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Comparative study of microstructure evaluation and mechanical

properties of 4043 aluminum alloy fabricated by wire-based
additive manufacturing

Qiuyu Miao, Dongjiang Wu, Dongsheng Chai, Yu Zhan, Guijun

Bi, Fangyong Niu, Guangyi Ma

PII: S0264-1275(19)30643-4
DOI: https://doi.org/10.1016/j.matdes.2019.108205
Reference: JMADE 108205

To appear in: Materials & Design

Received date: 10 June 2019

Revised date: 3 August 2019
Accepted date: 10 September 2019

Please cite this article as: Q. Miao, D. Wu, D. Chai, et al., Comparative study of
microstructure evaluation and mechanical properties of 4043 aluminum alloy fabricated
by wire-based additive manufacturing, Materials & Design(2019), https://doi.org/10.1016/
j.matdes.2019.108205

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© 2019 Published by Elsevier.

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Comparative Study of Microstructure Evaluation and Mechanical

Properties of 4043 Aluminum Alloy Fabricated by Wire-based Additive

Manufacturing

Qiuyu Miao1, Dongjiang Wu1, Dongsheng Chai1, Yu Zhan1, Guijun Bi2, Fangyong Niu1,

Guangyi Ma1*

1 Key Laboratory for Precision and Non-traditional Machining Technology of Ministry of Education,

Dalian University of Technology

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2 Singapore Institute of Manufacturing Technology

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Abstract: 4043 Al-Si alloy samples are fabricated by laser-arc hybrid additive
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manufacturing and wire arc additive manufacturing. To investigate the influence of

laser energy on the fabricated sample, the microstructure evaluation and mechanical
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properties are studied. After the input of laser energy, there are laser zones with finer
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grains and reduced Si segregation. As a result, the Si phases at grain boundaries in

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laser zone are smaller than that in other zones. And it is found that semi-coherent

interface between Al and Si phases with crystal orientation relations, [110]Al∥[110]Si

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and (111)Al∥(220)Si, indicating the Si phase tends to grow along (111)Al plane. The
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results of mechanical properties show that the micro-hardness in laser zone is 54.3

HV0.05, with the increment of 19.08% compared to that in heat-affected zone. And the

tensile strength, yield strength and elongation after the input of laser energy are

163.39±1.68 MPa, 75.60±4.91 MPa and 17.38±5.44 %, which are 7.56%, 8.45% and

3.45% higher than that without laser. The improved mechanical properties are due to

the finer gains, reduced Si segregation and the crack deflection in LAHAM samples.

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Keywords: Laser-arc hybrid additive manufacturing; Wire arc additive manufacturing;

Aluminum alloy; Microstructure; Mechanical properties

1. Introduction

With the development of lightweight applications, additive manufacturing of

aluminum alloys has become a hot topic and is facing time for rapid growth. The

materials studied include Al-Cu [1-2], Al-Zn [3], Al-Mg [4-5], Al-Si-Mg [6], Al-Si [7]

and other unconventional Al-based alloys [8-9]. The significant problems are crack

defects and low relative density of the additive manufactured samples, and no

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commercial materials available. Al-Si alloys are widely used in aerospace and

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automotive engineering, for their good formation ability, high specific strength and
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excellent corrosion resistance [10-11]. And there are also works to investigate the
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effect of the content of Si on the microstructure, mechanical and thermal properties

[7]. 4043 is a kind of Al-Si alloy commonly used as weld filler, which has good
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fluidity and no significant defects in additive manufactured samples [12].

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The main methods of additive manufacturing include wire arc additive

manufacturing (WAAM), selective laser melting (SLM), laser additive manufacturing

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(LAM) and so on. WAAM is drawing more and more attention all over the world
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because of the high deposition rate, low cost of equipment and materials. Compared

with SLM, the second dendrite arm spacing of Al-Si alloy sample fabricated by

WAAM can reach to 8 μm, which is ten times larger than the cell size of sample

fabricated by SLM [12-13], greatly weakening the mechanical properties [14]. SLM

can fabricate samples with complex shapes [15], while the cost of SLM is much

higher due to the cost of powder and low deposition rate. LAM, including laser metal

deposition (LMD) and laser engineered net shaping (LENS), has a high cooling rate

around 106 K/s, three orders higher than that of WAAM [16-17]. But because of the
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high reflectivity to laser and high thermal conductivity of Al and its alloys, high

power laser up to kilowatts should be used which increases the cost of LAM

significantly [18].

While there is very little research on the laser-arc hybrid additive manufacturing

(LAHAM). LAHAM, combining the advantages of WAAM and LAM, has the

features of low cost, high deposition rate and high cooling rate. The input of laser

energy can constrict and stabilize the arc [19], which can help to improve the

deposition rate and the macroscopic quality with stable geometric dimensions [20].

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And the input of laser energy can refine grains in keyhole [21],which will improve the

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mechanical properties. Liu et al. used laser-MIG hybrid heat source to fabricate
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Al-Mg alloy, and found that the microstructure of fabricated sample is more uniform
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than that fabricated by MIG [22]. However, researches mainly focused on the

macro-morphology of LAHAM sample, which has neither the detailed microstructure

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evaluation nor the relationship between microstructure and mechanical properties.

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In this paper, LAHAM was explored to fabricate 4043 Al-Si alloy, and the

WAAM samples were fabricated as a comparison. The aim of this paper was to study
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the characteristics of microstructure and mechanical properties after the input of laser
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energy, including the grain morphology, phase compositions, element distribution,

micro-hardness and tensile properties.

2. Experimental methods

2.1 Material and equipment

4043 aluminium alloy wire with 1.2 mm diameter was used in both WAAM and

LAHAM, and the substrate was used 6061 aluminium alloy plate with a thickness of

15 mm. LAHAM system is composed of GSI JK701H Nd:YAG pulsed laser and a

Dynasty200 DX arc welding machine, and WAAM system is formed minus the pulsed
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laser. Fig. 1 (a) shows schematic diagram of the LAHAM system with the wire fed

against the scan direction into the arc zone. The pulse energy, pulse duration, focal

spot size and de-focal distance of laser was 17.5 J, 3 ms, 0.6 mm and -1.0 mm,

respectively. And the angle of wire feeding was 25 °. The deposition within a layer

was going on with an overlap ratio (choosing according to the experimental results

and geometric calculation) which was 33% of the single-track width, and the vertical

distance was 2 mm between the tip of tungsten electrode and the surface of deposited

part all the time. The scanning strategy is shown in Fig.1 (b) which is same in all

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tracks and layers. Before additive manufacturing, the substrate was polished

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mechanically to remove the surface oxide layer and then cleaned with ethanol. Fig.1
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(c) shows the LAHAM sample with a dimension of 70 mm × 25 mm × 6 mm, five
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layers in all, with the average height of 1.2 mm per layer. The chemical compositions

of 4043 wire and 6061 substrate are shown in Table 1, respectively. And the process
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parameters are shown in Table 2.

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Fig. 1. The schematic diagram of LAHAM process and sample fabricate by LAHAM. (a)

LAHAM system; (b) scanning strategy; (c) 4043 aluminum alloy sample fabricated by LAHAM

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Table 1 Chemical composition (mass fraction, %)

Al Si Fe Cu Mn Mg Zn Cr Ti

4043 Bal. 4.5-6 0.8 0.3 0.05 0.05 0.1 - 0.2

6061 Bal. 0.4-0.8 0.7 0.15-0.4 0.15 0.8-1.2 0.25 0.04-0.35 0.15

Table 2 Process parameters

WAAM LAHAM

Laser power/W - 350

Frequency/Hz - 20
-1
Wire feeding rate/mm·min 1000 1000

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Scan speed/mm·min-1 250 250

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Initial current/A 150 150

Change of current Decrease 5 A by layer Decrease 5 A by layer

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Overlap ratio 33% 33%
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2.2 Testing method
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The microstructure of samples were characterized using a Olympus MX40F

optical microscope (OM), a VK-X100/X200 Keyence confocal microscope, a Zeiss

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scanning electron microscope Supra 55 (SEM) and a JXA-8530F Plus field emission
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electron microprobe (EPMA). The cutting plane was orientated parallel to xz-plane
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for microstructure analysis, corresponding to the coordinate system in Fig.1 (a). Phase

compositions were analyzed by a Lab XRD-6000 with Cu-Kα radiation, using a scan

rate of 0.04 °/min with the 2 Theta angle varying from 20 ° to 100 °. A JEM-2100F

field transmission electron microscope (TEM) was used to characterize the

morphology and composition of each phase, and the interface between phases. TEM

samples with the thickness less than 100 nm were prepared by focused ion beam

(FIB). Micro-hardness test was performed using a MVS-1000Z type micro-hardness

tester with a loading force of 50 g and dwelling time of 10 s. Tensile tests were carried

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out using a WDW-50E microcomputer controlled electronic universal testing machine

with a tensile rate of 2 mm/min. Three tensile coupons with standard dimensions were

taken from the samples along the scanning direction as shown in Fig. 2. And the

fracture surfaces were captured by OM and SEM.

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Fig. 2. Tensile coupons: (a) tensile coupons location; (b) the diagram of tensile coupon; (c) tensile
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coupons; (d) fractured coupon
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3 Results and discussion

3.1 Microstructure
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The microstructure of LAHAM and WAAM samples perpendicular to the

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scanning direction are shown in Fig. 3. In Fig. 3 (a) and (b), it can be observed that

the microstructure shows a periodical pattern according to the number of deposited

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layers. According to the microstructure characteristic in a single-layer, it can be

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divided into the arc zone (AZ), laser zone (LZ), heat-affected zone (HAZ) and light

strip in LAHAM sample. And the notable differences of microstructure compared

with WAAM sample are the LZ and the decreased HAZ. The boundary between LZ

and adjacent layer’s AZ in LAHAM sample is clear without HAZ (Fig. 3 (c)), while

there are HAZ and light strip between adjacent layers’ AZ in WAAM sample (Fig. 3

(d)). In the process of LAHAM, the arc melts most of the metal, and the laser

increases the depth of the molten pool through the formation of keyhole [23]. So there

is LZ in the bottom of the molten pool in LAHAM sample. It should be noted that the
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presence of LZ reduces the area of HAZ.

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Fig. 3. Microstructure of LAHAM and WAAM samples perpendicular to the scanning direction.
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(a)(c)(e)(g) LAHAM sample; (b)(d)(f)(h) WAAM sample; the (c)(e)(g) are the magnification of

area A-C in (a), the (d)(f)(h) are the magnification of area A-C in (b), respectively. AZ: the region
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forms with arc energy as the main heat source. LZ: the region forms with laser energy as the main
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heat source. HAZ: the region forms under the reheating process and belongs to the previous

deposited layers.

Non-uniformity of microstructure is significant due to the heat accumulation in

additive manufacturing [24-25]. The microstructure morphology in different zone is

different. Grains in AZ (Fig. 3 (c)-(h)) are in typical columnar shape, and the size

decreases with the distance away from molten pool boundary. Grain size is

determined by the product of temperature gradient G and solidification rate R. It has

been calculated by H.L.Wei that the G·R is increasing with distance from the molten

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pool boundary [26], causing the decrease of grain size. And the grain morphology is

determined by G/R. The G/R is decreasing with the distance away from molten pool

boundary, but grains will change from columnar shape into equiaxed only when G/R

is lower than the critical value to form equiaxed grains [26]. Grains in AZ are all in

columnar shape in this work (Fig. 4). Because the cross-section is not parallel to the

growth direction of all grains, it seems the morphology is not identical, with both

columnar and equiaxed. Grains are often mistaken for changing from columnar to

equiaxed in the section, which coincides with the simulation of H.L.Wei [27]. In

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addition, it is interesting to find that the grain boundaries in AZ are connected to each

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other to form a network structure [13,28]. -p
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Fig. 4. Microstructure in different cross-sections of the same location in sample (above the red
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dotted line). (a) and (b) are views as shown in the upper-right corner, respectively.
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In HAZ (Fig. 3 (e)-(h)), the morphology and size of grains are all different from

that in AZ. The formation of HAZ is due to the reheating process in additive

manufacturing, in which region belonging to the previous deposited layers the

temperature is no higher than the melting point. Grains in HAZ are larger than that in

AZ, and some discrete particles can be found. And grain size in HAZ is still

nonuniform which can be explained through the temperature distribution. HAZ is

outside of the molten pool with high temperature but lower than liquid temperature.

While the grain growth in HAZ is related to the G and the time stay in high
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temperature [29]. Different locations in HAZ has the different thermal cycles, so

grains in HAZ is nonuniform [30].

It is interesting to find a light strip (Fig. 3 (d), (g)-(h)) in the edge of every HAZ

bottom. The grain in light strip is about 10 μm in size, which is almost equal to the

grain size in AZ. Some literatures also report the light strip, and consider the

complicated heat history is the reason for the generation of light strip, with different

grains’ morphology on each side [31]. Bai et al. found decreasing grain boundaries in

the junction between inter-layer and inner-layer, similar to growth stopping of grains

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[32]. Grains of light strip in this paper also shows growth stopping phenomenon with

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discontinuous grain boundary, causing by the high diffusion rate of atoms in grain
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boundary under high temperature [33]. It can be observed that light strip is clear due
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to the decreasing of black grain boundaries. The region in light strip shows lighter

color after etching due to the different element segregation. And the microstructure
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morphology is different on each side of light strip, which is between the HAZ and the
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AZ.

LZ in LAHAM sample, with finer grains, separates HAZ into two discontinuous
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regions which are continuous in WAAM sample (Fig. 3 (a)-(b)). There are two
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reasons for the significantly finer grains. On one hand, G in LZ can reach to the order

of 106 K/m [34], while the G in AZ is one or two order of magnitude lower than that

in LZ [35]. The product of G and R named cooling rate in LZ increases and makes

grains refined [13]. On the other hand, the large surface tension gradient caused by

large G in keyhole can strengthen the fluid flow in molten pool, which contributes to

dendrite fragmentation. These dendrite fragments are carried into the molten pool and

act as nuclei for new grains. The increasing of nucleation rate makes grains refined

[36-37]. Meantime, laser beam with high energy density and high cooling rate can
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decrease the residence time in high temperature, making no significant HAZ at the

bottom of LZ.

3.2 Phase structure

Fig. 5 shows the XRD pattern of LAHAM sample, WAAM sample and 4043

wire. The α-Al and Si phases are obtained, which are consistent with the phase

compositions of Al-Si alloy (Fig. 6). From the XRD results, we can see that the

preferential orientation of the α-Al phase in wire, WAAM sample and LAHAM

sample has changed from (220), (200) to (111). The α-Al is a fcc structure, and (111)

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is the close-packed plane [31]. And because the surface energy of close-packed plane

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(111) is smaller than that of other planes, the preferred orientation of close-packed
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plane (111) is attributed to the minimization of surface energy [38]. The peak intensity
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of Al (111) in LAHAM sample increases significantly, which indicates that the input

of laser energy propagates the growth of α-Al on (111) plane.

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Fig. 5. XRD pattern Fig. 6. Al-Si phase diagram [39]

In order to identify the phase structure of LAHAM sample, the selected area

electron diffraction (SAED) and high resolution transmission electron microscopy

(HRTEM) were used. Fig. 7 (a)-(b) show the TEM images and the SAED patterns

determining the Al and Si phases, respectively. The interface of eutectic Si and Al

phases by HRTEM and its FFT are shown in Fig. 8 (a) which is not perfectly coherent.

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The lattice spacing of (220)Si plane is determined to be 0.1949 nm and the lattice

spacing of (111)Al plane is determined to be 0.2376 nm by the inverse FFT in Fig. 8

(b). It can be calculated that four times of the lattice spacing of (220)Si equals three

times that of (111)Al, so there must be edge dislocation in the phase interface (Fig. 8

(c)). The crystal orientation relations can be referred from Fig. 8 (a)-(b), with [110]Al

∥[110]Si and (111)Al∥(220)Si. Because (111) plane is the close-packed plane of Al

phase, the eutectic Si tends to grow along (111)Al plane [40]. Fig. 9 shows the stacking

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fault of Al phase through HRTEM and its inverse FFT. It is not easy for aluminium to

generate stacking fault for the high stacking fault energy [41]. But stacking fault

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exists in Al phase in all region, it may be caused by the solid solution of Si in Al [42]
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and the non-equilibrium solidification process of additive manufacturing [43].
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Fig. 7. TEM images and the SAED patterns (a) Al phase along [110] zone axis; (b) Si phase along
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[111] zone axis

Fig. 8. HRTEM image and its inverse FFT patterns along [110]Si zone axis: (a) HRTEM and its

FFT; (b)-(c) inverse FFT

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Fig. 9. HRTEM with stacking fault and its inverse FFT in Al phase

3.3 Element distribution

Fig. 10 shows the back-scatter images and element distribution of Al and Si in

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LAHAM sample and WAAM sample. It is found that element Si is enriched at grain

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boundaries. Grains are mainly constituted by element Al. And the Al-Si eutectic is

mainly at grain boundaries. During the solidification of 4043 Al-Si alloy, α-Al firstly
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forms. When the Al-Si reaches to eutectic ratio, Al-Si eutectic finally forms at grain
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boundaries and forms fine network which can improve the crack resistant [27,44].
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Fig. 10. Distribution of Al and Si Elements in LAHAM and WAAM samples, (a)-(c) for LAHAM

sample and (d)-(f) for WAAM sample. (a) and (d) back-scatter images; (b) and (e) distribution of

element Al; (c) and (f) distribution of element Si

Segregation is directly related to cooling rate [45]. When cooling rate increases

to a certain extent, the element diffusion in liquid phase is limited [46]. So larger
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cooling rate can inhibit the diffusion of solute and reduce the segregation of LAHAM

sample compared with WAAM sample [47]. For LAHAM sample, it can be found that

the distribution of Si is more uniform in LZ, with the decreased segregation of Si.

According to the microstructure analysis, grains in HAZ have significant change

in morphology. And the reason for the change can be explained combining with the

element distribution. The HAZ can be divided into two parts: partially melted zone

and over-heated zone. As we all know, the typical features of eutectic is that its

melting point is lower than that of every component. Partially melted zone is close to

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the molten pool boundary, with the temperature between eutectic temperature TE and

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liquid temperature TL. So the Al-Si eutectic is melted [31], causing the phenomenon
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of coarse grains and thick grain boundaries (Fig. 10 (f)) which also occurs in the
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welding of aluminium alloys [48-49]. As the diffusion rate of Si increases in high

temperature, the network structure breaks into small particles in over-heated zone
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with the temperature lower than TL [13,27]. With the long time staying at high
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temperature in over-heated zone, small eutectic particles form at grain boundaries

aggregating and spheroidizing to form larger particles. Because most of the grain
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boundaries are broken, the phases of α-Al are connected with each other causing
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grains coarsened remarkably.

To further analysis the distribution of element Al and Si at the grain boundary,

the LAHAM sample was tested by TEM. Fig. 11 (a)-(b) show the TEM images and

EDS-mapping containing grain boundaries of AZ and LZ, respectively. The coupled

growth of Al and Si phases [50] can be clearly observed in the grain boundaries in AZ,

proving to be eutectic Al-Si. Eutectic Si phases are in slender shape and distribute

discretely (Fig. 11 (a)). Si phase is hard and brittle, so the change of both shape and

size of Si phase may have great influence in the mechanical properties [51-52,10]. It
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remains eutectic Al-Si in LZ, but the size of eutectic Si is smaller than that in AZ with

the reduced thickness (Fig. 11 (b)). Fig. 11 (c)-(d) show the TEM images and

EDS-mapping of HAZ with large discrete particles and thick grain boundaries

corresponding to Fig. 10 (f), respectively. According to the analysis of the

microstructrue, it has been known that grains in HAZ are coarse with thick grain

boundaries or the eutectic Si gathering to form large discrete particles. In HAZ, the

eutectic Si of discrete particles is surrounded by each other (Fig. 11 (c)). And the

significantly larger eutectic Si of thick grain boundaries can be seen in Fig. 11 (d). It

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can be concluded that the size and morphology of Si phase in grain boundaries is

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related to the cooling rate which has been reported by O.El Sebaie [53].
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Fig. 11. TEM analysis of EDS-mapping in the region containing grain boundaries: (a) AZ; (b) LZ;

(c) HAZ with discrete particles; (d) HAZ with thick grain boundaries

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3.4 Micro-hardness Analysis

Fig.11 shows the micro-hardness distribution along building direction (red dotted

lines represent measuring position). Due to the periodic distribution of the

microstructure along the building direction (Fig. 3), and the close relationship

between the microstructure and micro-hardness has been confirmed in many

literatures [54-56], the micro-hardness values of samples are also periodically

distributed. The average micro-hardness of LAHAM sample is 51.59±2.29 HV0.05

along the building direction higher than that of 49.97±4.12 HV0.05 of WAAM sample.

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It can be calculated that the average micro-hardness in the building direction increases

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by 3.24% with the input of laser energy. In order to further analyze the influence of
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the microstructure on the micro-hardness, the micro-hardness in different zones of
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LAHAM samples are measured (Fig. 12). The micro-hardness in HAZ and LZ are

determined to be 45.6 HV0.05 and 54.3 HV0.05, respectively. It can be calculated that
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the micro-hardness in LZ is 19.08% higher than that in HAZ. Because of the existence
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of LZ in LAHAM sample, the reducing area of HAZ can also improve the

micro-hardness.
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Fig. 12. Micro-hardness distribution along building direction and images of LAHAM

micro-hardness in LZ and HAZ

From the micro-hardness distribution, it can be seen that the micro-hardness

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distribution of WAAM sample fluctuates greatly, with the large difference between

maximum micro-hardness and minimum micro-hardness. Due to the existence of

HAZ in the measuring position, micro-hardness values fluctuates greatly. In LAHAM

sample, the micro-hardness values are more uniformly distributed on both sides of the

average line, and the micro-hardness values fluctuate less because there are LZ and

AZ in the measuring position.

The factors affecting micro-hardness value include grain size and element

distribution [56-57]. The irregular arrangement of atoms at grain boundaries hinders

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the movement of dislocations. The decreasing grain size increases the possibility of

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hindering effect [57], which is beneficial to the resistance of plastic deformation. So
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the micro-hardness at grain boundary is higher than that in grain body, also known as
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fine-grain strengthening. The grain size in LZ is significantly smaller than that in

HAZ, so the strengthening effect of fine grains is one of the reasons that the
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micro-hardness in LZ is higher than that in HAZ. For 4043 Al-Si alloy, Si is

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distributed in α-Al matrix as a hard element, and the distribution of Si also has some

influence on the micro-hardness. As the solid solubility of Si in α-Al matrix increases

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during rapid solidification, more Si atoms displace Al atoms in Al lattice. Because the
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atomic radius of Si is slightly smaller than that of Al, the lattice of Al is distorted,

which is beneficial to the increase of micro-hardness, also known as solid-solution

strengthening. From the results of element distribution, it can be seen that the

distribution of Si element in LZ is more uniform than that in HAZ. As a strengthening

element, the more uniform distribution of Si may also contribute to the improvement

of micro-hardness.

3.5 Mechanical Property Analysis

The tensile strength, yield strength and elongation of the samples are listed in
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Table 3. Compared with WAAM sample, the tensile strength, yield strength and

elongation of LAHAM sample increase by 7.56%, 8.45% and 3.45%, respectively.

The fracture surfaces of tensile coupons are shown in Fig. 13. There are small

and shallow dimples in all fractures, and there are tear ridges which are more notable

in LAHAM (Fig. 13 (a)-(b)). In Fig. 13 (b), the distance between adjacent tear ridges

is about 8 μm, which is corresponding to the grain size in AZ. This indicates that the

fracture process is not continuous. The discontinuous fracture is attributed to the soft

α-Al with low deformation resistance yielded under force loading and the brittle Si in

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eutectic. Therefore, the fracture prefers to generate from Si phases [58]. The large Si

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particles tend to crack first because of the lower nucleation stress, easy to decrease the
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strength [14,59]. The probability of Si particle cracking can be calculated as follows
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[60]:

  2.14d  
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
p  1  exp    
eq
(1)
  d 0 0  
  
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which shows that the probability of cracking is the function of particle size d, particle

aspect ratio α, the shear modulus of the matrix μ, the equivalent tensile strain  eq , and
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the reference stress  0 and particle size d 0 in Eqs. (1). So the Si particles with
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large d in HAZ weaken the tensile strength. The segregation of Si in LZ is not so

serious than that in HAZ (Fig. 9), so the reduced HAZ and the existence of LZ is

beneficial to mechanical properties. It can be observed from the fractures there are

rough surfaces and smooth surfaces (Fig. 13 (d)). The rough surface is proved to be

rich in element Si by EDS, while the smooth surface is α-Al (Fig. 14). Segregation of

element Si in LAHAM fractures has a significant decrease (Fig. 9 (c)) which can also

account for the improved mechanical properties.

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Fig. 13. SEM of tensile fractures. (a)-(b) for LAHAM sample; and (c)-(d) for WAAM sample
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Fig. 14. Results of EDS in fractures: (a) rough surface; (b) smooth surface

The results of tensile tests are compared with other literatures in Table 3 (both

thin wall and block samples). The strength of sample fabricated by LAHAM in this

work is higher than that in other literatures [12,61]. While the effects of sample’s

structure on the mechanical properties are complex [62]. Despite the structure

difference, comparing the mechanical properties of different additive manufacturing

methods can be useful when evaluating the applicability.

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Fig. 15. Tensile stress-strain curves of samples fabricated by WAAM and LAHAM

Table 3 Tensile test results and comparison with other literatures

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Tensile
sample Yield Strength/MPa Elongation/%
Strength/MPa

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LAHAM (this work) 163.39±1.68 75.60±4.91 17.38±5.44
WAAM (this work) 151.91±1.28 69.71±4.01 16.80±0.61
Y：145.5
-p - Y：23.65
WAAM [61]
Z：148.2 - Z：21.96
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WAAM [12] 141±4 61±3 17±3
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Fig. 15 shows the tensile stress-strain curves of LAHAM and WAAM samples. In

order to analysis the relationship between microstructure and tensile properties, the
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fracture coupons were cut along the axial direction. Fig. 16 shows the microstructure
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under the tensile fracture of LAHAM coupons and WAAM coupons, respectively. The
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fracture surface of LAHAM coupon is not so smooth than that of WAAM coupon, with

the crack deflection in LZ (Fig. 16 (a)-(b)). Compare AZ and HAZ (Fig. 16 (c)-(d) and

(e)), there are both intercrystalline fracture and transcrystalline fracture in AZ, while

HAZ is dominated by intercrystalline fracture. From Fig. 3 and Fig. 10, we have known

that grain size in HAZ is larger than that in AZ, with the thicker Si phase. So it can be

concluded that the eutectic Si is the weak position under the tensile loading, and the

large eutectic Si phases are easier to break, forming the intercrystalline fracture. So, the

appearance of thicker eutectic Si in HAZ is unfavorable to the mechanical properties.

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Fig. 16. Microstructure of fracture surfaces: (a)(c)(e) for LAHAM sample, (b)(d)(f) for WAAM
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sample; (a)-(b) Optical microscope pictures of fracture; (c)-(f) back-scatter images

While for LAHAM sample, it is clear that there is no significant deflection of crack
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in the border between AZ and LZ (Fig. 16 (c)). In other words, the presence of LZ
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doesn’t cause extra stress concentration to propagate crack propagation. In Fig. 16 (e),

crack propagates along horizontal grain boundaries in the upper side of LZ, while crack
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propagates across the grain in the direction perpendicular to the tensile direction. After
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further observation, it can be seen that grains grow in different directions (on both sides

of red dotted line in Fig. 16 (e)), meaning that crack deflection is related to the direction
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of grains. It has been studied that the propagation of crack is related to the

misorientation of grains [63]. As we all know, the propagation of crack tends to seek the

path requiring lowest energy, so the presence of LZ with finer and disordered grains is

good for tensile properties.

4. Conclusion

The microstructure evolution and mechanical properties of LAHAM and WAAM

samples have been studied in this paper. And the relationship between microstructure

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and mechanical properties is analyzed, getting the following conclusions:

(1) Compare LAHAM sample with WAAM sample, the significant difference in

microstructure between the samples is the LZ with finer grains and the decreased

HAZ in LAHAM sample, which are caused by the high cooling rate and strengthened

fluid flow in laser zone. The distribution of Si is more uniform in LZ, while the Si

phases in HAZ are in large size at grain boundary and form large discrete particles.

Through HRTEM, it is found that semi-coherent interface between Al and Si phases,

with [110]Al∥[110]Si and (111)Al∥(220)Si indicating the Si tends to grow along the

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direction of (111)Al.

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(2) The mechanical properties can be clearly related to microstructure through
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the analysis of micro-hardness and tensile properties. The micro-hardness in LZ is
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54.3 HV0.05 which is significant lager than that in HAZ with the increment of 19.08%,
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caused by the finer grains and more uniform element distribution in LZ. The tensile

strength, yield strength and elongation of LAHAM sample are 163.39±1.68 MPa,
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75.60±4.91 MPa, and 17.38±5.44%, with the increment of 7.56%, 8.45% and 3.45%

compared with WAAM sample, respectively. There are amounts of rough surfaces in
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the fracture of WAAM sample determined to be regions rich in Si, which are
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significantly decrease in LAHAM sample. Crack tends to propagate along grain

boundaries, especially large Si phases in HAZ. While the crack deflection in LZ can

explain the improvement of tensile properties of LAHAM sample. So the input of

laser energy on the fabrication of 4043 alloy samples can improve mechanical

properties.

Acknowledgements

This work was supported by the National Key R & D Program of China (No.

2018YFB1107801), the National Natural Science Foundation of China (No. 51805070,

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No. 51790172), and Science Fund for Creative Research Groups of NSFC (No.

51621064).

Conflicts of interest

There are no conflicts to declare.

Data availability

The raw/processed data required to reproduce these findings cannot be shared at

this time as the data also forms part of an ongoing study.

Reference

of
[1] J. Gu, J. Bai, J. Ding, S. Williams, L. Wang, K. Liu, Design and cracking susceptibility of additively

ro
manufactured Al-Cu-Mg alloys with tandem wires and pulsed arc, J. Mater. Process. Technol. 262 (2018)
210-220. -p
[2] H. Zhang, H. Zhu, T. Qi, Z.Hu, X. Zeng, Selective laser melting of high strength Al–Cu–Mg alloys:
Processing, microstructure and mechanical properties, Mater. Sci. Eng. A. 656 (2016) 47-54.
re
[3] N. Kaufmann, M. Imran, T.M. Wischeropp, C. Emmelmann, S. Siddique, F. Walther, Influence of process
parameters on the quality of aluminium alloy EN AW 7075 using selective laser melting (SLM), Physics
procedia. 83 (2016) 918-926.
lP

[4] Y. Shi, P. Rometsch, K. Yang, F. Palm, X. Wu, Characterisation of a novel Sc and Zr modified Al–Mg alloy
fabricated by selective laser melting, Mater. Lett. 196 (2017) 347-350.
na

[5] H. Geng, J. Li, J. Xiong, X. Lin, Optimisation of interpass temperature and heat input for wire and arc additive
manufacturing 5A06 aluminium alloy, Sci. Technol. Weld. Join. 22 (2017) 472-483.
[6] M. Tang, P.C. Pistorius, Oxides, porosity and fatigue performance of AlSi10Mg parts produced by selective
ur

laser melting, Int. J. Fatigue. 94 (2017) 192-201.

[7] T. Kimura, T. Nakamoto, M. Mizuno, H. Araki, Effect of silicon content on densification, mechanical and
Jo

thermal properties of Al-xSi binary alloys fabricated using selective laser melting, Mater. Sci. Eng. A. 682
(2017) 593-602.
[8] K.G. Prashanth, H.S. Shahabi, H. Attar , V.C. Srivastava, N. Ellendt, V. Uhlenwinkel, J. Eckert, S.Scudinoa,
Production of high strength Al85Nd8Ni5Co2 alloy by selective laser melting, Addit. Manuf. 6 (2015) 1-5.
[9] K.G. Prashanth, S. Scudino, A.K. Chaubey, L. Löber, P. Wang, H. Attar, F.P. Schimansky, F. Pyczak, J. Eckert,
Processing of Al–12Si–TNM composites by selective laser melting and evaluation of compressive and wear
properties, J. Mater. Res. 31 (2016) 55-65.
[10] S. Hegde, K.N. Prabhu, Modification of eutectic silicon in Al–Si alloys, J. Mater. Sci. 43 (2008) 3009-3027.
[11] H. Ye, An overview of the development of Al-Si-alloy based material for engine applications, J. Mater. Eng.
Perform. 12 (2003) 288-297.
[12] A.S. Haselhuhn, M.W. Buhr, B. Wijnen, P.G. Sanders, J.M. Pearce, Structure-property relationships of
common aluminum weld alloys utilized as feedstock for GMAW-based 3-D metal printing, Mater. Sci. Eng. A.
673 (2016) 511-523.
[13] L. Thijs, K. Kempen, J.P. Kruth, J.V. Humbeeck, Fine-structured aluminium products with controllable texture
22
 Journal Pre-proof

by selective laser melting of pre-alloyed AlSi10Mg powder, Acta Mater. 61 (2013) 1809-1819.
[14] H. Attar, M.J. Bermingham, S. Ehtemam-Haghighi, A. Dehghan-Manshadi, D. Kent, M.S. Dargusch,
Evaluation of the mechanical and wear properties of titanium produced by three different additive
manufacturing methods for biomedical application, Mater. Sci. Eng. A. 760 (2019) 339-345.
[15] I. Maskery, N.T. Aboulkhair, A.O. Aremu, C.J. Tuck, I.A. Ashcroft, R.D. Wildman, R.J. Hague, A mechanical
property evaluation of graded density Al-Si10-Mg lattice structures manufactured by selective laser melting,
Mater. Sci. Eng. A. 670 (2016) 264-274.
[16] W. Ou, T. Mukherjee, G.L. Knapp, Y. Wei, T. Debroy, Fusion zone geometries, cooling rates and solidification
parameters during wire arc additive manufacturing, Int. J. Heat Mass Transf. 127 (2018) 1084-1094.
[17] Y. Li, D. Gu, Parametric analysis of thermal behavior during selective laser melting additive manufacturing of
aluminum alloy powder, Mater. Des. 63 (2014) 856-867.
[18] M. Froend, V. Ventzke, S. Riekehr, N. Kashaev, B. Klusemann, J.Enz, Microstructure and Microhardness of
Wire-based Laser Metal Deposited AA5087 using an Ytterbium Fibre Laser, Mater. Charact. 143 (2018) 59-67.

of
[19] W.M. Steen, Arc augmented laser processing of materials, Journal of Applied Physics. 51 (1980) 5636-5641.
[20] M. Ono, Y. Shinbo, A. Yoshitake, M. Ohmura, Development of laser-arc hybrid welding, NKK TECHNICAL

ro
REPORT-JAPANESE EDITION. 86 (2002) 70-74.
[21] G. Casalino, M. Mortello, P. Leo, G. Casalino, M. Mortello, P. Leo, K.Y. Benyounis, A.G. Olabi, Study on arc
-p
and laser powers in the hybrid welding of AA5754 Al-alloy, Mater. Des. 61 (2014) 191-198.
[22] Z.L. Zhuang, G. Song, M.L. Zhu, L.M. Liu, Interlayer rapid forming aluminum alloy by Laser-MIG hybrid
heat source, Transactions of the China welding institution. 34 (2013) 71-74.
re
[23] J. Dowden, P. Kapadia, N. Postacioglu, An analysis of the laser-plasma interaction in laser keyhole welding, J.
Phys. D-Appl. Phys. 22 (1989) 741-749.
lP

[24] B. Wu, Z. Pan, S. Li, D.Cuiuri, D. Ding, H. Li, The anisotropic corrosion behaviour of wire arc additive
manufactured Ti-6Al-4V alloy in 3.5% NaCl solution, Corrosion Sci. 137 (2018) 176-183.
[25] J. Ge, T. Ma, Y. Chen, T. Jin, H. Fu, R. Xiao, Y. Lei, J. Lin, Wire-arc additive manufacturing H13 part: 3D
na

pore distribution, microstructural evolution, and mechanical performances, J. Alloy. Compd. 783 (2019)
145-155.
[26] H.L. Wei, J.W. Elmer, T. DebRoy, Origin of grain orientation during solidification of an aluminum alloy, Acta
ur

Mater. 115 (2016) 123-131.

[27] H.L. Wei, J.W. Elmer, T. DebRoy, Three-dimensional modeling of grain structure evolution during welding of
Jo

an aluminum alloy, Acta Mate. 126 (2017) 413-425.

[28] H. Rao, S. Giet, K. Yang, X. Wu, C.H.J. Davies, The influence of processing parameters on aluminium alloy
A357 manufactured by Selective Laser Melting, Mater. Des. 109 (2016) 334-346.
[29] S. Mishra, T. DebRoy, Non-isothermal grain growth in metals and alloys, Mater. Sci. Technol. 22 (2006):
253-278.
[30] M. Ohno, T. Yamaguchi, D. Sato, K. Matsuura, Existence or nonexistence of thermal pinning effect in grain
growth under temperature gradient, Comput. Mater. Sci. 69 (2013) 7-13.
[31] H. Suo, Z. Chen, J. Liu, S. Gong, J. Xiao, Microstructure and mechanical properties of Ti-6Al-4V by electron
beam rapid manufacturing, Rare Metal Mat. Eng. 43 (2014) 780-785.
[32] J.Y. Bai, C.L. Fan, C.L. Yang, B.L. Dong, Effects of thermal cycles on microstructure evolution of 2219-Al
during GTA-additive manufacturing, The International Journal of Advanced Manufacturing Technology. 87
(2016) 2615-2623.
[33] A. Suzuki, Y. Mishin, Atomic mechanisms of grain boundary diffusion: Low versus high temperatures, J.
Mater. Sci. 40 (2005) 3155-3161.
23
 Journal Pre-proof

[34] F. Verhaeghe, T. Craeghs, J. Heulens, L. Pandelaers, A pragmatic model for selective laser melting with
evaporation, Acta Mater. 57 (2009) 6006-6012.
[35] J. Xiong, Y. Lei, R. Li, Finite element analysis and experimental validation of thermal behavior for
thin-walled parts in GMAW-based additive manufacturing with various substrate preheating temperatures,
Appl. Therm. Eng. 126 (2017) 43-52.
[36] R.F Niu, B.H. Lin, Y.N. Wang, X.F. Yang, Burning behavior of Mg element and hardness distribution of joints
in aluminum alloy pulsed laser welding, Journal of Welding. 31 (2010) 81-84.
[37] S. Kou, Welding metallurgy, New Jersey. USA, 2003 431-446.
[38] B. Wang, J.M. Zhang, Y.D. Lu, X.Y. Gan, B.X. Yin, K.W. Xu, Anisotropy analysis of surface energy and
prediction of surface segregation for fcc metals, Acta Phys.Sin. 60 (2011) 16601-016601.
[39] M. Warmuzek, Aluminum-Silicon Casting Alloys, Atlas of Microfractographs. 2004.
[40] M. Zhao, Q. Jiang, B.S. Xu, Interface morphology of nanosized Si embedded in Al matrix, Mater. Sci.
Technol. 23 (2007) 577-581.

of
[41] X.Z. Liao, S.C. Srinivasan, Y.H. Zhao, M.I. Baskes, Y.T. Zhu, Formation mechanism of wide stacking faults
in nanocrystalline Al, Appl. Phys. Lett. 84 (2004) 3564-3566.

ro
[42] H. Suzuki, Segregation of solute atoms to stacking faults, J. Phys. Soc. Jpn. 17 (1962) 322-325.
[43] S. Zhou, R. Hu, J. Li, H. Chang, H. Kou, L. Zhou, Stress induced deformation in the solidification of
-p
undercooled Co80Pd20 alloys, Mater. Sci. Eng. A. 528 (2011) 973-977.
[44] J.W. Yeh, W.P. Liu, The cracking mechanism of silicon particles in an A357 aluminum alloy, Metall. Mater.
Trans. A. 27 (1996) 3558-3568
re
[45] Y.C. Zhang, Z.G. Li, P.L. Nie, Y.X.Wu, Effect of ultrarapid cooling on microstructure of laser cladding IN718
coating, Surf. Eng. 29 (2013) 414-418.
lP

[46] J.A. Sarreal, G.J. Abbaschian, The effect of solidification rate on microsegregation, Metallurgical Transactions
A. 17 (1986) 2063-2073.
[47] H. Xiao, S.M. Li, W.J. Xiao, Y.Q. Li, L.M. Cha, J. Mazumder, L.J. Song, Effects of laser modes on Nb
na

segregation and Laves phase formation during laser additive manufacturing of nickel-based superalloy, Mater.
Lett. 188 (2017) 260-262.
[48] A. Squillace, U. Prisco, Influence of filler material on micro-and macro-mechanical behaviour of
ur

laser-beam-welded T-joint for aerospace applications. Proceedings of the Institution of Mechanical Engineers,
Proc. Inst. Mech. Eng. Pt. L-J. Mater.-Design Appl. 223 (2009) 103-115.
Jo

[49] Y.B. Chen, Z.B. Yang, W. Tao, J. Chen, L.Q. Li, S. Liu, L. Chen, Microstructure characteristics and
mechanical properties of double-sided laser beam welded aluminium alloy T-joints, Chinese journal of lasers.
40 (2013) 0503009.
[50] M. Pierantoni, M. Gremaud, P. Magnin, D. Stoll, W. Kurz, The coupled zone of rapidly solidified Al Si alloys
in laser treatment, Acta metallurgica et materialia. 40 (1992) 1637-1644.
[51] S. Milenkovic, V. Dalbert, R. Marinkovic, A.W. Hassel, Selective matrix dissolution in an Al–Si eutectic,
Corrosion Sci. 51 (2009) 1490-1495.
[52] Y.C. Chen, S.Q. Zhang, X.J. Tian, H.M. Wang, Microstructure and Microhardness of 4045 Aluminum Alloy
Fabricated by Laser Melting Deposition, Chinese journal of lasers. 42 (2014) 0303008.
[53] O.E. Sebaie, A.M. Samuel, F.H. Samuel, H.W. Doty, The effects of mischmetal, cooling rate and heat
treatment on the eutectic Si particle characteristics of A319. 1, A356. 2 and A413. 1 Al-Si casting alloys, Mater.
Sci. Eng. A. 480 (2008) 342-355.
[54] N.Q. Wu, C. Xia, M. Li, N. Perrusquia, S.X. mao, Interfacial structure and micro and nano-mechanical
behavior of laser-welded 6061 aluminum alloy blank, J. Eng. Mater. Technol. 126 (2004) 8-13.
24
 Journal Pre-proof

[55] E.L. Stevens, J. Toman, A.C. To, M. Chmielus, Variation of hardness, microstructure, and Laves phase
distribution in direct laser deposited alloy 718 cuboids, Mater. Des. 119 (2017) 188-198.
[56] M.L. Zhu, F.Z. Xuan, Correlation between microstructure, hardness and strength in HAZ of dissimilar welds
of rotor steels, Mater. Sci. Eng. A. 527 (2010) 4035-4042.
[57] T. Inoue, Z. Horita, H. Somekawa, K. Ogawa, Effect of initial grain sizes on hardness variation and strain
distribution of pure aluminum severely deformed by compression tests, Acta Mater. 56 (2008) 6291-6303.
[58] Q.G. Wang, Microstructural effects on the tensile and fracture behavior of aluminum casting alloys A356/357,
Metall. Mater. Trans. A. 34 (2003) 2887-2899.
[59] Q.G. Wang, D. Apelian, D.A. Lados, Fatigue behavior of A356/357 aluminum cast alloys, Part II–Effect of
microstructural constituents, Journal of light metals. 1 (2001) 85-97.
[60] Q.G. Wang, C.H. Caceres, J.R. Griffiths, Damage by eutectic particle cracking in aluminum casting alloys
A356/357, Metall. Mater. Trans. A. 34 (2003) 2901-2912.
[61] J.Y. Bai, J.H. Wang, J.H. Shi, S.B. Lin, C.L.Yang, C.L. Fan, Microstructure and mechanical properties of 4043

of
aluminum alloy thin-walled parts made by TIG additive manufacturing, Welding & Joining. (2015) 23-26.
[62] B. Cong, Z. Qi, B. Qi,H.Sun, G. Zhao, J. Ding, A comparative study of additively manufactured thin wall and

ro
block structure with Al-6.3% Cu alloy using cold metal transfer process, Appl. Sci.-Basel. 7 (2017) 275.
[63] Y.Q. Chen, S.P. Pan, M.Z. Zhou, D.Q. Yi, D.Z. Xu, Y.F. Xu, Effects of inclusions, grain boundaries and grain
-p
orientations on the fatigue crack initiation and propagation behavior of 2524-T3 Al alloy, Mater. Sci. Eng.A.
580 (2013) 150-158.
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Credit author statement

The authors, Qiuyu Miao, Dongjiang Wu, Dongsheng Chai, Yu Zhan, Guijun Bi, Fangyong

Niu, Guangyi Ma in this paper declare that this paper 《Comparative Study of Microstructure

Evaluation and Mechanical Properties of 4043 Aluminum Alloy Fabricated by Wire-based

Additive Manufacturing》 is the results of our research unpublished. All authors have read and

approved the text and consent to its publication by Materials and Design, and that it is not under

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consideration for publication elsewhere.

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Authors:
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Qiuyu Miao, Dongjiang Wu, Dongsheng Chai, Yu Zhan, Guijun Bi, Fangyong Niu, Guangyi Ma
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Graphical Abstract

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Highlights

1. There is laser zone with refined grains and more uniform element distribution in

sample fabricated by laser-arc hybrid additive manufacturing.

2. Outstanding micro-hardness and tensile strength can be obtained by laser-arc

hybrid additive manufacturing compared with wire arc additive manufacturing.

3. The finer grains and significant decreasing of element segregation in laser zone can

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help to strengthen the mechanical properties.

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