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Journal of Materials Processing Technology 211 (2011) 396401

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Journal of Materials Processing Technology


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

Inuence of shallow and deep cryogenic treatment on the residual state of


stress of 4140 steel
D. Senthilkumar a,1 , I. Rajendran a, , M. Pellizzari b , Juha Siiriainen c,2
a
Department of Mechanical Engineering, Dr. Mahalingam College of Engineering and Technology, Udumalai Road, Pollachi 642 003, Tamil Nadu, India
b
Department of Materials Engineering and Industrial Technologies, University of Trento 38050, Italy
c
Stresstech Oy, Tikkutehtaantie 1, 40800 Vaajakoski, Finland

a r t i c l e i n f o a b s t r a c t

Article history: The present research work studies the effect of cryogenic treatment on the residual stress state in
Received 8 April 2010 4140 steel. Two kinds of cryogenic treatment, namely shallow (SCT, 80 C 5 h) and deep cryogenic
Received in revised form 13 October 2010 treatment (DCT, 196 C 24 h) were carried out between quenching and tempering in conventional
Accepted 21 October 2010
heat treatment process. The results evidenced an increase in the compressive residual stress in steel
are subjected to cryogenic treatment before tempering. X-ray diffractometry revealed that residual
stresses are relieved during tempering, according to the redistribution of carbon in martensite and
Keywords:
the precipitation of transition carbides. While conventional heat treatment (CHT) and shallow cryo-
Cryogenic treatment
Residual stress
genic treatment (SCT) promote a tensile state of residual stress, DCT shows a compressive residual
Steel stress.
2010 Elsevier B.V. All rights reserved.

1. Introduction ual stress in steels is important in the component design eld.


It not only leads to improve fatigue resistance but also improves
In recent years material scientists and engineers devoted their the dimensional stability. It can also lead to improve the con-
efforts in enhancing the fatigue and impact properties of met- temporary drop in resistance against stress corrosion cracking.
als by deliberately producing compressive residual stresses in to In polycrystalline and/or multiphase materials, residual stresses
the surface of engineering materials. Residual stresses are the can be classied as microstresses and macrostresses. Almer et al.
stresses that remain within a part after the original cause of (1998) stated that the microstresses are formed due to incompat-
the stresses (external forces, heat gradient) has been removed. ibilities between grains or between phases and the macrostresses
Kalpakjian (1985) pointed out that the residual stresses remain are formed by differential plastic deformation over a large scale
along a cross-section of the component, even without the exter- relative to microstructure. Prevey (1996) explained that the macro-
nal cause. Samant and Dahotre (2008) described that these internal scopic stresses or macrostresses are extended over large distances
stresses become evenly balanced by themselves. They existed in a relative to the grain size. Macrostresses vary within the body of the
free body that had no external forces or constraints acting on its component over a range larger than the grain size of the material.
boundary. These stresses are of general interest in design and failure analysis.
Residual stresses are caused by means of load or thermal Macrostresses are tensor quantities. These stresses are determined
gradients or both. These stresses are developed during differ- for a given location and direction by measuring the strain in that
ent processes like non uniform plastic deformation during cold direction at a single point. Microscopic stresses or microstresses are
working, shot peening, surface hammering, grinding, welding, treated as scalar properties of the material. These microstresses are
phase transformations, and high thermal gradients. Over the past related to the degree of cold working or hardness, and the result of
few years, much interest has been shown in the properties and imperfections in the crystal lattice. Microstresses arise from vari-
improvement of compressive residual stress. Knowledge of resid- ations in strain between the crystallites bound by dislocation
tangles within the grains. They are acting over distances less than
the dimensions of the crystals. Hoffmann et al. (1997) pointed out
that the microstresses vary from point to point within the crystals.
Corresponding author. Tel.: +91 04259 236030/236040; fax: +91 04259 236070. They are producing a range of lattice spacing and broadening of the
E-mail addresses: kumarsen 2001@rediffmail.com (D. Senthilkumar), diffraction peak. These micro-residual stresses are generated dur-
irus rajendran@yahoo.co.in (I. Rajendran), massimo.pellizzari@ing.unitn.it
ing diffusionless martensitic transformation by dislocations and by
(M. Pellizzari), juha.siiriainen@stresstech. (J. Siiriainen).
1
Tel.: +91 04259 236030/236040; fax: +91 04259 236070. solute carbon atoms remaining in their octahedral sites without
2
Tel.: +358 014 333 0037; fax: +358 014 333 0099. diffusion.

0924-0136/$ see front matter 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.jmatprotec.2010.10.018
D. Senthilkumar et al. / Journal of Materials Processing Technology 211 (2011) 396401 397

During the last decade, cryogenic treatment techniques have RAW MATERIAL CHT
been developed and are now broadly used by industry to improve
the mechanical properties of steel components. Barron Randall
SCT
(1974) and Harish et al. (2009) studied that deep cryogenic treat-
CHEMICAL COMPOSITION ANALYSIS
ment of SAE 52100 bearing steel enhances wear resistance. Collins
DCT
and Dormer (1997) investigated the inuence of deep cryogenic
treatment on D2 cold work tool steel. Dong et al. (1998) stud-
ied the effect of DCT with respect to the microstructure of T1 HARDENING (875C, 1 hour)
high speed steels. It was proved that deep cryogenic treatment
can improve wear resistance by the precipitation of nano-sized DEEP
SHALLOW
eta-carbides in the primary martensite. It was also observed by QUENCHING IN CRYOGENIC
CRYOGENIC
Stratton (2007). Tamas Reti (2002) found that the amount of OIL (30C) TREATMENT
TREATMENT
(-196C, 24
retained austenite present in steel plays a signicant inuence (-80C, 5 hours)
hours)
on the magnitude of the residual stresses and dimensional sta-
bility. They also pointed out that the effect of retained austenite TEMPERING (200C, 1
on component performance is still a controversial issue. Some of hour)

the key factors inuencing the retained austenite transformation


include grain size, quenching temperature, hardening temperature, Fig. 1. Research methodology.
chemical composition, quenching cooling rates, and stress reliev-
ing or tempering. Retained austenite causes a decrease in tensile
and yield strength in steels and reduces the maximum achiev- treatment at 93 K, soaking for 24 h, imparts 110% improvement in
able surface compressive stresses relative to the amount of this tool life of T1 type high speed steel.
phase. Tempering at sufciently high temperature promotes the The main objective of the present work is to evaluate the
transformation of retained austenite, accompanied by increased inuence of two cryogenic treatments, namely shallow cryogenic
hardness. The contemporary loss in hardness due to the tempering treatment (SCT, 80 C for 5 h) and deep cryogenic treatment
of primary martensite partially hides the positive effect of former (DCT, 196 C for 24 h) on surface residual stress, hardness and
transformation. Alexandru and Bulancea (2002) have pointed out impact toughness of 4140 steel. It nds application in axle shafts,
that cryogenic treatments have been proposed as a useful method crankshafts, connecting rods, gears, and many other automotive
to transform retained austenite prior to tempering and to overcome components.
the problems related to austenite stabilization. The transformation
of retained austenite into martensite inuences the residual stress, 2. Material and experimental procedure
which will have an effect on the performance of the material. How-
ever, Preciado et al. (2006) stated that because of rather low amount The material considered in study was obtained in the form of
of retained austenite (less than 15%) left by conventional quenching 20 mm diameter rod. The composition of the 4140 chrome molyb-
in the microstructure of alloy steels, it appears that the cryogenic denum steel was obtained by optical emission spectroscopy (OES).
cooling would not cause additional microstructure improvements The chemical composition of the alloy considered is reported in
compared to ordinary quenching. So, cryogenic treatments are nec- Table 1. The experimental procedure adopted in the present study
essary to create a molecular change in alloy steels, making the most is schematically shown in Fig. 1. Samples were subjected to con-
retained austenite into martensite, a denser, rened mix, smaller ventional heat treatment (CHT) consisting of quench hardening in
and a more uniform than austenite. Besides, cryogenic treatment oil at 875 C for 1 h. Part of samples was then subjected to shal-
would induce the precipitation of very ne carbides of dimensions low cryogenic treatment (SCT) and deep cryogenic treatment (DCT)
less than 1 m, which occupies the microvoids so that it contributes as indicated in Bensely et al. (2007). By shallow cryogenic treat-
to the increase of both coherence and density within the metal. ment the conventionally quench hardened samples were directly
Molinari et al. (2001) studied that carbide precipitation occurs with put in a freezer kept at 80 C and soaked for 5 h to attain ther-
a higher activation energy thus leading to a higher nucleation rate mal equilibrium. Samples were then extracted and left to reach
which in turn leads to ner dimensions and a more homogenous room temperature in air. By deep cryogenic treatment, the conven-
distribution. A new phenomenon referred as tempered martensite tionally quench hardened samples were slowly cooled from room
detwinning occurred in AISI M2 steel, which showed a reduction temperature to 196 C in 3 h, soaked at 196 C for 24 h and nally
of twins after soaking at 196 C for 35 h. Deep cryogenic treat- heated back to room temperature in 6 h. All samples were nally
ment reduces the wear rate of the hot work tool steel. This result subjected to tempering or stress relieving at 200 C for 60 min.
was interpreted on the basis of increased toughness, because in X-ray diffraction techniques exploit the fact that when a metal
the presence of delamination, the ability of materials to oppose is under stress, applied or residual, the resulting elastic strains
crack propagation can really increase the mechanical stability on cause the atomic planes in the metallic crystal structure to change
the wear surface and load bearing capacity. Therefore, even if the their spacing. When a beam of X-rays is incident on a polycrys-
deep cryogenic treatment does not inuence hardness, it increases talline material, crystographic planes diffract X-rays and Braggs
both toughness and wear resistance. This is usual with no or low law n = 2dh k l sin  is satised, which was put forward by Martinez
amount of retained austenite present in steel. et al. (2003). Here n is an integer indicating the order of diffraction,
Mohan Lal et al. (2001) analyzed the inuence of cryogenic treat-  is the X-ray wave length, dh k l is lattice spacing of the h k l planes,
ment on T1 type-high speed steel and concluded that the cryogenic and  is the diffraction angle on the h k l planes.

Table 1
Chemical composition of 4140 steel (wt%).

Sample description %C % Si % Mn %P %S % Cr % Mo

Raw material 0.45 0.35 0.75 0.017 0.019 1.19 0.21


Uncertainty 0.010 0.013 0.012 0.003 0.007 0.007 0.018
398 D. Senthilkumar et al. / Journal of Materials Processing Technology 211 (2011) 396401

In this analysis, X-ray diffraction measurements were car-


Hardness (HRC)
ried out on X-stress 3000 diffractometer (Stresstech Oy/Finland)
to nd out the residual micro- and macro-stresses. This anal-
ysis has been conducted by using solid-state linear sensor

56.7

60.3
technique (MOS, Dual 512 pixels) with a gonimeter in modi-

64

66

55
60

ed psi geometry (symmetry side inclination). According to the


instructions given by Stresstech (2006), X-ray diffraction tests
Average FWHM

were carried out at room temperature in ambient air using


Cr K radiation for residual micro- and macro-stress measure-
ments. Cylindrical samples of size 15 mm diameter and 10 mm
4.48

5.67

2.59

4.71
5.20

2.80
thick were used for the measurements. The purpose of the
present investigation is to determine surface residual stress after
CHT, SCT and DCT conditions. The residual stresses can be classied
Phi = 90

into three types based on the length scale. These stresses remain
FWHM

4.46
4.47

5.18
5.22
5.19

5.81
5.62
5.58

2.58
2.59

2.79
2.78
2.82

4.69
4.72
4.71
4.50

2.60 homogenous over a large number of grains and equilibrium forces


are assumed over a large number of crystals. Here uniform strain
occurs over large distances. Macrostresses are strongly related with
macroscopic structures such as grain boundary area, grain shape,
Average
FWHM

grain size, cracks, porosity, and several other features.


4.41

5.18

5.75

2.54

2.74

4.73
De Oliveira et al. (2007) pointed out that the microstresses are
given by two distincts. The rst one remains homogenous within
one grain and the forces are assumed to be in balance among adjoin-
ing grains. The second one is homogenous over some inter atomic
distances and the internal forces remain in equilibrium around
crystalline defects. Microstresses are formed by non-uniform strain
4.37
4.43
4.43

5.11
5.29
5.16

5.91
5.66
5.67

2.52
2.55
2.54

2.66
2.76

4.76
4.72
4.72
2.80
Phi = 0
FWHM

occurs over short distances. This strain is typically within few grains
or within a single grain of type 2 and type 3, respectively. The
present study measures the micro- and macro-stresses in both lon-
gitudinal and transverse directions with respect to the bar axis
Average longitudinal

by the X-ray diffraction techniques. This technique measures the


macrostress (MPa)

+148.76 (tensile)

+49.83 (tensile)

changes in interplanar spacing caused by the residual stress. These


changes in the crystals (grains) are corresponding to the elastic
107.97

175.00

constants and the residual stress of the material. Prevey (1996)


65.26

88.53

mentioned that macrostresses produce uniform distortion of many


crystals simultaneously, shifting the angular position of the diffrac-
tion peak selected for residual stress measurement.
The data were obtained at beam angle in the range comprising
macrostress Phi = 90

between 45 and 45 and the residual stresses were found out


by using the Chi-method (-method) which is derived from the
Longitudinal

classical sin2 ( ) method. The test method for residual stress anal-
ysis by X-ray diffraction is described in SFS-EN 15305 (2008). The
107.9

80.7
67.4
47.7

146.5
208.1
170.4

134.7
159.8
151.8

52.3
45.3
51.9

89.9

86.7
109.0
107.0
(MPa)

89

diffraction peak position was found out by using cross-correlation


algorithm. Macroscopic stresses are displayed in MPa. Micro-
scopic stresses are presented as a relative result, by expressing the
peak broadening. With this kind of measurements, the absolute
Average transverse
macrostress (MPa)

microstress value in MPa would not be obtained. The behavior of


+19.43 (tensile)
+108.1 (tensile)

microstresses is more or less a scalar quantity, apart from vector


form macroscopic stresses.
125.67

184.06

The properties and parameters chosen for the experimen-


136.9

69.1

tation are Poissons ratio = 0.3, Youngs modulus = 211,000 MPa,


diffraction angle = 156.4 , and exposure time = 5 s. Due to restricted
penetration of Cr K radiation in steel (4 m), only the stresses in
Transverse macrostress

the outermost surface region could be determined. Hence, stresses


at 3 locations approximately 120 degree apart were determined
on the surface of the outer diameter of the samples. Microstruc-
Phi = 0 (MPa)

ture analysis on the CHT, SCT and DCT samples (before and after
tempering) were examined by using scanning electron micro-
141.9
134.6
134.2

137.2
123.9
115.9

148.3
193.3
210.6

119.6
107.6
97.1

19.4
18.7
20.2

68.8
66.6
71.9
Residual stress measurements.

scope. Furthermore, the tempered CHT, SCT and DCT samples were
also subjected to Charpy test at room temperature as per ASTM
standards E23 (2002).
Sample description

3. Results and discussions


tempering

tempering

tempering

tempering

tempering

tempering
CHT prior

DCT prior

CHT after

DCT after
SCT prior

SCT after
Table 2

The results of the residual stress measurements and the tough-


ness values for CHT, SCT and DCT conditions are discussed below.
D. Senthilkumar et al. / Journal of Materials Processing Technology 211 (2011) 396401 399

3.1. Residual stress (2003) and Vanvlack (1998) have explained that the tempering
reduces hardness and residual stress but it increases ductility
The micro- and macro-stresses measured in both, longitudi- and toughness and also it provides dimensional stability. Data in
nal and transverse directions, for CHT, SCT and DCT samples are Table 2, evidence a progressive reduction in compressive stresses
tabulated in Table 2. from CHT (+245 MPa), to SCT (+145 MPa) and DCT (+115 MPa),
respectively. In the case of CHT and SCT samples, tensile stresses
1. Residual stress after CHT: Compressive stresses after quenching develop after tempering. The same does not occur in DCT sample,
(137 2 MPa). where residual macrostresses remain compressive. It is observed
2. Residual stress after SCT (inuence of 80 C 5 h): No inu- that the different behavior of CHT, SCT and DCT is not caused
ence of SCT in view of the measured experimental scatter by the different amount of retained austenite, because the tem-
(125 10 MPa). pering temperature is too low to cause the transformation of
3. Residual stress after DCT (inuence of 196 C 24 h): The lower this phase into ferrite and cementite. The inuence of cryogenic
temperature and longer soaking time in DCT promote higher treatment on the martensitic microstructure seems to be the
compressive stresses (184 30 MPa). sole factor affecting present value of residual stress after temper-
ing.
Bhadeshia (2002) pointed out that the strains due to phase Huang et al. (2003) pointed out that the substantial relief of
transformations can alter the state of residual stress. It is known compressive residual stress occurred in the SCT and DCT sam-
that the martensitic transformation of a steel component puts the ples after stress relieving or tempering. The reason is due to the
surface under compression. It is argued that this is because of the occurrence of ner carbide precipitates throughout the matrix and
expansion at the surface due to formation of the lower density bct the loss of tetragonality of martensite. However, the stress relief
martensite from fcc austenite. is higher for the CHT sample, which was not subjected to sub
Present results highlight that hardness is higher in SCT and zero treatment. Grachev (2009) explained that the structural and
DCT than in CHT, of 4 and 6HRC, respectively, given in Table 2. As phase transformations can promote the process of shear forma-
proposed by Collins and Dormer (1997), the increase in hardness tion and also raise the shear resistance due to hardening of the
produced by subzero treatment is given by the transformation of alloy in the process of phase transformations that stabilize the
retained austenite to martensite. After studying most reliable the- structure, as in decomposition of super saturated solid solutions.
ories, it is inferred that through the carbon redistribution at low It should be noted that an alloy with less stable structure necessar-
temperature, DCT further promotes the formation of nucleation ily relaxes more intensely than an alloy with more stable structure.
sites for subsequent precipitation of large numbers of very ne The rate of transition of the system to a more stable state has great
carbide particles, during tempering. This effect has been claimed importance. Higher relaxation of stresses corresponds to a higher
as low temperature conditioning of martensite, which was inves- rate of transition to a more stable state. The mechanism of this
tigated by Meng et al. (1994). Our previous study reports about process responsible for stabilization of the structure has substan-
retained austenite present in the samples of 4140 subjected to CHT, tial signicance. This stress is caused by the spatial variation in
SCT and DCT after tempering, respectively, by X-ray diffraction composition and microstructure which leads to different thermal
techniques. It was reported that 6.5% austenite is retained in the contraction and also by the transformation of retained austenite
CHT sample. After SCT, the retained austenite is reduced from 6.5% to martensite. The martensite needs to be cooled below a certain
to 5.1%. Further, after DCT results in a further reduction of retained temperature to develop internal stress high enough to generate
austenite from 6.5% (CHT) to 2.7%. It is found that the SCT and crystal defects. The required long holding time suggests a local-
DCT promoted the transformation of retained austenite to marten- ized carbon distribution occurring by clustering of carbon atoms to
site and cause an increase in compressive residual stresses. The lattice defects (dislocations). The martensite becomes more super-
reduction of retained austenite from CHT samples does not develop saturated with decreasing temperature. This increases the lattice
compressive residual stress in SCT samples (prior and after temper- distortion and thermodynamic instability of the martensite, both
ing) whereas an increase in compressive residual stress is observed of which drive carbon and alloying atoms to segregate nearby
in DCT samples (prior and after tempering). This is contributed to defects. These clusters act as or grow into nuclei for the forma-
the conversion of available retained austenite to martensite. The tion of carbides when tempered subsequently. Fig. 2 shows the
process of treating samples with shallow cryogenic freezer is totally martensite microstructure of CHT, SCT and DCT samples before and
different from deep cryogenic system from the level of temper- after tempering. There are no microstructural changes observed
ature reduction. Cryogenic treatment reduces retained austenite between CHT, SCT and DCT samples before and after tempering.
and the volume decreases as treatment temperature is lowered. No appreciable differences could be detected by scanning electron
The decrease in the temperature of cryogenic treatment will lead to microscopy. However, the changes in lattice parameters are proved
more transformation of austenite to martensite and hence, greater by recent in situ neutron diffraction study indicating that the lattice
compressive residual stress will be developed. The temperature parameters a and c of the martensite behave differently during
to which the metal has been cooled is more important than the the cooling and warming-up processes. The lattice parameter a
holding time, because of the athermal character of the marten- changes with temperature almost linearly, following almost the
sitic transformation. The transformation of retained austenite to same curve during the cooling and warming-up process, indicat-
martensite is depends on the cooling temperature. Bozidar Liscic ing that it is not only a pure thermal effect. This was stated by
(1997) pointed out that the further transformation will take place Huang et al. (2003). It is inferred from the above result that carbon
only if the temperature is lowered further. However, martensite atoms segregation occurred up to 0.2%, during the deep and shallow
nish temperature (Mf ) for 4140 steel should not be lower than treatment process, which was put forward by Mittemeijer and Van
80 C, so that no difference should be observed between SCT and Doorn (1983). Because carbon atoms predominantly occupy the
DCT sample; i.e., both treatment temperatures are lower than Mf . octahedral or tetrahedral site to the defect regions mainly affecting
In light of the present difference stabilization phenomenon has the c lattice parameter. The capacity of carbon atoms to diffuse
to be taken into account. increases as the temperature rises back to room temperature. Dur-
Cryogenic treatment is not a nal heat treatment process since ing this stage carbon atoms move along short distance to segregate
successive stress relieving or tempering is absolutely necessary on the twin crystal surface or on other defects, form ne carbides of
to attain the stress relieving of brittle primary martensite. Avner diameter 2660 A leading to relief of residual stress in cryogenically
400 D. Senthilkumar et al. / Journal of Materials Processing Technology 211 (2011) 396401

Fig. 2. Microstructure of (a) CHT prior tempering, (b) CHT after tempering, (c) SCT prior tempering, (d) SCT after tempering, (e) DCT prior tempering and (f) DCT after
tempering, at 5000 magnication.

treated samples, as explained in Bensely et al. (2008) and Huang 3.2. Impact test
et al. (2003).
Microstresses were also estimated by the prediction of full The impact energy for all the samples is tabulated in Table 3.
width at half-maximum of the peaks (FWHM) from the X-ray In the light of the experimental scatter, CHT, SCT and DCT samples
diffraction patterns of processed samples. FWHM illustrate the have practically the same toughness. However, the slightly higher
microstresses and or hardness and plastic deformation. When toughness of SCT and DCT must be considered in view of the lower
the value of FWHM increases, the hardness of steel also will
be increasing. FWHM values are the average values from psi
angles. The hardness values are also reported in Table 2. The Table 3
Impact energy.
reduction of retained austenite from CHT samples increases both
compressive microstresses and hardness of SCT samples and DCT Conditions Sample Absorbed Average J
samples. This is attributed to the transformation of austenite to identication energy J
martensite. Raw material (Group A) A 31 31 1.5
The untempered samples have the highest microstresses and B 32
hardness in all the cases but the material is more brittle due to C 29
D 32
the untempered martensite. Hence tempering should be done to
reduce the brittleness by sacricing some hardness and tensile CHT (Group B) E 8 8.0 1
strength to relieve internal stress and to increase toughness and F 9
G 7
ductility. During tempering, martensite rejects carbon in the form H 8
of nely divided carbide phases. The end result of tempering is a
SCT (Group C) J 9 9.5 0.5
ne dispersion of carbides in the -iron matrix, which bears little
K 10
structural stability to the original as-quenched martensite. Hence, L 9
the microstresses and hardness of all the samples are reduced after M 10
tempering. It is observed that the SCT and DCT of both tempered and
DCT (Group D) N 10 9.5 0.5
un-tempered samples show increased hardness and microstresses O 9
when compared with the conventionally treated samples, respec- P 10
tively. Q 9
D. Senthilkumar et al. / Journal of Materials Processing Technology 211 (2011) 396401 401

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