4.4. Notch Tensile Test
The notch tensile curves and fracture morphology of X52 steel pipes at different sampling positions under air, 6.3 MPa hydrogen, and 10 MPa hydrogen conditions are shown in
Figure 9. From the tensile curves, it can be seen that, compared to the base metal, the notch tensile strength of the X52 steel base metal, girth weld, and girth weld heat-affected zone changes little in the 6.3 MPa hydrogen environment, while the notch tensile strength of the straight weld and straight weld heat-affected zone significantly decreases. This may be due to the presence of defects and stress concentration in the tensile specimens, resulting in lower tensile strength. Under the 10 MPa hydrogen condition, the notch tensile strength at all positions decreases, but the change is not significant. The reduction in cross-sectional shrinkage at all positions of the X52 steel pipe under the 6.3 MPa hydrogen condition is higher than that under the 10 MPa hydrogen condition, indicating that the material’s cross-sectional shrinkage significantly decreases with the increase in hydrogen partial pressure.
Figure 10 shows the micro-fracture morphology of the post-tensile specimens. From this figure, it is evident that under the 10 MPa hydrogen condition, the fracture edge exhibits an obvious brittle fracture, and a brittle fracture is also observed at the straight weld position and the heat-affected zone of the girth weld under the 6.3 MPa hydrogen condition. This indicates that X52 steel is at a higher risk of hydrogen embrittlement under the 10 MPa hydrogen environment.
Figure 11 displays the microstructural fracture in X52 steel pipes across different regions under varying hydrogen concentrations. The fracture surface of the X52 steel base material in an air environment (
Figure 11a) is predominantly characterized by a ductile fracture, exhibiting a large number of uniformly distributed dimples. The significant depth and size of these dimples indicate that the material possesses a high plastic deformation capability under hydrogen-free conditions. In a 6.3 MPa hydrogen environment (
Figure 11b), the density of dimples on the fracture surface decreases, with shallow dimples or quasi-cleavage surfaces appearing in localized regions (as indicated by arrows in
Figure 11b). This suggests that hydrogen introduction reduces local plasticity. Hydrogen atoms tend to accumulate at ferrite–pearlite interfaces, acting as microcrack initiation sites, which aligns with the findings in reference [
40] that “the pearlite band serves as a hydrogen diffusion barrier, whereas the ferrite band acts as the preferred diffusion path.” In a 10 MPa hydrogen environment (
Figure 11c), the fracture surface exhibits pronounced brittle characteristics, dominated by quasi-cleavage and intergranular fractures, with nearly no observable dimples. The elevated hydrogen pressure enhances hydrogen adsorption at grain boundaries, leading to significant grain boundary weakening. This observation correlates well with the experimental data in
Table 6, where the cross-sectional reduction rate markedly decreases (from 0.30 to 0.37) under a 10 MPa hydrogen environment.
The fracture surface of the straight weld zone exhibits a mixed morphology of dimples and cleavage due to welding residual stress and micro-defects such as pores and inclusions (
Figure 11d). Under a hydrogen environment at 6.3 MPa, the proportion of cleavage areas significantly increases, with cracks propagating along the weld centerline (as indicated by the arrow in
Figure 11e). This phenomenon may be attributed to the high hardness of the weld zone (with a hardness value of 202.8 HV at the center of the straight weld, as shown in
Table 4) and its banded structure. At 10 MPa hydrogen pressure, the fracture surface becomes entirely brittle, and the crack propagation path exhibits bifurcation characteristics (
Figure 11f), indicating that increased hydrogen pressure further reduces the fracture resistance of the weld. The non-uniformity of the microstructure in the heat-affected zone of the straight weld (
Figure 6) results in varying sensitivities to hydrogen embrittlement. Under a 6.3 MPa hydrogen environment, intergranular cracking is observed on the fracture surface (
Figure 11h), consistent with the findings in reference [
25] that the pearlite–ferrite non-banded structure in the HAZ offers weak resistance to hydrogen diffusion. At 10 MPa hydrogen pressure, the fracture surface displays continuous cleavage steps (
Figure 11i), suggesting an accelerated hydrogen-induced crack propagation rate.
The fracture surface of the circumferential weld in an air environment is predominantly characterized by dimples; however, the size of these dimples is smaller than that observed in the base material (
Figure 11j). This difference may be attributed to the formation of acicular ferrite during the welding process (
Figure 7). In a hydrogen environment, the dimple morphology is progressively replaced by cleavage surfaces. Notably, under a 10 MPa hydrogen pressure, secondary cracks extending along the welding direction emerge on the fracture surface (
Figure 11k), which highlights the hydrogen enrichment effect in the high-stress regions of the circumferential weld. The heat-affected zone (HAZ) of the circumferential weld exhibits ductile fracture characteristics similar to those of the base material in an air environment (
Figure 11m). However, under a 6.3 MPa hydrogen pressure, localized cleavage surfaces begin to appear (
Figure 11n), and at 10 MPa hydrogen pressure, the HAZ becomes entirely brittle (
Figure 11o). According to the data presented in
Table 6, the reduction in the area for the HAZ of the circumferential weld in a 10 MPa hydrogen environment is only 7.23%, significantly lower than 16.74% observed for the base material. This discrepancy suggests that the HAZ has a higher susceptibility to hydrogen embrittlement, potentially due to the hydrogen trapping effect at the coarse austenite grain boundaries within the HAZ (
Figure 7).
The relevant mechanical properties of the material can be obtained through tensile curves and fracture measurements, as shown in
Table 6.
Figure 12 can be derived from the data presented in
Table 6. As shown in
Figure 12, compared with the air environment, the notch tensile strength and cross-sectional shrinkage of the material are significantly reduced under hydrogen pressures of 6.3 MPa and 10 MPa.
According to the relevant standards and literature reviews [
49,
62], the hydrogen embrittlement sensitivity can be evaluated by the mechanical properties of identical specimens exposed to hydrogen-containing environments and non-hydrogen (ambient) environments. The greater the deviation of the ratio, the higher the cracking sensitivity. Based on the results in
Table 6, the ratios of the notch tensile strength and reduction in the area between hydrogen-containing environments and air are calculated, as shown in
Figure 13. As observed from the figures, the notch tensile strength of the X52 steel at the straight weld and HAZ shows a significant decrease in hydrogen environments. The reduction in the area at the straight weld, girth weld, and girth weld HAZ is also significantly lower in both environments. The ratios of these indicators are all less than 1. Under 6.3 MPa hydrogen pressure, the reduction in the area ratios for the base metal, straight weld, straight weld HAZ, girth weld, and girth weld HAZ are 0.77, 0.51, 0.80, 0.50, and 0.52, respectively. Under 10 MPa hydrogen pressure, the reduction in the area ratios for these positions are 0.84, 0.30, 0.52, 0.41, and 0.37, respectively. The results indicate that the X52 steel pipe exhibits a higher hydrogen embrittlement sensitivity and a higher risk of hydrogen embrittlement under the 10 MPa hydrogen pressure environment.
4.5. Smooth Round-Bar Tensile Test
The results of the notch tensile tests are relatively conservative, as the stress concentration at the notch location exhibits higher sensitivity to hydrogen. To accurately investigate the sensitivity of the X52 steel pipe in hydrogen environments, smooth round-bar tensile tests were performed on the base metal of the X52 steel pipe under 6.3 MPa hydrogen pressure. The tensile curves are shown in
Figure 14. As seen from the figure, the tensile strength of the smooth tensile specimen of the X52 steel base metal fluctuates slightly in both air and 6.3 MPa hydrogen environments, indicating that the impact of 6.3 MPa hydrogen on the plasticity of the base metal is minimal, and the strain variation is also small. Macro-appearance observations of the tensile-tested smooth specimens are shown in
Figure 15, where no brittle fracture zone was observed under hydrogen exposure.
By measuring the tensile curve and fracture, the related mechanical properties of the material can be obtained, as detailed in
Table 7. It can be seen from
Table 7 that the post-fracture elongation of the smooth round-bar specimens in air and hydrogen environments is not much different. Although the post-fracture elongation in the hydrogen environment is slightly higher than that in the air environment, the reason is that the different sampling positions of the materials will lead to differences in the internal microstructure of the specimens, which further affects the tensile properties of the materials. Coupled with the testing error of the instrument, the above-mentioned abnormal result eventually occurred. It can also be seen from
Figure 14 that hydrogen has a weak influence on the post-fracture elongation of the material. Comparisons of the mechanical performance data are shown in
Figure 15.
Figure 16 indicate that the tensile strength, reduction in area, and elongation after a fracture of the smooth specimen of the X52 base metal show minimal changes.
The hydrogen embrittlement sensitivity can be evaluated by the mechanical properties of identical specimens exposed to hydrogen-containing environments and non-hydrogen (ambient) environments. The greater the deviation in the ratio, the higher the cracking sensitivity. Based on the results in
Table 7, the ratios of the tensile strength, reduction in area, and elongation after a fracture between the hydrogen-containing environments and air are calculated. As shown in
Figure 17, the ratios for the different indicators in both environments are close to one, indicating that the hydrogen embrittlement risk for the smooth specimen of the X52 base metal in a 6.3 MPa hydrogen environment is relatively low.
In order to accurately investigate the sensitivity of the X52 steel pipe’s girth weld in a hydrogen environment, smooth round-bar tensile tests were conducted on the X52 steel pipe’s girth weld under 6.3 MPa hydrogen conditions. The tensile curve is shown in
Figure 18. As seen from the figure, the tensile strength of the smooth tensile specimens from the X52 steel pipe’s girth weld shows some fluctuation in both air and 6.3 MPa hydrogen environments, but the variation is small, indicating that 6.3 MPa hydrogen has little impact on the plasticity of the base metal smooth specimens. The strain values show minimal changes under the 6.3 MPa hydrogen environment. Macroscopic observations of the fractured smooth specimens are shown in
Figure 19, where no brittle fracture zones were observed in the hydrogen environment. The relevant mechanical property indicators of the materials were obtained through tensile curve and fracture measurements, as shown in
Table 8.
Hydrogen embrittlement sensitivity can be evaluated by comparing the mechanical properties of identical specimens exposed to hydrogen and non-hydrogen (normal temperature and pressure) environments. The ratios of the tensile strength, reduction in area, and elongation after a fracture in hydrogen environments to those in air are calculated and shown in
Figure 20. It can be seen that the ratios of different indicators in both environments are close to one, indicating that the hydrogen embrittlement risk of the X52 steel base metal smooth specimens is relatively low under 6.3 MPa hydrogen partial pressure conditions.
4.6. Fracture Toughness Test
The fracture toughness tests of the X52 steel base metal under both ambient conditions and 6.3 MPa hydrogen partial pressure were conducted using the CTOD (crack tip opening displacement) method. The F-V curves at different loading levels are shown in
Figure 21. The corresponding force (F) and plastic displacement component (Vp), which is the intersection point of the F-V curve with the horizontal axis, were used to calculate the respective δ values for each sample’s shutdown point. The calculation results are presented in
Table 9.
In the formula, μ is the Poisson’s ratio, taken as 0.3; σy is the yield stress, with the actual yield strength of X52 steel pipe taken as 455 MPa; E is the Young’s modulus, taken as 2.06 × 105 MPa; Z is the notch thickness, taken as 0 mm; W is the specimen width, 24 mm; a0 is the initial crack length of the specimen, 12 mm.
Figure 21.
The P-V curves of the X52 steel base metal under different environments. (a) air; (b) 6.3 MPa H2.
Figure 21.
The P-V curves of the X52 steel base metal under different environments. (a) air; (b) 6.3 MPa H2.
Table 9.
Loading data of fracture toughness tests for X52 steel base metal.
Table 9.
Loading data of fracture toughness tests for X52 steel base metal.
Material | Test Environment | Vp/mm | P/N | δ/mm |
---|
X52 base metal | air—1 | 3.02 | 17,535 | 1.28 |
air—2 | 2.7 | 19,321 | 1.16 |
air—3 | 2.77 | 19,252 | 1.19 |
6.3 MPa H2—1 | 2.39 | 18,601 | 1.03 |
6.3 MPa H2—2 | 2.49 | 17,676 | 1.06 |
6.3 MPa H2—3 | 2.82 | 18,671 | 1.20 |
The CTOD values for the two conditions are shown in
Table 10. As the hydrogen content increases, the material’s
KQ values remain relatively unchanged. According to the pipeline steel requirements for pipeline transport, the CTOD value must exceed 0.254 mm for the pipeline to be usable. All four conditions meet this requirement. The
KQ values were calculated according to the relevant provisions in ASME B31.12, where
KQ values were calculated using F
Q values. The results show that the CTOD values of the X52 steel base metal in air and 6.3 MPa hydrogen environments are 1.21 mm and 1.10 mm, respectively; the fracture toughness
KQ values are 68.0 MPa·m
1/2 and 66.6 MPa·m
1/2, respectively. ASME B31.12 specifies that the
KQ values are related to the sample thickness, with
KIH values exceeding 55 MPa·m
1/2. The
KQ values for all four conditions fall within the standard range.
The fracture toughness tests of the X52 steel girth weld under H
2-free and 6.3 MPa H
2 environments were also performed using the CTOD method. The
F-V curves at different loading levels are shown in
Figure 22. Similarly, the force (
F) and plastic displacement component (
VP) at each sample’s shutdown point were used to calculate the respective δ values. The calculation results are shown in
Table 11.
In the Formula (1), μ is the Poisson’s ratio, taken as 0.3; σy is the yield stress, with the actual yield strength of the X52 steel pipe taken as 476 MPa; E is the Young’s modulus, taken as 2.06 × 105 MPa; Z is the notch thickness, taken as 0 mm; W is the specimen width, 24 mm; a0 is the initial crack length of the specimen, 12 mm.
The CTOD values for the two conditions are presented in
Table 12. As the hydrogen content increases, the material’s
KQ values show little change. The CTOD values for all four conditions meet the usage requirements. According to ASME B31.12, the
KQ values are calculated using
FQ values. The results indicate that the CTOD values for the X52 steel girth weld in air and 6.3 MPa hydrogen environments are 0.47 mm and 0.51 mm, respectively, and the fracture toughness
KQ values are 52.0 MPa·m
1/2 and 52.3 MPa·m
1/2, respectively. The ASME B31.12 standard states that
KQ values are related to the sample thickness, and
KIH values greater than 55 MPa·m
1/2 are required. The
KQ values for all four conditions are within the standard range.
The fracture toughness parameters of the X52 pipeline steel welds in hydrogen environments were measured and compared to those in air. The hydrogen environment was generated by on-site hydrogen charging, using a simulated soil solution as the electrolyte, with three different current densities: 1, 5, and 10 mA/cm2. A specially designed electrolytic cell mounted on a three-point bending setup was used to facilitate hydrogen charging during the monotonic loading of the samples. The measurement of ductility was based on the J0 integral. In all cases, slight changes in toughness were measured according to KQ. An increase in current density was associated with a reduction in ductility, particularly in the base metal. A more complex phenomenon was observed in the HAZ metal, where ductility slightly decreased at two current densities (1 and 5 mA/cm2), but the reduction was more pronounced at the third current density (10 mA/cm2). The hydrogen degradation effect was found to be more pronounced in the banded ferrite–pearlite microstructure, as observed through the microstructural analysis of the X52 base and HAZ metals.
The ferrite had a hardness of 154.5 HV, while the banded pearlite had a hardness of 245.5 HV. The average hardness of the X52 HAZ metal was 173 HV, with ferrite grains having a hardness of 160 HV and pearlite grains having a hardness of 212 HV. The HAZ exhibited a non-banded ferrite–pearlite microstructure, with grains of varying sizes [
25].
Fracture toughness tests were conducted on the X52 steel base metal and the HAZ under different hydrogen-charging concentrations.
Figure 23 presents the force–displacement curves of the X52 base metal in air and under all hydrogen-charging conditions. The results of the X52 base metal samples are shown in
Table 13. Regarding the base metal, the reduction in plasticity (as indicated by a decrease in
J0) was seen with an increase in current density. Compared to
J0 in air, the dispersion of the hydrogen-induced reduction in
J0 at current densities of 1 and 5 mA/cm
2 suggested a significant reduction in ductility (
Table 14). At a current density of 10 mA/cm
2, the average reduction in
J0 was greater than that at 5 mA/cm
2, but the dispersion of results can be attributed to the fact that, for a current density of 5 mA/cm
2, critical hydrogen concentrations may have accumulated at the crack tip. Higher current densities facilitate greater hydrogen absorption, with minimal impact on fracture toughness.
Figure 24 shows the force–displacement curves for the X52 HAZ metal in air and under all hydrogen-charging conditions, and
Table 15 presents the results of the X52 HAZ metal samples. Compared to the base metal, the HAZ demonstrated greater resistance to hydrogen-induced reduction in
J0. As shown in
Table 16, when a current density of 1 mA/cm
2 was applied, the change rate in
J0 was 6.4%, compared to 9.2% for the base metal. At a current density of 5 mA/cm
2, the relative reduction in
J0 for HAZ metal was 12.8%, while the base metal exhibited a relative reduction of 46.9%. Finally, for a current density of 10 mA/cm
2, the relative reduction in
J0 was more pronounced, at 33.4%.
The banded ferrite–pearlite microstructure of the X52 base metal affects hydrogen diffusion and permeation. During diffusion tests, it was found that hydrogen permeability was lower when diffusion occurred perpendicular to the bands compared to when it occurred parallel to the bands or in randomly distributed ferrite–pearlite microstructures, indicating that the pearlite layers act as barriers to hydrogen diffusion. The ferrite layers between the pearlite bands are described as preferential hydrogen diffusion paths. When hydrogen diffuses through the ferrite layers, the ferrite–pearlite interfaces become hydrogen-saturated, and hydrogen interacts with the deformation between the ferrite and pearlite bands.
Regarding the different behaviors of the X52 base metal and the X52 HAZ, there is a microhardness difference between the ferrite–pearlite bands in the X52 base metal and the ferrite–pearlite grains in the HAZ. The hardness difference between ferrite and pearlite in the X52 steel base metal is approximately 90 HV, while the hardness difference between ferrite and pearlite in the HAZ is about 52 HV. The values for the base metal suggest that there is a significant deformation gradient between the ferrite and pearlite bands, and the deformation gradient between the ferrite and pearlite grains in the HAZ appears to be enhanced by the hydrogen promotion effect at the ferrite–pearlite interfaces between the bands. The synergistic effect of hydrogen diffusion paths is increased by the banded structure and the higher ferrite–pearlite deformation gradient, which increases with hydrogen accumulation at the ferrite interface. To illustrate this, at a current density of 1 mA/cm
2, the fracture morphology is characterized by cracks tearing into strips, perpendicular to the direction of the bag-shaped texture and parallel to the ferrite–pearlite banding, as shown in
Figure 25.
The materials studied in the literature [
25] are X52 steel pipes, where the base metal has a banded ferrite–pearlite microstructure. The HAZ has a non-banded ferrite–pearlite microstructure, with pearlite grains located further from the weld, and more pronounced banding effects in areas farther from the weld. This ferrite–pearlite banding causes the base metal to be more susceptible to hydrogen embrittlement than the HAZ metal. The continuous interfaces between ferrite and banded pearlite in the X52 base metal act as hydrogen traps, as hydrogen is forced to follow the ferrite bands during diffusion. With the aid of the large deformation gradient between the ferrite and pearlite bands, the interfaces become oversaturated, further increasing the deformation gradient. In contrast to the X52 base metal, the X52 HAZ exhibits a non-banded ferrite–pearlite microstructure, with smaller microhardness differences between the ferrite and pearlite grains, and greater resistance to hydrogen reduction in
J0.