ISSN (Print): 0974-6846

ISSN (Online): 0974-5645

Indian Journal of Science and Technology, Vol 11(28), DOI: 10.17485/ijst/2018/v11i28/130792, July 2018

Enhancement of Mechanical Properties of Bulk

Copper Processed by Room Temperature
Rolling and Cryorolling
Ravi Kumar1*, Manik2 , Bhagel Singh2 and Jasbir Singh Gill1
1
Department of Mechanical Engineering, Chandigarh University, Gharuan Mohali – 140413, Punjab, India; ravipaul.
iit@gmail.com, jsgill.cgc@gmail.com
2
Department of Aerospace Engineering, Chandigarh University, Gharuan Mohali – 14041, Punjab, India;
manikasharma786@gmail.com, singh92bhagel@gmail.com

Abstract
Objectives: In the present work, we have examined and reported the mechanical and microstructures properties of bulk
Cu subjected to Room Temperature Rolling (RTR) and Cryorolling (CR) in Liquid Nitrogen temperature (LN2). Samples
deformed plastically to obtain 90% Reduction in Area (RA). Methods/Statistical analysis: The mechanical properties of
samples at room temperature rolling and cryorolled samples investigated by tensile testing and hardness measurement.
Brittle type of fracture was identified for 90% RA cryorolled samples from fractography analysis, whereas the presence of
the small dimples in the fractured surfaces of Room Temperature Rolled (RTR) tensile specimens shows a ductile failure.
Findings: The increase in tensile strength is due to the refinement of the grains due to collective effect of inhibition of
dynamic recovery and the recrystallization processes, an increase of the high density dislocations in the cryorolling. The
grain size refinement has been confirmed by TEM analysis. Application/Improvements: Cryorolled samples with 90% RA
show tensile yield strength (380 MPa) with an elongation only ~3.2%. The enhancement in yield strength of the cryorolled
samples were found more compared to the Room Temperature Rolled (RTR) samples (YS = 230 MPa).

Keywords: Cryorolling (CR), Electron Microscopy, Room Temperature Rolling (RTR), Tensile Yield Strength, Ultrafine
Grains, Work Hardening

1. Introduction tion of material and cost factor. Thus, it is very difficult

It is well recognized that there is a huge technological
interest in bulk-size ultrafine grain material because
of superior mechanical properties1-3. Sever Plastic
Deformation (SPD) processes such as High Pressure
Torsion (HPT)4, Equal Channel Angular Pressing
(ECAP)5, are used to make bulk ultrafine grained met-
als for the functional and the structural applications.
However, the majority of these require very sever plas-
tic deformation with the strains higher than unity. Major
problems in SPD techniques are that it needs sever plastic
strain, costly tooling, design difficulties, low produc-
to be used for manufacturing applications. Metal with
Ultrafine grain such as6, and alloys of Cu, Al are obtained
from its bulk metals/alloys by deforming them plastically
at low temperatures using cryorolling. Plastic deforma-
tion of metals and alloys in liquid nitrogen temperature
suppresses the dynamic recovery and the recrystalliza-
tion; and the concentration of accumulated dislocations
increases to very high steady state level.
It is the arrangement of ultrafine and nanocrystalline
grains in pure Aluminium and Cu by the process of cryor-
olling followed by the short term annealing7,8. Microstructure
refinement brings about higher mechanical properties

*Author for correspondence

 Enhancement of Mechanical Properties of Bulk Copper Processed by Room Temperature Rolling and Cryorolling

such as improved strength and toughness9. Ultrafine grain 2.2  Microstructure Analysis
materials with grain size of less than 500 nm, in general
Chemical analysis was performed by the optical emis-
have better mechanical properties in terms of yield tensile
sion spectrometer TJA 181/81 (chemical composition as
strength than their coarse grained counterparts. But, one of
shown in Table 1). Microstructure analysis completed
the major problems associated with ultrafine grain materials
by the optical microscopy, XRD analysis and the TEM
for structural applications is its low ductility that might be
investigation. Optical microstructures were analyzed by
connected to the intrinsic properties of material10.
LEICA DMI 5000 M optical microscope with polarized
Therefore, it increases the work hardening rate and
light. XRD analysis of the as received annealed, room tem-
correspondingly higher strength as reported in literature11.
perature rolling and cryorolled samples was performed by
Copper is the metal with good combination of mechanical
Bruker AXS D8 instrument with Cu Kα radiation. TEM
and corrosion resistant properties for industrial applications.
analysis was carried out on FEI Technai 20 G2S - Twin
These mechanical properties further can be improved by
transmission electron microscope operated at 200 kV.
rolling at low temperature for high strength industrial appli-
TEM sample was prepared on the plane in rolling direc-
cations. Commercial grade bulk copper is extensively used
tion. Electro polishing was carried out by using FEI twin
in manufacturing of marine fittings, precision screws, auto-
jet electro polisher with in a solution of methanol + 10%
mobile and electrical components. Therefore, aim of present
nitric acid at -30°C temperature. Fractography exami-
study is to examine the collective effect of work hardening
nation after tensile testing carried out by the scanning
rate and the dynamic recovery of pure Copper deformed by
electron microscope (SEM) ZEISS, 51-ADD0048.
the room temperature rolling and the cryorolling on tensile
properties and the microstructure evolution. Table 1.  Chemical composition of alloy used in
present study
2.  Materials and Methods Components Zn Al Ni Mg Cu
wt.% 0.005 0.001 0.001 0.002 Balance
Commercially available bulk pure Cu plate has been
taken the material in this work. Initially, the copper
was annealed at 850°C for 5h for homogenization of the 3.  Results and Discussion
microstructures. Cryorolling was done in multi pass by
dipping the samples in container containing liquid N2. 3.1  Microstructural Investigation
Before starting the rolling the bulk rectangular specimens The XRD patterns of starting received annealed, room
(cross sectional area = 25×5 mm) were dipped under temperature rolling and cryorolled copper are shown in
liquid N2 until reaches saturation temperature of liquid Figure 1. It is seen that with same reduction in area 90%,
nitrogen. Reduction in Area (RA) per pass was at ~2.5% peak intensity of (200), (220) and (311) reduce and breadth
and many passes were given to obtain maximum reduc- of the peak increased for the room temperature and CR
tion. In between every passes the specimen was dipped in samples respectively. The X-ray broadening of peak is due
liquid nitrogen for sufficient period to obtain saturation to the collective effect of structural improvement (finer
temperature. Room temperature rolling was performed crystallite size) and raise in the residual strain12; whereas,
on same size sample. the intensity of peak (222) increased, and it is also broad-
ened with RA. This clearly shows the preferred orientation
2.1  Mechanical Properties of the grains along (222) with the RA.
Size of the average grain of the starting annealed
Mechanical properties were investigated by per-
specimen was observed from the optical microstruc-
forming tensile testing at a constant strain rate
ture, is shown in Figure 2(a). The presence of equiaxed
(5 × 10 - 4 S - 1) and Vickers hardness for both samples.
grains found with a regular grain size of 200 µm, calcu-
Sample for tensile testing was machined along the plane
lated by line intercept technique. Many twins can be seen
parallel to rolling direction. Samples were set according
from optical micrograph (Figure 2a). The optical micro-
to ASTM E8 standards having 12.5 mm gauge length.
graphs of RTR and CR specimens are also shown in same
To take Vickers hardness, minimum three readings were
Figure 2. Intersecting slip bands may be seen because of
taken with a load of 5 kg with dwell time of 15 s.

2 Vol 11 (28) | July 2018 | www.indjst.org Indian Journal of Science and Technology

Figure 1.  XRD patterns of copper of (a) starting received
annealed (b) RTR-90% RA (c) CR-90%RA.
Figure 2.  Optical micrographs of copper (a) starting
received annealed (b) RTR-90% RA (c) CR-90% RA,
specimen.
plastic strain in Figure 2b and Figure 2c. But the optical
micrographs showed tremendously deformed grains and
not possible to observe the grain boundaries at all. Therefore,
average crystallite size of the RTR and CR samples was cal-
culated by X-ray peak broadening from 3 major peaks.
However, the sample after deformation up to 90%
RA, crystallite size was calculated to be 600 nm for RTR.
Whereas, cryorolling with deformation up to 90% RA,
the sample characterized by elongated grains and corru-
Vol 11 (28) | July 2018 | www.indjst.org
Ravi Kumar, Manik , Bhagel Singh and Jasbir Singh Gill
Figure 3.  TEM micrographs of CR-90% (a) bright field
image of dislocation cells/ substructures with deformation
twins (b) SEAD pattern from the central region of image 3a.
gated boundaries. Crystallite size of cryorolling with 90%
RA sample was calculated to be 100 nm by XRD data.
Therefore, it is observed that with increase in the percent-
age of RA, the crystallite size decreases and lattice strain
increases. However, the dynamic recovery suppression in
the LN2 temperature preserve the very high density of
the dislocations, which might act as large number of sites
for recrystallization to create fine grain structure13. XRD
grain size estimation is usually not reliable to compute
crystallite size beyond 50 nm. Therefore, TEM analy-
sis was performed to validate the grain size refinement
achieved by CR process. The bright field TEM micro-
graphs with Selected Area Diffraction (SAED) pattern of
CR sample after reduction up to 90% RA are shown in
Figure 3. Extremely deformed structures with large den-
sity dislocations may also be seen from Figure 3a. The
sub structural grains (size of ~100 nm) and deformation
twins (as indicated by arrow marks) may be seen in the
TEM image in Figure 3a. Selected area diffraction pattern
(Figure 3b) was observed with an aperture size of 500
nm within the central region of the micrograph (Figure
3a). The SAED ring pattern clearly shows that the sizes of
average grain are in nanometer level with 90% reduction
in area under liquid nitrogen temperature. It is observed
from bright field micrograph of the CR sample that a lot
of fine dislocation cells/substructures may be observed.
The large equiaxed dislocation cells structure after CR up
to 90% RA can be seen in Figure 3a. These cells/ substruc-
tures further subdivided into cell blocks by development
of dense dislocation walls with increasing strain14. The
dislocation density of the CR sample enhanced with
increase in the % reduction in area.
Indian Journal of Science and Technology 3
 Enhancement of Mechanical Properties of Bulk Copper Processed by Room Temperature Rolling and Cryorolling
3.2  Mechanical Properties
3.2.1 Hardness
Vickers hardness in the starting annealed material was
found to be 0.44 GPa. Maximum RA achieved by cry-
orolling was 90%, and consequently measured hardness
values is 1.61 GPa. We have already examined that there
is an immense grain size refinement produced by cryor-
olling, which cannot be achieved by room temperature
cold rolling. Cryorolling (CR) of the alloys and metals
under the cryogenic temperatures suppresses the rate
of dynamic recovery and hence the recrystallization15.
Accumulated dislocations density gets its maximum
saturation level by highest possible reduction in area.
Therefore, materials reach strain hardened to its maxi-
mum level with maximum possible RA. The CR material
has ultrafine-grain like substructures by means of grain
boundaries with low angle16 than room temperature cold
rolling. Therefore, grain size refinement takes place in CR
technique. Thus, the enhance in hardness is not only due
to strain hardening in the material but also because of
grain size reduction17. In fact, enhancement in hardness
was possibly dominated by the huge grain size refinement.
3.2.2 Tensile
Tensile mechanical behavior of starting received annealed,
Room Temperature Rolled (RTR) and the Cryorolled
(CR) samples are shown in Figure 4. It is found that
Yield Strength (YS) and Ultimate Tensile Strength (UTS)
of the starting received annealed specimen were 75 and
182 MPa, respectively. After RTR up to 90% RA, YS and
UTS were found to be 230 and 340 MPa, respectively. The
tensile strength UTS and Yield strength YS of the same
material with maximum reduction (90% RA) under LN2
were found to be 380 and 430 MPa, respectively. High
plastic deformation at sub-ambient temperature results
Figure 4.  Engineering stress-strain curves of (a) starting
received annealed (b) RTR with 90% and CR- 90% RA.
4 Vol 11 (28) | July 2018 | www.indjst.org
in suppression of dynamic recovery, promotion of twin
activity, higher dislocation density, and hence, it is esti-
mated a higher strength accompanied by good ductility.
Decreased value of the stacking fault energy restricts dislo-
cation movement by slip, and hence twinning mechanism
is preferential for plastic deformation. Thus, it is observed
to improve work hardening rates and origin the imme-
diate enrichment in the strength and the ductility. Low
stacking fault energy material have better grain refine-
ment and improved mechanical properties compared to
high stacking fault energy alloys18. The elongation % of
the starting received material was 35% by an average size
of grain 200 μm (Figure 2a). The ductility was decreased
to ~3.2% corresponding to its UTS of 430 MPa with 90%
RA by cryorolling. It is a universal phenomenon found in
highly deformed metals and alloys because of inverse rela-
tionship between strength and ductility. Hence although
tensile YS enhanced to a high value (380 MPa), due to its
very low ductility, the material cannot be useful for struc-
tural applications. Therefore, it is required to compromise
the tensile strength a bit to enhance the elongation to get a
best alliance of the strength and ductility.
3.2.3  Fractography Analysis
The fractured surface of the tensile sample after tensile test
was examined under SEM and the fractographs taken from
the different samples are shown in Figure 5. The presence
of dimple marks in the room temperature rolling sample
Figure 5.  Fracture surface morphologies of tensile samples
of (a) starting received annealed (b) RTR-90% RA (c) CR-
90% RA, sample.
Indian Journal of Science and Technology

indicates a ductile type of fracture. With 90% reduction
in area in cryorolling, the dimple marks size decreased,
because of the increase in brittleness because of the refine-
ment in grain and the work hardening connected with the
sever plastic deformation19 as shown in Figure 5 (c). The
Cryorolled sample with 90% RA shows approximately
brittle appearance fracture with a few number of small size
dimple marks in the fractograph (Figure 5c).
4. Conclusion
Ultrafine grain copper sample was produced from the
commercially bulk copper by rolling at LN2 tempera-
ture. Systematic examination of microstructure and the
mechanical properties were made. Based on the results
obtained and their analysis, the following conclusions can
be drawn.
• CR samples with 90% RA show highest value of
mechanical properties (YS-380 MPa and UTS-430
MPa) with a ductility of 3.2 % than Room Temperature
Rolling (RTR). It is due to the grain size refinement
by the collective effect of dynamic recovery suppres-
sion and the then recrystallization as the accumulated
dislocations density get its maximum saturation state
with highest possible reduction in area.
• With maximum 90% RA, the dimple marks size
reduced, because of the increase in brittleness due to
grain refinement and work hardening associated with
the large plastic deformation. Fractography analysis
of CR (90% RA) samples showed a brittle appearance
fracture with a few dimple marks. This is also corrob-
orated the tensile behavior of the cryorolled samples
with reduction in area.
5. Acknowledgement
The authors thankfully acknowledge the Chandigarh
University, Gharuan for the supports of this work.
Authors owe special thanks to Dr. Suhrit Mula, Assistant
Professor, IIT Roorkee for their valuable contributions in
microstructural characterizations.
6. References
1. Valiev RZ, Islamgaliev RK, Alexandrov IV. Bulk nano-
structured materials from severe plastic deformation.
Progress in Material Science. 2000 May; 45:103-89.
https://doi.org/10.1016/S0079-6425(99)00007-9.
Vol 11 (28) | July 2018 | www.indjst.org
Ravi Kumar, Manik , Bhagel Singh and Jasbir Singh Gill
2. Valiev RZ, Langdon TG. principles of equal-channel angu-
lar pressing as a processing tool for grain refinement.
Progress in Material Science. 2006 August; 51:881-81.
https://doi.org/10.1016/j.pmatsci.2006.02.003.
3. Zhilayev AP, Langdon TG. Using high-pressure torsion
for metal processing: Fundamentals and applications.
Progress in Material Science. 2008 April; 53:893-979.
https://doi.org/10.1016/j.pmatsci.2008.03.002.
4. Valiev RZ, Ivanisenko YZ, Rauch EF, Baudelet B. Structure
and deformation behavior of Armco iron subjected to
severe plastic deformation. Acta Materialia. 1996 May; 44:
4705-711. https://doi.org/10.1016/S1359-6454(96)00156-5.
5. Noda M, Hirohashi M, Funami K. Low temperature
super-plasticity and its deformation mechanism in grain
refinement of Al-Mg alloy by multi-axial alternative forg-
ing. Material Transaction. 2003 August; 44:2288-97.
https://doi.org/10.2320/matertrans.44.2288.
6. Wang Y, Chen M, Zhou F, Ma E. High tensile ductility in a
nanostructured metal. Nature. 2002 September; 419:912-17.
https://doi.org/10.1038/nature01133. PMid:12410306
7. Lee TR, Chang CP, Kao PW. The tensile behavior and deforma-
tion microstructure of cryo-rolled and annealed pure nickel.
Material Science Engineering A. 2005 May; 408;131-35.
https://doi.org/10.1016/j.msea.2005.07.045.
8. Shanmugasundaram T, Murty BS, Sarma VS. Development
of ultrafine grained high strength Al-Cu alloy by cry-
orolling. Scripta Materialia. 2006 April; 54:2013-17.
https://doi.org/10.1016/j.scriptamat.2006.03.012.
9. Bahmanpour H, Kauffmann A, Khoshkhoo MS, Youssef
KM, Mula S, Freudenberger J, Eckert J, Scattergood RO,
Koch CC. Effect of stacking fault energy on deforma-
tion behavior of cryorolled copper and copper alloys.
Material Science Engineering A. 2011 May; 529:230-36.
https://doi.org/10.1016/j.msea.2011.09.022.
10. Li XM, Stranik MJ. Effect of compositional variations on
characteristics of coarse intermetallic particles in overaged
7000 aluminium alloys. Material Science Technology. 2001;
p. 1324-28.
11. Guduru RK, Murty KL, Youssef KM. Scattergood R.O.,
Koch C.C., Mechanical behavior of nanocrystalline cop-
per. Material Science Engineering A. 2007; 463:14-12.
https://doi.org/10.1016/j.msea.2006.07.165.
12. Koch CC. Nanostructured materials: processing, proper-
ties, and applications, 2nd edition.  Norwich, N.Y.: William
Andrew Publications. 2007.
13. Koch CC, Youssef KM, Scattergood RO, Murty
KL. Breakthroughs in optimization of mechani-
cal properties of nanastructured metals and alloys.
Advanced Engineering Materials. 2005; p. 787-94.
https://doi.org/10.1002/adem.200500094.
14. Conrad H, Narayan J. The grain size softening in nano-
crystalline materials. Scripta Materialia. 2000; 42:1025-30.
https://doi.org/10.1016/S1359-6462(00)00320-1.
Indian Journal of Science and Technology 5
 Enhancement of Mechanical Properties of Bulk Copper Processed by Room Temperature Rolling and Cryorolling
15. Dao M, Lu L, Shen YF, Suresh S. Strength, strain-
rate sensitivity and ductility of copper with
nano-scale twins. Acta Materialia. 2006; 54:5421-32.
https://doi.org/10.1016/j.actamat.2006.06.062.
16. Zehetbauer M. Effects of nonequilibrium vacancies on
strengthening. P. Lukac (Ed.) Plasticity of Metals and Alloys
- Ispma 6. Trans Tech Publications, Clausthal Zellerfe. 1994;
p. 287-306. PMid:7913711 PMCid:PMC296315
17. Cizek J, Janecek M, Srba O, Kuzel R, Barnovska Z, Prochazka
I. Evolution of defects in copper deformed by high pres-
sure torsion. Acta Materialia. 2011 April; 59:2322-29.
https://doi.org/10.1016/j.actamat.2010.12.028.
6 Vol 11 (28) | July 2018 | www.indjst.org
18. Venugopal T, Prasad rao K, Murty BS. Mechanical
and electrical properties of Cu-Ta nanocomposites
prepared by high-energy ball milling. Acta Materialia.
2007 August; 55:4439-45. https://doi.org/10.1016/j.acta-
mat.2007.04.025.
19. Chartterjee Arnomitra, Sharma Garima, Sarkar A,
Singh JB, Chakravartty JK. A study on cryogenic
temperature ECAP on the microstructure and
mechanical properties of Al-Mg alloy. Material
Science Engineering A. 2012 May; 556:653-57.
https://doi.org/10.1016/j.msea.2012.07.043.
Indian Journal of Science and Technology