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Materials Chemistry and Physics 132 (2012) 216–222

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Materials Chemistry and Physics


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

Welding heat input effect on the hydrogen permeation in the X80 steel
welded joints
Y.D. Han a,b , H.Y. Jing a,b , L.Y. Xu a,b,∗
a
School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
b
Tianjin Key Laboratory of Advanced Joining Technology, Tianjin 300072, China

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

Article history: In this study, the effect of microstructure at the base metal (BM), the fine grain heat affected zone (FGHAZ),
Received 22 December 2010 the coarse grain HAZ (CGHAZ) and weld metal (WM) under different welding heat input on hydrogen
Received in revised form 15 October 2011 permeation in X80 steel weldments have been investigated. Base metal showed the highest effective dif-
Accepted 16 November 2011
fusivity. With each heat input, the effective hydrogen diffusivity in FGHAZ is comparable to that of the base
metal. The effective hydrogen diffusivity in weld metal was lower than that in CGHAZ. With increasing
Keywords:
the welding heat input, the effective diffusivity in different zones of the weldment decreased correspond-
Microstructure
ingly. Non-metallic inclusions were not detected in each specimen. Constituents in microstructure under
Hydrogen permeation
Welding heat input
low heat input are likely to agglomerate during accelerated cooling. The retained hydrogen may create
Effective diffusivity an unpredictable susceptibility to hydrogen cracking at the CGHAZ even existing during service.
© 2011 Elsevier B.V. All rights reserved.

1. Introduction Due to melting and solidification, the weld metal microstruc-


ture is changed. Meanwhile, due to recrystallization and grain
The consumption of petroleum and natural gas is increasing growth in the heat affected zone (HAZ) caused by thermal cycles,
with upgraded standards of living and industrial advancements [1]. the work hardening of base metal is almost lost. Hence, they will
Hence, the usage of pipeline steels to transport oil and gas is increas- affect the local property of hydrogen embrittlement resistance at
ing correspondingly. Based on the yield strength, pipeline steels are the joints of a pressure vessel or a piping structure. During weld-
often classified into API grades by the American Petroleum Institute ing process, difficulties were experienced in controlling the heat
(Washington, DC). X80 pipeline steel is a low carbon, micro-alloyed input [5]. Heat input depends on applied voltage, current and travel
high-grade steel and a fairly new steel used as pipeline material speed. Heat input can be calculated by the following equation: heat
[2]. Due to its high-intensity and high-toughness, the material has input (J mm−1 ) = (voltage (V) × current (A))/travel speed (mm s−1 ).
the potential to be widely used in the gas transmission pipelines. The higher values of the heat input, the slower the cooling rate.
Hydrogen is one of the most common contaminants to metals. The microstructure of different zones in the welded joints can be
Hydrogen absorbed by steels, in particular, high strength steels, affected by different welding heat input and hence the hydrogen
results in considerable loss of their overall performances [3]. Hence, permeation behavior. Wang et al. [4] studied the hydrogen per-
the application of X80 steel to a piping for transporting petroleum meation behavior in different zones of a submerged arc weldment
and a pressure vessel for storing petroleum would be closely bound of TMCP steel. It was observed that the base metal has the high-
up with the hydrogen problem [4]. Diffusible hydrogen embrittles est hydrogen permeation rate. The HAZ shows the lowest values of
the steel microstructure and enhances the crack propagation. It has permeation rate. The weld metal near the fusion line yields a higher
been investigated that the concept of threshold hydrogen concen- permeation rate. Park et al. [3] investigated the effect of microstruc-
tration is crucial to understand the HIC phenomena in terms of ture on the hydrogen trapping efficiency and hydrogen induced
both hydrogen and metallurgical factors. A larger hydrogen entry cracking of X65 pipeline steel. It was observed that the hydrogen
flux to the steel leads to a faster build-up in the local concentration trapping efficiency is increased in the order of degenerated pearlite,
of hydrogen to some threshold level necessary to initiate cracking. ferrite/bainite and acicular ferrite. Results of literature search indi-
cate that no study is conducted to determine the effect of welding
heat input on the hydrogen permeation behavior of X80 welded
joints.
∗ Corresponding author at: School of Materials Science and Engineering, Tianjin Accordingly, in the present study, comparative studies of
University, Tianjin 300072, China. microstructural changes and hydrogen permeation behavior of
E-mail address: xulianyong@tju.edu.cn (L.Y. Xu). X80 welds were conducted with different heat inputs. Particular

0254-0584/$ – see front matter © 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.matchemphys.2011.11.036
Y.D. Han et al. / Materials Chemistry and Physics 132 (2012) 216–222 217

Table 1
Chemical composition of tested steel.

Element C P S Si Mn Ni Cr Al Nb V Mo

wt.% 0.04 0.10 0.001 0.19 0.18 0.24 0.020 0.19 0.072 0.001 0.267

Table 2 the cathodic side, or hydrogen entry side, of the cell. After the cur-
Average heat input (kJ mm−1 ) of X80 steel welded joints.
rent is stabilized in the extraction side, the hydrogen entry side was
No. Average heat input/kJ mm−1 galvanostatically polarized at a constant charging current (10 mA)
H1 1.8 in 1% NaCl and 5 ml acetic acid with 0.4 g L−1 Na2 S·H2 O at 25 ◦ C. The
H2 2.4 anodic current (exit side) gave a direct measure of the hydrogen
flow rate (permeation flux), is proportional to the anodic current
detected [7]. At last, the morphology of the surface after hydrogen
emphasis was placed to understand the effect of heat input on the permeation tests was observed under FE-SEM (FEI Nanosem 430).
hydrogen permeation rate.
2.3. Data analysis
2. Experimental procedures
For this study, the flux of hydrogen through the specimen was
2.1. Materials and FCAW welding measured in terms of the steady-state current density, Ip∞ (A cm−2 ),
and was converted to the steady-state hydrogen permeation flux,
The nominal chemical composition of API 5L X80 steel for weld- J∞ (mol cm−2 s−1 ), according to the following equation and results
ing are given in Table 1. X80 steel pipe (yield strength: 573 MPa, directly from the Fick’s first law:
tensile strength: 719 MPa, elongation: 23%) of 1219 mm O.D. and  
∂C Ip∞
22 mm thickness with suitable V-groove preparation was used for J∞ = −D = (1)
Fluxed-Cored Arc Welding (FCAW) welding. The butt joint geome- ∂x nF
x=L
try is illustrated in Fig. 1. The welding parameters of (FCAW) are
The permeation flux (mol cm−2 s−1 ) was defined by
listed in Table 2. The welded specimens including BM, FGHAZ,
CGHAZ and WM were cut to desired dimensions. Then the cross- Ip∞ L
section of the sample was metallographically grinded, polished and J∞ L = (2)
nF
etched for a few seconds with 4 vol.% nitric acid in 96 vol.% ethanol
where D is the hydrogen diffusion coefficient (cm2 s−1 ), Ip∞ indicates
for microstructure and hydrogen permeation tests.
the steady-state permeation current density, n is the number of
electrons transferred, F is the Faraday’s constant, L is the specimen
2.2. Electrochemical permeation
thickness and J∞ is the steady-state flux.
The effective hydrogen diffusivity, the rate-limiting step Deff can
After microstructure analysis, different zones (BM, FGHAZ,
be calculated by
CGHAZ and WM) in the welded joint was observed and labelled (see
Fig. 2(a)). Then the different zones were cut from the welded joint L2
Deff = (3)
using wire cutting. The sampling of different zones in the welded 6tL
joint for electrochemical permeation experiments was schemati-
where L is the specimen thickness and tL the time-lag in seconds for
cally shown in Fig. 2(b). They were finally machined to dimensions
0.63 saturation, which is extrapolated from the permeation curve
of 0.5 mm × 20 mm × 50 mm. These specimens were ground and
[8].
polished through sand paper and 0.3 ␮m alumina, then rinsed with
distilled water and ultrasonically cleaned in acetone, and dried
quickly by warm air blowing. The exit side of each specimen was 3. Results and discussions
electroplated with a 0.2 ␮m thick nickel layer, in order that the
background current density was minimized and significant hydro- 3.1. Microstructure analysis
gen permeation current density was obtained.
The modified ISO17081 (2004) standard method was used to In order to determine the effect of heat input on the hydrogen
measure the hydrogen permeation flux. The hydrogen permeation permeation behavior, the optical metallographs of the weldment
measurements were performed in a two cell system based on the at 4 distinct zones, namely the WM, CGHAZ, FGHAZ and BM were
Devanathan-Stachurski technique [6]. Firstly, the hydrogen extrac- examined. The microstructure of X80 welded joints under differ-
tion side (the side with a thin Ni layer) was constantly polarized at ent heat input was shown in Figs. 3 and 4, respectively. In X80 base
0.15 V vs Ag/AgCl in order to oxidize the hydrogen atoms which metal, they are ferrite (F)/degenerated pearlite (DP)/bainite (B). The
retained in the specimens. The other side of the specimen acted as unaffected base metal is characterized by the fine equiaxed fer-
rite grain with finely scattered pearlite and bainite. The structure
is produced by the thermo-mechanical controlled rolling (TMCP)
with an accelerated cooling process. The FGHAZ formed by the nor-
malization during welding appears essentially as fine ferrite grain
and bainite. The CGHAZ produced by the reheated thermal welding
cycle appears as coarse ferrite and bainite. The typical microstruc-
ture of the solidified and phase transferred weld metal displays
acicular ferrite surrounded by coarse grain boundary block ferrite.
Similar microstructure was obtained for X80 welded joints with
different heat inputs. With respect to the heat inputs, the variation
in microstructure from base metal toward the weld metal with sig-
Fig. 1. X80 steel joint geometry of the single-v-groove weld. nificant grain coarsening is shown in Figs. 3 and 4. During welding
218 Y.D. Han et al. / Materials Chemistry and Physics 132 (2012) 216–222

process, as cooling rates decreases, with higher heat input, there Table 3
The data of hydrogen permeation effective diffusivity in different zones of weld-
is an increasing amount of grain growth in the weld region, which
ments under different heat input.
produces a larger grain size and a wider weld region.
Sample location Deff (×10−7 cm2 s−1 )

Base metal 2.77


3.2. Hydrogen permeation behavior FGHAZ 2.28
Low heat input (H1)
CGHAZ 2.15
Hydrogen diffusion in metal is mainly influenced by two factors: Weld metal 1.71

one is the concentration of hydrogen at the surface and the other FGHAZ 1.91
is the hydrogen trapping sites which are various defects such as High heat input (H2) CGHAZ 1.73
Weld metal 1.62
solute atoms, vacancies, inclusions and precipitate present in the
metal [9].
In this study, hydrogen permeation test was conducted to inves-
tigate the welding heat input effect on hydrogen diffusion of X80 revealed the same observation as that reported by other researchers
welded joints. The results of hydrogen permeation behavior at dif- [4].
ferent zones of the X80 weldment are presented in Table 3. From With the same heat input, the effective hydrogen diffusivity in
Table 3 and Fig. 3, base metal with refined equiaxed ferrite and scat- FGHAZ with fine ferrite grain and bainite is comparable to that of
tered fine grain pearlite showed the highest effective diffusivity. It the base metal. This could be attributed to the similar microstruc-
is attributed to the large volume fraction of grain boundary avail- ture in FGHAZ and base metal. The effective hydrogen diffusivity
able as hydrogen high diffusivity path. The results in this study also in weld metal with acicular ferrite/block ferrite was lower than

Fig. 2. (a) Different zones (BM, FGHAZ, CGHAZ and WM) in the welded joint. (b) Schematic diagram of sampling different zones in the welded joints for hydrogen permeation
tests.
Y.D. Han et al. / Materials Chemistry and Physics 132 (2012) 216–222 219

Fig. 3. Optical microstructure of the X80 weld metal with low heat input: (a) base metal; (b) FGHAZ; (c) CGHAZ; (d) weld metal.

Fig. 4. Optical microstructure of the X80 weld metal with high heat input: (a) FGHAZ; (b) CGHAZ; (c) weld metal.
220 Y.D. Han et al. / Materials Chemistry and Physics 132 (2012) 216–222

Fig. 5. SEM morphologies and EDS spectra after hydrogen permeation test (low heat input): (a) base metal; (b) FGHAZ; (c) CGHAZ; (d) weld metal; (e) EDS spectra.

that in CGHAZ. This means that the hydrogen trapping efficiency hydrogen transport. The cooling rate of high heat input was lower
of acicular ferrite is higher than that of bainite in CGHAZ and more than that of low heat input and thus the carbon diffusion during
hydrogen can be trapped in the weld metal, thus the diffusion of cooling was sufficient to form the lamellar structure of cementites,
hydrogen is retarded. Meanwhile, the presence of retained austen- the decrease in hydrogen permeation and diffusivity in the welded
ite affords more sites for hydrogen trapping and results in a lower joints under higher heat input can also attributed to the lamellar
effective diffusivity. structure of cementites as an obstacle for hydrogen transport. In
With increasing the welding heat input, the effective diffusiv- a word, under the premise of good mechanical properties of the
ity of different zones in the weldment decreased correspondingly. welded joints, increasing the heat input can improve the hydrogen
It can be explained as follows. During welding, with increasing induced crack resistance.
the heat input, the cooling rate decreased correspondingly. Thus,
the amount of martensite decreased while bainite and retained 3.3. HIC resistance and fractography analysis
austenite increased. The higher solubility and the low diffusiv-
ity in austenite led to the higher diffusible hydrogen content. The For the specimens which had undergone a standard hydro-
retained austenite and the interfaces between the M/A constituents gen permeation test, the surface of hydrogen extraction side was
existed between the acicular ferrites can significantly trap the observed under SEM. No internal cracks were observed in different
Y.D. Han et al. / Materials Chemistry and Physics 132 (2012) 216–222 221

Fig. 6. SEM morphologies after hydrogen permeation test (high heat input): (a) FGHAZ; (b) CGHAZ; (c) weld metal.

zone of welded joints under different heat input. The morphologies fractions, under fluctuating temperatures and load conditions dur-
and EDS spectra were shown in Figs. 5 and 6. Non-metallic inclu- ing service.
sions, usually reported as the typical initiation sites of cracks, were
not detected in each specimen. It implies that the HIC initiation site
may be more closely related to the local enrichment of M/A agglom- 4. Conclusions
erates rather than the uniform distribution of M/A constituents [3].
Constituents in microstructure under low heat input are likely to The effects of the welding heat input on hydrogen permeation
agglomerate during accelerated cooling since the carbon enriched and hydrogen solubility were evaluated in X80 weldment using
prior-austenite in ferrite/austenite two-phase region does not have the electrochemical permeation method. The surface of hydrogen
enough time to diffuse and may result in the agglomeration of hard extraction side was also observed under SEM. Base metal with
phases. refined equiaxed ferrite and scattered fine grain pearlite showed
During welding process, due to the high temperature effect of the highest effective diffusivity. With each heat input, the effective
heat source, much hydrogen was dissolved in the weld metal. The hydrogen diffusivity in FGHAZ with fine ferrite grain and bainite is
hydrogen tried to diffuse and escape during cooling. Phase transfor- comparable to that of the base metal. The effective hydrogen dif-
mation was occurred at high temperature in weld metal because of fusivity in weld metal with acicular ferrite/block ferrite was lower
lower carbon content compared to that in the base metal. Austen- than that in CGHAZ. With increasing the welding heat input, the
ite decomposed into ferrite, pearlite, bainite and martensite. At effective diffusivity in different zones of the weldment decreased
the same time, the austenite decomposition in the base metal and correspondingly. Non-metallic inclusions were not detected in each
HAZ was not started due to the higher carbon content. When the specimen. Constituents in microstructure under low heat input
austenite in the weld metal transformed into ferrite and pearlite, are likely to agglomerate during accelerated cooling. Hence, under
the solubility of hydrogen will decrease significantly. As diffusion the premise of good mechanical properties of the welded joints,
rate of hydrogen in ferrite and pearlite is fast, it can easily trans- increasing the heat input can improve the resistance of HIC.
port from weld metal to fusion line. Because the low diffusion
rate of hydrogen in austenite, it cannot diffuse into the base metal
far from fusion line. Hence, high hydrogen concentration site was Acknowledgements
formed near the fusion line. Based on this hydrogen permeation
diffusivity and welding process analysis, the retained hydrogen The authors acknowledge the research funding by National
may create an unpredictable susceptibility to hydrogen cracking Natural Science Foundation of China (Grant nos. 50975196 and
in a welded joint at the CGHAZ even existing in small volume 50805103), Key Project in the Science & Technology Pillar Program
222 Y.D. Han et al. / Materials Chemistry and Physics 132 (2012) 216–222

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