CN112666066B - 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 rise of temperature, so that the hydrogen atoms which are separated out and enter a pipeline steel matrix are increased. It can be inferred that the base hydrogen concentration c is increased o Is advantageous forThe hydrogen atoms are gathered around the defect, thereby enhancing the hydrogen embrittlement of the pipeline steel and making the fracture more likely 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 σ hyd Is the hydrostatic pressure around the crack, omega H Is the volume of the hydrogen atom component in the steel for a line pipe, k B Is Boltzmann constant, T is temperature, and c eq Is the equilibrium hydrogen concentration around the defect. Only upon filling the region saturated with stress concentrations caused by tensile stress can hydrogen atoms continue to collect toward the crack tip and cause cracking. However c eq Is subjected to c o And the effect of T in the exp () term. It is understood that as the temperature rises, c o Will increase, whereas the exp () term will decrease, so the temperature pair c eq The 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, Ω H Is the component volume of hydrogen atoms, v is the Poisson's ratio of iron, K I Representing 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 a 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. Therefore, 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 more severe the 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 fill 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 the content of the first and second substances,l z for 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, a o Is the lattice constant,. Alpha. z For the actual specimen thickness, the measurement is carried out automatically according to the specimen selection H Is the volume of the constituent of a hydrogen atom, K I Representing the stress intensity at the crack tip, determined according to experimental or engineering conditions, k B Representing Boltzmann constant, taking the value of 1.380649 × 10 -23 J/K。
c eq Is 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 hydrogen concentration c of the substrate at a certain temperature can be obtained by the formula (3) o . So that the equilibrium hydrogen atom concentration c in a particular force field sigma can be obtained eq Can be expressed as
Wherein σ hyd Can be expressed as
By the formula (4), for c eq Integration 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 -7 exp(-0.8×1.6×10 -19 /k B t) (5), wherein K B Representing boltzmann's constant.
In some embodiments of the present invention, the hydrogen atom diffusivity versus 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 and the temperature of the hydrogen atoms is obtained through molecular dynamics simulation, namely the hydrogen atoms are added in a body-centered cubic structure at different temperatures in a memory, the change relation of the 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, K I Representing 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 centigrade 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 carburization current density test.
In a second aspect, the method for predicting the hydrogen embrittlement temperature threshold of the pipeline based on hydrogen diffusion kinetics is applied to the fields of integrity management and risk evaluation of the pipeline. The influence of the temperature on the hydrogen brittleness 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 c o To obtain the equilibrium concentration c of hydrogen atoms at the tip of the crack eq Further obtaining the total number N of hydrogen atoms required by the filling force field; obtaining the relation between the diffusivity D and the temperature through molecular dynamics simulation, and obtaining the diffusion speed V of hydrogen atoms to the crack tip; the hydrogen embrittlement threshold temperature of the pipeline steel is predicted through the ratio of N/V, and is verified through a slow stretching experiment in an 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 a hydrogen permeation current density versus 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 temperature meter 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 exemplary 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 value prediction method based on hydrogen diffusion kinetics is shown in fig. 6, and the specific flow process comprises:
determination of matrix hydrogen concentration c in pipeline steel by using hydrogen permeation current density experiment o Temperature, and thus the number of hydrogen atoms N required to saturate the defect force field,
determination of the relationship of the diffusivity of hydrogen atoms D to the temperature D = 1.5X 10 by molecular dynamics simulation -7 exp(-0.8×1.6×10 -19 /k B T), 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 pipe 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 160nm. v is the value of Poisson's ratio of 0.31 o Is a lattice constant
l z Is the actual specimen thickness. Omega H Value of 1.99X 10 -30 m 3 。
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, the value for bulk diffusion being equal to 3, 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 determination of the time dependence of MSD. The slope of the curve is the diffusivity D value at different temperatures. After fitting, a formula of the diffusivity and the temperature of the hydrogen atom can be obtained:
D＝1.5×10 -7 exp(-0.8×1.6×10 -19 /k B T) (5)
wherein k is B Representing 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 more hydrogen embrittlement. So that X90 is most hydrogen brittle at 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 utilized 2 And carrying out oxygen removal treatment on the solution for 1h.
After deoxidization, put into the corrosion case with the pipeline steel, the submergence is in NS4 solution 3, and the both ends of sample set up silica gel coating 5, and the sample passes through silica gel seal on the corrosion case, and silica gel supports the sample, plays sealed effect simultaneously. Subjecting the corrosion chamber to a constant temperature treatment, introducing 5% CO through a pH adjusting tube 2 +95％N 2 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 -6 s -1 . A preload of 490N was applied to eliminate the reduction teeth before the experimentWheel, clamp, 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 (6)
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;
quantifying the hydrogen embrittlement temperature threshold value of the pipeline by quantifying the minimum value of the N/V ratio;
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 l z F is the Faraday constant and D is the hydrogen diffusivity;
the saturated number of hydrogen atoms N is obtained according to formula (4):
wherein R value is 160nm, v is Poisson's ratio, a o Is the lattice constant,. Alpha. z Omega for actual specimen thickness H Is the component volume of a hydrogen atom, K I Representing the stress intensity, k, of the crack tip B Represents the boltzmann constant; the hydrogen atom diffusivity is fitted to the temperature in a relationship shown by the formula (5):
D＝1.5×10 -7 exp(-0.8×1.6×10 -19 /k B T)(5)，
wherein, K B Represents the boltzmann constant;
the temperature threshold of the pipeline steel is in the range of-10 to 60 ℃;
the relation between the hydrogen atom enrichment movement speed V and the hydrogen atom diffusion rate is shown as the formula (2):
wherein D is the diffusivity of a hydrogen atom, Ω H Is the volume of the hydrogen atom component, v is the Poisson's ratio of iron, k I Representing the stress intensity at the crack tip.
2. The hydrogen diffusion kinetics-based pipeline hydrogen embrittlement temperature threshold prediction method of claim 1, wherein: the method for determining the relation between the hydrogen atom diffusivity and the temperature comprises the following steps: 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 (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 by fitting.
3. The hydrogen diffusion kinetics-based pipeline hydrogen embrittlement temperature threshold prediction method of claim 1, wherein: and performing mechanical test on the pipeline steel before performing a hydrogen permeation current density experiment to obtain the stress intensity of the crack tip.
4. The use of the hydrogen diffusion kinetics-based pipeline hydrogen embrittlement temperature threshold prediction method of any one of claims 1 and 2 in the fields of pipeline integrity management and risk assessment.
5. The use of claim 4, wherein: the pipe comprises ferrite-pearlite line steel, acicular ferrite line steel, bainite-martensite line steel.
6. The use of claim 5, wherein: the pipeline steel is 5LB, X42, X52, X60, X70, X80, X100 and X120.
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