is associated with an increase of the failure load, suggesting that the crack path complexity positively affects the SLJ strength. Fig. 9 presents the AE activity recorded during a tensile test performed on a Seq A joint, with a -45 orientation (0 layer in fourth position). The first high amplitude events appear when the load is around 2 kn. There is a slow increase of the number of events before the first failure of a ply. This appears as a step on the load curve, associated with very high amplitude events. Acoustic emission The AE activity monitored during the tests provided numerous data. The use of two transducers allowed locating the acoustic events sources. The major part of the recorded events came from the adhesive layer zone, and particularly from both ends of the overlap (Fig. 8). Fig. 9. AE events recorded during a tensile test (Seq. A, -45 ). Fig. 8. AE location Fig. 10. Examples of AE activity recorded during the tensile tests: cumulated counts vs load (N) 5

These observations can be summarized in term of cumulated counts versus load curves (Fig. 10-abcd). This set of curve appears as a confirmation of the failure mechanisms inferred from the optical observations. When the fracture happens in the first 0 layer (Fig. 10-a), very few events are recorded. On the contrary, when several layers are involved in the failure process, an intense acoustic activity is observed (Fig. 10-bcd). This suggests that the layer cracking and delamination involved in the failure process do not occur simultaneously. There is a temporal succession in the advance of the crack through the different layers. In the case of joints made from QIQH laminates, the more layers the cracks have to go through, the higher the breaking strength is. 4 Discussion Results show that the two studied sequences differ only by the values of the failure strength, since the fracture mechanisms are identical. The hypothesis that can be made is that two phenomena occur in combination during the failure process: a local effect, depending on the order of the layers near the adhesive, and a global effect, coming from the elastic properties and depending also on the layer order but this time in the whole laminate. The local effect is readily assessed from the sequence A results, since they were unaffected by change in elastic properties. This effect was described above. The problem here is that it is impossible to assess the global elastic properties influence from the sequence B results, since local effects are also implied in the failure. Therefore, we chose to analyze this influence using the closed form solution proposed by Hart-Smith [7]. This analysis is based on the global elastic properties of the laminates and, as such, unable to predict the real failure strength in the present case. But it allows us to compute the peel stress and the bending stress in the adherends at the ends of the overlap for a given load in the bonded joint. Since the experimental observations indicate that the peel stress is certainly playing a major role in the fracture initiation, we will consider only this stress in the following. Hart-Smith solution was later modified by Kairouz and Matthews []. They introduced a change in the bending term to take into account the difference between tensile Poisson s ratio and bending Poisson s ratio. This derivation is recalled below: The average stress is given by av P / t (2) where P is the failure load per unit joint width and t is the adherend thickness. The adhesive peel stress is given by 2 t E(1 m) t a 1/ 2 p k av(1 )[ ] () t 2k E t where: b m a - E is the adhesive elastic modulus, - E m is the effective membrane elastic modulus of the adherends - k is the eccentricity factor given by 2 ( c) 1 k (1 c ) (4) 6 P with D, and c the half length of the overlap. - t a is the adhesive layer thickness - D is the flexural rigidity as modified in [] E t D b 2 12( 1 ν ) (5) b with b the bending Poisson s ratio and E b the effective bending modulus of the adherends k b - and finally k b is the non-dimensionalized bending stiffness parameter for composite adherends introduced by Hart-Smith [7] and modified in []: - 2 2 2 Ebt /12(1 b ) 12d11( a11 a12) (6) 2 2 2 2 E t /12(1 ) t a ( d d ) m m s where a ij and b ij are respectively the membrane and bending compliance terms of the laminate compliance matrix. 11 11 12

GLOBAL AND LOCAL INFLUENCE OF STACKING SEQUENCE ON THE STRENGTH OF ADHESIVELY BONDED JOINTS OF CFRP LAMINATES Values of k b corresponding to the different adherend orientations are presented in table 2. k b is of course equal to unity for each orientation in the case of sequence A. failure strengths of sequence B joints according to tensile direction vary less markedly that what could have been predicted from either bending stiffness or local fracture mechanism considerations. Sequence A B Orientation - 0 45 90-45 k b 1.00 1.22 1.15 0.84 0.77 Table 2. Values of the bending stiffness parameter k b The global properties influence linked to this bending stiffness was arbitrarily estimated by the method described thereafter. First, a mean failure peel stress (49 MPa) was computed from the average failure load (4250 N) of all the tested specimens, using equation () with sequence A elastic properties (i.e. k b =1). Then this value of peel stress was used to find the corresponding failure loads for the different orientations of sequence B. The percent deviation of the four computed failure loads from the average value allowed quantifying and ranking the global properties effect. The same treatment was applied to sequence A results (deviation in percent from the average failure load). Both local and global influences are presented together on Fig. 11. As it is well known and considering only global effects, when the bending stiffness of the adherends is increased, the peel stress is reduced and the predicted failure load is increased. So the global influence presented in Fig. 11 is not surprising. The local fracture mechanisms explained previously have a somewhat different influence, and, in the case of 0 and -45 orientations, a totally opposite effect. As mentioned above, the experimental failure loads measured in the case of sequence B joints cannot be explained by considering only global or local properties, but by taking into account the combination of both effects. That is the reason why we tried to superpose these effects by simply adding their influences in term of percent deviation. Fig 12 shows the results of this superposition compared to experimental results. While the agreement is not totally satisfactory, this superposition goes a long way to explain why the Fig. 11. Failure strength deviations from the average value according to local and global influences Fig. 12. Failure strength deviations from the average value as measured (sequence B) and predicted 5 Conclusion The purpose of the study was to investigate the role of the stacking sequences in the tensile failure of adhesively bonded joints made from carbon/epoxy laminates. In each studied case, the mechanism of crack propagation in the first four plies was reconstructed from the examination of the failure surfaces of the bonded joint and the recorded AE data. The 0 layer is the locus of an intralaminar crack resulting in a rapid fracture of the specimen, so the position of this layer with respect to the adhesive layer has a real influence on the joint strength when considering 7

QIQH sequence. Both failure load and AE activity (cumulative counts) are shown to increase with the distance of the 0 layer from the adhesive/laminate interface. This is explained by the increased complexity of the crack path ending in the 0 layer. The comparison with sequence B results shows the same failure mechanisms associated with the same AE activity, with respect to the local ply orientations, but different failure load values. This is due to the concurrent influence of the strengthening effect of the adherend bending stiffness in single lap joints. Bonded Carbon/Epoxy Laminate Joints International Journal of Adhesion and Adhesives, Vol. 5, pp 68-75, 2012. [7] L. J. Hart-Smith, Adhesive-bonded single-lap joints, Douglas Aircraft Co., NASA CR-11226, 197. As the failure strength of the adhesively bonded joints is dependent on both the local orientations and the global properties of the laminates, it is therefore important to separate these interactions in order to draw a correct interpretation of the influence of the stacking sequence on the failure process. The elastic strengthening effect can be accounted for using a simple closed form solution, but the assessment of the local effect requires an experimental approach using special QIQH sequences. References [1] F. Matthews and R. Tester Influence of stacking sequence on bonded CFRP SLJ, International Journal of Adhesion and Adhesives, Vol. 5, No. 1, pp 1-18, 1985. [2] W. S. Johnson and S. Mall Influence of interface ply orientation on fatigue damage of adhesively bonded composite joints, Journal of Composites Technology and Research, Vol. 8, No. 1, March 1986, pp -7, 1986. [] K. C. Kairouz and F. L. Matthews Strength and failure modes of bonded single lap joints between cross-ply adherends Composites, Vol. 24, No. 6, pp 475-484, 199. [4] M.-G. Song, J.-H. Kweon, J.-H. Choi, J.-H. Byun, M.-H. Song, S.-J. Shin and T.-J. Lee Effect of manufacturing methods on the shear strength of composite single-lap bonded joints, Composite Structures, Vol. 92, No. 9, pp 2194-2202, 2010. [5] P. Vannucci and G. Verchery A New Method for Generating Fully Isotropic Laminates Composite Structures, Vol. 58, No. 1, pp 75-82, 2002. [6] C. Galliot, J. Rousseau and G. Verchery Drop Weight Tensile Impact Testing of Adhesively