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Scripta Materialia 60 (2009) 76–79

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A new route to fabricate ultrafine-grained structures in carbon steels

without severe plastic deformation
Yoshitaka Okitsu,a,* Naoki Takatab and Nobuhiro Tsujic
a
Automobile R&D Center, Honda R&D Co., Ltd., 4930 Shimotakanezawa, Haga-machi, Haga-gun, Tochigi 321-3393, Japan
b
Department of Metallurgy and Ceramics Science, Graduate School of Science and Engineering, Tokyo Institute of Technology,
2-12-1-S8-8 Ookayama, Meguro-ku, Tokyo 152-8552, Japan
c
Department of Adaptive Machine Systems, Graduate School of Engineering, Osaka University,
2-1 Yamadaoka, Suita, Osaka 565-0871, Japan
Received 16 July 2008; revised 1 September 2008; accepted 1 September 2008
Available online 10 September 2008

A new route to fabricate ultrafine-grained ferritic steel without severe plastic deformation is described. A low-carbon steel sheet
with a duplex microstructure composed of ferrite and martensite was cold-rolled to 91% reduction in thickness, and then annealed at
620–655 °C. The microstructure obtained via this process was fully annealed ultrafine grains of ferrite including homogenously dis-
persed cementite particles. The mean ferrite grain sizes obtained were 0.49–0.85 lm.
Ó 2008 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Keywords: Ultrafine grain; Ferritic steels; Severe plastic deformation (SPD); Dual phases; Martensite

It has been shown that ultrafine-grained (UFG)
steels with grain sizes smaller than a few micrometers
have superior mechanical properties such as high
strength [1], good fracture toughness at low temperature
[2] and high dynamic strength (strength at very high
strain rates around 103 s 1) [3,4]. Therefore UFG steels
are expected to be new structural materials in the near
future. In many cases UFG metals have been fabricated
by so-called severe plastic deformation (SPD) processes.
However, it has been difficult to apply UFG steel sheets
to automobile body parts, because of the limited dimen-
sions of the samples fabricated by SPD processes such as
equal channel angular extrusion (ECAE) [5,6], high-
pressure torsion (HPT) [7] and ARB [1]. In addition,
the SPD processes do not seem suited to the conven-
tional mass-production routes for steels. In this paper,
the authors have found a new route to fabricate bulky
UFG steel sheets through conventional rolling and
annealing procedures without SPD. The process is char-
acterized by the starting microstructure before rolling,
which is a duplex microstructure composed of ferrite
and martensite. The process and the obtained micro-
structures are introduced and the mechanism of micro-
* Corresponding author. Tel.: +81 28 687 1360; fax: +81 28 687
1356; e-mail: Yoshitaka_Okitsu@n.t.rd.honda.co.jp
structure formation through the process is discussed in
this paper.
The chemical composition of the steel studied is
shown in Table 1. The two-phase region of ferrite and
austenite during cooling from austenite at 2 °C s 1,
which was important to obtain the duplex starting
microstructure, was clarified to be between 465 and
625 °C by dilatometry. An ingot of the steel was hot-
rolled to the thickness of 6.8 mm in the austenite region
followed by air-cooling to 540 °C and substantial cool-
ing by water spray to room temperature to obtain a du-
plex microstructure of ferrite and martensite. The hot-
rolled sheets were cold-rolled in multi-passes at room
temperature using a four-high rolling mill with lubri-
cant. The total reduction in thickness through the
cold-rolling was 91%, corresponding to an equivalent
plastic strain of 2.8. In order to obtain UFG microstruc-
tures, the cold-rolled sheets 150 mm wide and 0.6 mm
thick were annealed at various temperatures ranging
from 620 to 655 °C in a salt bath followed by water-
cooling. In addition, to fabricate a coarse-grained fer-
ritic microstructure for comparison, some of the cold-
rolled sheets were annealed at 650 °C for 57.6 ks in a
nitrogen atmosphere.
Microstructural observations for the specimens at
each stage of the process were carried out by optical
microscopy, scanning electron microscopy (SEM) and

1359-6462/$ - see front matter Ó 2008 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.scriptamat.2008.09.002
 Y. Okitsu et al. / Scripta Materialia 60 (2009) 76–79 77

Table 1. Chemical composition of the steel studied (mass%) Figure 2a shows a TEM microstructure of the 91%
C Si Mn P Si Al Nb B N cold-rolled specimen. The ‘‘F” and ‘‘M” in the figure
0.10 0.01 1.98 0.002 0.001 0.018 0.018 0.0015 0.0011
represent ferrite and martensite, respectively. In the fer-
rite region neighboring to martensite phase, a fine lamel-
lar structure with a mean spacing of 0.14 lm was
observed. Figure 2b shows a selected area diffraction
transmission electron microscopy (TEM). All micro-
(SAD) pattern taken from the ferrite region indicated
structures were observed on the longitudinal sections
by the dotted circle (b) in Figure 2a. The SAD pattern
from the transverse direction (TD) of the sheets. Elec-
shows ring-like spots, which indicates that various orien-
tron backscatter diffraction (EBSD) analysis was also
tations exist within the selected area. Similar lamellar
carried out by FEI XL30S field-emission SEM (FE-
structures have been previously observed in heavily de-
SEM) equipped with a TSL orientation image micros-
formed materials. Hansen and Jensen [8] have shown a
copy (OIM) system. The EBSD scanning was carried
lamellar microstructure with a mean spacing of about
out at the center of thickness on the TD sections, and
0.3 lm in a commercial purity aluminum heavily cold-
in a 30 lm  50 lm area at a step size of 0.1 lm on a
rolled to a strain of 5. Tsuji et al. [9] have reported an
hexagonal grid. Tensile properties were investigated at
elongated UFG microstructure with mean grain thick-
a nominal strain rate of 10 2 s 1 at room temperature.
ness of 0.21 lm in an ultra-low-carbon, interstitial-free
Tensile specimens 6 mm in gauge length and 2 mm in
(IF) steel ARB processed for 5 cycles (plastic strain is
gauge width, with the tensile direction parallel to the
4.0) at 773 K. However, it should be emphasized that
rolling direction (RD), were used. The total elongation
in the present work the ultrafine lamellar structure of
of the specimens was measured from the difference in
ferrite was obtained only after conventional 91% rolling
the gauge length before and after testing.
(e = 2.8). This fact indicates that the hard martensite
The hot-rolled specimen showed a duplex microstruc-
phase caused strain concentration in the ferrite matrix,
ture composed of ferrite matrix and martensite islands.
resulting in the formation of the fine lamellar structure
The average ferrite grain size and martensite island size
with large misorientations. Figure 2c shows a SAD pat-
observed in the optical micrograph of the hot-rolled
tern taken from the martensite region indicated by the
specimen were 2.8 and 2.2 lm, respectively. The area
dotted circle (c) in Figure 2a. The pattern is again
fraction of martensite islands was 42%. The TEM obser-
ring-like, which suggests large local misorientations in
vation confirmed that the martensite was typical ‘‘lath-
the martensite regions. As shown in Figure 1, the mar-
martensite” including a high density of dislocations.
tensite regions were also deformed to some extent in
The average thicknesses of martensite laths and blocks
cold-rolling. The strain introduced into martensite
were 0.4 and 1.5 lm, respectively. Cementite particles
should be smaller than that into ferrite matrix, because
were not observed in the hot-rolled specimen. Figure 1
martensite is much harder than ferrite. Nevertheless,
shows a SEM image of the 91% cold-rolled specimen.
the martensite regions contained large misorientations.
The ferrite matrix (dark gray region) exhibited a wavy
Ueji et al. [10] have reported that 50% cold-rolled low-
microstructure elongated roughly in the RD and bent
carbon martensite exhibited a fine lamellar structure
along the martensite islands (light gray region). This
involving large misorientations. This is thought to be
indicated that complex plastic flow had occurred and
attributed to the complicated and fine microstructure
higher strain had been introduced in the softer ferrite
of the martensite, which also involves a high density of
matrix by the existence of the hard martensite phase.
dislocations [10]. It can be concluded therefore that
Such a strain distribution between soft phase (ferrite)
the strain applied to martensite in this study was not
and hard phase (martensite) is the key factor for the for-
very large but probably sufficient to introduce large lo-
mation of UFGs in the present thermomechanical treat-
cal misorientations.
ment, as will be discussed later.

Figure 2. (a) TEM microstructure of the low-carbon steel cold-rolled

Figure 1. SEM image of the low-carbon steel cold-rolled to 91% to 91% reduction. The starting microstructure was a duplex structure
reduction. The starting microstructure was a duplex structure com- composed of ferrite and martensite. Observed from TD. (b) SAD
posed of ferrite and martensite. Observed from TD. pattern taken from ferrite. (c) SAD pattern taken from martensite.
78 Y. Okitsu et al. / Scripta Materialia 60 (2009) 76–79

Figure 3a and b show SEM images of the specimens

after annealing at 620 and 655 °C for 120 s, respectively.
The cold-rolled microstructure changed to equiaxed
UFG ferrite grains including fine cementite particles
during annealing. The cementite particles were homoge-
neously dispersed within the UFG ferrite matrix. Figure
4a and b show the boundary misorientation maps ob-
tained by EBSD measurement of the specimens an-
nealed at 620 and 655 °C for 120 s, respectively. The
bold lines show high-angle grain boundaries (HAGBs)
of which misorientation angles are higher than 15°,
while the narrow gray lines show low-angle grain
boundaries (LAGBs) of which misorientation angles
are 2–15°. The EBSD measurement revealed that the
UFGs in the annealed specimens were mostly sur-
rounded by HAGBs. The fraction of HAGBs of the
specimens annealed at 620 and 655 °C were 77.4% and
85.1%, respectively. The fraction of HAGBs gradually
increased with increasing annealing temperature. The
mean ferrite grain diameter of the specimens in the pres-
ent work annealed at 620 and 655 °C for 120 s were 0.49
and 0.85 lm, respectively.
In the present process, UFG ferritic microstructures
were obtained by relatively low plastic strain through
conventional cold-rolling. It is known that an extremely
high equivalent strain of over 4 or 5 is required to pro-
Figure 4. Boundary misorientation maps obtained by EBSD measure-
duce the UFG microstructure through SPD [11]. The ment of the low-carbon steel cold-rolled to 91% reduction, annealed at
microstructural analysis of the present cold-rolled spec- (a) 620 °C and (b) 655 °C for 120 s and cooled to room temperature in
imen revealed that large misorientations existed at the water. Observed from TD. The bold lines show high-angle grain
cold-rolled state although the rolling strain was only boundaries and the narrow gray lines low-angle grain boundaries.
2.8. Through the substantial annealing, continuous
coarsening of the finely subdivided regions together with
recovery happened to form the UFG equiaxed micro-
structure shown in Figure 3. It is difficult to distinguish discussed above, the ultrafine ferrite grains could origi-
clearly which area in Figure 3 was originally ferrite or nate from both ferrite and martensite. On the other
martensite, but according to the supposed mechanism hand, some coarse grains larger than 1 lm located in
an arc-like row seen in the lower part of Figure 3a prob-
ably formed mainly by recovery of ferrite regions such
as the elongated and bent ferrite seen in the lower part
of Figure 1. Those ferrite regions in the cold-rolled
microstructure seem to be deformed to smaller plastic
strain because of the relatively low density of surround-
ing martensite islands. Furthermore, the fact that the
coarse ferrite grains in the annealed microstructure con-
tained few cementite particles suggests that they were
originally ferrite.
In addition, it should be noted that the equiaxed
UFGs do not involve substructures within the grains,
as shown in Figure 4. That is, UFG structures equiva-
lent to fully recrystallized grains with submicrometer
grain sizes could be obtained through the present pro-
cess. Such a structure has not been achieved before. In
a previous study, when fully annealed and equiaxed
grain structures were obtained through SPD and subse-
quent annealing, the grain sizes became over 1 lm [1].
Basically the ultrafine structures with submicrometer
grain sizes formed through SPD processes are simulta-
neously deformation structures, and naturally contain
dislocation substructures inside [1] though they are sub-
divided by HAGBs on the submicrometer scale. As a re-
Figure 3. SEM images of the low-carbon steel cold-rolled to 91% sult, it has been difficult to separate the effects of grain
reduction, annealed at (a) 620 °C and (b) 655 °C for 120 s and cooled refinement and dislocation substructures on the mechan-
to room temperature in water. Observed from TD. ical properties of the UFG materials.
 Y. Okitsu et al. / Scripta Materialia 60 (2009) 76–79
Table 2. Grain sizes and tensile properties of the low-carbon steel specimens obtained by various annealing conditions
Annealing temperature Mean ferrite 0.2% offset
and time grain size (lm) stress (MPa)
625 °C, 120 s 0.49 966
655 °C, 120 s 0.85 658
650 °C, 57.6 ks 2.6 457
Besides the SPD processes, several studies have at-
tempted to achieve ultrafine grain refinement by rolling
and annealing of carbon steels with various carbon con-
tents and starting microstructures. In the cases of fer-
rite–pearlite [12], martensite [10,13] and tempered
martensite [14] as starting microstructures before roll-
ing, submicrometer ferrite microstructures have been
obtained, but the ferrite grains contained residual dislo-
cations inside. The dislocation density was decreased by
annealing at elevated temperatures, but ferrite grain
coarsening over 1 lm occurred simultaneously. In con-
trast, in this study, the grain growth of the ultrafine fer-
rite grains during annealing was considerably
suppressed. This is probably because of the high density
of finely subdivided regions in the cold-rolled micro-
structure and the fact that the ferrite grains formed dur-
ing annealing were already surrounded mostly by
HAGBs. Recently, Azizi-Alizamini et al. [15] fabricated
a ferritic microstructure with bimodal ferrite grain size
distribution by 50% cold-rolling and substantial anneal-
ing of a ferrite–martensite dual-phase microstructure.
The microstructure they obtained was a mixture of fine
grains with grain sizes of 2 lm and coarse grains with
sizes of 3–15 lm, but the strength of the material was
unfortunately not so high (tensile strength of
550 MPa). This is probably because the rolling reduc-
tion they took (50%) was smaller than the present case
(91%), and not enough to obtain uniform UFG struc-
tures like those shown in Figure 3. In addition, Furuha-
ra et al. [16] have obtained fully annealed submicrometer
ferrite with a large amount of cementite particles by 90%
cold-rolling and substantial annealing at 700 °C of high-
carbon pearlite. The microstructure they obtained
showed good balance of tensile strength and tensile
elongation (950 MPa, 14%). However, it seems to be dif-
ficult to apply pearlitic steels to automobile body parts
because of poor spot-weldability caused by the high car-
bon content of these materials.
Table 2 shows the mechanical properties of the an-
nealed specimens obtained at various conditions of
annealing in the present study. The strength of the spec-
imen with a mean grain size of 0.49 lm was about twice
that of the coarse-grained specimen with a mean grain
size of 2.6 lm. This means that significant strengthening
by grain refinement was achieved in the present UFG
steel. It is also noteworthy that the UFG steel with a
0.49-lm grain size exhibits total elongation of 8.4%,
which is considerably larger than that of the submicrom-
eter ferrite single phase structures fabricated by SPD [1].
79
Tensile strength Uniform Total elongation
(MPa) elongation (%) (%)
966 0.6 8.4
672 4.1 16.7
476 19.6 35.1
This is probably because the present UFG structures are
fully annealed grains without substructures inside.
In summary, a new route to fabricate UFG ferritic
steel sheets through conventional cold-rolling and
annealing procedures was shown. UFG ferrite–cement-
ite steel sheets with sufficient dimensions (150 mm wide
and 0.6 mm thick) could be produced by conventional
cold-rolling and subsequent short-time annealing of
the duplex microstructure composed of ferrite and mar-
tensite. A plastic strain of only 2.8 by cold-rolling was
enough to obtain the fully annealed and equiaxed
UFG ferrite with submicrometer grain sizes throughout
the specimen. The formation of the UFG ferrite was
considered to be attributed to the strain concentration
in the soft ferrite matrix and also the mild deformation
of the martensite regions in the cold-rolling. It is con-
cluded that the present process effectively provides the
UFG steel sheets with sufficient dimensions, and is not
only applicable to industrial production of UFG steel
sheets (from a practical viewpoint) but is also useful
for the further systematic study of the mechanical prop-
erties of UFG steels (from an academic viewpoint).
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