Short communication

Fabrication of MoCu composites by a diffusion-rolling procedure

Yihang Yang, Gaoyong Lin, Xiaoying Wang, Diandian Chen, Aokui Sun, Dezhi Wang
Key Laboratory of Ministry of Education for Non-ferrous Materials Science and Engineering, School of Material Science and Engineering, Central South University, Changsha 410083, PR China
a b s t r a c t a r t i c l e i n f o
Article history:
Received 25 September 2013
Accepted 9 November 2013
Keywords:
MoCu
Refractory composite
Laminates
Microstructure
Diffusion-rolling
A plastic deformation approach to Mo matrix composites remains a longstanding challenge in the processing of
refractory metal. Toward this objective, we explored a selective fabrication of the diffusion-rolling procedure.
With diffusion bonding initially, a primary sandwich sheet was achieved. The interfacial strength of Mo/Cu
was enhanced by the plastic deformation after rolling. Ultrathin CuMoCu sheet and MoCu alloy sheet with
Cu matrix containing distributed uniformly brous Mo were fabricated. HR-TEM analysis revealed that atomic-
level interdiffusion of Mo and Cu was present at the interface. Therefore, it is concluded that the diffusion-
rolling procedure can be potentially employed as a joining method for the fabrication of MoCu composites.
2013 Elsevier Ltd. All rights reserved.
1. Introduction
MoCu composites combine the refractory properties of Mo withthe
high conductivity of Cu and can be tailored to specic applications by
adjusting the relative amounts of these constituents [1]. These materials
that have high thermal conductivity and a lowcoefcient of thermal ex-
pansionhave become desirable. MoCu composites are used inindustri-
al applications as electrical contacts, electroerosion segments for hard
metals and heat sinks for packaging microelectronic devices [16].
In general, good solid solubility is essential for sound bond proper-
ties [7,8]. In the case of low inter-solubility metals of Mo and Cu [911],
well-designed bonding procedure remains a challenge. MoCu compos-
ites are traditionally processed by Cu inltration of Mo preforms
[4,5,12]. Laminated composites of MoCu are processed by explosion
bonding [13]. In1998, Saito et al. invented a process, named accumulative
roll bonding (ARB), to impose severe plastic strain onto metallic materials
through the rolling process [14,15]. Different from ARB, the authors now
propose an alternative plastic deformation procedure of diffusion-rolling
[16] for refractory metal composite manufacturing at high productivity
and quality. In this paper, the principle of the diffusion-rolling procedure
and some convincing experimental results are presented.
2. Experimental
Fig. 1 schematically represents the multi-stages of diffusion-rolling.
In order to obtain one-body solid material and avoid cracks during
rolling of refractory metal Mo, the diffusion bonding employed initially
was not only a bonding process but also a constraint on its surface. First,
a Mo sheet and two Cu sheets were stacked in the order of CuMoCu.
Before stacking, the sheet surfaces were degreased with acetone and
cloth polished. Then, the three sheets were bonded together by diffu-
sion at 900 C and 10 MPa process pressure for a time of 30 min.
Multi-pass rolling with a thickness reduction of 35% was conducted
for thinner sheet fabrication and bonding strength improvement. At
this stage, ultrathin CuMoCu sheets can be achieved. After that, the
length of rolled composites was sectioned into three partitions. The sec-
tioned sheets were again surface-treated, stacked, diffusion bonded and
rolled. The whole process was repeated again and again. At last, MoCu
alloy sheets can be achieved.
As-received commercially pure Mo sheets with a thickness of
3.6 mm and a purity of 99.95 wt.% were used as the core materials.
Oxygen-free copper sheets with a thickness of 2.0 mm and a purity of
99.99 wt.% were used as the cladding materials. The dimension of Mo
sheet was 50 100 mm
2
, and two Cu sheets were 15 mm longer
than Mo plate for the convenience of roll bite.
Single lap shear specimens were prepared for the evaluation of inter-
facial strength. These specimens were tested in tension using an Instron-
3369 machine, such that the 1 mm long bond line was subjected to a
shear stress. The tests were carried out at room temperature and at a
loading rate of 1 10
3
m/min. A scanning electron microscope (SEM,
Quanta-200) was used to examine the interface. Image of high resolution
transmission electron microscopy (HR-TEM) was collected on a FEI
Tecnai G2 F20 operated at 200 kV. The cross-sectional TEM sample was
prepared by tripod polishing and Ar ion beam thinned to perforation.
3. Results and discussion
3.1. Layer structures evolution
The layer structures of all-stages of diffusion-rolling procedure were
shown in Fig. 2. Fig. 2a shows the diffusion bonded CuMoCu sheet.
Int. Journal of Refractory Metals and Hard Materials 43 (2014) 121124
Corresponding author. Tel.: +86 731 88877221; fax: +86 731 88830202.
E-mail address: dzwang@csu.edu.cn (D. Wang).
0263-4368/$ see front matter 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.ijrmhm.2013.11.003
Contents lists available at ScienceDirect
Int. Journal of Refractory Metals and Hard Materials
j our nal homepage: www. el sevi er . com/ l ocat e/ I JRMHM
After diffusion bonding, ultrathin sheets were achieved by multi-pass
rolling. Fig. 2b shows the roll processed CuMoCu sheet with a thick-
ness of 600 m. The interface of Mo/Cu was at. Fig. 2c shows the roll
processed CuMoCu sheet with a thickness of 350 m. But the inter-
face of Mo/Cu has a slightly wave-like structure.
When the thickness of CuMoCu sheet approaches to the limit of
rolling mill, the procedure of diffusion-rolling was repeated again and
again. Fig. 2d shows the two-cycle processed MoCu laminate with a
thickness of 230 m. The interface of Mo/Cu has a severe wave-like
structure, but the layers were uniform and coherent. When the process
repeated once again, Mo layers became fragmented, displaying multiple
necking due to inhomogeneous deformation of layers and shear bands
crossing the layers. Finally, a composite sheet with Cu matrix containing
uniformly distributed brous Mo was fabricated, as shown in Fig. 2e.
3.2. Bond strength
In order to evaluate the diffusion-rolling effect on the bond strength
of CuMoCu clad sheet, the shear tensile test was conducted. Fig. 3
shows the shear tensile specimen and bond strengths of two types of
Mo/Cu interface. It reveals that the diffusion-rolling processed Mo/Cu
interface was twice as strong as the diffusion bonded one, and that
it reached a maximum tensile strength equivalent to 70% of that of
Cu (about 250 MPa), which suggests that interfacial strength was
Fig. 1. Schematic illustration of diffusion-rolling procedure.
Fig. 2. CuMoCu sheets and multi-stages processed MoCu alloy.
122 Y. Yang et al. / Int. Journal of Refractory Metals and Hard Materials 43 (2014) 121124
enhanced by the subsequent rolling deformation. This canbe interpreted
as the high rolling strain accelerated the diffusion between the different
layers [17,18]. Besides, it potentially provide more opportunity for the
establishment of atom-to-atom bond between two pieces [19,20].
3.3. Microstructure of Mo/Cu interface
After the three-cycles (Fig. 2e), a SEM image of the Mo/Cu interface
area is shown in Fig. 4a. It exhibits good bonding along the interface of
the joints. The interface was free of discontinuities, microcracks and
microvoids. There was a distinct interface of Mo/Cu in the cross-
sectional backscatter electron image with a magnication of 10,000.
This result was consistent with the previous work [1]. It was the typical
bonding example between two metals with the low inter-solubility,
which is immiscible phases in the solid state.
Fig. 4b shows a high-resolution TEM lattice image of the interfacial
layer. There were some dislocations in Cu area, which can be distin-
guished by crystallographic orientation of dislocation boundaries. A re-
gion of interdiffusion with about 10 nm in width was shown at the
interface, which shows the diffusion bonding of Mo and Cu. Therefore,
in view of the mechanism of metallic bond [21] and solid solution
strengthening, the interfacial strength was enhanced.
4. Conclusion
In summary, by diffusion-rolling procedure, a CuMoCu sheet with
a thickness of 350 mand a MoCu alloy sheet with Cu matrix contain-
ing uniformly distributed brous Mo were fabricated. With diffusion
bonding initially, a primary sandwich sheet is achieved. The following
plastic deformation by rolling potentially provides more opportunity
for the establishment of atom-to-atom bond between two pieces, and
the interfacial strength was enhanced. The bond mechanism of
diffusion-rolling processed MoCu involves metallic bond and solid so-
lution strengthening.
Acknowledgment
This work was nancially supported by the National Natural Science
Foundation of China (No. 51274246).
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