Journal of Non-Crystalline Solids 483 (2018) 94–98

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Journal of Non-Crystalline Solids

journal homepage: www.elsevier.com/locate/jnoncrysol

A CuZr-based bulk metallic glass composite with excellent mechanical T

properties by optimizing microstructure
⁎ ⁎⁎
Song-Shan Jianga,b, Yong-Jiang Huanga, , Fu-Fa Wub, , Peng Xuea, Jian-Fei Suna
a
School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001, China
b
School of Materials Science and Engineering, Liaoning University of Technology, Jinzhou 121001, China

A R T I C L E I N F O A B S T R A C T

Keywords: The dependence of microstructure and mechanical properties on alloy composition of a series of
Bulk metallic glass composites Cu48Zr48−xAl4Nbx (x = 0, 0.3, 0.8, 1.2, 1.5, 2.0 at.%) bulk metallic glass composites (BMGCs) was studied in
Doping element detail. It was found that the doping element Nb exerts a crucial role on the mechanical properties of the studied
Mechanical properties BMGCs. By adjusting Nb content, a BMGC possessing an excellent combination of high strength (~1.3 GPa) and
Martensitic transformation
significant tensile plasticity (~8%) was obtained. Such superior mechanical performance can be attributed to the
formation of multiple shear bands and the deformation-induced martensitic transformation from a cubic pri-
mitive B2 phase to a monoclinic B19′ phase.

1. Introduction introducing minor elements can effectively favor the formation of

Bulk metallic glasses (BMGs) have attracted considerable attention
due to their unique properties, such as high strength, high elastic limit,
and excellent wear resistance [1–5]. However, the plastic deformation
of BMGs is highly localized within narrow shear bands of ~20 nm thick
under quasi-static uniaxial loading at room temperature, which results
in rapid propagation of shear bands and thus catastrophic failure [6, 7].
Limited plasticity severely hinders the industrial applications of BMGs
as engineering materials [8–14]. To address this issue, extensive in-
terests have focused on the exploration of ductile bulk metallic glass
composites (BMGCs) due to their favorable effect on the improvement
of ductility [15–21]. So far, BMGCs fabricated mainly by ex-situ and in-
situ methods have been explored in various alloy systems [7, 22–30], in
which most exhibit remarkable ductility under compression [22, 27,
28] and some even possess large tensile plasticity [29, 30]. However,
the lack of work-hardening mechanism for these BMGCs often involves
unstable deformation with the occurrence of work-softening once
yielding. In order to overcome the shortcoming, the concept of trans-
formation-induced plasticity (TRIP) has been proposed into the BMGCs
[10, 14, 31]. According to the TRIP effect, B2 phase reinforced CuZr
based and TiCuNi based BMGCs have been achieved, undergoing
martensitic transformation during deformation, which possess en-
hanced toughness and obvious work-hardening properties [10, 16, 32,
33]. For CuZr-based BMGCs, tuning the morphology, volume fraction
and distribution of second phase precipitating from the glassy matrix by
multiple shear bands, which significantly stabilizes their plastic de-
formation [34–37]. Meanwhile, the microstructure and mechanical
properties can also be optimized by tailoring stacking fault energy
through addition of minor elements [38]. B2 phase reinforced CuZr-
based BMGCs possess excellent plasticity and high strength. A question
arises here: can we further improve their mechanical properties? Due to
a positive mixing enthalpy with Cu and Zr, Nb element plays an im-
portant role in promoting the precipitation of crystals and inhibiting
their coarsening for CuZr-based BMGCs [28, 39, 40]. Meanwhile, minor
Nb addition can improve tensile plasticity and work-hardening cap-
ability of B2 phase reinforced BMGCs by tailoring stacking fault energy
[38]. Therefore, to accelerate the precipitation of single B2 phase,
modify the microstructure and thus enhance the tensile properties of B2
phase reinforced CuZr-based BMGCs, Nb is selected as the doping ele-
ment to replace Zr element in the CuZrAl alloy system. The effect of Nb
addition on the microstructure and mechanical properties of
Cu48Zr48Al4 alloys was studied. The results indicated that a BMGC with
a combination of high strength, significant tensile plasticity and strong
work-hardening capability can be achieved by finely tuning the Nb
content. Also, morphology and distribution of B2 phase play important
roles on the mechanical properties of the studied BMGCs.
2. Experimental detail
Alloy ingots with nominal compositions of Cu48Zr48−xAl4Nbx

⁎
Corresponding author.
⁎⁎
Corresponding author.
E-mail addresses: yjhuang@hit.edu.cn (Y.-J. Huang), ffwooxy@163.com (F.-F. Wu).

https://doi.org/10.1016/j.jnoncrysol.2018.01.006
Received 31 October 2017; Received in revised form 24 December 2017; Accepted 7 January 2018
Available online 10 January 2018
0022-3093/ © 2018 Elsevier B.V. All rights reserved.
S.-S. Jiang et al.
(x = 0, 0.3, 0.8, 1.2, 1.5, 2.0 at.%) were prepared by arc melting a
mixture of constituent elements with purity higher than 99.9% in a Ti-
gettered argon atmosphere. The ingots were re-melted at least four
times in order to guarantee the compositional homogeneity, followed
by drop casting the molten alloy into a copper mold. Cylinder rods of
3 mm in diameter and ~40 mm in length were then produced. The
microstructure of the as-cast rods was characterized by X-ray diffraction
(XRD) using a Rigaku D/max 2200 diffractometer with Cu Kα radiation,
a Leica DM 4000M optical microscope (OM) and a JEM-2100 trans-
mission electron microscopy (TEM). The crystalline volume fraction of
the as-cast rods was quantitatively calculated by an Image-Pro Plus 6.0
software. The dog-bone shaped tensile samples with a cross section of
1 × 1 mm2 and a gauge length of 2 mm were electric discharging ma-
chined from the as-cast samples. The room temperature tensile tests
were carried out by a CMT5305 testing machine at an initial strain rate
of 6 × 10−4 s−1. In order to ensure reproducibility, each test was re-
peated at least five times. The fracture features of tensile samples were
examined by scanning electron microscopy (SEM) in a Helios Nanolab
600i instrument.
3. Results and discussion
3.1. Composition–microstructure relationship
Fig. 1 shows the XRD patterns obtained from the as-cast
Cu48Zr48−xAl4Nbx (x = 0, 0.3, 0.8, 1.2, 1.5, 2.0 at.%) rods with 3 mm in
diameter. The XRD spectrum for the Cu48Zr48Al4 alloy exhibits a sharp
Bragg peak superimposed on a broad halo (2θ = 38°), corresponding to
a mixture of precipitated crystal and amorphous matrix. The crystalline
phase is characterized as CuZr phase with a body-centered cubic (bcc)
structure (i.e., the B2 phase), consistent with the previous report [11].
For the 0.3% Nb sample, the intensity of crystalline peaks increases,
indicating the increase in the volume fraction of B2 phase. With further
increasing Nb content (x = 0.8–1.5), the intensity of the B2 phase de-
creases in comparison to that of the Nb-free alloy, showing the in-
hibition on the precipitation of the crystal. However, beside the peak at
2θ = 38°, there exists a sharp peak at the position of 2θ = 56.7° for
Cu48Zr46.5Al4Nb1.5 alloy, which may result from the preferential or-
ientation of B2 phase. Contrarily, for the 2.0% Nb sample, the broad
halo almost disappears and crystalline phases dominate the whole
structure of the cast sample. Furthermore, there is another crystalline
phase (Al2Zr) precipitating from the glassy matrix.
Fig. 2 shows the OM images obtained from the cross sections of the
Fig. 1. XRD pattterns of as-cast Cu48Zr48−xAl4Nbx (0 ≤ x ≤ 2.0) alloys with a diameter of
3 mm, with inset showing the selected area electron diffraction pattern of B2 CuZr phase.
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Journal of Non-Crystalline Solids 483 (2018) 94–98
as-cast Cu48Zr48−xAl4Nbx (0 ≤ x ≤ 2.0) alloy samples. For the Nb-free
sample (Fig. 2(a)), round B2 phases with sizes ranging 30–120 μm and
homogeneous distribution are embedded in the glassy matrix. The 0.3%
Nb alloy displays a significant increase of crystalline volume fraction. In
addition, most grains coarsen and agglomerate each other to form
patch-like framework (Fig. 2(b)). For 0.8% Nb-added sample, round B2
phases reappear and distribute homogeneously in the glassy matrix.
With further increasing the Nb content, the amount of crystalline
phases for Cu48Zr48−xAl4Nbx (x = 1.2 and 1.5) alloys decreases
(Fig. 2(d)–(e)), indicating an improvement of the glass forming ability
(GFA) for these alloys. For the 2.0% Nb sample, crystalline phases
connecting with each other come into prominence and only small area
of glassy matrix exists at the edge of the sample. The above micro-
structural observations show that, at the same cooling rate (casting
diameter), Nb content has a strong effect on the morphology, dis-
tribution and volume fraction of crystalline phases for the current
BMGCs, and single round B2 CuZr phase can be achieved by fine ad-
justing the Nb content.
3.2. Mechanical properties
In order to study the mechanical properties of the current BMGCs
with different Nb content, tensile tests were conducted on the dog-
bone-shaped samples machined from the as-cast rods with 3 mm dia-
meter. As shown in Fig. 3, the tensile mechanical properties of the
samples strongly depend on both their microstructures and the different
crystalline volume fraction. The characteristic deformation parameters
are summarized in Table 1. As can be seen, the alloys exhibit a yield
strength ranging 416–1727 MPa and a plastic strain of 0.1%–16.7%.
The Cu48Zr48Al4 alloy exhibits ~2% plastic strain with a tensile
strength of 1060 ± 15 MPa. With increasing the volume fraction of
crystalline phases, the Cu48Zr47.7Al4Nb0.3 alloy shows relatively large
plasticity but low yield strength. As the Nb content increases, the high
yield strength of 1332 ± 18 MPa and a significant plasticity of
7.8 ± 0.2% can be obtained in the alloy containing 0.8% Nb with
homogeneous distribution of B2 particles embedded in the glassy ma-
trix. In contrast, the Nb-free sample, possessing similar morphology and
distribution of crystalline phases, exhibits lower strength and plastic
strain. It should be attributed to the decrease in the stacking fault en-
ergy of the B2 phase in the 0.8% Nb-added sample, which can promote
phase transformation and hence improve the tensile plasticity and
work-hardening capability [38]. Furthermore, for the 1.2% and 1.5%
Nb samples, brittle fracture occurs without remarkable yielding. The
lack of plasticity should result from heterogeneous distribution of
crystalline phase [11]. While the Cu48Zr46Al4Nb2 alloy displays the
nature of crystalline materials with relatively low strength due to the
high crystalline volume fraction of ~80%. There is brittle Al2Zr phase
precipitating from the glassy matrix (Fig. 1), which results in the poor
tensile plasticity of Cu48Zr46Al4Nb2 alloy. Hence, the morphology,
distribution and volume fraction of B2 CuZr phase play important roles
in tensile deformation of the current BMGCs. Furthermore, as men-
tioned in previous literatures [40, 41], the deformability of BMGCs is
closely related to the normalized strain hardening rate K K = ( dσ
σy dε ).
Here, K values of all alloys are calculated and also listed in Table 1. If K
is ≥1, the stable plastic deformation of BMGCs can be achieved under
tension [41]. As shown in Table 1, all the alloys except brittle failure
samples (x = 1.2 and 1.5) exhibit strong strain hardening ability and
stable deformability. Thus, a BMGC (x = 0.8) with single B2 CuZr phase
exhibiting optimal tensile properties has been achieved by tuning Nb
addition.
3.3. Mechanisms of enhanced deformability
To understand the intrinsic mechanisms of the current CuZr based
BMGCs with enhanced mechanical properties, a comparative analysis
S.-S. Jiang et al. Journal of Non-Crystalline Solids 483 (2018) 94–98

(a) (b) (c)

Matrix

B2
B2 Matrix

B2 Matrix

(d) (e) (f)

B2
Matrix

Matrix
B2 B2
Matrix

Fig. 2. Optical micrograph images for the Cu48Zr48−xAl4Nbx BMGCs: (a) Nb-free; (b) 0.3% Nb; (c) 0.8% Nb; (d) 1.2% Nb; (e) 1.5% Nb and (f) 2.0% Nb.

2000 region, where high density shear bands can be observed (Fig. 4(c)).
Moreover, severe plastic deformation occurs not only around the B2/
matrix interface but also inside the B2 phase, as can be seen from the
1600 magnified image of the lateral surface (Fig. 4(d)). In B2 phase re-
Engineering stress (MPa)

inforced CuZr-based BMGCs, the elastic strain limit of glassy matrix is

approximately 2% whereas the B2 CuZr phase exhibits an elastic limit
1200 of far < 1% [39]. Therefore, the B2 phase undergoes earlier plastic
deformation than glassy matrix upon tensile loading, which is re-
strained by the interface between crystalline phase and glassy matrix.
800 Hence, stress concentration sites are formed at the interface. With
further loading, when the total strain is up to ~2%, shear bands ori-
ginating from stress concentration sites at the interface initiate. Then
400 x=0 x=0.3 x=0.8 x=1.2x=1.5 x=2.0 primary shear bands propagate away from the B2 phase, indicating the
2% beginning of plastic deformation of glassy matrix [41]. B2 phase can
retard the rapid propagation of shear bands during deformation [12,
0 40]. Therefore, the shear bands will deflect around the interface be-
Engineering strain tween B2 phase and glassy matrix, and facilitate the formation of
Fig. 3. Tensile engineering stress-strain curves of the Cu48Zr48−xAl4Nbx alloy samples at multiple shear bands (Fig. 4(d)), which would improve the ductile of
room temperature. current BMGC. Meanwhile, the morphology of B2 phase evolves from
round to ellipse-like shape along the loading direction (Fig. 4(d)). In
order to further explore the effect of shape evolution of B2 phase on the
Table 1
The yielding strength (σy), fracture strength (σf), plastic strain (εp), normalized strain plastic deformation of the studied BMGC, the TEM images of B2 phase
hardening rate (K) and volume fraction of B2 phase (VB2) for Cu48Zr48−xAl4Nbx before and after tensile deformation are observed, as shown in Fig. 1
(0 ≤ x ≤ 2.0) samples with 3 mm in diameter. inset and Fig. 4(d) and (e). It can be seen that the deformation-induced
martensitic transformation from B2 phase (bcc) to B19′ phase (mono-
x/% σy/MPa σf/MPa εp/% K VB2/%
clinic) occurs with the shape evolution of B2 phase, which will lead to
0 1060 ± 15 1205 ± 10 1.6 ± 0.2 9.8 18 ± 2 the release of the stress concentration near the interface and thus
0.3 556 ± 25 1232 ± 22 16.7 ± 0.3 9.4 34 ± 2.5 suppress the formation of cracks [12]. Martensitic transformation of B2
0.8 1332 ± 18 1595 ± 20 7.8 ± 0.2 2.3 10 ± 1.5 phase also plays an important role in improving the tensile properties. It
1.2 1686 ± 20 1709 ± 17 0.1 ± 0.1 – 17 ± 1
has been generally accepted that the crystals will be strengthened
1.5 1727 ± 22 1763 ± 25 0.3 ± 0.1 – 4±2
2.0 416 ± 12 707 ± 15 3.0 ± 0.4 10 80 ± 3 during martensitic transformation [15], and require higher stress for
further deformation. Besides, nano-scale twinned structure can be ob-
served inside the lath martensite after tensile deformation, shown in
for the deformation features of two representative alloys (x = 0.8 and Fig. 4(f), which also favors the notable work-hardening behavior of
x = 1.5) is carried out, as shown in Fig. 4. As for Cu48Zr46.5Al4Nb1.5 CuZr-based BMGCs [36]. From the above results, it can be concluded
alloy, Fig. 4(a) exhibits a brittle fracture along a shear angle θ, which that the formation of multiple shear bands and deformation-induced
equals to 81° larger than 45°, between the loading axis and the fracture martensitic transformation contributed to the enhanced mechanical
plane, and few shear bands on the lateral surface. Apparently, the single performance of the current BMGC materials.
shear band has little effect on the brittle fracture (Fig. 4(b)). In contrast,
for Cu48Zr47.2Al4Nb0.8 alloy, the shear angle θ equals to 47° corre-
4. Conclusions
sponding approximately to the plane of maximum shear stress. The
homogeneous plastic deformation can be achieved in the entire gauge
In summary, by investigating the microstructure and mechanical

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S.-S. Jiang et al. Journal of Non-Crystalline Solids 483 (2018) 94–98

Fig. 4. Lateral surface and magnified SEM images showing the tensile deformation features of Cu48Zr46.5Al4Nb1.5 (a), (b) and Cu48Zr47.2Al4Nb0.8 (c), (d) BMGC; the TEM images showing
(e) the B19′ phase and (f) nanoscaled-twins respectively (inset showing the corresponding select area electron diffraction (SAED) patterns), the martensite and twins are symbolized by M
and T in the subscript, respectively.

properties of Cu48Zr48−xAl4Nbx (0 ≤ x ≤ 2.0) alloys, the correlation and martensitic transformation of B2 CuZr phase.
among doping element, microstructure and tensile properties is estab-
lished. Doping element Nb plays a dual role in precipitation of B2 CuZr
phase. BMGCs with optimal tensile properties can be obtained by ad- Acknowledgements
justing Nb content. In addition, homogenized microstructure can be as a
main criterion for the current BMGCs with enhanced mechanical This work was financially supported by the National Natural Science
properties. We have successfully prepared the Cu48Zr47.2Al4Nb0.8 BMG Foundation of China (NSFC) [Grant Nos. 51571106, 51671070 and
composite showing high strength, large plasticity and obvious work- 51371065], the Natural Science Foundation of Liaoning Province
hardening behavior. According to the exploration for the deformation [Grant No. 2015020244], and the Program for Liaoning Excellent
mechanisms of the B2 phase reinforced BMGC, it can be drawn that Talents in University [Grant No. LJQ2014064].
excellent tensile properties of Cu48Zr47.2Al4Nb0.8 BMGC should be at-
tributed to the combination of the formation of multiple shear bands

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