J. Mater. Sci. Technol., 2012, 28(3), 241248.

Analytical Investigation of Prior Austenite Grain Size Dependence of Low Temperature Toughness in Steel Weld Metal
X.F. Zhang1) , P. Han2) , H. Terasaki1) , M. Sato2) and Y. Komizo1)
1) Joining and Welding Research Institute, Osaka University, 11-1 Mihogaoka, Ibaraki, Osaka 567-0047, Japan 2) Technical Development Department, Welding Business, Kobe Steel Ltd., 100-1, Miyamae, Fujisawa, Kanagawa 2518551, Japan
[Manuscript received September 14, 2011, in revised form November 9, 2011]

Prior austenite grain size dependence of the low temperature impact toughness has been addressed in the bainitic weld metals by in situ observations. Usually, decreasing the grain size is the only approach by which both the strength and the toughness of a steel are increased. However, low carbon bainitic steel with small grain size shows a weakening of the low temperature impact toughness in this study. By direct tracking of the morphological evolution during phase transformation, it is found that large austenite grain size dominates the nucleation of intragranular acicular ferrite, whereas small austenite grain size leads to grain boundary nucleation of bainite. This kinetics information will contribute to meet the increasing low temperature toughness requirement of weld metals for the storage tanks and oshore structures. KEY WORDS: In situ observation; Prior austenite grain size; Low temperature toughness;
Intragranular nucleation; Grain boundary nucleation

1. Introduction Recently, the required low temperature toughness of weld metals used for the storage tanks to transport the crude oils and natural gases has become higher and higher due to extreme weather conditions and the stresses arising in these processes. For example, a liqueed natural gas storage tank (LNG storage) should have the ability to store LNG at the very low temperature of 162 C. Meanwhile, oshore structures have recently been constructed with larger designs and operated in colder and deeper seas to explore energy resources. Usually, the brittle fracture is considered more dangerous than the ductile fracture in the low temperature. The rapid sinking of the Titanic is a typical example, because the low temperature brittle fracture made the hull steel and the wrought iron rivets failed[1] . Thus, improving the low temperature toughness of weld metal gets very important.
Corresponding author. Ph.D.; Tel./Fax: +81 6 6879 4377; E-mail address: xfzhang@jwri.osaka-u.ac.jp (X.F. Zhang).

Grain renement is an eective means for improving the strength and lowering the ductile-brittle transition temperature of structural alloys[2,3] . Generally, the smaller the grain size, the stronger the material. In the case of the HallPetch eect, decreasing the grain size can impede dislocation movement and increase yield strength; in the same time, it also decreased microcrack size and increased the toughness[2] . It seems that decreasing the grain size is the only approach by which both the strength and the toughness of a steel are increased. However, low carbon bainitic steel with small prior austenitic grain size shows a weakening of the low temperature toughness in this study. It means that there are certainly other factors contributing to the weakening eect during bainite transformation. The aim of the present study is to address prior austenite grain size dependence of the low temperature toughness and the inuence of the nucleation and growth mechanisms of bainite ferrite on the toughness. Therefore, the 780 MPa grade high tensile strength low carbon bainitic steels were selected for

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Table 1 Chemical compositions of the investigated weld metals (in mass%) with balance Fe Sample B11 B22 B1 B2 B3 M1 M2 M3 C 0.04 0.03 0.09 0.07 0.10 0.11 0.10 0.09 Si 0.28 0.34 0.18 0.24 0.17 0.92 0.80 0.62 Mn 1.77 1.86 1.72 1.57 1.26 1.73 1.76 1.75 Ni 2.54 2.53 2.46 2.38 2.49 2.37 2.49 2.50 Mo 0.74 0.78 0.71 0.71 0.73 0.72 0.73 0.73 Al 0.004 0.004 0.008 0.008 0.008 0.068 0.046 0.036 B 0.0003 0.0003 0.0006 0.0006 0.0005 0.0026 0.0022 0.0017 N 0.0039 0.0042 0.0055 0.0055 0.0055 0.0054 0.0056 0.0055 O 0.0016 0.007 0.019 0.030 0.046 0.010 0.014 0.015

Fig. 1 (a) Schematic illustration of optical system in LSCM, (b) thermal cycle applied to the weld metals

investigation. For a reference, the martensitic steels were also taken into account. To better understand it, an advanced observation system, which combines an infrared image furnace with laser scanning confocal microscopy (LSCM), was developed to direct tracking of the morphological evolution at the micrometer scale under a rapid heating and cooling cycle. This technique has made it possible to identify microstructural changes at any temperature in real time. Finally, the results were compared and analyzed with previous reports in order to provide further insight into the correlation of grain size with the low temperature toughness. 2. Experimental The test materials were low carbon submerged arc weld (SAW) metals with varied oxygen content. In order to obtain the weld metals with less oxygen content, gas tungsten arc welding (GTAW) method was also used in this study. The chemical compositions of the weld metals used in this investigation are shown in Table 1. The SAW samples of B1, B2, and B3 represent the bainitic weld metals, while those of M1, M2, and M3 characterize the martensitic weld metals. The GTAW weld metals with bainitic microstructure were marked as B11 and B22. The objectives were to determine how oxygen content might aect the prior austenite grain size and the low temperature toughness. LSCM system was used to in situ observe morphological development of grain growth and phase transformation, as shown in Fig. 1(a). De-

tails of this system have been described elsewhere[4,5] . The specimen was machined into 5 mm in diameter and 1 mm in height, and the observed plane was mirror polished. Then, this disc sample was set in the infrared image furnace and continuously heating and cooling along a heat history, as displayed in Fig. 1(b). The atmospherics was lled with high purity argon shielding gas after evacuating to 1102 Pa. The LSCM images were recorded in the time resolution of 0.03 s throughout the thermal cycle. The samples were also submitted to the Charpy V-notch impact test for impact toughness analysis. The test temperature was 60 C. Furthermore, to detect the chemical compositions and particle diameter distribution of the inclusions, electron probe microanalyzer with energy dispersive X-ray spectroscopy (EPMA-EDX) was used in this study. 3. Results and Discussion Fig. 2 displays the relationship among the oxygen content, prior austenite grain size, and absorbed energy. More than one samples were carried out for impact test, and the detailed absorbed energy data are displayed in Table 2. The average absorbed energy data were used in Fig. 2. For martensitic weld metals, the prior austenite grain size decreases with increasing oxygen content, whereas the absorbed energy increases. It means that increasing the oxygen content can inhibit the austenite grain growth and improve the low temperature toughness. It also suggests that decreasing the grain size can decrease microcrack

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Table 2 Detailed absorbed energy data, oxygen content, and grain size of the investigated weld metals Sample B11 B22 B1 B2 B3 M1 M2 M3 318 227 128 111 70 58 60 70 Absorbed energy at 60 C/J 316 222 121 104 67 53 59 66 Oxygen content /106 16 70 190 300 460 100 140 150 Grain size /m 198 150 112.5 100 90 110 90 85

301 187 115 101 65 52 53 64

Fig. 2 Relationship among the oxygen content, prior austenite grain size, and absorbed energy in the weld metals

size and increase the impact toughness. This satised the knowledge described in the section 1. However, decreasing the austenite grain size does not guarantee good low temperature toughness of the bainitic weld metals. As displayed in Fig. 2, both the austenite grain size and absorbed energy decrease with increasing oxygen content in the bainitic weld metals. This indicates that increasing the oxygen content can also inhibit the austenite grain growth for bainitic weld metals, but reduce the low temperature toughness. Thus, the larger the grain size, the better the toughness. This is clearly contrary to the knowledge described in the section 1. In a word, decreasing austenite grain size can improve low temperature toughness in martensitic weld metals, while the reverse eect presents in the bainitic weld metals. To understand the above paradox, one can rst explore the eect of the oxygen content on the grain growth. Fig. 3 shows the chemical compositions of the inclusions in bainitic weld metals and their particle diameter distribution. The equivalent diameter of the inclusions was determined by EPMA-EDX analysis. The letter N represents the number of inclusions whose size is more than 0.3 m. The number of inclusions was counted in a eld of view of 96800 m2 . For B1 weld metal, the number of the inclusions is about 448 and the oxygen content is 190106 . EDX analysis shows that the inclusions are mainly AlO, MnO, SiO and AlN, as shown in Fig. 3(a). For

B2 weld metal, the number of the inclusions is about 632 and the oxygen content is 300106 . The inclusions are distinguished to be AlO, MnO, SiO and AlN, as shown in Fig. 3(b). In the case of B3 weld metal, the inclusions are similar to those of B1 and B2 weld metals. But the number of the inclusions in B3 weld metal is increased to 746 with 460106 oxygen content, as shown in Fig. 3(c). Based on the above, the number of the inclusions increases with increasing oxygen content. To make it clear, the relationship between equivalent particle diameter and the inclusions number density is characterized in Fig. 3(d). The largest number of the inclusions is presented in B3 weld metal, while the least is contained in B1 weld metal. As the Zener pinning eect described, the grain boundary migration can be retarded by the presence of particles[3,6] . Small particles act to prevent the motion of such boundaries by exerting a pinning pressure which counteracts the driving force pushing the boundaries. The second phase particles, such as non-metallic inclusions, have a strong pinning eect on grain boundary, thereby inhibiting the grain growth[3,6] . In a word, the greater the number of the inclusions, the stronger the inclusions on the grain boundary pinning eect, so the crystal grain size gets rened. Thus, the prior austenite grain size decreases with increasing oxygen content. This is also applied to the martensitic weld metals. Since low carbon bainitic steel with small grain size shows a weakening of the low temperature impact toughness as shown in Fig. 2, it means that there are certainly other factors contributing to the weakening eect during bainite transformation. Fig. 4 displays in situ morphological evolution at the micrometer scale under the cooling cycle. Fig. 4(a)(d) show the bainite transformation of B1 weld metal during the cooling process, while Fig. 4(e)(h) display the transformation of B3 weld metal. In the case of B1 metal, the nucleation site of bainite can be divided into two categories, one is grain boundary and inclusions where primary bainitic ferrite nucleates, and the other is surface of the primary bainitic ferrite where sympathetic nucleation occurs. In Fig. 4(a) and (b), the bainitic ferrite rst takes place at the inclusion and grain boundary, but the main nucleation sites are at the inclusions, as designed by the arrows. Subse-

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Fig. 3 Chemical compositions of the inclusions in bainitic weld metals and their particle diameter distribution. The letter N represents the number of inclusions whose size is more than 0.3 m. The number of inclusions was counted in a eld of view of 96800 m2 . (a) B1 weld metal, (b) B2 weld metal, (c) B3 weld metal, (d) relationship between equivalent particle diameter and the inclusions number density

quently, the secondary bainitic ferrites nucleate sympathetically on the surface of the primary bainitic ferrite, as indicated in Fig. 4(c). With the growth of bainitic ferrites, impingement events take place between the ferrite plates. In fact, this interlocking nature and the impingement of the bainitic ferrites can be clearly observed in Fig. 4(d). Usually, this intragranular bainitic ferrite is called acicular ferrite. Acicular ferrite is formed in the interior of the original austenitic grains by direct nucleation from the inclusions, resulting in randomly oriented short ferrite needles with a basket weave appearance. This interlocking nature, together with its ne grain size, provides the maximum resistance to crack propagation by cleavage. So, this microstructure is advantageous over other microstructures because of its chaotic ordering, which increases toughness[79] . Thus, the low temperature toughness of B1 weld metal is good. Based on in situ observations, it seems that intragranular transformation tends to occur in the large grains. For B3 weld metal with small grain size, the nucleation mechanism is dierent from that of B1 weld

metal with large grain size. This can be distinguished in Fig. 4(e)(h). In Fig. 4(e) and (f), the bainitic ferrite rst takes place at the grain boundary. Almost all of the bainitic ferrites nucleate at the grain boundaries, and only a ferrite nucleates at the inclusion, as shown in Fig. 4(g). Usually, the bainitic ferrite nucleated at austenite grain boundary is called grain boundary ferrite. From Fig. 4(g) and (h), it can be seen that the grain boundary ferrites grow in the same direction parallel to each other. Although the growth of the grain boundary ferrite can also cause impingement between the plates, the microstructure seems more orderly (Fig. 4(g) and (h)). Compared to acicular ferrite, the grain boundary ferrite has a smaller contribution to the low temperature toughness. Thus, the toughness of B3 weld metal is not so good as that of B1 weld metal. To better grasp the correlation of prior austenite grain size with the nucleation of bainite, B11 sample with large grain size was selected for study. Meanwhile, B1 sample with slightly larger scale inclusions was also re-examined to obtain the typical acicular

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Fig. 4 In situ observations of the morphological evolution and microstructural changes of bainitic ferrite. (a)(d) snapshots of the LSCM images for B1 weld metal, (e)(h) snapshots for B3 weld metal

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Fig. 5 In situ observations of the intragranular transformation evolution of bainitic ferrite. (a)(e) snapshots of the LSCM images for B11 weld steel with large austenite grain size, (f)(j) snapshots for B1 weld metal with slightly larger scale inclusions

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ferrite structure. Fig. 5(a)(e) display the microstructure evolution of B11 sample during cooling, while Fig. 5(f)(j) show the typical acicular ferrite formation in the sample of B1. For B11 sample with large austenite grain size, a clear polygonal grain boundary can be observed in Fig. 5(a). With decreasing temperature, intragranular bainite nucleation and growth occur (Fig. 5(b)(d)), and then impingement events take place between the ferrite plates with the growth of bainitic ferrites (Fig. 5(e)). In the case of B1 sample with slightly larger scale inclusions, the potential nucleation sites are marked in Fig. 5(f). Subsequently, the acicular ferrites nucleate on the potential sites (that is, inclusions), as shown in Fig. 5(g)(i). Finally, the randomly oriented short ferrite needles with a basket weave appearance are presented in Fig. 5(j). In addition, when the austenite grain size is large, the number density of inclusions becomes large relative to boundary nucleation sites promoting the formation of acicular ferrite at the expense of bainite. Similarly, a small grain size has a relatively large number density of grain boundary nucleation sites so bainite dominates the microstructure. Therefore, although the grain sizes of B1 and B11 weld metals with small number of inclusions are large, their toughness are better than that of B3 weld metal. These observations are consistent with the previous results[10] . Oxides in steel weld metals can initiate fracture by inuencing the microstructures. For example, the non-metallic particles can initiate brittle cracks or voids during ductile failure, both events leading to a deterioration in mechanical properties[11,12] . In the same time, the non-metallic inclusions also contribute to the formation of acicular ferrite, which improves the toughness[10,13] . Thus, changes in toughness with oxygen concentrations also need be highlighted except for prior austenite grain size dependence of low temperature toughness. In this study, excess oxygen content (from 16106 to 460106 ) prefers to decrease the toughness for 780 MPa grade high strength bainitic weld metals, while increasing oxygen content in martensitic weld metals contributes to improve the toughness. Terashima and Bhadeshia[14] reviewed the investigation of oxygen content on the toughness, and they pointed out that the absorbed energy decreases up to 100106 oxygen content and then peaks occur at 300106 in the high strength alloy (778 MPa). This non-monotonic change of the toughness is due to the microstructure changes with varied oxygen content. They considered that the microstructure is dominated by grain boundary nucleating upper and lower bainite, respectively, along with martensite. With increasing oxygen content, the acicular ferrite is absent from the microstructure, so that oxides simply serve to nucleate fracture. But for this study, the microstructures of B1, B2, B3, B11, and B22 are bainite based on in situ observations. Although the intragranular acicular ferrite is also absent from the microstructure with increasing oxygen content, the oxide

particles mainly serve to form acicular ferrite not to nucleate fracture. In Figs. 4(a)(d) and 5, intragranular nucleation is the main phase transition mechanism in the weld metals with 190106 and 16106 oxygen content, respectively. Although grain boundary nucleation is main transition mechanism in the weld metal with 460106 oxygen content (Fig. 4(e) (h)), intragranular nucleation still appears. Thus, the toughness improves monotonically as the oxygen concentration is reduced, which is dierent from the previous study by Terashima and Bhadeshia[14] . By contrast, it can be seen that the changes in grain size caused by varied oxygen content lead to the dierence of the low temperature toughness in bainitic weld metals. Above mentioned show that intragranular transformation tends to occur in the large grains, that is, the larger the grain, the easier the acicular ferrite generation. And the formation of acicular ferrites will greatly contribute to increase the toughness. As reported, the nucleation of intragranular formation acicular ferrite is aided by non-metallic inclusion, in particular oxygen-rich inclusions[10] . In this study, the inclusions in B1, B2, B3, B11, and B22 are distinguished to be AlO, MnO, SiO and AlN, which must be responsible for the nucleation of acicular ferrite. In general, compared to the grain renement, the special microstructure is more important for the improvement of the toughness. Therefore, although the grain sizes of B1 and B11 weld metals are larger than that of B3 weld metal, the low temperature toughness of B1 and B11 is better than that of B3. Thus, based on the experimental observations, intragranular acicular ferrite is regarded as the most desirable microstructure feature than the grain boundary ferrite, in view of its strength and the low temperature toughness. Finally, appropriate increase in the austenite grain sizes by composition control, which enhances the low temperature toughness of bainitic steels, is extremely important in engineering application. 4. Conclusion In conclusion, the relationship among the oxygen content, prior austenite grain size, and absorbed energy were investigated in steel weld metals. For martensitic weld metal, the austenite grain size decreased with increasing oxygen content, but the low temperature toughness increased. It conformed to the HallPetch eect. But for the bainitic weld metal, both austenite grain size and the low temperature toughness decreased with increasing oxygen content. It was ascribed to large austenite grain size dominating the nucleation of intragranular acicular ferrite, whereas small austenite grain size leads to grain boundary nucleation of bainite.
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