CN112862148A - Method for estimating red oil explosion accident release source item of high-level radioactive waste liquid evaporator of post-treatment plant - Google Patents
Method for estimating red oil explosion accident release source item of high-level radioactive waste liquid evaporator of post-treatment plant Download PDFInfo
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Abstract
The invention relates to a method for estimating a red oil explosion accident release source item of a high-level radioactive waste liquid evaporator of a post-treatment plant, which comprises the following steps: estimating the generation amount of the red oil in the high-level radioactive waste liquid evaporator; calculating the energy generated by explosion of the red oil; evaluating the integrity of the high-level waste liquid evaporator; if the high-level radioactive waste liquid evaporator is damaged, calculating the initial release amount and the natural evaporation release amount, and if the high-level radioactive waste liquid evaporator is not damaged, ending the estimation process; calculating the mass of the concentrated solution evaporated instantly after explosion: after the high-level radioactive waste liquid evaporator is broken, the explosion energy of the red oil is completely used for evaporating part of the concentrated solution, and the mass of the concentrated solution instantaneously evaporated at the moment is calculated; calculating the mass of the concentrated solution of the subsequent evaporation: and after the high-level waste liquid evaporator is broken, spreading the leaked concentrated solution on the ground of the equipment room, and calculating the quality of the concentrated solution subsequently evaporated on the ground of the equipment room. According to the method provided by the invention, the release source item of the red oil explosion accident of the high-level radioactive waste liquid evaporator of the post-treatment plant can be quickly obtained.
Description
Technical Field
The invention belongs to the technical field of research on release source items of emergency working conditions of a post-treatment plant, and particularly relates to an estimation method for a release source item of a red oil explosion accident of a high-level radioactive waste liquid evaporator of the post-treatment plant.
Background
When a solution containing an organic solvent and uranium and plutonium metals is evaporated, the organic solvent and degradation products thereof can chemically react with a nitric acid solution of the uranium and plutonium metals at a certain temperature to cause explosion, namely red oil explosion. It is generally accepted that "red oil" is a complex compound of nitrated TBP and uranium and plutonium heavy metals, the main component being nitroso compounds (red being the colour of nitroso compounds in the diluent). Although evaporator explosion events occurred at foreign aftertreatment facilities, the literature does not report quantitative data on the composition of "red oil". When the red oil is accumulated to a certain amount, the red oil can be decomposed violently by self catalysis and explode when heated to a temperature of more than 130 ℃. The material amount and the radioactivity processed by the high-level radioactive waste liquid concentration evaporator are the largest in the evaporator of the post-processing plant, so that the red oil explosion accident is taken as a typical design benchmark accident to be analyzed.
Aiming at the thermal decomposition reaction of TBP and a nitric acid mixture containing heavy metal, experimental research is carried out abroad. Experiments were conducted by the atomic force research institute of japan, and studies were made on the thermal decomposition reaction behavior of a solvent in which a solvent containing nitric acid and uranium nitrate is heated and nitrated under various temperature conditions. In addition, the reaction rate was investigated by measuring the rate of gas generation during thermal decomposition, and the heat of reaction between the solvent and nitric acid was measured using a calorimeter. After a solvent containing nitric acid is heated at a high temperature, the solvent reacts with nitric acid (a nitric acid compound containing heavy metals) to produce nitrate compounds, nitro compounds and the like. These compounds are thermally unstable and cause thermal decomposition reactions after oxidation by nitric acid. In a thermal decomposition reaction test for investigating a solvent, a solvent containing nitric acid and uranium nitrate is stored in a reaction tank of a development system, a thermal decomposition reaction is carried out by raising the temperature of the solvent at a constant rate, and a thermal decomposition gas generated from a nitrating solvent is measured by a quantitative gas meter installed outside the reaction tank, and the generation rate of the gas is determined as a function of the temperature. In the thermal decomposition reaction test, the generated gas was extracted and analyzed for chemical composition. Russian researches show that the irradiated TBP/nitric acid solution starts to generate exothermic reaction at 90 ℃ and generate gas, and the reaction is severe at 110 ℃; the non-irradiated TBP/nitric acid solution starts to react after being within the temperature range of 110-120 ℃ for several hours, and cannot be out of control; below 110 ℃, the reaction releases only gas and is not exothermic.
NUREG/CR-7232 presents a non-reactor nuclear facility source term calculation method that uses a multiplication of five parameters, namely MAR × DR × ARF × RF × LPF, where: MAR-material-at-risk, which is a waste liquid inventory for the sump; DR-the Damage ratio, the fraction released from the sump; ARF-air release fraction, airborne release fraction; RF-respirable fraction, breath fraction; LPF, leak path factor, refers to the fraction of MAR released outside the facility, considering the release path, mainly affected by filtration and sedimentation. However, DR, ARF, RF are difficult to acquire; it is questionable to use a scale experimental apparatus to simulate a cubic meter scale post-treatment plant. Furthermore, these 5 parameters do not relate to the size of the aerosol particles. In addition, the results of the proportion experiments are not found to be applied to post-treatment facilities, and no open literature reports release source item analysis software and method special for red oil explosion accidents.
Disclosure of Invention
Aiming at the defects in the prior art, the invention provides a method for estimating a red oil explosion accident release source item of a high-level radioactive liquid waste evaporator of a post-treatment plant, which is used for quickly acquiring the release source item of the red oil explosion accident of the high-level radioactive liquid waste evaporator of the post-treatment plant and providing support for the analysis and the response of the accident.
In order to achieve the above purposes, the invention adopts the technical scheme that: the method for estimating the release source item of the high-level radioactive waste liquid evaporator red oil explosion accident in the post-treatment plant is provided, and comprises the following steps:
estimating the generation amount of red oil in a high-level radioactive waste liquid evaporator;
step (2), calculating the energy generated by explosion of the red oil;
step (3), evaluating the integrity of the high-level radioactive waste liquid evaporator;
step (4), if the high-level radioactive waste liquid evaporator is damaged, calculating an initial release amount and a natural evaporation release amount; if the high-level radioactive waste liquid evaporator is not damaged, ending the estimation process;
and (5) calculating the mass of the concentrated solution instantaneously evaporated after explosion: after the high-level radioactive waste liquid evaporator is broken, the explosion energy of the red oil is completely used for evaporating part of the concentrated solution, and the mass of the concentrated solution instantaneously evaporated at the moment is calculated;
and (6) calculating the mass of the concentrated solution subjected to subsequent evaporation: and after the high-level waste liquid evaporator is broken, spreading the leaked concentrated solution on the ground of the equipment room, and calculating the quality of the concentrated solution subsequently evaporated on the ground of the equipment room.
Further, the specific method of the step (1) is as follows:
estimating the amount of red oil produced according to the following formulas (1) and (2):
Vred_oil＝VTBP(1-e-kt) Formula (1);
k＝3.66×1012e-14746.2/Tformula (2);
in the formula:
VTBPthe amount of TBP entrained into the evaporator, L;
k is the solution reaction rate, s-1;
t is the reaction time, s;
t is the temperature of the concentrated solution in the high-level waste liquid evaporator, K.
Further, the specific method of the step (2) is as follows:
calculating the explosion energy of the red oil according to the following formulas (3) and (4):
WTNT＝0.016Vred_oilformula (3);
E＝1000*WTNTQTNTformula (4);
in the formula:
WTNTin kg, explosive TNT equivalent;
e is the explosion energy, J;
QTNTfor the explosive heat of TNT, 4520kJ/kg is generally used.
Further, the specific method for evaluating the integrity of the evaporator in the step (3) comprises the following steps:
step (a), calculating the overpressure of the wall surface of the high-level waste liquid evaporator according to the formulas (5) and (6):
in the formula:
Δ p is the positive phase overpressure of the shock wave, Pa; r' is a dimensionless distance;
d is the distance m from the wall surface of the high level radioactive waste liquid evaporator to the center of explosion;
pais at atmospheric pressure, 1.01X 105Pa。
And (b) if the normal-phase overpressure delta p of the shock wave borne by the wall surface of the high-level radioactive waste liquid evaporator is greater than the design pressure, the high-level radioactive waste liquid evaporator is broken.
Further, the method for calculating the quality of the concentrated solution instantaneously evaporated after explosion in the step (5) comprises the following steps:
step (a), calculating the saturated temperature of the concentrated solution corresponding to the current pressure of the equipment room according to a formula (7):
TWto concentrate saturation temperature, K;
P0is the equipment room pressure, Pa;
and (b) calculating the mass of the concentrated solution instantaneously evaporated after explosion according to the formula (8):
Mevapkg of concentrate which is evaporated instantly after explosion;
cpthe specific heat capacity of the concentrated solution is J/(kg.K);
t is the temperature of the concentrated solution, K;
Hfgthe vaporization latent heat of the concentrated solution is J/kg.
Further, the method for calculating the quality of the concentrated solution of the subsequent evaporation in the step (6) comprises the following steps:
step (a), calculating the saturation pressure of the concentrated solution according to the formula (9)
pw1000 × exp (a-B/(T + C)), formula (9)
In the formula: t is the temperature of the concentrated solution, K; A. b, C are all constants, and when the temperature of the concentrated solution is more than 483K, the value of A, B, C is 17.65216, 5204.082 and 32.5 respectively; when the temperature of the concentrated solution is less than or equal to 483K, the values of A, B, C are 16.37379, 3876.659 and-43.42 respectively.
Step (b), calculating the evaporation rate of the concentrated solution according to the formula (10):
in the formula:
MWthe evaporation rate of the concentrated solution is kg/s;
d is the diffusion coefficient of the concentrated solution, m2/s；
P0Is an equipment roomPressure, Pa;
RWis the gas constant of the vapour of the concentrate, m2/(s·K)；
h is the height of the equipment room, m;
s is the floor area of the equipment room, m2。
And (c) multiplying the evaporation rate calculated in the step (b) by the evaporation time, namely the quality of the subsequently evaporated concentrated solution, wherein once an explosion accident occurs, the concentrated solution can be scattered to the ground of the equipment room if the evaporator is damaged, so that the time of the accident start is the time of the evaporation start, and the evaporation time is the accident duration.
Further, the method further comprises:
and (7) calculating the activity of each nuclide instantaneously released to the equipment room after explosion and the activity of each nuclide instantaneously released to the external environment from the equipment room after explosion according to the mass of the concentrated solution instantaneously evaporated after explosion calculated in the step (5).
Further, the method further comprises:
and (8) calculating the activity of each nuclide released to the equipment room subsequently by explosion and the activity of each nuclide released to the external environment from the equipment room subsequently by explosion according to the mass of the concentrated solution evaporated subsequently by explosion calculated in the step (6).
Further, if the discharge filter of the equipment room is judged to be invalid in the step (4), after the concentrated solution is evaporated, each nuclide is directly discharged to the environment from the equipment room; if the filter is not failing, then the decontamination factor of the filter for each nuclide is considered when calculating the activity of each nuclide released from the equipment room to the external environment.
The invention has the beneficial effects that: aiming at the blank of the prior art, the invention provides the method for estimating the release source item of the red oil explosion accident of the high-level radioactive liquid waste evaporator of the post-treatment plant, which can quickly obtain the release source item of the red oil explosion accident of the high-level radioactive liquid waste evaporator of the post-treatment plant and provide powerful support for the safety evaluation and emergency research of the red oil explosion accident of the high-level radioactive liquid waste evaporator of the post-treatment plant.
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FIG. 1 is a block diagram of a flow chart of a method for estimating a red oil explosion accident release source item of a high level radioactive waste liquid evaporator of a post-treatment plant provided by the invention.
Detailed Description
The following further describes embodiments of the present invention with reference to the accompanying drawings.
As shown in fig. 1, the invention provides a method for estimating a red oil explosion accident release source item of a high level radioactive waste liquid evaporator of a post-treatment plant, which comprises the following steps:
step 100: estimating the amount of red oil generated in the high-level radioactive waste liquid evaporator, wherein the specific method comprises the following steps:
estimating the amount of red oil produced according to the following formulas (1) and (2):
Vred_oil＝VTBP(1-e-kt) Formula (1);
k＝3.66×1012e-14746.2/Tformula (2);
in the formula: vTBPThe amount of TBP entrained into the evaporator, L; k is the solution reaction rate, s-1; t is the reaction time, s; t is the temperature of the concentrated solution in the high-level waste liquid evaporator, K.
Step 200: the method for calculating the energy generated by the explosion of the red oil comprises the following steps:
calculating the explosion energy of the red oil according to the following formulas (3) and (4):
WTNT＝0.016Vred_oilformula (3);
E＝1000*WTNTQTNTformula (4);
in the formula: wTNTIn kg, explosive TNT equivalent; e is the explosion energy, J; qTNTFor the explosive heat of TNT, 4520kJ/kg is generally used.
Step 300: evaluating the integrity of the high-level waste liquid evaporator, and the specific method comprises the following steps:
firstly, according to the formulas (5) and (6), calculating the overpressure of the wall surface of the high-level waste liquid evaporator:
in the formula: Δ p is the positive phase overpressure of the shock wave, Pa; r' is a dimensionless distance; d is the distance m from the wall surface of the high level radioactive waste liquid evaporator to the center of explosion; p is a radical ofaIs at atmospheric pressure, 1.01X 105Pa。
And if the positive overpressure delta p of the shock wave borne by the wall surface of the high-level radioactive waste liquid evaporator is greater than the design pressure, the high-level radioactive waste liquid evaporator is broken.
Step 400: and if the high-level radioactive waste liquid evaporator is damaged, judging whether the discharge filter of the equipment room is invalid, and if the high-level radioactive waste liquid evaporator is not damaged, ending the estimation process.
Step 500: calculating the mass of the concentrated solution evaporated instantly after explosion: after the high-level radioactive waste liquid evaporator is broken, the explosion energy of the red oil is completely used for evaporating part of the concentrated solution, and the mass of the concentrated solution instantaneously evaporated at the moment is calculated; the method comprises the following steps:
step 501, calculating the saturation temperature of the concentrated solution corresponding to the current pressure of the equipment room according to the formula (7):
TWto concentrate saturation temperature, K; p0Is the equipment room pressure, Pa;
step 502, calculating the mass of the concentrated solution instantaneously evaporated after explosion according to the formula (8):
Mevapkg of concentrate which is evaporated instantly after explosion; c. CpThe specific heat capacity of the concentrated solution is J/(kg.K); t is the temperature of the concentrated solution, K; hfgThe vaporization latent heat of the concentrated solution is J/kg.
Step 600: calculating the mass of the concentrated solution of the subsequent evaporation: and after the high-level waste liquid evaporator is broken, spreading the leaked concentrated solution on the ground of the equipment room, and calculating the quality of the concentrated solution subsequently evaporated on the ground of the equipment room. The method comprises the following steps:
step 601, calculating the saturation pressure of the concentrated solution according to the formula (9)
pw1000 × exp (a-B/(T + C)), formula (9)
In the formula: t is the temperature of the concentrated solution, K; A. b, C are all constants, and when the temperature of the concentrated solution is more than 483K, the value of A, B, C is 17.65216, 5204.082 and 32.5 respectively; when the temperature of the concentrated solution is less than or equal to 483K, the values of A, B, C are 16.37379, 3876.659 and-43.42 respectively.
Step 602, calculating the evaporation rate of the concentrated solution according to the formula (10):
in the formula: mWThe evaporation rate of the concentrated solution is kg/s; d is the diffusion coefficient of the concentrated solution, m2/s；P0Is the equipment room pressure, Pa; rWIs the gas constant of the vapour of the concentrate, m2V (s · K); h is the height of the equipment room, m; s is the floor area of the equipment room, m2。
Step 603, the evaporation rate calculated in step 602 is multiplied by the evaporation time, that is, the quality of the subsequently evaporated concentrated solution, once an explosion accident occurs, if the evaporator is damaged, the concentrated solution will be scattered to the ground of the equipment room, so the time when the accident starts is the time when the evaporation starts, and the evaporation time is the accident duration.
Step 700: the activity of each species released into the apparatus chamber and the activity of each species released from the apparatus chamber into the external environment are calculated.
The mass of the concentrate instantaneously evaporated after explosion calculated in step 500, the activity of each nuclide instantaneously released to the equipment room after explosion, and the activity of each nuclide instantaneously released from the equipment room to the external environment after explosion are calculated.
The mass of the concentrate subsequently evaporated by the explosion calculated in step 600 is used to calculate the activity of each nuclide subsequently released to the equipment room by the explosion, and the activity of each nuclide subsequently released to the external environment from the equipment room by the explosion.
It will be apparent to those skilled in the art that various changes and modifications may be made in the present invention without departing from the spirit and scope of the invention. Thus, if such modifications and variations of the present invention fall within the scope of the claims of the present invention and their equivalents, the present invention is intended to include such modifications and variations. The above-described embodiments are merely illustrative of the present invention, and the present invention may be embodied in other specific forms or other specific forms without departing from the spirit or essential characteristics thereof. The described embodiments are, therefore, to be considered in all respects as illustrative and not restrictive. The scope of the invention should be indicated by the appended claims, and any changes that are equivalent to the intent and scope of the claims should be construed to be included therein.
Claims (8)
1. A method for estimating a release source item of a red oil explosion accident of a high-level radioactive waste liquid evaporator of a post-treatment plant is characterized by comprising the following steps:
estimating the generation amount of red oil in a high-level radioactive waste liquid evaporator;
step (2), calculating the energy generated by explosion of the red oil;
step (3), evaluating the integrity of the high-level radioactive waste liquid evaporator;
step (4), if the high-level radioactive waste liquid evaporator is damaged, calculating the mass of the concentrated solution evaporated at the moment of explosion and the mass of the concentrated solution evaporated subsequently; if the high-level radioactive waste liquid evaporator is not damaged, ending the estimation process;
and (5) calculating the mass of the concentrated solution instantaneously evaporated after explosion: after the high-level radioactive waste liquid evaporator is broken, the explosion energy of the red oil is completely used for evaporating part of the concentrated solution, and the mass of the concentrated solution instantaneously evaporated at the moment is calculated;
and (6) calculating the mass of the concentrated solution subjected to subsequent evaporation: and after the high-level waste liquid evaporator is broken, spreading the leaked concentrated solution on the ground of the equipment room, and calculating the quality of the concentrated solution subsequently evaporated on the ground of the equipment room.
2. The method for estimating the release source term of the high level radioactive waste liquid evaporator red oil explosion accident of the post-treatment plant according to claim 1, wherein the specific method of the step (1) is as follows:
estimating the amount of red oil produced according to the following formulas (1) and (2):
Vred_oil＝VTBP(1-e-kt) Formula (1);
k＝3.66×1012e-14746.2/Tformula (2);
in the formula:
VTBPthe amount of TBP entrained into the evaporator, L;
k is the solution reaction rate, s-1;
t is the reaction time, s;
t is the temperature of the concentrated solution in the high-level waste liquid evaporator, K.
3. The method for estimating the release source term of the high level radioactive waste liquid evaporator red oil explosion accident of the post-treatment plant according to claim 1, wherein the specific method of the step (2) is as follows:
calculating the explosion energy of the red oil according to the following formulas (3) and (4):
WTNT＝0.016Vred_oilformula (3);
E＝1000*WTNTQTNTformula (4);
in the formula:
WTNTin kg, explosive TNT equivalent;
e is the explosion energy, J;
QTNTfor the explosive heat of TNT, 4520kJ/kg is generally used.
4. The method for estimating the release source term of the red oil explosion accident of the high level radioactive waste liquid evaporator of the post-processing plant according to claim 1, wherein the specific method for evaluating the integrity of the evaporator in the step (3) comprises the following steps:
step (a), calculating the overpressure of the wall surface of the high-level waste liquid evaporator according to the formulas (5) and (6):
in the formula:
Δ p is the positive phase overpressure of the shock wave, Pa; r' is a dimensionless distance;
d is the distance m from the wall surface of the high level radioactive waste liquid evaporator to the center of explosion;
pais at atmospheric pressure, 1.01X 105Pa。
And (b) if the normal-phase overpressure delta p of the shock wave borne by the wall surface of the high-level radioactive waste liquid evaporator is greater than the design pressure, the high-level radioactive waste liquid evaporator is broken.
5. The method for estimating the release source term of the high level wastewater evaporator red oil explosion accident of the post-processing plant according to claim 1, wherein the method for calculating the quality of the concentrated solution instantaneously evaporated after explosion in the step (5) comprises the following steps:
step (a), calculating the saturated temperature of the concentrated solution corresponding to the current pressure of the equipment room according to a formula (7):
TWto concentrate saturation temperature, K;
P0is the equipment room pressure, Pa;
and (b) calculating the mass of the concentrated solution instantaneously evaporated after explosion according to the formula (8):
Mevapkg of concentrate which is evaporated instantly after explosion;
cpthe specific heat capacity of the concentrated solution is J/(kg.K);
t is the temperature of the concentrated solution, K;
Hfgthe vaporization latent heat of the concentrated solution is J/kg.
6. The method for estimating the red oil explosion accident release source item of the high level radioactive waste liquid evaporator of the post-processing plant according to claim 1, wherein the method for calculating the quality of the concentrated solution of the subsequent evaporation in the step (6) comprises the following steps:
step (a), calculating the saturation pressure of the concentrated solution according to the formula (9)
pw1000 × exp (a-B/(T + C)), formula (9)
In the formula: t is the temperature of the concentrated solution, K; A. b, C are all constants, and when the temperature of the concentrated solution is more than 483K, the value of A, B, C is 17.65216, 5204.082 and 32.5 respectively; when the temperature of the concentrated solution is less than or equal to 483K, the values of A, B, C are 16.37379, 3876.659 and-43.42 respectively.
Step (b), calculating the evaporation rate of the concentrated solution according to the formula (10):
in the formula:
MWthe evaporation rate of the concentrated solution is kg/s;
d is the diffusion coefficient of the concentrated solution, m2/s；
P0Is the equipment room pressure, Pa;
RWis the gas constant of the vapour of the concentrate, m2/(s·K)；
h is the height of the equipment room, m;
s is the floor area of the equipment room, m2。
And (c) multiplying the evaporation rate calculated in the step (b) by the evaporation time, namely the quality of the subsequently evaporated concentrated solution, wherein once an explosion accident occurs, the concentrated solution can be scattered to the ground of the equipment room if the evaporator is damaged, so that the time of the accident start is the time of the evaporation start, and the evaporation time is the accident duration.
7. The method for estimating the release source term of the red oil explosion accident of the high level radioactive waste liquid evaporator of the post-processing plant according to claim 1, wherein the method further comprises the following steps:
and (7) calculating the activity of each nuclide instantaneously released to the equipment room after explosion and the activity of each nuclide instantaneously released to the external environment from the equipment room after explosion according to the mass of the concentrated solution instantaneously evaporated after explosion calculated in the step (5).
8. The method for estimating the release source term of the red oil explosion accident of the high level radioactive waste liquid evaporator of the post-processing plant according to claim 1, wherein the method further comprises the following steps:
and (8) calculating the activity of each nuclide released to the equipment room subsequently by explosion and the activity of each nuclide released to the external environment from the equipment room subsequently by explosion according to the mass of the concentrated solution evaporated subsequently by explosion calculated in the step (6).
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