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Microstructure and Mechanical Properties of Mg–14Li–

3Al–2Gd Alloy Processed by Multilayer Accumulative Roll
Bonding
Haipeng Zheng, Ruizhi Wu,* Legan Hou, Min Qiu, Fan Gao, Jinghuai Zhang, and
Milin Zhang

However, due to their low strength, the

Herein, evolution of the grain refinement mechanism, interface behavior, and application of Mg–Li alloys is restricted.
mechanical properties of Mg–14Li–3Al–2Gd sheets prepared by multilayer The processing of severe plastic defor-
accumulative roll bonding (MARB) is investigated. The grain refinement mation (SPD) can bring about improve-
ment in mechanical properties of alloys.
mechanism mainly consists of continuous dynamic recrystallization (CDRX)
The accumulative roll bonding (ARB)
caused by violent dislocation movement under restrictive conditions and high- process, which was invented by Saito,[6]
energy interfaces. The bonding mechanism changes from pressure bonding and has been widely used to manufacture
metallurgical bonding to dynamic recrystallization bonding with increase in the ultrafine-grained alloys and multilayered
MARB cycle. A new process, two-step rolling in one MARB cycle, sufficiently composites, such as Mg/Mg,[7] Al/Al,[8]
improves the bonding of new interfaces introduced in the previous cycle. With the Ti/Ti,[9] Al/Mg,[10] Al/Cu,[11] Zn/Sn,[12]
Cu/Ag,[13] Al/Al2O3,[14] Al/B4C,[15] and
increase in MARB cycles, the strength and hardness of the Mg–14Li–3Al–2Gd
Ti/TiO2.[16] Recently, research on ARB
sheets are enhanced. Fine grain strengthening, strain hardening, and dispersion has mainly been based on the traditional
strengthening are the strengthening mechanisms. In the first stage, fine grain double-layer and cyclic rolling to achieve
strengthening dominates. In the later period, the strengthening effect is governed grain refinement, interface bonding, and
by strain hardening. At the same time, the interface bonding performance is the improvement of comprehensive mechani-
basis for the strengthening effect. cal properties. Ghalandari et al.[17] success-
fully fabricated Al/Sn composites by ARB
and studied the fracture behavior of dissim-
ilar metal composites in detail. Alizadeh
1. Introduction and Dashtestaninejad[18] successfully fabricated Cu matrix,
Al/Mn-reinforced, multilayered composites with a homogenous
Magnesium alloy, as the lightest commercialized metallic struc- microstructure by ARB, which was a successful application of
tural material, possesses many advantages, such as high specific ARB in the fabrication of metal matrix composites. The research
strength, high specific rigidity, and good electromagnetic shield- on Mg–Li alloys processed by ARB in recent years is summarized
ing effectiveness.[1] A magnesium–lithium (Mg-Li) alloy, with a in detail by Wu et al.[10,19–21] However, little work has focused on
density between 1.30 and 1.60 g cm
3, is lighter by more than optimizing the ARB process to improve the mechanical proper-
25% than the conventional magnesium alloys.[2] Therefore, ties of Mg–Li sheets. At the same time, the refinement mecha-
Mg–Li alloys have extensive application prospects in the military, nism, interface behavior, and bonding mechanism of Mg–Li
alloys with a high Li content are rarely involved.
electronics, pharmaceutical, and automotive industries.[3–5]
The traditional ARB process with double-layer and one-step
rolling in one cycle has an excessive workload, lower efficiency
of accumulated strain, and especially poor interface bonding of
Dr. H. Zheng, Prof. R. Wu, Dr. L. Hou, Dr. J. Zhang, Prof. M. Zhang the latest interface brought by the last cycle, which severely limit
Key Laboratory of Superlight Materials & Surface Technology the strengthening effect of the traditional ARB process.
Ministry of Education
Harbin Engineering University
Based on the above problems, we propose the multilayer
No. 145 Nantong Street, Nangang District, Harbin 150001, P. R. China accumulative roll bonding (MARB) process with two-step rolling
E-mail: ruizhiwu2006@yahoo.com, rzwu@hrbeu.edu.cn in one cycle (TSRC) to further optimize the traditional ARB
Prof. R. Wu, Dr. M. Qiu, Dr. F. Gao, Prof. M. Zhang process.
Science College In this study, Mg–14Li–3Al–2Gd sheets with a fine-grained,
Heihe University homogeneous microstructure and high strength were fabricated
No. 1 Xueyuan Road, Heihe 164300, P. R. China
by MARB. The evolution of the microstructure, refinement
The ORCID identification number(s) for the author(s) of this article mechanism, interface bonding mechanism, and mechanical
can be found under https://doi.org/10.1002/adem.201900774. properties of the MARB-processed Mg–14Li–3Al–2Gd sheets
DOI: 10.1002/adem.201900774 was investigated.

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2. Experimental Section
The raw materials for the Mg–14Li–3Al–2Gd alloy were commer-
cial pure (CP) Mg (purity 99.9 wt%), CP Li (purity 99.9 wt%),
CP Al (purity 99.9 wt%), and the master alloy of Mg–20 wt%
Gd. They were melted in a graphite crucible in a vacuum induc-
tion furnace at an argon atmosphere. Then, the melt was poured
into a cuboid mould.
The density of the Mg–14Li–3Al–2Gd alloy measured by
Archimedes drainage was 1.392 g cm
3. The liquid used in
the Archimedes drainage was deionized water. Although the cor-
rosion resistance of Mg–Li alloys is relatively poor, the contact
time between the sample and the water was very short in the test.
Therefore, the change of the sample caused by water corrosion
could be almost neglected in such a short contact time.[22]
The as-received ingot was cut into plates of dimensions
60 mm  40 mm  2 mm for MARB processing. To eliminate
component segregation and obtain a uniform microstructure
and properties, the as-cast ingot was homogenized at 473 K
for 10 h.
To solve the problem of poor interface bonding caused by the
last cycle and the insufficient reduction of single rolling and the
cracking phenomenon caused by the excessive reduction of sin-
gle rolling, improved accumulative roll bonding (MARB) with
TSRC was introduced, as shown in Figure 1.
To remove the surface oxide film and achieve excellent inter-
face bonding between sheets, the surfaces of the sheets were
degreased with acetone and brushed with a stainless steel brush.
The surface treatment process was described in detail by
Wang et al. in a previous article.[19] After surface treatment, four
smooth sheets were stacked and fixed with aluminum wire. After
the stacked sheets were preheated at 473 K for 15 min, the
stacked sheets were rolled with a reduction ratio of 50%. After
annealing at 473 K for 20 min, the sheets were rolled again with
the second 50% reduction. To avoid the static recrystallization
caused by residual temperature and preserve the rolled structure
as much as possible, the MARB-processed sheets were water
cooled. Finally, the roll-bonded sheets were cut into four
equal-sized sheets for the next rolling cycle.
Figure 1. Schematic illustration of the MARB process.
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A LEICA DM IRM optical microscope and an FEI Quanta 200
scanning electron microscope were utilized for the microstruc-
tural investigations. The phases of the alloys were measured with
a Rigaku TTR-III X-ray diffraction (XRD) machine at 40 kV and
150 mA and energy-dispersive spectrometry (EDS). A JEM-2100
transmission electron microscope (TEM) was utilized to observe
the dislocation behavior and analyze the grain refinement
mechanism. The tensile properties were analyzed on a
WDW-200D electrouniversal tester machine with an initial
strain rate of 10
3 s
1, and the tensile axis was parallel to the
rolling direction. The Vickers microhardness (HV) on the rolling
direction–transverse direction (RD–TD) plane and the rolling
direction–normal direction (RD–ND) plane was measured with
a microhardness tester under a loading of 50 gf and a holding
time of 15 s.
3. Results
3.1. Microstructure and Phase Analysis of the As-Cast Alloy
The microstructure, EDS, and XRD of the as-cast Mg–14Li–
3Al–2Gd alloy are shown in Figure 2 and 3. As shown in
Figure 2a and 3, the matrix alloy possesses a single β-Li phase
and the grains are coarse and polygonal with an average grain
size of 200–400 μm. Figure 2b shows that the fine second phases
are mainly located at the grain boundaries, whereas the coarse
second phases are mainly located at the grain interior.
To accurately confirm the component of the second phases,
the EDS for the second phases was analyzed, as shown in
Figure 2b–d. It is well-known that the difficulty of forming a com-
pound between different elements can be judged by the differ-
ence in electronegativity. The larger the difference, the greater
the bonding force between the elements, which leads to interme-
tallic compounds forming more easily between the elements.
Because lithium elements cannot be detected by conventional
EDS and it is difficult for lithium to form intermetallic com-
pounds with rare earth elements, only the Mg, Al, and Gd in
the alloy were analyzed, as shown in Figure 2c,d. The analysis
of bright white particles in the grain interior and at the grain
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Figure 2. Microstructure and EDS of the as-cast LAGd1432 alloy: (a) OM micrograph of the as-cast LAGd1432 alloy, (b) SEM micrograph of the as-cast
LAGd1432 alloy, and (c), (d) the EDS of the marked spots in (b).
Figure 3. XRD pattern of the as-cast Mg–14Li–3Al–2Gd alloy.
boundary of the β-Li phase of the alloy shows that the compounds
of A and B mainly contain Mg, Al, and Gd (possibly containing
Li). Mg is most likely the Mg element dissolved in Li metal. If the
influence of the Mg element is excluded, the compounds of
A and B are composed of Al and Gd, and the atomic ratio of
Al to Gd is about 2:1.
Combined with the relevant research result,[23,24] the electro-
negativity differences between the metal atoms Gd and Al, Gd
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and Mg, and Gd and Li are 0.41, 0.1, and 0.22, respectively.
Therefore, combined with the XRD pattern shown in
Figure 3, the compounds of A and B in Figure 2b are both Al2Gd.
3.2. Microstructure Evolution of MARB-Processed Sheets
Figure 4 illustrates the microstructure of the RD–ND plane in
different cycles. The number N in MARBN represents the num-
ber of cycles. In Figure 4a, the interface between sheets is clearly
visible. With the increase of rolling cycles, new interfaces gener-
ate; at the same time, the old interfaces gradually disappear.
Due to the improved process with TSRC resulting in SPD, the
dynamic recrystallization is very severe. At the same time, defor-
mation continues in the region where dynamic recrystallization
has occurred. The severe interaction brings about the elongated
grains along the RD caused by SPD and the equiaxed grains
caused by dynamic recrystallization, as shown in Figure 4.
Figure 5 provides a more intuitive view of the interface
changes. As shown in Figure 5, there are some continuous inter-
faces, at the same time, in the 70 μm range on the left; there is no
interface or only intermittent interfaces can be observed, which
proves the breakage and disappearance of the interface during
the MARB cycle.
To intuitively depict the interface bonding and the variation
of precipitated compounds, the microstructures of the MARB-
processed sheets under different cycles were observed by scan-
ning electron microscopy (SEM), as shown in Figure 6. After the
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Figure 4. Microstructure of MARB-processed Mg–14Li–3Al–2Gd sheets: a) MARB1, b) MARB2, c) MARB3, and d) MARB4.
Figure 5. Microstructure of MARB3-processed Mg–14Li–3Al–2Gd sheets.
MARB1 cycle, continuous interfaces are clearly observed, as
shown in Figure 6a. With increase of the rolling cycle, the
interface bonding lines become discontinuous and gradually dis-
appear, as shown in Figure 6b–d. After four cycles, 255 interfa-
ces, that is (44
1), are produced. Only the discontinuous
interfaces introduced in the last cycle can be observed blurrily;
the previous interfaces disappear almost completely. It is shown
that multilayer rolling and TSRC can sufficiently improve the
bonding performance of interfaces introduced in the last cycle
and the previous cycle.
The evolution of the Al2Gd phase in different cycles is also
shown in Figure 6. As shown in Figure 6a, the Al2Gd phase
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appears to agglomerate and grow in size. With the deformation
continuing, the agglomeration is significantly improved. At the
same time, because of its high melting point, the Al2Gd phase
remains stable without dissolution at the rolling temperature
of 473 K. However, during the deformation process, hard par-
ticles are crushed and dispersed in the matrix, as shown in
Figure 6b–d. With the increase of MARB cycles, the Al2Gd
phases are crushed and the size gradually decreases. At the same
time, the agglomeration phenomenon and dispersivity of Al2Gd
phases are also improved significantly, due to the increase of
accumulated strain and the disappearance of interfaces with
the increase of MARB cycles. However, although the increase
of MARB cycles significantly improves the uniformity of
Al2Gd phases, the larger accumulated strain of the MARB4 cycle
still keeps the Mg–14Li–3Al–2Gd sheet in an obvious rolling
morphology along the RD, which leads to the distribution
of Al2Gd phases along the RD. The fine-grained Al2Gd
phases enhance the mechanical properties by dispersion
strengthening.
To intuitively analyze the interface morphology, the number of
grains between interfaces, and the effect of interfaces on the
grain size, the MARB-processed Mg–14Li–3Al–2Gd sheets were
annealed at 300  C for 30 min, and the microstructures are
shown in Figure 7. In Figure 7a,b, the average grain size is about
30–50 μm. At this stage, a dozen grains (Figure 7a) and four
or five grains (Figure 7b) exist in a layer along the ND.
However, the finer grains form between the interfaces, as shown
in Figure 7c,d. At this stage, two or three grains exist between the
interfaces along the ND. In Figure 7d, only a single grain with an
average grain size of about 5–10 μm exists between the interfaces
along the ND.
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Figure 6. SEM micrographs of MARB-processed Mg–14Li–3Al–2Gd sheets. a) MARB1, b) MARB2, c) MARB3, and d) MARB4.

Figure 7. Microstructure of MARB-processed Mg-14Li-3Al-2Gd sheets annealed at 300  C for 30 min: a) MARB1 b) MARB2 c) MARB3, and d) MARB4.

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3.3. Mechanical Properties

3.3.1. Strength and Elongation

Figure 8a,b shows stress–strain curves and the yield strength

(YS), ultimate tensile strength (UTS), and elongation (EL) of
Mg–14Li–3Al–2Gd sheets at different cycles, respectively. The
YS, UTS, and EL of the as-cast Mg–14Li–3Al–2Gd sheets are
73.2  3.8 MPa, 125.6  4.2 MPa, and 38.2  1.7%, respectively.
The strength of the MARB-processed Mg–14Li–3Al–2Gd sheets
is significantly improved compared to that of the as-cast
Mg–14Li–3Al–2Gd sheets; at the same time, the sheets still
possess good plasticity.
With the increase of MARB cycles, the YS and UTS are sig-
nificantly enhanced. The MARB4 sheet possesses the highest YS
(232.2  5.3 MPa). Compared to the as-cast alloy, the strength of
the MARB sheets is significantly enhanced, by 317%. For
MARB1, the elongation declines seriously. After MARB2, the Figure 9. The specific strength of MARB-processed Mg–14Li–3Al–2Gd
elongation value still has a slight decrease. However, after sheets and commercial Mg alloys.
MARB3 and MARB4, the elongation begins to increase continu-
ously, which is mainly due to the significant improvement of
interface bonding performance in high cycles. The Mg–14Li–3Al–2Gd sheets strengthened by MARB process-
In addition, as shown in Figure 8a, the MARB-processed ing with TSRC exhibit especially valuable benefits when they are
Mg–14Li–3Al–2Gd sheets exhibit distinct stress–strain curves used in transportation vehicles and aircraft because of their
compared with the as-cast alloy. The uniform plastic deformation lightweight and high-strength characteristics.
of stress–strain curves of the MARB-processed Mg–14Li–
3Al–2Gd sheets is relatively small, and is followed by enormous
localized deformation after necking. The overall plastic deforma- 3.3.2. Hardness
tion of the sample is large but mostly localized in the neck.
Figure 8 shows that the MARB process can significantly The hardness of Mg–14Li–3Al–2Gd sheets at different cycles is
improve the strength of the Mg–14Li–3Al–2Gd alloy. At the same shown in Figure 10. Compared to the as-cast Mg–14Li–3Al–2Gd
time, the MARB-processed Mg–14Li–3Al–2Gd sheets also have a sheet, the hardness of the MARB-processed Mg–14Li–3Al–2Gd
high yield ratio. For a metal structural material, the yield strength sheets is significantly improved. After four MARB cycles, the
is an important manifestation of the material resistance to plastic hardness is enhanced from 48.1  1.7 to 80.3  3.4 HV0.05.
deformation. Therefore, it is of great engineering significance to However, the hardness fluctuates along the ND and the low-
use the ratio of yield strength to density as the specific strength hardness values mainly exist in the interface bonding regions
value to measure the resistance of materials to plastic deforma- because of the large number of structure defects in these regions.
tion.[25] Figure 9 shows that the MARB-processed Mg–14Li– As the rolling cycle increases, the fluctuation gradually decreases,
3Al–2Gd sheets have low density and high specific strength which is mainly attributed to the improvement of the interface
compared with as-used commercial Mg-based alloys.[25–27] bonding with the increase of the MARB cycle.

Figure 8. The stress–strain curve and variation trend of MARB-processed Mg–14Li–3Al–2Gd sheets along the RD: a) stress–strain curve and b) variation
trend image.

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Figure 10. The hardness of MARB-processed Mg–14Li–3Al–2Gd sheets at
different distances from the surface along the ND.
4. Discussion
4.1. Refinement Mechanism
Figure 11 shows the TEM micrographs of MARB4-processed
Mg–14Li–3Al–2Gd sheets. Because of the great accumulated
Figure 11. TEM micrographs of MARB4-processed Mg–14Li–3Al–2Gd sheets: (a), (b) grain morphology and (b), (c) dislocation substructures.
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strain of MARB4-processed Mg–14Li–3Al–2Gd sheets, the mor-
phology and the size of grains could not be observed directly and
accurately through optical microscopy, so transmission electron
microscopy was used to observe the morphology and size of
MARB4-processed Mg–14Li–3Al–2Gd sheets, as shown in
Figure 11a,b. After MARB4, the size of MARB4-processed grains
in the ND was relatively stable, with an average size of 0.5 μm.
However, in the RD, the size of MARB-processed grains fluctu-
ated in a larger range of several microns and the smallest size
was about 2 μm along the RD.
The low stacking fault energy of magnesium alloys can signif-
icantly promote dynamic recrystallization during hot deforma-
tion, especially during SPD.[19,23,28] At the same time,
compared to the close-packed hexagonal (hcp) of Mg–Li alloys
with low Li content, the body-centered cubic (bcc) of
Mg–14Li–3Al–2G alloys has more slip systems.[29] When the
alloy is deformed under a large force with an extremely high
speed, SPD occurs, during which a large amount of slip systems
are stimulated. Thereby, the dislocation increment and disloca-
tion density increase rapidly, which makes the dislocation pile-up
form easily.[30] At the same time, as a hard phase, the Al2Gd
phase obstructs the movement of dislocation and accelerates
the dislocation pile-up during the SPD process. With the defor-
mation proceeding, the dislocation pile-up gradually transforms
into a dislocation wall, and then dislocation cells are formed by
dislocation walls. The dislocation cells gradually transform into a
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subgrain. Finally, the sub-boundary transforms into a high-angle

grain boundary. This continuous dynamic recrystallization
(CDRX) is the main dynamic recrystallization mode and grain
refinement method in the MARB process. The continuous occur-
rence of the phenomenon in the rolling cycle leads to grain
refinement. The results of the above analysis show that, in the
MARB cycle, the grain size is controlled by the complicated inter-
action of the dynamic recrystallization and dispersion of the
Al2Gd phase.
In initial cycles, such as MARB1 and MARB2, due to the large
thickness of the single layer, the interface has no significant effect
on grain refinement. During subsequent cycles, the thickness of
the single layer decreases rapidly until about 8 μm in the MARB4
cycle. However, the phenomenon of inhomogeneous deformation
also exists, which results in a slight difference in the thickness of
the single layer. At this stage, the interface begins to have a
significant effect on grain refinement. As shown in Figure 7c,
finer grains start forming between the interfaces due to the
obstruction of the interface. At the same time, because of the exis-
tence of the intermittent interfaces, the obstruction of grain
growth along the ND is significantly stronger than along the
RD, which makes the as-annealed grains still possess an elongated
shape along the RD. At the same time, with decrease of the thick-
ness of the single layer and obstruction of the interfaces to grain
growth, the number of grains in a single layer gradually decreases.
As shown in Figure 7d, only a single grain with the average size of
about 5–9 μm exists between the interfaces along the ND.
Figure 12. The interface behavior of the MARB cycle: a) MARB1,
4.2. Interface Behavior and Bonding Mechanism b) MARB2, c) MARB3, and d) MARB4.

The interface behavior and the accumulative number of layers in

different cycles are depicted in detail in Figure 12 and Formula 1.
Compared to the traditional two-layer accumulative roll bonding
(TARB), the distribution of the interface has a significant differ-
ence. During the TARB process,[20,31] the latest interface always
exists in the middle thickness of the sheet, whereas the old inter-
faces gradually move to the sides of the sheet and these interfaces
become blurred and gradually disappear. However, in each
MARB cycle, three new interfaces are produced, and the new
interfaces always exist in the middle thickness and one-quarter
thickness of the sheet. At the same time, in the MARB cycle, the
relationship between the accumulative layers and the number of
cycles can be expressed by the following formula
FðLÞ ¼ 4n ðn∶1, 2, 3, 4 : : : nÞ (1)
where F(L) and n represent the accumulative layers and the num-
ber of cycles, respectively. Due to the exponential relationship,
with the increase of the MARB cycle, the accumulative number
of layers increases sharply, which is especially noticeable in high
cycles.
In Figure 12, the different colors represent the interfaces pro-
duced by the different cycles. With the increase of the MARB
cycle, the interface gradually fragments and disappears.
Figure 13 shows the microstructure of the MARB-processed
Mg–14Li–3Al–2Gd sheets after annealing. There are obvious
bonding zones and fault zones. The bonding zone is further
divided into the grain bonding zone and the grain boundary
bonding zone. The grain boundary bonding zone is connected
by the shared grain boundary, and the fault zone is pressure
bonding.
In the whole interface bonding process, there are four main
stages. In the first stage of deformation, such as the MARB1 cycle,
the reduction of deformation and the accumulated strain are
small, which is not enough to provide sufficient power for com-
plete bonding between interfaces. Under the action of rolling
force, mainly shear force, the hardened layer produced by the
stainless steel brush and the oxide layer produced during brushing
and heating gradually rupture, leading to the exposure and mutual
contact of fresh metal in some areas. Under the action of flow
stress, the flow of fresh metal promotes the contact degree
between fresh metals, which makes the atomic distance of the
interface metal atoms instantaneously reduce to the extent of
the formation of metallurgical bonding. When the energy instan-
taneously provided by SPD is sufficient to overcome the energy
barrier of the metallic bond, metallurgical bonding occurs between
the interfaces. Previous studies[32,33] have indicated that overcom-
ing the energy barrier is a necessary condition for interface bond-
ing in the ARB process. Under a lower accumulated deformation,
in MARB1, for example, metallurgical bonding does not occur
within the entire interface. The interface bonding mode of the
locations that are not exposed to fresh metal and the locations that
are exposed to fresh metal but cannot provide enough energy to
overcome the energy barrier is mainly pressure bonding.
With the rolling cycle increasing, the accumulated deforma-
tion gradually increases, under the action of normal stress,

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Figure 13. Microstructure of MARB-processed Mg–14Li–3Al–2Gd sheets annealed at 300  C for 30 min: a) MARB2 and b) MARB3.
and the residual hardened layer and oxide layer are further rup-
tured at some locations of pressure bonding surfaces. Under the
action of shear stress, the interface metals that have completed
metallurgical bonding rapidly expand around the pressure bond-
ing points. Due to the squeezing action of metal flow, some
cracks form at pressure bonding locations.
Due to the irregular atomic arrangement compared to the
matrix, the interfaces exhibit a metastable state with higher
energy.[34] The metastable state with higher energy causes the
rearrangement of atoms, which leads to dynamic recrystalliza-
tion with a larger nucleation rate compared to the matrix.[35]
After nucleation, nuclei grow up rapidly. However, because of
the large nucleation rate, the obstruction of second phases
and discontinuous interfaces, the growth of the grains is
obstructed. With the accumulated deformation increasing fur-
ther, for example, in MARB4, dynamic recrystallization occurs
again on the basis of the previous cycle structure, which results
in the previous structure being replaced by the new dynamic
reorganization structure. The structure replacement leads to
completely losing the interface structure. Accordingly, a transfor-
mation between metallurgical bonding and recrystallization
bonding happens.
4.3. Mechanical Properties
The strengthening mechanism of magnesium alloy during the
ARB process mainly includes strain strengthening and grain
refinement. Strain hardening is a significant strengthening
method.[36] Mineta and Sato[37] study the mechanical properties
of a Mg–Li–Al alloy produced by SPD where the principle of the
strengthening method mainly includes dislocation multiplica-
tion and mutual dislocation interaction.
During the deformation process, a large number of disloca-
tions form in grains. Dislocation pile-up brings about a signifi-
cant increase in the mechanical properties. Moreover, the grain
size has a significant effect on the strengthening of the metallic
material.[38] The MARB4 sheet possesses the smallest grain size,
about 0.5 μm in the ND and 2–6 μm along the RD, as shown in
Figure 11a,b, which is much smaller than that of the as-cast
Mg–14Li–3Al–2Gd sheet. The decrease of the grain size leads
to a significant increase of grain boundaries acting as obstacles
to dislocation motion. Due to grain refinement, the YS, UTS, and
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hardness are continuously enhanced during the MARB cycle, as
shown in Figure 7 and 8. Furthermore, the fine and dispersed
second phase also significantly enhances the mechanical
properties of the metallic material.[39] The Al2Gd phase can also
effectively obstruct dislocation motion.
As shown in Figure 7, significant refinement of the grains
mainly happens in the first cycle, although the obvious strength-
ening of the mechanical properties always occurs throughout the
whole MARB process, which indicates that strain strengthening
caused by the high accumulated strain efficiency of MARB
becomes the main strengthening factor for the MARB-processed
Mg–14Li–3Al–2Gd sheets after the second cycle. At the same
time, with the deformation proceeding, the Al2Gd phases are
gradually crushed and dispersed in the matrix; therefore, the
effect of dispersion strengthening is gradually improved.
It is well-known that dynamic recrystallization has a certain
softening effect; however, CDRX is the main mode of grain
refinement in this study, resulting in fine grain strengthening.
In addition, dynamic recrystallization and dramatic plastic defor-
mation occur simultaneously, which results in there being no
recrystallized microstructure after each cycle and a deformed
microstructure due to great accumulative deformation, as shown
in Figure 4, 5, and 11. At this point, there are still a large number
of dislocation tangles and pile-ups, which leads to strain strength-
ening still playing an important strengthening role.
It should be noted that, as for multilayered materials, the
interface bonding performance has a critical impact on the
mechanical properties. Only under the condition that the inter-
face bonding performance is good can the strengthening factors
mentioned earlier produce significant effects.
In addition, the tensile curves of MARB-processed Mg–14Li–
3Al–2Gd sheets exhibit rather typical behavior, rapid necking and
strain softening, as shown in Figure 8a, frequently reported for
SPD-treated materials, and compared with traditional strain-
hardened materials, SPD materials exhibit a smaller work hard-
ening index.[40–46] SPD is an effective way to refine grain size,
especially to obtain nanocrystalline or ultrafine-grained metals.
Compared with strain hardening, strain softening has also been
observed frequently in tensile and compressive tests recently for
nanocrystalline or ultrafine-grained metals, such as copper with
grain sizes of 100–800 nm.[47–52] Tang and Schoenung[45] found
that the main reason for strain softening is the formation of
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com
residual internal stresses caused by the generation of dislocations
and the absorption of dislocations at grain boundaries in nano-
crystalline or ultrafine-grained metals. At this time, during the
plastic deformation of a nanocrystalline or ultrafine-grained
metal, when a dislocation created at the grain boundary of a grain
sweeps through the grain and is absorbed at the other side grain
boundary, a residual stress field is established around this
grain. With this residual internal stress field, to create new dis-
locations at grain boundaries for the surrounding grains, lower
external stress is required when compared with that without the
internal stress field, and thus, strain softening occurs.
Although the grain size of MARB-processed Mg–14Li–
3Al–2Gd sheets is still relatively large, there are a large number
of substructures with ultrafine grain size and storage dislocations
in the alloy after MARB processing. The substructures with ultra-
fine grain size, especially subgrains, may have similar effects to
the ultrafine grains described earlier. Chrominski et al.[44] found
that a large number of substructures are formed in multislip sys-
tem metals by the SPD process, and at the same time significant
dynamic softening occurs in tensile tests. After reaching
yielding, the storage dislocations begin to move and interact with
substructures, which results in larger stress and a larger stress
field in the grain, and then the gradual reduction of the external
stress required for the grain to continue to deform, thus resulting
in softening. The softening effect caused by the residual stress
field weakens the strain hardening effect of materials and
advances the time when the softening effect plays a dominant
role in competition with strain hardening, which may be an
important reason for the weak strain hardening effect of
MARB-processed Mg–14Li–3Al–2Gd sheets, the rapid hardening
just after exceeding the YS, and the continuous softening after
reaching the UTS.
In summary, the improvement of mechanical properties of
MARB-processed Mg–14Li–3Al–2Gd sheets can be attributed
to fine grain strengthening, strain hardening, and dispersion
strengthening. Additionally, the interface bonding performance
is the basis for the strengthening effect.
5. Conclusions
In this study, Mg–14Li–3Al–2Gd sheets with a fine-grained,
homogeneous microstructure and high strength were success-
fully fabricated by multilayer accumulative roll bonding.
MARB efficiently refines the grains of the Mg–14Li–3Al–2Gd
alloy. The MARB4-processed Mg–14Li–3Al–2Gd sheets possess
the smallest grain size, about 0.5 μm in the ND; however, the size
of MARB4-processed grains fluctuates in a larger range of several
microns along the RD, with the smallest size being about 2 μm.
The refinement mechanism is CDRX. CDRX is caused by the
dislocation movement and the high energy interface, respec-
tively. The MARB-processed sheets possess excellent bonding
performance. The bonding mechanisms include pressure bond-
ing, metallurgical bonding, and dynamic recrystallization bond-
ing. TSRC can sufficiently improve the bonding performance of
new interfaces introduced in the last cycle. With the increase of
MARB cycles, the YS, UTS, and hardness are enhanced signifi-
cantly. The strengthening mechanisms mainly include fine grain
strengthening, strain hardening, and dispersion strengthening.
Adv. Eng. Mater. 2019, 1900774 1900774 (10 of 11)
www.aem-journal.com
Additionally, the interface bonding performance is the basis for
the strengthening effect. In the first stage (MARB1 and MARB2),
the strengthening is dominated by fine grain strengthening. In
the later period (MARB3 and MARB4), the strengthening is
governed by strain hardening.
Acknowledgements
This work was supported by the National Natural Science Foundation
(51671063, 51771060, and 51871068), the Heilongjiang Province
Natural Science Foundation (ZD2017010), and the Fundamental
Research Funds for the Central Universities (HEUCFG201834).
Conflict of Interest
The authors declare no conflict of interest.
Keywords
grain refinement mechanisms, interface bonding mechanisms, multilayer
accumulative roll bonding, strengthening mechanisms
Received: July 2, 2019
Revised: September 19, 2019
Published online:
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