J. Cent. South Univ. (2022) 29: 38363846 DOI: https://doi.org/10.1007/s11771-022-5218-z Role of oxides in the formation of hole defects in friction stir welded joint of 2519-T87 aluminum alloy YI Tie(易铁)1, LIU Sheng-dan(刘胜胆)1, 2, 3*, FANG Chen(方晨)1, JIANG Geng-duo(江耿铎)4 1. School of Materials Science and Engineering, Central South University, Changsha 410083, China; 2. National Key Laboratory of Science and Technology on High-strength Structural Materials (Central South University), Changsha 410083, China; 3. Key Laboratory of Non-ferrous Metals Materials Science and Engineering of Ministry of Education (Central South University), Changsha 410083, China; 4. School of Mechanical and Automotive Engineering, South China University of Technology, Guangzhou 510640, China © Central South University 2022 Abstract: The role of oxides in the formation of hole defects in friction stir welded joint of 2519-T87 aluminum alloy has been investigated by using optical microscope, scanning electron microscope, electron backscatter diffraction and electron probe microanalyzer to examine the distribution of oxides and the features of hole defects, and using ABAQUS 3D thermo-mechanical coupling finite element model based on arbitrary Lagrangian-Eulerian method to simulate the material flow behavior. Oxides exist at the edge of tunnel hole and in the micropores in the joint. Based on distribution of oxygen and material flow behavior, it is believed that the oxides on the surface of the alloy tend to flow down into the bulk along the flow direction of plastic material during friction stir welding, aggregate in the weak region of material flow at the intersection of the shoulder affected zone and the stir pin-tip affected zone, and consequently prevent the material from contacting and diffusing. Due to the insufficient material flow and therefore the small plastic deformation, the pressure is not high enough to compress the accumulated oxides, resulting in hole defects. Key words: aluminum alloy; friction stir welding; arbitrary Lagrangian-Eulerian method; hole defects; oxides Cite this article as: YI Tie, LIU Sheng-dan, FANG Chen, JIANG Geng-duo. Role of oxides in the formation of hole defects in friction stir welded joint of 2519-T87 aluminum alloy [J]. Journal of Central South University, 2022, 29(12): 3836−3846. DOI: https://doi.org/10.1007/s11771-022-5218-z. 1 Introduction Friction stir welding (FSW) is a solid-phase welding technology and especially suitable for aluminum alloys welding, because it can avoid solidification defects caused by traditional fusion welding [1 − 3]. However, there are still some problems in friction stir welded aluminum alloys, such as tunnel hole and micropores. These defects are prone to stress concentration and become crack initiation region, resulting in the deterioration of mechanical properties in the joints [4−6]. Therefore, it is essential to understand the formation of hole defects in friction stir welded aluminum alloys to improve the joint quality. In some investigations, the formation of hole defects was believed to be related to the insufficient plastic flow of the material. For instance, HUANG et al [7] investigated the formation of defects in Received date: 2022-05-05; Accepted date: 2022-08-20 Corresponding author: LIU Sheng-dan, PhD, Professor; E-mail: lsd_csu@csu.edu.cn; ORCID: https://orcid.org/0000-0001-8547-0180 3837 J. Cent. South Univ. (2022) 29: 38363846 friction stir welded joints of Al-Mg-Si aluminum alloy and thought that the main reason for tunnel hole defects is that the plastic material could not fully backfill the cavity on the advancing side. HAN et al [8] found that insufficient heat input results in poor fluidity in friction stir welded powder metallurgy 2024 aluminum alloy, and hole defects form if the plastic materials cannot reach the position of the hole in time during welding. SHOJAEEFARD et al [9] found that low rotation and welding rates during FSW lead to low heat input and increase the possibility of formation of defects in friction stir welded joints of 7075-O and 5083-O aluminum alloys. In other investigations, it is believed that the oxides on the surface of aluminum alloy weldment mainly contribute to the formation hole defects [10 − 14]. For instance, DAI et al [13] examined the micropores in friction stir welded joints of 6082-T6 aluminum alloy and found a higher oxygen concentration on the edges of the micropores, indicating the presence of oxide particles near the micropores. ZHOU et al [14] found the same phenomenon in friction stir welded 6082-T6 alloy joint. During welding, the oxides may flow with the plastic materials, and then exert complex effect on the formation of hole defects; therefore, more investigations are needed to clarify this issue. Recently, some attempts have been made to investigate material flow behavior during friction stir welding or friction stir processing (FSP) using numerical model to understand the formation of hole defects better. For instance, CHAUHAN et al [15] used a coupled Eulerian and Lagrangian method to simulate the friction stir welding process of 6061-T6 aluminum alloy and used volume of fluid principle to predict the formation of defects during the process. WEN et al [16] used an arbitrary Lagrangian-Eulerian coupling method to simulate the friction stir welding of 5052 aluminum alloy and showed that increasing the tool rotating rate can enhance the fluidity of materials and thus effectively eliminate hole defects. AKBARI et al [17] used Deform-3DTM software to simulate the material flow during FSP and found that the materials on the advancing side experience a higher amount of effective strain than on the retreating side, and the material deformation near the top surface is higher than the near bottom area. In this work, the role of oxides in the formation of hole defects in friction stir welded joint of 2519T87 aluminum alloy has been investigated based on experimental results of distribution of oxides and the features of hole defects and the material flow behavior simulated by finite element method. This can help to better understand the formation mechanism of hole defects and then eliminate them in the FSW of aluminum alloys. 2 Experimental procedure 2519-T87 aluminum alloy sheets with a thickness of 2.5 mm were used for FSW and the chemical compositions are listed in Table 1. During welding, the inclination angle of the rotation axis and the press amount of the stir tool were 2.5° and 0.3 mm, respectively; the stir tool was inserted into the weldment with a rotation rate of 1600 r/min and a welding rate of 80 mm/min. Preheating to a low temperature can soften the material and decrease the axial downward pressure of the stir tool [18]. During welding, the weldment was preheated to 75 ℃ without causing grain coarsening of the base metal. The weldments were all cooled to room temperature in the air after welding. Table 1 Chemical compositions of 2519-T87 aluminum alloy wt% Cu Mn Mg Ti Zr Fe Si Al 5.80 0.30 0.20 0.05 0.02 0.10 0.02 Bal. Samples with sizes of 30 mm×15 mm×2.5 mm were cut along the direction vertical to the welding direction from the joint. The metallographic samples were mechanically polished and etched in 30% NaOH solution for about 30 s, and then immersed in 3% HNO3 solution to remove the corrosion products on the surface. The samples were cleaned in water, dried in still air, and examined by Leica DM2700M optical microscope. Some samples were mechanically polished first and then electrolytically polished in an electrolyte of 10% HClO4+90% CH3OH at 20 V for 6−8 s, and finally examined by JSM-7900F scanning electron microscope with an electron backscatter diffraction (EBSD) detector to investigate grain structure. The distribution of oxides in joint was examined by JXA-8230 electron probe microanalyzer (EPMA). The morphology of 3838 J. Cent. South Univ. (2022) 29: 38363846 hole defects in the joints were examined by Zeiss MA 10 scanning electron microscope (SEM) and Oxford EDS energy spectrum detector. 3 Mathematical modeling 3.1 Geometrical conditions and mesh generation Because the adaptive remeshing of ALE maintains high accuracy in large deformation during FSW process, ABAQUS 3D thermo-mechanical coupling finite element model (FEM) was used to investigate the plastic flow behavior of welded material [19−21]. The weldment was set as an undivided sheet in the simulation process. To prevent meshes distortion caused by excessive deformation in the process of stir tool pressing down, a conical through hole matching the stir pin was preset for the welding part. To prevent the model meshes distortion caused by the geometric corner of the stir pin-tip, the length of the stir pin was set to be greater than the thickness of the sheet. The stir tool was set as an analytical rigid body and no meshing was carried out. The geometry is shown in Figure 1. Physical properties of H13 steel for stir tool can be found in Ref. [22]. Figure 2 Displacement boundary condition alloy are similar to 2219 aluminum alloy, so the mechanical and physical parameters of 2219 aluminum alloy from Refs. [23 − 24] were used in this work (see Figure 3). The Johnson-Cook semiempirical formula was used to describe the relationship of flow stress, strain rate and temperature [25] (see Eqs. (1) and (2)). Figure 3 Mechanical and physical properties of 2219 aluminum alloy σ = (A + Bεˉnp1 )(1 + Cln Figure 1 Stir tool geometry in mm used in the simulation and dimensions (Unit: mm; All corner radii are 0.2 mm) In ALE model, non-uniform meshes were used, i.e., fine meshes of 0.2 mm in the center zone of the joint and coarser meshes in other zones; there are 6032 meshes and 7980 nodes (see Figure 2). C3D8RT eight-node hexahedron reduced integral displacement/temperature coupling solid element were used. 3.2 Material properties The chemical compositions of 2519 aluminum εˉ̇ pl )(1 - T *m ) ε̇ 0 ì 0 T < T 0 ï ï T - Tm * T0 £ T £ Tm T =í ï Tm - T0 ïî1 T 0 > T m (1) (2) where σ is the flow stress; εˉpl is the effective plastic strain; εˉ̇ pl is the effective plastic strain rate; ε̇ 0 is the normalized strain rate; T is the temperature; T0 is the initial temperature (75 ℃ ); Tm is the melting temperature (542 ℃). The values of constants A, B, C, n, m for 2519 aluminum alloy are from Ref. [26] and presented in Table 2. The elastic part of the material was described by Hooke’s law. The mass scaling technique was applied in the simulation [27] and the mass scaling coefficient was 107. It is worthy to mention that the J. Cent. South Univ. (2022) 29: 38363846 3839 Table 2 Constants of Johnson-Cook model for 2519 aluminum alloy A/MPa B/MPa C n m ε̇ 0/s−1 452.7 282.6 1.42×10−2 0.42 0.74 1.0 mass scaling does not change the volume of heat generated by plastic deformation work and friction slip. 3.3 Boundary conditions A thermo-mechanical finite element based on the ALE formulation and adaptive remeshing were applied in this work. The weldment was set as the adaptive region. The upper and lower surfaces of the weldment were set as the sliding surface. The surface perpendicular to the joint was set as the Eulerian surface to facilitate the inflow of materials. In ALE model, velocity boundaries were used in the Eulerian region to prevent material from flowing out of the surface (see Figure 2). The welding conditions used in the model, including the inclination angle, press amount, rotation speed and welding speed, were the parameters used for welding in Section 2. The penalty function friction model was used for contact boundary and the coulomb law of friction was applied. The friction coefficient between the stir tool and the weldment was 0.4. The contact type was finite slip friction. The rigid surface of the stir tool was the principal surface and the surface of the weldment was the minor surface. The initial temperature of the weldment was 75 ℃ . The heat transfer coefficient between the bottom and side of the weldment and the fixture was 200 W/(m2·℃) and the heat transfer coefficient between the weldment and the air was 30 W/(m2·℃). 4 Results 4.1 Features of hole defects According to the characteristics of the stir tool action zone, the nugget zone (NZ) is divided into shoulder affected zone (SAZ) and stir pin-tip affected zone (SPTAZ) (see Figure 4). There are micropores and tunnel hole on the advancing side (AS) of the joint. The tunnel hole exhibits a wedged shape from zone I in Figure 4. Micropores exhibit small irregular shapes near the boundary between NZ and the thermal mechanical affected zone Figure 4 Local morphology of the advancing side of the joint (TMAZ). These defects are solid bonding defects that located on the bonding line between SAZ and SPTAZ. The edge of the tunnel hole exhibits bright contrast (see Figure 5(a)), and EDS results show that oxygen element is densely distributed here (see Figure 5(b)). Therefore, oxides are likely present in this region. Oxygen element is also visible at the micropores (see Figures 5(c) and (d)), and some oxide particles in the micropores are detected. It is related to the deterioration of material flow and the accumulation of oxides and will be discussed in Section 5. It was found that the regions surrounding the tunnel hole exhibit different grain structures (see Figure 6(a)). Equiaxed grains are present in the SAZ on the upper side of the hole, and their sizes are (1.27±0.87) μm. Finer equiaxed grains exist in the SPTAZ on the lower side of the hole, and their sizes are (0.78±0.41) μm. It is because the shear rate and heat generation on the top of the weld are higher than that on the bottom of the weld [28]. Downward migrating materials and upward migrating extruded materials intersect here, but do not mix well, leading to tunnel hole. The compacted bonding line exhibits a good metallurgical binding, but the grain structure is different in this region (see Figure 6(b)). It is seen that some ultra-fine grains are present in the center of bonding line (see the arrows in Figure 6(b)), and their sizes are about (0.47±0.11) μm. It is because the flowing materials in compacted bonding line experience severe plastic deformation, and the 3840 J. Cent. South Univ. (2022) 29: 38363846 Figure 5 SEM images and oxygen mapping for hole defects of joint: (a) Tunnel hole from zone I in Figure 4; (b) Oxygen distribution mapping of (a); (c) Micropores from zone III in Figure 4; (d) Oxygen distribution mapping of (c) Figure 6 EBSD map of the regions surrounding the tunnel hole and compacted bonding line: (a) Tunnel hole in the purple dotted frame of Figure 5(a); (b) Compacted bonding line from zone II in Figure 4 prolific dislocation wall and significant difference in the stored energy between the neighboring grains provide a favorable crystallographic condition for the formation of ultra-fine grains [29]. The features of streamline and distribution of oxygen in AS-TMAZ and NZ are shown by EPMA images in Figure 7. The oxides flow path is roughly consistent with the outer edge of the stir pin. RAJAKUMAR et al [30] and ZHOU et al [31] found that the internal oxides of joint mainly come from the oxide film on the original weldment surface and the oxidation products of aluminum alloy form at high welding temperature. From Figures 7(b) and (d), during welding, after being broken and stirred, the oxide film and oxidation products flow along the plastic flow direction of material indicated by arrows, and continuous streamline arrays of oxide particles form on the cross-section of the joint. 4.2 Simulation results The cross-section of the joint was examined. The starting point is the time when the semicircle behind the stir pin passes through the studied surface, and the ending point is the time when the semicircle behind the stir pin finally leaves the studied surface. Figure 8 shows the flow velocity distribution on the cross-section of the weldment around the stir tool. The flow velocity of materials on the joint surface is the highest and decreases with the depth increasing. At the starting point (see Figure 8(a)), the material flows slowly near the stir J. Cent. South Univ. (2022) 29: 38363846 3841 Figure 7 EPMA map showing oxygen distribution: (a) Images of AS-TMAZ from zone IV in Figure 4; (b) Oxygen distribution mapping of (a); (c) Images of NZ from zone V in Figure 4; (d) Oxygen distribution mapping of (c) Figure 8 The material flow velocity profiles around the stir tool during FSW: (a) Starting point; (b) Mid-point; (c) Ending point pin-tip on the AS, as shown in the purple dotted frame. This indicates that the shear speed at the stir pin-tip is low, and the deformation resistance of the edge material is large. In Figure 8(b), as the stir pin leaves the studied surface, the material flow velocity near the stir pin-tip on the AS is much lower. After the stir pin completely leaves the studied surface (see Figure 8(c)), the material near the stir pin-tip on the AS stops flowing. Based on the experimental results in Section 4.1, the hole defects tend to form in the purple dotted frame in Figure 4 near the stir pin-tip on the AS of the joint. Therefore, it is essential to focus on this zone, and the equivalent plastic strain field is shown in Figure 9. At the starting point (see Figure 9(a)), the equivalent plastic strain at the edge of the bonding line near the base material is relatively small, which is caused by the greater 3842 J. Cent. South Univ. (2022) 29: 38363846 Figure 9 The equivalent plastic strain field at the stir pin-tip on the advancing side during FSW: (a) Starting point; (b) Mid-point; (c) Ending point deformation resistance of the material due to lower temperature. However, the equivalent plastic strain tends to increase with the distance increasing away from the base material (see the black dotted frame of Figure 9(b)); it is likely due to the higher temperature and reduced material deformation resistance of the zone compared to the NZ edge (Figure 9(a)). Then, as the stir pin moves away from the studied surface, the equivalent plastic strain near the stir pin-tip becomes smaller (see the purple dotted frame of Figure 9(b) and (c)). 5 Discussion It is an effective way to understand the formation of defects by analyzing the material flow behavior [32]. According to previous investigations [33−35], the instantaneous cavity behind the stir pin on the AS is filled with the down flow of plastic material and upward flow of the extruded material, and consequently, the joint forms after periodically filling. During this process, if the materials cannot fully contact and diffuse at the intersection on the AS, e. g., prevented by oxides, it is easy for hole defects to form. Based on the experimental and simulation results in Sections 4.1 and 4.2, respectively, the role of oxides in the formation of hole defects during FSW can be inferred. Firstly, from the distribution of streamline arrays of oxides in the joint crosssection (Figures 7(b) and (d)), at the starting point, it is reasonable that some dispersed oxides can flow down with the plastic material, as described schematically in Figure 10(a). Near the bonding line of the base material, plastic flow deteriorates (see the purple dotted frame of Figure 8(a)), and therefore, the dispersed oxides accumulate to form a discontinuous oxide film (Figure 5(c)). The differences in the melting point and crystal structure between aluminum and alumina make it impossible for atomic diffusion to occur [36 − 37]. Therefore, the oxide film hinders material contact and diffusion, as described schematically in Figure 10(b). Meanwhile, the pressure force produced by small plastic deformation (Figure 9(a)) is not high enough to compress these materials, leading to the micropores in zone III in Figure 4. After the stir pin moves, the plastic deformation becomes larger in the black dotted frame of Figure 9(b), indicating strong intersection of the materials; as a result, the bonding line is pressed tightly, which can be seen in zone II in Figure 4 and Figure 6(b). As the stir pin moves away, the material flow and the plastic deformation decrease in the purple dotted frame of Figures 9(b) and (c). A number of J. Cent. South Univ. (2022) 29: 38363846 3843 Figure 10 Schematic of plastic flow at the stir pin-tip on AS during FSW: (a) Starting point; (c) Mid-point; (e) Ending point; (b) Details of micropore in the purple dotted frame of (a); (d) Details of tunnel hole in the purple dotted frame of (b) oxide particles begin to accumulate and form a sharp oxide layer edge in the purple dotted frame of Figure 5(a), and therefore a higher pressure is essential to form a strong metallurgical bonding. However, this is unlikely to occur because as the welding proceeds, the material flow becomes more difficult, as shown in the purple dotted frame of Figure 8(b). Then, the hole gradually expands through the gap and the oxide layer separates the material flow, as described schematically in Figures 10(c) and (d). Finally, when the stir pin completely leaves the studied surface, as described schematically in Figure 10(e), the welded material stops flowing (Figure 8(c)), and the cavity cannot be fully filled, resulting in the tunnel hole from zone I in Figure 4. Therefore, to effectively eliminate the hole defects during friction stir welding of aluminum alloy, it is essential to reduce the content of oxide in the weld and simultaneously increase the material fluidity. It is known that mechanical cleaning or chemical cleaning before FSW may be used to eliminate the oxide film on the surface of aluminum alloy weldments [38], to reduce the content of oxide. And the material flow can be improved by optimizing the process parameters and the geometry of stir tool [39]. Recently, the auxiliary energy method, such as laser and TIG assisted FSW, has been developed to evaporate the oxide film on the surface of aluminum alloy weldments and simultaneously enhance the material flow [40 − 41]. This is a worthwhile topic for future investigations. 6 Conclusions In this work, ABAQUS 3D thermo-mechanical coupling FEM based on ALE method was used to analyze the material flow of friction stir welded joint, the synergistic role of oxides and material flow in the formation of hole defects during FSW was investigated. 1) In the friction stir welded joint of 2519 aluminum alloy, the hole defects are present on the AS and located on the bonding line between SAZ J. Cent. South Univ. (2022) 29: 38363846 3844 and SPTAZ at the bottom of joint. The hole defects are covered with dense oxides. The grains are larger on the upper side than the lower side of the hole defects. 2) During welding, oxides flow along the direction of plastic flow of the material and accumulate in the weak flow zone at the intersection of SAZ and SPTAZ and contribute to the formation of tunnel holes and micropores by preventing materials contact and diffusion. 3) At the intersection of SAZ and SPTAZ, the pressure generated by insufficient material flow cannot compress the accumulated oxides, resulting in hole defects; however, the pressure generated by sufficient material flow can compress the accumulated oxides, resulting in a compacted bonding. [5] [6] [7] [8] [9] Contributors The overarching research goals were developed by LIU Sheng-dan and YI Tie. FANG Chen and JIANG Geng-duo established the models and analyzed the measured data. YI Tie conducted the literature review and wrote the first draft of the manuscript. LIU Sheng-dan checked and proofread the draft of manuscript. 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Eliminating hole defects and improving microstructure and mechanical properties of friction stir welded joint of 2519 aluminum alloy via TIG arc [J]. Journal of Materials Processing Technology, 2022, 310: 117773. DOI: 10.1016/j. jmatprotec. 2022.117773. (Edited by YANG Hua) 3846 J. Cent. South Univ. (2022) 29: 38363846 中文导读 氧化物在 2519-T87 铝合金搅拌摩擦焊接头孔洞缺陷形成中的作用 摘要使用光学显微镜、扫描电子显微镜、电子背散射衍射仪和电子探针显微分析仪研究了氧化物在 2519-T87 铝合金搅拌摩擦焊接接头孔洞缺陷形成中的作用并采用基于任意拉格朗日-欧拉方法的 ABAQUS 三维热力耦合有限元模型对材料流动进行分析。氧化物存在于接头隧道孔洞的边缘和微孔洞 中。根据氧元素的分布和材料的流动行为可知在搅拌摩擦焊接过程中合金表面的氧化物往往沿着 塑性材料的流动方向向下流动聚集在肩部影响区和搅拌针端部影响区交汇处的材料流动薄弱区域 并因此阻碍材料的接触和扩散。由于材料流动不足因此塑性变形较小导致产生的压力不足以压合 积累的氧化物从而导致孔洞缺陷产生。 关键词铝合金搅拌摩擦焊接任意拉格朗日-欧拉方法孔洞缺陷氧化物
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