CN112666066A - Pipeline hydrogen embrittlement temperature threshold prediction method based on hydrogen diffusion dynamics and application - Google Patents
Pipeline hydrogen embrittlement temperature threshold prediction method based on hydrogen diffusion dynamics and application Download PDFInfo
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Abstract
The invention belongs to the technical field of pipeline hydrogen embrittlement temperature influence prediction, and relates to a pipeline hydrogen embrittlement temperature threshold prediction method based on hydrogen diffusion dynamics and application. The method comprises the following specific steps: determining the relation between the matrix hydrogen concentration and the temperature in the pipeline steel by adopting a hydrogen permeation current density experiment, thereby finally determining the number N of hydrogen atoms required for saturating the defect force field; determining the relation between the diffusivity and the temperature of the hydrogen atoms through molecular dynamics simulation, thereby finally determining the enrichment movement speed V of the hydrogen atoms; and determining the hydrogen embrittlement temperature threshold of the pipeline, wherein the temperature at which the N/V ratio reaches the minimum value is the temperature at which hydrogen embrittlement is most severe. The method solves the unpredictability of the influence of the temperature on the service life of the pipeline, and has great significance on the integrity management and the risk evaluation of the pipeline.
Description
Technical Field
The invention belongs to the technical field of pipeline hydrogen embrittlement temperature influence prediction, and particularly relates to a pipeline hydrogen embrittlement temperature threshold prediction method based on hydrogen diffusion dynamics and application.
Background
The information in this background section is only for enhancement of understanding of the general background of the invention and is not necessarily to be construed as an admission or any form of suggestion that this information forms the prior art that is already known to a person of ordinary skill in the art.
The hydrogen embrittlement of the pipeline steel is caused by cathodic hydrogen evolution reaction in the corrosion process, and the corrosion reaction is more severe along with the increase of the temperature, so that the hydrogen atoms which are separated out and enter the steel matrix of the pipeline are increased. It can be inferred that the base hydrogen concentration c is increasedoThe method is beneficial to the accumulation of hydrogen atoms around the defects, so that the hydrogen brittleness of the pipeline steel is enhanced, and the fracture is easier to occur.
However, the temperature increase effect on the equilibrium hydrogen concentration around the defect follows the form of the arrhenius equation as follows:
wherein sigmahydIs the hydrostatic pressure around the crack, omegaHIs the volume of the hydrogen atom component in the steel for a line pipe, kBIs Boltzmann constant, T is temperature, and ceqIs the equilibrium hydrogen concentration around the defect. Only if the filling saturates the stress concentration zone caused by the tensile stress can the hydrogen atoms continue to accumulate towards the crack tip and cause cracking. However ceqIs subjected to coAnd the effect of T in the exp () term. It is understood that as the temperature rises, coWill increase, whereas the exp () term will decrease, so the temperature pair ceqThe effect of (a) is non-linear.
In addition, the effect of temperature on the migration rate of hydrogen atoms is difficult to define. The migration rate of hydrogen atoms to the crack tip can be derived from newton's law:
wherein D is the diffusivity of a hydrogen atom, ΩHIs the component volume of hydrogen atoms, v is the Poisson's ratio of iron, KIRepresenting the stress intensity at the crack tip. Wherein the diffusivity, D, increases with increasing temperature, while the 1/T term decreases. The influence of the temperature on the velocity V of the movement of the hydrogen atoms to the crack tip is therefore also non-linear.
As described above, the inventors found that the influence of temperature on hydrogen embrittlement cannot be quantified because the conventional studies cannot determine not only the relationship between the hydrogen concentration around the crack and the temperature, but also the relationship between the hydrogen atom aggregation rate to the crack tip and the temperature.
Disclosure of Invention
In view of the problems in the prior art, the present invention aims to provide a method for predicting a pipeline hydrogen embrittlement temperature threshold based on hydrogen diffusion kinetics.
In order to solve the technical problems, the technical scheme of the invention is as follows:
in a first aspect, a pipeline hydrogen embrittlement temperature threshold prediction method based on hydrogen diffusion dynamics comprises the following specific steps:
determining the relation between the matrix hydrogen concentration and the temperature in the pipeline steel by adopting a hydrogen permeation current density experiment, thereby finally determining the number N of hydrogen atoms required for saturating the defect force field;
determining the relation between the diffusivity and the temperature of the hydrogen atoms through molecular dynamics simulation, thereby finally determining the enrichment movement speed V of the hydrogen atoms;
and determining the hydrogen embrittlement temperature threshold of the pipeline by quantifying the minimum value of the N/V ratio.
And quantifying the influence of the temperature on hydrogen embrittlement by a prediction method, and determining the threshold value of the hydrogen embrittlement temperature of the pipeline, wherein the minimum value of the N/V ratio is the temperature with the most severe hydrogen embrittlement. After the hydrogen atoms fill the stress concentration area of the saturated crack tip, namely the number of the hydrogen atoms exceeds N, the residual hydrogen atoms can continue to move to the free surface of the crack tip, and further the growth of the crack is promoted. Thus, the smaller the value of N/V, the faster the hydrogen atoms fill the stress concentration zone at the front of the crack, i.e., the more hydrogen embrittlement.
The number of hydrogen atoms N required to saturate the defect force field is also referred to hereinafter as the saturated number of hydrogen atoms in the tensile force field around the microcrack or the total number of hydrogen atoms required to saturate the filled defect force field or simply the saturated number of hydrogen atoms N.
In some embodiments of the invention, the maximum current density value i of the pipeline steel at different temperatures is obtained by a hydrogen permeation current density experiment∞Then obtaining the concentration of matrix hydrogen according to the formula (1);
wherein lzFor the actual sample thickness, F is the Faraday constant and D is the hydrogen diffusivity.
In some embodiments of the invention, the hydrogen atom saturation number N is obtained according to formula (4):
wherein the R value is a fixed value and is selected to be 160nm, v is the Poisson's ratio, aoIs the lattice constant,. alpha.zFor the actual specimen thickness, the self-determination is carried out according to the specimen selectionHIs the volume of the constituent of a hydrogen atom, KIRepresenting the stress intensity at the crack tip, determined according to experimental or engineering conditions, kBRepresenting boltzmann constant, 1.380649 × 10-23J/K。
ceqIs the equilibrium hydrogen concentration around the defect. The effect of the existing temperature on the equilibrium hydrogen concentration is non-linear. Through a hydrogen permeation current density experiment, the equilibrium current density i of the pipe at a specific temperature can be obtained∞The matrix hydrogen at a certain temperature can be obtained by the formula (3)Concentration co. So that the equilibrium hydrogen atom concentration c in a particular force field sigma can be obtainedeqCan be expressed as
Wherein sigmahydCan be expressed as
By the formula (4), for ceqIntegration is performed in the range of 0-R. The total number of hydrogen atoms N required for saturation of the filling force field-induced hydrogen atoms can be obtained within the range of 0-R.
In some embodiments of the invention, the hydrogen atom diffusivity is fitted to the temperature relationship shown in equation (3):
D＝1.5×10-7exp(-0.8×1.6×10-19/kBt) (5), wherein KBRepresenting boltzmann's constant.
In some embodiments of the present invention, the relationship between the hydrogen atom diffusivity and the temperature is determined by: the variation relation of the Mean Square Displacement (MSD) of the hydrogen atoms along with the time is obtained by calculation and is substituted into the formula (6),
where d denotes the axial direction of the model involved in the calculation, the value for bulk diffusion being equal to 3, N is the total number of hydrogen atoms, r (to) is the initial position of the H atoms, r (t)0+ Δ t) is the position of the hydrogen atom after the time interval Δ t;
the slope of the curve is the diffusivity D value at different temperatures, and the relational expression shown in the formula (5) is obtained after fitting.
The relation between the diffusion rate of hydrogen atoms and the temperature is obtained through molecular dynamics simulation, namely the hydrogen atoms are added in a body-centered cubic structure at different temperatures, the change relation of Mean Square Displacement (MSD) of the hydrogen atoms along with time can be obtained through calculation, the change relation is substituted into a formula (6) to obtain the relation shown in a formula (5), and then the relation between the enrichment movement speed V of the hydrogen atoms and the temperature can be obtained through a formula (2).
In some embodiments of the present invention, the hydrogen atom enrichment movement velocity V is related to the hydrogen atom diffusion rate as shown in formula (2):
wherein D is the diffusivity of a hydrogen atom, Ω is the volume of the hydrogen atom's constituent, v is the Poisson's ratio of iron, KIRepresenting the stress intensity at the crack tip.
In some embodiments of the invention, the temperature threshold of the pipeline steel is in the range of-10 to 60 ℃. When the temperature reaches above 60 ℃, hydrogen atoms in the pipeline can be desorbed from the pipeline, and the hydrogen embrittlement effect can be greatly reduced. Therefore, the hydrogen embrittlement threshold temperature is selected and calculated for the pipe temperature range of 60 degrees celsius or less.
In some embodiments of the invention, the pipeline steel is mechanically tested for stress intensity at the crack tip prior to being subjected to the hydrogen permeation current density test.
In a second aspect, the hydrogen embrittlement temperature threshold value prediction method based on hydrogen diffusion dynamics is applied to the fields of integrity management and risk evaluation of pipelines. The influence of the temperature on the hydrogen embrittlement of the pipeline steel is obtained through the prediction method, so that the temperature control of the pipeline steel can be realized, the service life of a pipeline at a certain temperature is predicted, and the use safety and the use planning are improved.
In some embodiments of the invention, the pipe comprises ferrite-pearlite line steel, acicular ferrite line steel, bainite-martensite line steel.
Optionally, 5LB, X42, X52, X60, X70, X80, X100, X120.
One or more technical schemes of the invention have the following beneficial effects:
hydrogen permeation current density experiment quantification temperature and pipeline steel matrix hydrogen concentration coTo obtain the equilibrium concentration c of hydrogen atoms at the tip of the crackeqFurther obtaining the total number N of hydrogen atoms required by the filling force field; amplification by molecular dynamics simulationThe dispersion rate D is related to the temperature, and the speed V of hydrogen atoms diffusing to the crack tip is obtained; the hydrogen embrittlement threshold temperature of the pipeline steel is predicted by the ratio of N/V and verified by slow-drawing experiments in NS4 solution. The method is based on hydrogen diffusion dynamics, the model theory is solid, the prediction is accurate, the unpredictability of the influence of the temperature on the service life of the pipeline is solved, and the method has great significance on the integrity management and the risk evaluation of the pipeline.
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The accompanying drawings, which are incorporated in and constitute a part of this specification, are included to provide a further understanding of the invention, and are incorporated in and constitute a part of this specification, illustrate embodiments of the invention and together with the description, serve to explain the invention and not to limit the invention.
FIG. 1 is a graph of the relationship between the hydrogen permeation current density and the temperature in example 1;
FIG. 2 is a graph of hydrogen diffusivity versus temperature for example 1;
FIG. 3 is a plot of the mean square displacement of hydrogen atoms as a function of time for example 1;
FIG. 4 is a graph showing the N/V value of the steel for a line pipe of example 1;
FIG. 5 is a device for verifying hydrogen embrittlement temperature threshold in tensile experiments;
FIG. 6 is a flow chart of a prediction method;
the device comprises a thermometer 1, a thermometer 2, a circulating medium 3, an NS4 solution 4, an air outlet pipe 5, a silica gel coating 6 and a pH adjusting pipe.
Detailed Description
It is to be understood that the following detailed description is exemplary and is intended to provide further explanation of the invention as claimed. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.
It is noted that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of example embodiments according to the present application. As used herein, the singular forms "a", "an" and "the" are intended to include the plural forms as well, and it should be understood that when the terms "comprises" and/or "comprising" are used in this specification, they specify the presence of stated features, steps, operations, devices, components, and/or combinations thereof, unless the context clearly indicates otherwise.
A specific flow of a pipeline hydrogen embrittlement temperature threshold prediction method based on hydrogen diffusion kinetics is shown in fig. 6, and the specific flow process is as follows:
determination of matrix hydrogen concentration c in pipeline steel by using hydrogen permeation current density experimentoTemperature, and thus the number of hydrogen atoms N required to saturate the defect force field,
the relation D of the hydrogen atom diffusivity D and the temperature is determined to be 1.5 multiplied by 10 through molecular dynamics simulation-7exp(-0.8×1.6×10-19/kBT), thereby finally determining the hydrogen atom enrichment movement velocity V;
by quantifying the minimum value of the N/V ratio, the temperature at which hydrogen embrittlement is most severe is determined.
The invention will be further illustrated by the following examples
Example 1
The material of the line steel was X90, and the results of the hydrogen permeation current density test are shown in FIG. 1. Obtaining the substrate hydrogen concentration according to formula (1);
the saturated number of hydrogen atoms N is obtained according to formula (4),
the R value was chosen to be 160 nm. v is the value of Poisson's ratio of 0.31, aoIs lattice constant
lzIs the actual specimen thickness. OmegaHValue of 1.99X 10-30m3。
The temperature and diffusivity relationship is shown in figure 2. The relation between the diffusion rate of hydrogen atoms and the temperature is obtained through molecular dynamics simulation, namely the relation of the change of the Mean Square Displacement (MSD) of the hydrogen atoms along with the time is obtained through calculation by adding the hydrogen atoms into the body-centered cubic structure at different temperatures and substituting the relation into the formula (6),
where d denotes the axial direction of the model involved in the calculation, this value being equal to 3 for bulk diffusion, N is the total number of hydrogen atoms, r (t)o) Is the initial position of the H atom, r (t)o+ Δ t) is the position of the hydrogen atom after the time interval Δ t. FIG. 3 shows the MSD as a function of time. The slope of the curve is the diffusivity D value at different temperatures. The formula of the diffusivity and the temperature of the hydrogen atoms can be obtained after fitting:
D＝1.5×10-7exp(-0.8×1.6×10-19/kBT) (5)
wherein k isBRepresenting boltzmann's constant.
And then obtaining the hydrogen atom enrichment movement speed V according to the relation between the hydrogen atom enrichment movement speed V and the hydrogen atom diffusion rate.
As shown in FIG. 4, the obtained N and V can be calculated to obtain a value of N/V, and the smaller the value of N/V, the faster the hydrogen atom fills the stress concentration region at the front end of the crack, i.e., the stronger the hydrogen embrittlement is. The hydrogen embrittlement of X90 is most severe at a temperature of 313K.
Example 2
The hydrogen embrittlement temperature of example 1 was verified by a tensile experiment using an apparatus for verifying the hydrogen embrittlement temperature threshold.
As shown in FIG. 5, the device for verifying the hydrogen embrittlement temperature threshold comprises an etching tank (model is DC-2006), a constant temperature layer is arranged on the side wall of the etching tank, a circulating medium 2 is introduced into the constant temperature layer, and the etching tank is connected with an air outlet pipe 4, a pH adjusting pipe 6 and a thermometer 1.
Before the tensile test, N with the purity of 99.5 percent is utilized2And carrying out oxygen removal treatment on the solution for 1 h.
After deoxidization, the pipeline steel is put into a corrosion box and immersed in NIn S4 solution 3, the two ends of the sample are provided with silica gel coatings 5, the sample is sealed on the corrosion box through silica gel, and the silica gel supports the sample and plays a role in sealing. The corrosion box is processed at constant temperature, and 5 percent CO is introduced through a pH adjusting pipe2+95％N2So as to maintain a near neutral pH environment (pH 6.6-7.1);
introducing constant-temperature liquid into the constant-temperature layer: alcohol is adopted at the temperature below 10 ℃, and purified water is adopted at the temperature above 10 ℃; the thermostatic layer controls the temperature of the NS4 solution from-20 to 50 ℃. Compared with the traditional research, the research aims at the hydrogen embrittlement research caused by the accumulation and diffusion of hydrogen around the defect at the room temperature. And the influences of effects such as creep deformation at high temperature and the like are not considered, and the hydrogen embrittlement threshold temperature phenomenon of metal parts which are mainly commonly used in long-distance pipelines and other oil and gas industries is observed.
The stretching is carried out by an ETM-105D type microcomputer control electronic universal tester, and the strain rates are all 1 multiplied by 10-6s-1. A preload of 490N was applied prior to the experiment to eliminate backlash in the reduction gears, clamps, etc.
And then stretching at different temperatures, ultrasonically cleaning the sample with a rust removing liquid after the sample is pulled off, wiping the sample with alcohol and drying the sample. And measuring the area and the elongation of the fracture of the sample, and calculating the reduction of area and the elongation of the sample. And observing the appearance of the fracture and the side surface of the sample by adopting a Scanning Electron Microscope (SEM).
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. A pipeline hydrogen embrittlement temperature threshold prediction method based on hydrogen diffusion dynamics is characterized by comprising the following steps: the method comprises the following specific steps:
determining the relation between the matrix hydrogen concentration and the temperature in the pipeline steel by adopting a hydrogen permeation current density experiment, thereby finally determining the number N of hydrogen atoms required for saturating the defect force field;
determining the relation between the diffusivity and the temperature of the hydrogen atoms through molecular dynamics simulation, thereby finally determining the enrichment movement speed V of the hydrogen atoms;
and quantifying the hydrogen embrittlement temperature threshold of the pipeline by quantifying the minimum value of the N/V ratio.
2. The hydrogen diffusion kinetics-based pipeline hydrogen embrittlement temperature threshold prediction method of claim 1, wherein: obtaining the maximum current density value i of the pipeline steel at different temperatures through a hydrogen permeation current density experiment∞Then obtaining the concentration of matrix hydrogen according to the formula (3);
wherein lzFor the actual sample thickness, F is the Faraday constant and D is the hydrogen diffusivity.
3. The hydrogen diffusion kinetics-based pipeline hydrogen embrittlement temperature threshold prediction method of claim 2, wherein: the saturated number of hydrogen atoms N is obtained according to formula (4):
wherein R value is 160nm, v is Poisson's ratio, aoIs the lattice constant,. alpha.zFor actual specimen thickness, ΩHIs the volume of the constituent of a hydrogen atom, KIRepresenting the stress intensity, k, of the crack tipBRepresenting boltzmann's constant.
4. The hydrogen diffusion kinetics-based pipeline hydrogen embrittlement temperature threshold prediction method of claim 3, wherein: the hydrogen atom diffusivity is fitted to the temperature in a relationship shown by the formula (5):
D＝1.5×10-7exp(-0.8×1.6×10-19/kBt) (5), wherein KBRepresents the boltzmann constant;
preferably, the relation between the hydrogen atom diffusivity and the temperature is determined by: the variation relation of the Mean Square Displacement (MSD) of the hydrogen atoms along with the time is obtained by calculation and is substituted into the formula (6),
where d denotes the axial direction of the model involved in the calculation, this value being equal to 3 for bulk diffusion, N is the total number of hydrogen atoms, r (t)o) Is the initial position of the H atom, r (t)0+ Δ t) is the position of the hydrogen atom after the time interval Δ t;
the slope of the curve is the diffusivity D value at different temperatures, and the relational expression shown in the formula (5) is obtained after fitting.
5. The hydrogen diffusion kinetics-based pipeline hydrogen embrittlement temperature threshold prediction method of claim 1, wherein: the relationship between the hydrogen atom enrichment movement speed V and the hydrogen atom diffusion rate is shown in the formula (2):
wherein D is the diffusivity of a hydrogen atom, ΩHIs the volume of the hydrogen atom component, v is the Poisson's ratio of iron, kIRepresenting the stress intensity at the crack tip.
6. The hydrogen diffusion kinetics-based pipeline hydrogen embrittlement temperature threshold prediction method of claim 1, wherein: the temperature threshold of the pipeline steel is in the range of-10 to 60 ℃.
7. The hydrogen diffusion kinetics-based pipeline hydrogen embrittlement temperature threshold prediction method of claim 5, wherein: and performing mechanical test on the pipeline steel before the hydrogen permeation current density experiment to obtain the stress intensity of the crack tip.
8. Use of the hydrogen diffusion kinetics-based pipeline hydrogen embrittlement temperature threshold prediction method according to any one of claims 1 to 7 in the field of pipeline integrity management and risk assessment.
9. The use of claim 8, wherein: the pipe comprises ferrite-pearlite line steel, acicular ferrite line steel, bainite-martensite line steel.
10. The use of claim 9, wherein: the pipeline steel is 5LB, X42, X52, X60, X60, X70, X80, X100 and X120.
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