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Effect of Interface on Mechanical Properties of Ti/Al/Mg/Al/Ti Laminated Composites

Abstract

Ti/Al/Mg/Al/Ti laminated composites were fabricated via hot-pressing at 350 °C, 400 °C and 450 °C successfully. The influences of interface morphology, diffusion zone, constraint effect on the mechanical properties were investigated. At Ti/Al interface, intermetallic compounds aren’t found. Whereas, they form at Al/Mg interface. With the increasing temperature, the bonding strength of Al/Mg interface doesn’t change linearly, and the maximum strength is obtained at 400 °C because of intermetallic compounds with appropriate thickness. With the increase of temperature, the hardness at both Ti/Al and Al/Mg interfaces increases owing to the solid solution and the intermetallic phases. Also, the ultimate tensile strength of LMCs increases with sacrificing the fracture elongation. The rule of mixture is used to predict the theoretical strength. It is found that the theoretical values are less than the measured, and the reasons may relate to interfaces in Ti/Al/Mg/Al/Ti laminated composites.

Keywords:
Hot-pressing; Interface; Bonding strength; Hardness; The rule of mixture

1. Introduction

Laminated composites, which possess excellent ductility, strength and density, have drawn growing attention11 Medeiros RJ, Nóbrega SHS, Aquino EMF. Failure theories on carbon/kevlar hybrid fabric based composite laminate: notch and anisotropy effects. Mater Res. 2019;22(3):1-11.,22 Ribeiro AH, Gomez JE, Hale DW, Tonatto MLP, Panzera TH, Thomas C, et al. Evaluation of the stiffening mechanism based on micro-sized particle inclusions in laminated composites. Mater Res. 2019;22(4):1-9.. And plenty of metals have been adopted to prepare metal laminated composites. Mg and its alloys have been widely used due to their high specific strength, damping performance and low density. However, the inferior corrosion resistance, stiffness and abrasion resistance severely confine their development33 Zhang J, Liu S, Wu R, Hou L, Zhang M. Recent developments in high-strength Mg-RE-based alloys: Focusing on Mg-Gd and Mg-Y systems. Journal of Magnesium and Alloys. 2018;6(3):277-91.. Ti and its alloys are preferred where excellent specific strength, fracture toughness, temperature resistance and corrosion resistance are required44 Bridier F, Villechaise P, Mendez J. Analysis of the different slip systems activated by tension in a α/β titanium alloy in relation with local crystallographic orientation. Acta Mater. 2005;53(3):555-67.. Coating Ti layer on the surface of Mg not only overcomes their shortcomings but also takes advantage of dissimilar metals. However, almost no solid solubility or chemical reaction between Ti and Mg alloys raises a challenge to metallurgical bonding. Consequently, an intermediate layer should be added at Ti/Mg interface to facilitate atomic diffusion or reaction. In reality, the in-depth studies had been done on Mg/Al55 Yang WW, Cao XQ, Wang LF, Chen ZQ, Wang WX, Wang DY. Microstructure and mechanical properties of AA6061/AZ31B/AA6061 composite plates fabricated by vertical explosive welding and subsequent hot rolling. Mater Res. 2018;21(6):1-9. and Ti/Al66 Qin L, Wang H, Cui S, Wu Q, Fan M, Yang Z, et al. Characterization and formability of titanium/aluminum laminate composites fabricated by hot pressing. J Mater Eng Perform. 2017;26(7):3579-87. composites in previous works. Accordingly, it is feasible to fabricate Ti/Al/Mg/Al/Ti laminated composites by using Al as a connection layer between Ti and Mg sheets77 Kaibyshev R, Musin F, Lesuer DR, Nieh TG. Superplastic behavior of an Al-Mg alloy at elevated temperatures. Mater Sci Eng A. 2003;42:169-77..

Currently, solid-solid synthesis has been widely used because of fewer pores, oxidation inclusions and higher bonding strength than traditional fusion techniques. Solid-solid synthesis includes rolling88 Zhang X, Yu Y, Liu B, Ren J. Mechanical properties and tensile fracture mechanism investigation of Al/Cu/Ti/Cu/Al laminated composites fabricated by rolling. J Alloys Compd. 2019;805:338-45., hot-pressing99 Qin L, Wang J, Wu Q, Guo X, Tao J. In-situ observation of crack initiation and propagation in Ti/Al composite laminates during tensile test. J Alloys Compd. 2017;712:69-75., explosive welding1010 Fronczek DM, Chulist R, Szulc Z, Wojewoda-Budka J. Growth kinetics of TiAl 3 phase in annealed Al/Ti/Al explosively welded clads. Mater Lett. 2017;198:160-3., extrusion1111 Tang J, Chen L, Zhao G, Zhang C, Yu J. Study on Al/Mg/Al sheet fabricated by combination of porthole die co-extrusion and subsequent hot rolling. J Alloys Compd. 2019;784:727-38.,1212 Feng B, Xin Y, Yu H, Hong R, Liu Q. Mechanical behavior of a Mg/Al composite rod containing a soft Mg sleeve and an ultra-hard Al core. Mater Sci Eng A. 2016;675:204-11. and two or more of them (such as explosive welding and rolling55 Yang WW, Cao XQ, Wang LF, Chen ZQ, Wang WX, Wang DY. Microstructure and mechanical properties of AA6061/AZ31B/AA6061 composite plates fabricated by vertical explosive welding and subsequent hot rolling. Mater Res. 2018;21(6):1-9., hot-pressing and rolling1313 Du Y, Fan G, Yu T, Hansen N, Geng L, Huang X. Laminated Ti-Al composites: processing, structure and strength. Mater Sci Eng A. 2016;673:572-80. and so on). For instance, Zhang et al.88 Zhang X, Yu Y, Liu B, Ren J. Mechanical properties and tensile fracture mechanism investigation of Al/Cu/Ti/Cu/Al laminated composites fabricated by rolling. J Alloys Compd. 2019;805:338-45. manufactured Al/Cu/Ti/Cu/Al laminated composites via cold-rolling, exploring the fracture mechanism. Qin et al.66 Qin L, Wang H, Cui S, Wu Q, Fan M, Yang Z, et al. Characterization and formability of titanium/aluminum laminate composites fabricated by hot pressing. J Mater Eng Perform. 2017;26(7):3579-87. applied hot-pressing method to fabricating Ti/Al composites and examined the formabilities. Saravanan et al.1414 Saravanan S, Raghukandan K, Hokamoto K. Improved microstructure and mechanical properties of dissimilar explosive cladding by means of interlayer technique. Arch Civ Mech Eng. 2016;16(4):563-8. researched the interface properties of Al/Cu composites prepared by explosive welding. In the study carried out by Chen et al.1515 Chen Z, Wang D, Cao X, Yang W, Wang W. Influence of multi-pass rolling and subsequent annealing on the interface microstructure and mechanical properties of the explosive welding Mg/Al composite plates. Mater Sci Eng A. 2018;723:97-108., the Al/Mg/Al composites were prepared by extruding, and the effects of temperature on interface and microstructure were investigated. Zhang et al.1616 Zhang XC, Wang CJ, Deng KK, Nie KB, Gan WM, Liang W. Fabrication, microstructure and mechanical properties of the as-rolled ZW31/PMMCs laminate. Mater Sci Eng A. 2019;761:138043. designed ZW31/PMMCs composites by extrusion followed by rolling to solve the rolling problem of micron particle reinforced magnesium matrix composites. Furthermore, explosive welding and rolling were used by Fronczek and Chulist1717 Fronczek DM, Chulist LL. Microstructure and kinetics of intermetallic phase growth of three-layered A1050-AZ31-A1050 clads prepared by explosive welding combined with subsequent annealing. Mater Des. 2017;(130):120-30. to fabricate Al1050/AZ31/Al1050 composites, and the evolution rule of interface structure and intermetallic phases was probed. Assari and Eghbali1818 Assari AH, Eghbali B. Interfacial layers evolution during annealing in Ti-Al multi-laminated composite processed using hot press and roll bonding. Met Mater Int. 2016;22(5):915-23. researched the structure sequence of Ti-Al multi-laminated composite produced by hot-pressing and rolling. Among the methods above, hot-pressing is a promising technique employed in the fabrication of Ti/Al/Mg laminated composites for the advantages of cheap manufacturing and easy operation, and the metallurgical bonding can be achieved on the basis of element diffusion at high temperature. Meanwhile, the stable and excellent mechanical properties can also be realized in this way.

So far, plentiful works on Ti/Al composites have been done, such as layer thickness ratio1919 Fan M, Domblesky J, Jin K, Qin L, Cui S, Guo X, et al. Effect of original layer thicknesses on the interface bonding and mechanical properties of Ti Al laminate composites. Mater Des. 2016;99:535-42., reaction kinetics of phases at the interface2020 Sun Y, Wan ZP, Hu LX, Wu BH, Deng TQ. Characterization on solid phase diffusion reaction behavior and diffusion reaction kinetic of Ti/Al. Rare Met Mater Eng. 2017;46(8):2080-6., annealing process2121 Yu H, Tieu AK, Li H, Godbole A, Kong C. Annealing effect on microstructure and mechanical properties of Al/Ti/Al laminate sheets. Mater Sci Eng A. 2016;660:195-204., deformation mechanism of monolithic metal2222 Nie H, Hao X, Chen H, Kang X, Wang T, Mi Y, et al. Effect of twins and dynamic recrystallization on the microstructures and mechanical properties of Ti/Al/Mg laminates. Mater Des. 2019;181:107948. and formability2323 Kaya İ, Cora ÖN, Acar D, Koç M. On the formability of ultrasonic additive manufactured Al-Ti laminated composites. Metall Mater Trans, A Phys Metall Mater Sci. 2018;49(10):5051-64.. And the researches on Mg/Al composites mainly focused on the preparation technology2424 Wang T, Nie H, Mi Y, Hao X, Yang F, Chi C, et al. Microstructures and mechanical properties of Ti/Al/Mg/Al/Ti laminates with various rolling reductions. J Mater Res. 2018;34(2):344-53., bonding quality2525 Liu CY, Wang Q, Jia YZ, Jing R, Zhang B, Ma MZ, et al. Microstructures and mechanical properties of Mg/Mg and Mg/Al/Mg laminated composites prepared via warm roll bonding. Mater Sci Eng A. 2012;556:1-8., precipitated phases1111 Tang J, Chen L, Zhao G, Zhang C, Yu J. Study on Al/Mg/Al sheet fabricated by combination of porthole die co-extrusion and subsequent hot rolling. J Alloys Compd. 2019;784:727-38., formability2626 Nie H, Chi C, Chen H, Li X, Liang W. Microstructure evolution of Al/Mg/Al laminates in deep drawing process. J Mater Res Technol. 2019;8(6):5325-35. and so on. However, the investigations on Ti/Al/Mg/Al/Ti laminated composites are rare, especially the comprehensive influences of Ti/Al and Al/Mg interfaces on the mechanical properties of Ti/Al/Mg/Al/Ti laminated composites still require to be enriched.

In present work, the Al layer located between Ti layer and Mg layer in order to achieve better interface bonding, and the hot-pressing was adopted to prepare Ti/Al/Mg/Al/Ti laminated composites. The influence of hot-pressing temperatures on the interface structure and the mechanical properties was discussed. In particular, the applicability of the rule of mixture (ROM) on evaluating strength was checked, and the reasons for the gap between the measured values and the theoretical values were also analyzed for the purpose of better understanding on mechanical behavior of Ti/Al/Mg/Al/Ti laminated composites. The above research fruits, as a supplement in the field of laminated composites, are thought to provide guidance for the industrial production of Ti/Al/Mg/Al/Ti laminated composites.

2. Experimental Procedures

2.1 Materials and laminate processing

Commercial TA1 pure Ti, 2024 Al and AZ31B Mg are chosen as the component layers of Ti/Al/Mg/Al/Ti laminated composites. The TA1, 2024 and AZ31B plates with original thickness of 0.3 mm, 0.5 mm and 1 mm, respectively, all are cut into the size of 100 mm × 60 mm (the rolling direction (RD) × the transverse direction (TD)). The initial grain sizes of TA1 and AZ31B are ~7.69 μm and ~3.83 μm, respectively, as illustrated in Figure 1. For convenience, LMCs, Ti, Al and Mg are used to represent Ti/Al/Mg/Al/Ti laminated composites, TA1, 2024 Al and AZ31B Mg, respectively.

Figure 1
The metallographic structure of the original sheets of (a) TA1 and (b) AZ31B.

LMCs are fabricated by hot-pressing, and the preparation processes are illustrated in Figure 2. (i) The surfaces of Ti, Al and Mg are cleaned and roughened with a steel brush to remove surface dirt and oxide layers. The following specific steps include ultrasonic cleaning and rapid drying. (ii) The above plates are stacked in the order of Ti/Al/Mg/Al/Ti along the same direction, then they are put into the hot-pressing mold. (iii) The preparation technology is explored firstly. Figure 3 shows the macro morphologies of LMCs fabricated at different pressures and temperatures. At 200 MPa, Ti and Al are not bonded at 300 oC, while Mg is crushed out of LMCs at 500 oC, as shown in Figure 3a, thus the suitable temperature is 400 oC. Once the temperature is set as 400 oC, the bonding of LMCs depends on the pressure. As presented in Figure 3b, the well-bonding between Ti and Al doesn’t occur at 175MPa, and obvious cracks in Ti are visible at 225MPa, therefore only the pressure of 200MPa is a suitable one. Referring to the above results, the pressure of 200 MPa is adopted in present work. In order to reveal the effects of hot-pressing temperatures on the interface structure and mechanical properties of LMCs, the temperatures of 350oC, 400oC and 450oC are selected, and well-bonded LMCs are obtained at these temperatures. Detailed hot-pressing processes are demonstrated in Figure 3c.

Figure 2
The schematic diagrams of fabricating Ti/Al/Mg/Al/Ti laminated composites.
Figure 3
Exploration of (a) temperature at 200 MPa and (b) pressure at 400 oC during the preparation of LMCs, (c) the preparation technology of Ti/Al/Mg/Al/Ti LMCs.

2.2 Microstructure observation

Metallographic samples are fabricated by standard mechanical grinding and polishing, and the RD-ND planes are observed. LMCs are etched in Keller reagent (3ml HF + 2ml HNO3 + 95ml H2O) and 3.5% nitrate + 4% oxalic acid solution. The metallographic tests of Mg and Ti are carried out via optical microscope (OM). And US8010 Scanning Electron Microscope (SEM) equipped with an energy dispersive spectrometer (EDS) is adopted to achieve interfacial microstructure observation.

2.3 Mechanical properties test

The mechanical properties of LMCs and monolithic Ti, Al and Mg are measured using MTS (E45.105) electronic universal testing machine. And the size of tensile specimens is shown in Figure 4a. An extensometer with a gauge of 25 mm is applied to tensile specimens, and three specimens under each condition are tested at a constant crosshead speed of 1mm/ min.

Figure 4
The schematic diagrams of specimens for (a) uniaxial tensile tests and (b) shear tests.

The vickers hardness is measured with HV-1000 Micro Vickers Hardness Tester under a load of 100g for 15s.

The shear tests are performed to evaluate the interface bonding quality according to GB/T 6396-2008 standard. The specimens with an overlap joint size of 2×5 mm (RD × TD) are cut using wire electrical discharge machines, as shown in Figure 4b. The shear tests are conducted on MTS (E45.105) electronic universal testing machine with a speed of 0.5mm/min. The formula for calculating interface bonding strength is as follow: P = F/S, where F is tensile load and S represents bonding area.

3. Results and Discussion

3.1 Microstructure

Figure 5 presents the SEM images of Ti/Al interface. As shown in Figure 5a, well-bonded interfaces are obtained and no conspicuous voids or delamination can be observed. It is interesting that the morphologies of Ti/Al interfaces exhibit significant differences. At 350 oC, flat Ti/Al interface is observed, but it becomes rough at 400 oC and 450 oC. Which is attributed to the nonuniform deformation of adjacent metals with different plastic deformation ability. The appearance of rough interfaces is considered to be a signal of enhanced bonding strength1919 Fan M, Domblesky J, Jin K, Qin L, Cui S, Guo X, et al. Effect of original layer thicknesses on the interface bonding and mechanical properties of Ti Al laminate composites. Mater Des. 2016;99:535-42.. Figure 5a shows the EDS line analysis results of Ti/Al interface at different temperatures, and the obvious diffusion layers indicate metallurgical bonding between Ti and Al. The width of diffusion layers are 1.0 μm, 1.5 μm and 2.1 μm at the temperatures of 350 oC, 400 oC and 450 oC, respectively. The higher the temperature is, the wider the diffusion layer is1515 Chen Z, Wang D, Cao X, Yang W, Wang W. Influence of multi-pass rolling and subsequent annealing on the interface microstructure and mechanical properties of the explosive welding Mg/Al composite plates. Mater Sci Eng A. 2018;723:97-108.. As illustrated in Figure 5b, EDS point analysis at Ti/Al interface is performed at 450 oC. Combining with the EDS line analysis results of no platform on the curves in Figure 5a, it can be concluded that intermetallic phases don’t form at Ti/Al interface when hot-pressed at 450 oC. Due to the insufficient atomic diffusion at 350 oC and 400 oC, the same results can be obtained.

Figure 5
The SEM images of Ti/Al interface in LMCs: (a) the EDS line analysis at different temperatures, (b) the EDS point analysis at 450 °C.

The SEM images of Al/Mg interface are given in Figure 6. As can be seen from Figure 6a, obvious intermetallic phases layers are found, and their thicknesses increase as the temperature increases. Also, two layers marked by yellow dotted line in Al/Mg interface can be identified. According to the EDS point analysis results of Figure 6c, Al3Mg2 phase near Al layer and Mg17Al12 phase near the Mg layer are found. Based on the Al-Mg phase diagram and the previous works2626 Nie H, Chi C, Chen H, Li X, Liang W. Microstructure evolution of Al/Mg/Al laminates in deep drawing process. J Mater Res Technol. 2019;8(6):5325-35.,2727 Choi DH, Ahn BW, Lee CY, Yeon YM, Song K, Jung SB. Formation of intermetallic compounds in Al and Mg alloy interface during friction stir spot welding. Intermetallics. 2011;19:125-30., the same conclusion can also be achieved. The thicknesses of intermetallic phases layers at Al/Mg interface are ~10.56 μm, ~25.12 μm and ~38.40 μm at 350 oC, 400 oC and 450 oC, respectively. The EDS analysis results in Figure 6b also display a thickened diffusion region.

Figure 6
The SEM images of Al/Mg interface in LMCs: (a) the EDS line analysis and (b) the EDS map analysis at different temperatures, (c) the EDS point analysis at 450 oC.

Both Ti/Al and Al/Mg interfaces are well-bonded displayed in Figure 5a and Figure 6a. The film theory2828 Ma M, Meng X, Liu WC. Microstructure and mechanical properties of Ti/Al/Ti laminated composites prepared by hot rolling. J Mater Eng Perform. 2017;26(7):3569-78. indicates two contacted surface layers (including oxide film and contaminant film formed by brush scraping) break up and virgin metals are extruded through cracks under high temperatures and pressures. However, the adjacent sheets may not be bonded even if the virgin metals are exposed, unless the deformation is larger than a certain threshold2929 Lyu S, Sun Y, Li G, Xiao W, Ma C. Effect of layer sequence on the mechanical properties of Ti/TiAl laminates. Mater Des. 2018;143:160-8.. According to the energy barrier theory, the energy such as dispersing surface contaminants, extruding virgin metals, rearranging atoms to reconstruct grain boundary and activation energy are required for bonding metals. In present work, the rough surface is obtained by scratching with a steel brush during pretreatment. Thus the mechanical interlocking is achieved at the early stage of hot-pressing. And the pressure of 200 MPa applied to LMCs could overcome the energy barrier required for bonding metals. In an analysis of the changes of Ti/Al interface morphology, the differences on crystal structure and mechanical properties between Al and Ti must be considered. Pure Ti with HCP lattice below phase transition temperature (882 oC) possesses higher deformation resistance as compared with Al with FCC lattice. During deformation, shear occurs at the interface, which becomes much more drastic with the increasing temperature. Eventually strain localization generates near Ti/Al interface, so that protrusion and retrusion form along the interface2929 Lyu S, Sun Y, Li G, Xiao W, Ma C. Effect of layer sequence on the mechanical properties of Ti/TiAl laminates. Mater Des. 2018;143:160-8.. Furthermore, the difference of the thermal expansion coefficients between Ti and Al (Al is 18 ~ 24×10-6/ K, and Ti is 8.4 ~ 8.6×10-6/ K) may cause a thermal stress at the interface during the cooling after hot-pressing2121 Yu H, Tieu AK, Li H, Godbole A, Kong C. Annealing effect on microstructure and mechanical properties of Al/Ti/Al laminate sheets. Mater Sci Eng A. 2016;660:195-204.. These may result in some elastic-plastic deformation near the interface and finally trigger uneven interface.

From the EDS analysis results of Ti/Al and Al/Mg interfaces in Figure 5a and Figure 6a, the diffusion layer thickens with the increase of temperature. Previous works had demonstrated that elements diffusion was promoted through three basic mechanisms: mechanically induced atomic displacement, pipe diffusion along dislocations and vacancy diffusion induced by plastic deformation3030 Sauvage X, Dinda GP, Wilde G. Non-equilibrium intermixing and phase transformation in severely deformed Al/Ni multilayers. Scr Mater. 2007;56(3):181-4.. During hot-pressing, a large number of dislocations and vacancies are induced by severe plastic deformation. However, it is hard for dislocations to move by carrying atoms under high pressure. While the concentration and the mobility of vacancies enhance with the increasing temperature. As a result, diffusion at the interface accelerates owing to the migration of vacancies.

It can be seen from the EDS point analysis results in Figure 5b that intermetallic phases don’t form at Ti/Al interface. Ma et al.2828 Ma M, Meng X, Liu WC. Microstructure and mechanical properties of Ti/Al/Ti laminated composites prepared by hot rolling. J Mater Eng Perform. 2017;26(7):3569-78. and Xia et al.3131 Xia HB, Wang SG, Ben HF. Microstructure and mechanical properties of Ti/Al explosive cladding. Mater Des. 2014;56:1014-9. also didn’t find intermetallic phases at Ti/Al peeling surface of rolled and explosive welded Ti/Al layered composites because of the shorter reaction time. While Du et al.3232 Du Y, Fan GH, Yu T, Hansen N, Geng L, Huang X. Effects of interface roughness on the annealing behaviour of laminated Ti-Al composite deformed by hot rolling. Mater Sci Eng A. 2015;89:7. detected TiAl3 phase with a DO22 structure at Ti/Al interface fabricated by vacuum hot-pressing and hot-rolled. Also, Yu et al.2121 Yu H, Tieu AK, Li H, Godbole A, Kong C. Annealing effect on microstructure and mechanical properties of Al/Ti/Al laminate sheets. Mater Sci Eng A. 2016;660:195-204. proved that TiAl3 was the only phase that could form and grow at Ti/Al interface after annealing at 873 K for 6 h for as-rolled Al/Ti/Al. Based on above analysis, the nucleation and growth of phases depend on thermodynamic and kinetic conditions. At low temperatures, the nucleation is mainly related to atoms diffusion along grain boundaries. It is hard for Ti and Al atoms to diffuse massively in a short time due to insufficient atomic concentration and energy. Therefore, the formation of Ti-Al intermetallic phases is impossible.

As marked by the yellow dotted line in Figure 6c, the intermetallic phases layer can be seen clearly. According to Al-Mg binary phase diagram, the maximum concentration of Mg in Al and Al in Mg are 18.9 at % (at 450 °C) and 11.8 at % (at 437 °C), respectively. At the beginning of diffusion, diffusion between Mg atoms and Al atoms will form solid solution due to the driving force of concentration gradient. When the concentration is more than the maximum equilibrium concentration, the Al3Mg2 and Mg17Al12 precipitate from supersaturated solid solution of Al (Mg) and Mg (Al), respectively. The similar results were also confirmed by Yang et al.’s investigation55 Yang WW, Cao XQ, Wang LF, Chen ZQ, Wang WX, Wang DY. Microstructure and mechanical properties of AA6061/AZ31B/AA6061 composite plates fabricated by vertical explosive welding and subsequent hot rolling. Mater Res. 2018;21(6):1-9.. During the subsequent reaction process, a large number of intermetallic phases precipitate continuously, which accumulate and form a thin layer along the interface. After that, due to the concentration gradient between Mg/Al layer and new phases, the new phases grow in the direction perpendicular to the interface. Finally, a thick intermetallic phases layer forms.

Figure 7 demonstrates the OM images and grain sizes distribution of Ti and Mg in LMCs at different hot-pressing temperatures. The grain sizes of Ti are ~7.01 μm, ~7.34 μm and ~7.89 μm at 350 oC, 400 oC and 450 oC, respectively, only slight growth occurs. Considering that the melting point of pure Ti is 1668 °C, the Ti can be categorized as a warm-deformed structure at current temperatures. So the influence of temperature on grain size of Ti is not evident. It is interesting that a small number of twins are observed in Ti at 450 oC. The twins may be associated with the strain distribution during hot-pressing1414 Saravanan S, Raghukandan K, Hokamoto K. Improved microstructure and mechanical properties of dissimilar explosive cladding by means of interlayer technique. Arch Civ Mech Eng. 2016;16(4):563-8.. The recrystallization occurs in Mg at various temperatures. The grain sizes of Mg are ~3.08 μm, ~4.75 μm and ~5.49 μm at 350 oC, 400 oC and 450 oC, respectively. At 350 oC, a host of equiaxial fine grains are found at grain boundaries, especially at trigeminal grain boundaries2525 Liu CY, Wang Q, Jia YZ, Jing R, Zhang B, Ma MZ, et al. Microstructures and mechanical properties of Mg/Mg and Mg/Al/Mg laminated composites prepared via warm roll bonding. Mater Sci Eng A. 2012;556:1-8.. With the increase of temperature, the migration rate of grain boundaries accelerates, the grain size reaches the maximum and the distribution becomes more uniform at 450 °C. As shown in Table 1, the deformation of LMCs increases with the increase of temperature. Moreover, at high temperature, the higher strain energy in LMCs also provides driving force for grains growth.

Figure 7
Metallographic structure and grain size distribution of (a) Ti and (b) Mg at different hot-pressing temperatures.
Table 1
The thickness of Ti, Al, Mg and Al/Mg intermetallic layers in LMCs after hot-pressing at different hot-pressing temperatures.

3.2 Bonding strength

Huang et al.3333 Huang M, Xu C, Fan G, Maawad E, Gan W, Geng L, et al. Role of layered structure in ductility improvement of layered Ti-Al metal composite. Acta Mater. 2018;153:235-49. suggested that the high ductility of Ti-Al composites benefited from strong bonded interface, which not only reduced the strain localization of Ti layer, but also effectively relieved the stress concentration of Al layer. However, Launey et al.3434 Launey ME, Ritchie RO. On the fracture toughness of advanced materials. Adv Mater. 2009;21(20):2103-10. stated that delamination occurred easily at weak bonded interface, which could effectively restrict the crack propagation via crack deflection and blunting, thus toughening was achieved. Therefore, it is indispensable to evaluate bonding strength. In present work, bonding strength is measured by shear tests. Figure 8. shows variations of interface bonding strength for LMCs prepared at different hot-pressing temperatures.

Figure 8
Variations of interface bonding strength for LMCs prepared at different hot-pressing temperatures: bonding strength-strain curves of (a) Ti/Al interfaces and (b) Al/Mg interfaces, (c) variations of bonding strength for Ti/Al and Al/Mg interfaces.

From bonding strength-strain curves of Ti/Al interface in Figure 8a and variations of Ti/Al interface bonding strength in Figure 8c, it is observed that both bonding strength and fracture strain of Ti/Al interface increase continuously with the temperature increases. At 350 oC, 400 oC and 450 oC, Ti/Al interface bonding strength are 8.75 MPa, 25.8 MPa and 29.1 MPa, respectively. Especially from 350 oC to 400 oC, interface bonding strength increased by 195%. At 350 oC, at low strain, interface debonding occurs because of weak bonding. With the temperature increases, the strong interface leads to an enhanced constraint effect between Ti layer and Al layer, so fracture strain increases. The changes of Ti/Al interface bonding strength can be explained by the following aspects. From the perspective of deformation, with the temperature increases, the deformation of LMCs increases (as shown in Table 1), and the oxide layer and the dirt layer at the interface rupture, so more virgin metal is available in the contact surfaces for atom-to-atom bonding. Bouaziz et al.3535 Bouaziz O, Sauvage X, Barcelo D. Steel-magnesium composite wire obtained by repeated co-extrusion. Mater Sci Forum. 2010;654-656:1263-6. also found that the higher strains can improve interface bonding. Moreover, the higher deformation can easily cause severe shear deformation at the interface, thereby rough interfaces are introduced. The rough interfaces increase the actual contact area between Ti and Al, and is conducive to improving bonding strength. From the perspective of diffusion, with the temperature increases, the diffusion rate of Ti and Al atoms accelerates, and the diffusion layer thickens, which leads to enhanced metallurgical bonding2525 Liu CY, Wang Q, Jia YZ, Jing R, Zhang B, Ma MZ, et al. Microstructures and mechanical properties of Mg/Mg and Mg/Al/Mg laminated composites prepared via warm roll bonding. Mater Sci Eng A. 2012;556:1-8.. Furthermore, intermetallic compounds don’t form at Ti/Al interface as shown in Figure 5b, so their adverse effects are unnecessary to consider.

Figure 8b and Figure 8c show bonding strength-strain curves of Al/Mg interface and variations of Al/Mg interface bonding strength, respectively. At 350 oC, 400 oC and 450 oC, Al/Mg interface bonding strength are 16.35 MPa, 25.45 MPa and 18.85 MPa, respectively. From 350 oC to 400 oC, interface bonding strength increases, while it reduces from 400 oC to 450 oC. The changes of fracture strain is consistent with bonding strength. Different from Ti/Al interface, the bonding quality of Al/Mg interface has close relationship with transition layer. The formation of intermetallic phases is a symbol of metallurgical bonding, while intermetallic phases layer with excessive thickness is negative for bonding quality1111 Tang J, Chen L, Zhao G, Zhang C, Yu J. Study on Al/Mg/Al sheet fabricated by combination of porthole die co-extrusion and subsequent hot rolling. J Alloys Compd. 2019;784:727-38.. With the increase of temperature, intermetallic phases layer at Al/Mg interface thickens gradually3636 Zhang XP, Tan MJ, Yang TH, Xu XJ, Wang JT. Bonding strength of Al/Mg/Al alloy tri-metallic laminates fabricated by hot rolling. Bull Mater Sci. 2011;34(4):805-10.. At 350 °C or 400 °C, intermetallic phases can be regarded as reinforced phases, thus bonding strength improves. However, intermetallic phases layer thickens transversely at 450 oC, which deteriorates the bonding strength of Al/Mg interface. Also quite a few microcracks can be seen in intermetallic phases layer, as shown by red arrows in Figure 6a. Hence, the bonding strength of Al/Mg interface decreases as the temperature increased to 450 °C. Choi et al.2727 Choi DH, Ahn BW, Lee CY, Yeon YM, Song K, Jung SB. Formation of intermetallic compounds in Al and Mg alloy interface during friction stir spot welding. Intermetallics. 2011;19:125-30. also confirmed that intermetallic phases layer with appropriate thickness had a positive effect on mechanical properties of Al-Mg welded joints.

3.3 Micro-hardness

Figure 9 exhibits the micro-hardness values of Ti layer, Ti/Al interface, Al layer, Al/Mg interface and Mg layer in LMCs. It indicates that the micro-hardness of Ti layer, Al layer and Mg layer reduces with the increase of temperature. As described in Figure 7, the grain sizes increase gradually with the increase of temperature, and coarse grains lead to low hardness values of monolithic sheet according to Hall-Petch relationship. However, the hardness increases with the rise of temperature at both Ti/Al and Al/Mg interfaces. Especially, the hardness of Al/Mg interface soars to 203.18HV at 450 °C. For Ti/Al interface, solution strengthening plays a vital role. Lyu et al.2929 Lyu S, Sun Y, Li G, Xiao W, Ma C. Effect of layer sequence on the mechanical properties of Ti/TiAl laminates. Mater Des. 2018;143:160-8. also reported that the hardness of Ti layer increased owing to the increase of solid solubility of Al in Ti. As to Al/Mg interface, Mgl7All2 and Al3Mg2 form at 450 °C. Chang et al.3737 Chang HW, Zhang MX, Atrens A, Huang H. Nanomechanical properties of Mg-Al intermetallic compounds produced by packed powder diffusion coating (PPDC) on the surface of AZ91E. J Alloys Compd. 2014;587:527-32. and Yang et al.3838 Yang H, Guo X, Wu G, Wang S, Ding W. Continuous intermetallic compounds coatings on AZ91D Mg alloy fabricated by diffusion reaction of Mg–Al couples. Surf Coat Tech. 2011;205(8-9):2907-13. had found that the Mg17Al12 and Al3Mg2 possessed higher elastic modulus and nano-hardness than the matrix. Thus, intermetallic phases are responsible for the high micro-hardness at Al/Mg interface.

Figure 9
The micro-hardness values of Ti layer, Ti/Al interface, Al layer, Al/Mg interface and Mg layer in LMCs fabricated at different hot-pressing temperatures.

3.4. Tensile properties

The thickness of LMCs decreases in the normal direction (ND), and the length increases along RD as well as TD during hot-pressing. Due to the difference of the yield strength (YS) of dissimilar metals, the volume fraction of each layer after hot-pressing must be distinguished from that before hot-pressing. In order to understand the mechanical properties of LMCs clearly, the thicknesses of Ti layer, Al layer, Mg layer and intermetallic phases layer at different hot-pressing temperatures are measured, as shown in Table 1. It serves to display that the deformations of Mg and Al are similar, while their deformations are greater than that of Ti at various temperatures.

The tensile properties of LMCs hot-pressed at different temperatures along RD are given in Figure 10. Figure 10a shows engineering stress-strain curves of LMCs. And Figure 10b shows variations of YS, the ultimate tensile strength (UTS) and the fracture elongation (FE) of LMCs along RD. It is noticed that UTS of LMCs increases with the temperature increases, however, at the expense of FE. The increase of UTS can be attributed to the following aspects. First of all, dislocation strengthening effect is the most significant. Dislocations with three types need to be considered during deformation. With the temperature increases, the deformation of LMCs increases. For example, the deformation of LMCs increases from 19.01% to 28.60% when temperature increases from 350 °C to 450 °C (as shown in Table 1). Which will cause severe shear deformation at the interface. Subsequently greater stress concentrations and more dislocations will generate at the interface. And at high temperature, the cooperative deformation ability of adjacent layers enhances owing to strong interface bonding. Therefore, dislocations easily interact with interface and plug at the interface during plastic deformation. Also, the difference in thermal conductivity between layers causes a local temperature increase. During cooling after deformation, due to different cooling rate, regions with severe thermal stresses are generated, which results in thermal unmatched dislocations at the interface3232 Du Y, Fan GH, Yu T, Hansen N, Geng L, Huang X. Effects of interface roughness on the annealing behaviour of laminated Ti-Al composite deformed by hot rolling. Mater Sci Eng A. 2015;89:7.. All above factors lead to high dislocation density at the interface, so dislocation strengthening theory can explain this strengthening behavior. Moreover, the back stress strengthening at the interface needs to be emphasized. Due to the difference of elastic-plastic properties between component metals and intermetallic compounds, an elastic-plastic deformation stage will be introduced during deformation, which results in the formation of strain gradient. The higher the temperature is, the more severe the shear is at the interface, and the larger strain gradient is. Subsequently, it is necessary to generate some geometrically necessary dislocations (GND) to alleviate the strain gradient. As a result, the back stress enhancement caused by the accumulation of GND leads to higher strength3939 Chen Y, Nie J, Wang F, Yang H, Wu C, Liu X. Revealing hetero-deformation induced (HDI) stress strengthening effect in laminated Al-(TiB2+TiC)p/6063 composites prepared by accumulative roll bonding. J Alloys Compd. 2020;815:1-8.. At elevated temperature, solid solutions at both Ti/Al and Al/Mg interfaces and intermetallic phases at Al/Mg interface tend to contribute significantly to the increase of strength. Furthermore, with the increasing temperature, high thickness ratio of Ti to LMCs enhances the overall strength of LMCs because of higher strength of Ti than Al and Mg2121 Yu H, Tieu AK, Li H, Godbole A, Kong C. Annealing effect on microstructure and mechanical properties of Al/Ti/Al laminate sheets. Mater Sci Eng A. 2016;660:195-204.. In addition, the bonding strength of both Ti/Al and Al/Mg interfaces increases when temperature increase from 350°C to 400°C. High bonding strength can delay necking and fracture of poorly ductile metal and improve its work hardening effect. Although the bonding strength of Al/Mg interface declines from 400 °C to 450 °C, the influence of other factors above may be more prominent.

Figure 10
The tensile properties of LMCs hot-pressed at different temperatures along RD: (a) engineering stress-strain curves and (b) variations of YS, UTS and FE.

Despite that, the fracture elongation (FE) of LMCs reduces visibly with the increasing temperature, which may be closely related to bonding strength. At 350 °C, debonding occurs easily due to the weak bonding, so more energy is needed for cracks initiation. Also, the weak interface blunts the crack tip and prolongs the crack propagation path. Thus the LMCs possess optimal plasticity at low temperature3131 Xia HB, Wang SG, Ben HF. Microstructure and mechanical properties of Ti/Al explosive cladding. Mater Des. 2014;56:1014-9.. Furthermore, intermetallic phases generate at Al/Mg interface. The higher the temperature is, the thicker the intermetallic phases layer is, and the harder it is to coordinate deformation with adjacent sheets. Therefore, it is likely to trigger stress concentration and initiate cracks, so plasticity of LMCs weakens at high temperature.

The fracture macro morphologies of tensile specimens of LMCs at different hot-pressing temperatures are displayed in Figure 11. During tensile, for all specimens, Ti and Al layers are well-bonded, while delamination occurs between Al and Mg layers. Mi et al.4040 Mi Y, Nie H, Wang T, Li X, Hao X, Liang W. Effect of anisotropy on microstructures and mechanical properties of rolled Ti/Al/Mg/Al/Ti laminates. J Mater Eng Perform. 2019;28(7):4143-51. also found the same phenomenon. As described by the magnified images of Figure 11a, Mg can be observed significantly under Ti/Al layer, which indicates the inhomogeneous deformation between Mg and Ti/Al layers. From the magnified images of Figure 11b, the delamination between Al and Mg as well as the fracture of Mg can be observed clearly. Based on above analysis, during tensile, at low strain, microcracks generate at Al/Mg interface owing to intermetallic compounds, and a large number of microcracks lead to local debonding of Al/Mg interface. With the strain increases, the local debonding extends and interconnects to form delaminations. After that, Mg layer and Ti/Al layer work independently. Subsequently, Mg fractures owing to its poor UTS. While Ti/Al layer deforms unceasingly after the fracture of Mg, because the crack tip is passivated by interface debonding and the renucleation of cracks requires to absorb more energy3434 Launey ME, Ritchie RO. On the fracture toughness of advanced materials. Adv Mater. 2009;21(20):2103-10.. From the partial enlarged views of Figure 11b, the fractured Mg and the well-bonded Ti/Al layer can be observed obviously. Sun et al.4141 Sun Y, Chen J, Ma F, Ameyama K, Xiao W, Ma C. Tensile and flexural properties of multilayered metal/intermetallics composites. Mater Charact. 2015;102:165-72. also demonstrated that local debonding of interface increased the damage tolerance and the absorbed energy of fracture of LMCs. At high strain levels, Ti layer and Al layer deform cooperatively, necking and breaking occur along the direction of 45o to RD. Ultimately, LMCs rupture. Therefore, the Ti/Al layer plays a key role in the later stages of tensile of LMCs.

Figure 11
The macro morphologies of tensile specimens of LMCs after rupture at different hot-pressing temperatures: (a) RD-TD surface and (b) RD-ND surface.

Furthermore, curling is noted at Ti/Al layer when hot-pressed at 400 °C and 450 °C, as described in the magnified images of Figure 11b. Which may be attributed to the different thermal expansion coefficients between Ti and Al. It is thought that the higher the temperature is, the more serious the thermal mismatching is, and the more residual stress is, so the curl is inevitable for Ti/Al layer at elevated temperature2323 Kaya İ, Cora ÖN, Acar D, Koç M. On the formability of ultrasonic additive manufactured Al-Ti laminated composites. Metall Mater Trans, A Phys Metall Mater Sci. 2018;49(10):5051-64..

3.5 Mechanical properties of LMCs analyzed by ROM

The strength of LMCs can be calculated by applying ROM1313 Du Y, Fan G, Yu T, Hansen N, Geng L, Huang X. Laminated Ti-Al composites: processing, structure and strength. Mater Sci Eng A. 2016;673:572-80.:

σ = σ T i ν T i + σ A l ν A l + σ M g ν M g (1)
ν T i + ν A l + ν M g = 1 (2)

Where σ is the flow stress of LMCs, σTi, σAl and σMg are the flow stresses of heat-treated Ti, Al and Mg, respectively, and νTi, νAl, νMg are volume fractions of Ti, Al, Mg after hot-pressing, respectively. Relevant dates can be calculate according to Table 1.

In order to understand the tensile properties of LMCs clearly, the component metals are heat-treated at 350 oC, 400 oC and 450 oC, and corresponding engineering stress-strain curves are given in Figure 12. The YS, UTS and FE of monolithic Ti, Al, Mg sheets are summarized in Table 2.

Figure 12
Engineering stress-strain curves of monolithic Ti, Al, Mg sheets and LMCs at the temperature of (a) 350 oC (b) 400 oC and (c) 450 oC.
Table 2
Mechanical properties of monolithic Ti, Al and Mg sheets heat-treated at different temperatures.

It can be clearly seen from Figure 12 that the ductility of LMCs is lower than any monolithic sheets, while the strength lies between Al sheet and Mg sheet. The YS and UTS of LMCs calculated by ROM are regarded as theoretical values. Table 3 exhibits the comparison between the theoretical values and the measured values of LMCs. As shown in Table 3, both theoretical YS and UTS of LMCs decline with the increase of temperature, which is contrary to the results of the measured. Both the measured values of YS and UTS of LMCs are higher than the theoretical, and the gap becomes much more obvious with the increase of temperature.

Table 3
Comparison of the theoretical values and the measured values of YS and UTS in LMCs at different hot-pressing temperatures.

The variation above may involve many causes and the following five aspects will be discussed emphatically. Firstly, it has been characterized by Figure 5a that Ti/Al interface is rough when hot-pressed at elevated temperature. This roughness may induce some strain, which may directly play on the improvement of strength. Secondly, the interface reaction layer is not considered by ROM. Both solution strengthening and precipitation strengthening should be emphasized. With the increase of temperature, the gap between the theoretical values and the measured values becomes wide because of the thickened solid solution zone and intermetallic phases layer. Thirdly, the deformations of component metals are not considered by ROM. Actually, due to the drastic deformation, both fine grain strengthening and work hardening may generate in monolithic metals. Fourth, according to ROM, the YS of LMCs is calculated based on the YS of monolithic metals. However, the actual yielding happens only when a layer with a high YS yields. In present work, Ti possesses the highest YS, so it is difficult to observe the yielding phenomenon of LMCs when monolithic Mg or Al yields. Therefore, deviation between the theoretical values and the measured values is reasonable. Fifth, the constraint effect is expected to be developed. Because of the different elastic-plastic behavior of Ti, Al, Mg, intermetallic phases layer and solid solution layer, the constraint strain will generate when LMCs are subjected to tensile strain4242 Wu H, Fan G, Huang M, Geng L, Cui X, Xie H. Deformation behavior of brittle/ductile multilayered composites under interface constraint effect. Int J Plast. 2017;89:96-109.. Both the variation of stress state and the formation of GND in different deformation stages will lead to the increase of measured strength.

4. Conclusions

LMCs were fabricated by hot-pressing at 350 °C, 400 °C and 450 °C in present work. The influences of interface morphology, diffusion layer and reaction product, constraint effect on the mechanical properties of LMCs were studied. The detailed conclusions were given as follows:

  1. 1

    With the increase of hot-pressing temperature, the morphologies of Ti/Al interface change from flat to waveform, and intermetallic phases don’t form. Whereas, the width of intermetallic phases layer at Mg/Al interface increases significantly with the increasing temperature.

  2. 2

    With the increase of hot-pressing temperature, both bonding strength and hardness of Ti/Al interface increase owing to the thickened diffusion layer. However, the bonding strength of Al/Mg interface doesn’t change linearly with the increasing temperature, and the maximum bonding strength is obtained at 400 °C.

  3. 3

    With the increasing temperature, UTS of LMCs increases, however, at the expense of FE. The dislocation strengthening, back stress strengthening, solution strengthening, precipitation strengthening, the delayed necking and the increased Ti content are all contributed to the increase of UTS. The variation of FE is attributed to the influence of interface on crack initiation and propagation.

  4. 4

    Both the measured YS and UTS of the LMCs are higher than that calculated by ROM. It is thought that the strain, solid solution, precipitated phases and stress at the interfaces as well as fine grains, work hardening, inconsistent yielding of monolithic sheets are all conducive to the improvement of the measured strength of LMCs.

5. Acknowledgments

This work was supported by “National Natural Science Foundation of China” (Grants. 51771128 and 51771129), Projects of International Cooperation in Shanxi (Grant no. 201703D421039), Shanxi province science and technology major projects (Grant no.20181101008) and the Program for the Outstanding Innovative Teams of Higher Learning Institutions of Shanxi.

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Publication Dates

  • Publication in this collection
    30 Mar 2020
  • Date of issue
    2020

History

  • Received
    26 Nov 2019
  • Reviewed
    20 Jan 2020
  • Accepted
    29 Jan 2020
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