CN117219301A - Uranium plutonium solution system critical safety control method - Google Patents

Uranium plutonium solution system critical safety control method Download PDF

Info

Publication number
CN117219301A
CN117219301A CN202311105250.7A CN202311105250A CN117219301A CN 117219301 A CN117219301 A CN 117219301A CN 202311105250 A CN202311105250 A CN 202311105250A CN 117219301 A CN117219301 A CN 117219301A
Authority
CN
China
Prior art keywords
uranium
plutonium
solution system
gadolinium
plutonium solution
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
CN202311105250.7A
Other languages
Chinese (zh)
Inventor
周旺
何润虎
郭云
周利华
杨立群
陈俊良
孙亚楼
王国辉
何燎原
龚伟
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
404 Co Ltd China National Nuclear Corp
Original Assignee
404 Co Ltd China National Nuclear Corp
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by 404 Co Ltd China National Nuclear Corp filed Critical 404 Co Ltd China National Nuclear Corp
Priority to CN202311105250.7A priority Critical patent/CN117219301A/en
Publication of CN117219301A publication Critical patent/CN117219301A/en
Pending legal-status Critical Current

Links

Abstract

The invention relates to a critical safety control method of a uranium-plutonium solution system, which is characterized in that the treatment capacity of containers such as a pulse extraction column, a solution storage tank and the like can be greatly improved by adding soluble neutron poison into the uranium-plutonium solution system at the head end of spent fuel post-treatment. The soluble neutron poison used in uranium plutonium solution systems is gadolinium nitrate and no boron-containing solution is used. The reason is that boron cannot be ensured to continuously exist according to a preset distribution state in the dissolving process of the spent fuel assembly; boron is soluble in 0.2-0.5 mol/L nitric acid, while cadmium, gadolinium, samarium and other rare earth elements are soluble in 1-3 mol/L nitric acid, and the soluble acidity range of the rare earth elements is more in line with the dissolution process of a post-treatment plant. Compared with the prior art, the invention can realize critical safety control of uranium-plutonium solution system by only using one soluble neutron poison gadolinium nitrate, and has simple control system and easy industrialization.

Description

Uranium plutonium solution system critical safety control method
Technical Field
The invention relates to the field of post-treatment professional nuclear critical safety, in particular to a critical safety control method of a uranium plutonium solution system.
Background
The post-treatment is an important component of closed fuel circulation, and in the post-treatment link of the spent fuel, the content of the fissionable nuclides in the treated spent fuel assembly is higher, and the post-treatment flow needs critical control. Before the fuel of power stack is irradiated 235 The mass fraction of U is generally about 3.5%, and the maximum mass fraction is not more than 5%. In the discharged spent fuel 235 The U average mass fraction is less than 1%, and the plutonium mass fraction is more than 0.5%. And some spent fuel is likely to 235 The mass fraction of U is more than 3 percent and is very close to that of the un-irradiated fuel 235 U mass fraction. There may also be some plutonium in the spent fuel by mass fraction greater than 1%.
According to the physical and chemical characteristics of the treatment object, U, pu components in the feed liquid are mixed from a dissolver to each device in the main process; a material state; the liquid phase (aqueous phase, organic phase) is in a homogeneous state or in a heterogeneous state; extracting equipment interface dirt; precipitation equipment plutonium oxalate scarring; plutonium can flow back and accumulate in the extraction equipment; the concentration (aqueous phase, organic phase) of the feed liquid, the concentration variation range and the like can adopt one or more of the following nuclear critical safety measures: 1) Concentration control; 2) Geometry control; 3) Neutron poison; 4) Controlling the total amount; 5) And (5) distance control.
At the same time, consideration of equipment critical safety measures also needs to be extended to the first downstream equipment to ensure that these fissionable nuclides do not inadvertently deposit on non-critical safety design elements, causing critical accidents. The equipment which can generate critical safety hazards due to accumulation, concentration and precipitation of fissile substances is listed as critical safety monitoring points, and the critical safety monitoring points are important means for preventing critical accidents from happening in spent fuel post-treatment plants by measuring neutrons generated by spontaneous fission of the plutonium and neutrons generated by reacting alpha particles with light nuclei (alpha, n) such as O, C in addition to measuring the concentration and controlling the loss of uranium and the plutonium by adopting an on-line monitoring technology, and even if the unexpected accumulation, concentration, precipitation or transfer of the plutonium is found in a gamma radiation field.
Absorption is a process in which neutrons interact with matter of paramount importance. All substances can absorb neutrons without fission, even if fissile isotopes are present. If neutrons are present in the system without fissile nuclides, then more fissile nuclear material is required to maintain the chain reaction of the system, i.e., to increase the critical mass of the system. Some materials are particularly good at absorbing neutrons, i.e., they have a particularly large neutron absorption cross section, such as boron, cadmium, gadolinium, etc., and the nuclides having particularly large neutron absorption cross sections are generally referred to as neutron poisons.
For the main process system of the existing post-treatment facility, the material liquid containing the fissionable nuclide has critical safety risk in the process of guiding the material from the geometric safety container to the non-geometric safety container, and the safety cannot be completely ensured if the type, the burnup depth and the initial enrichment degree of the processed spent fuel object are changed originally, which relates to equipment/containers with geometric safety. From the standpoint of eliminating critical risk points and facility utilization, a new method different from the traditional critical safety control measures is therefore proposed to ensure the nuclear critical safety of uranium-plutonium solution systems.
Disclosure of Invention
The invention aims to provide a critical safety control method of a uranium-plutonium solution system for solving the defects existing in the prior art, and the critical safety of the cores of the uranium-plutonium solution systems with different components is ensured, so that the critical safety of the cores of the processes of post-treatment facility head end, co-decontamination, chemical separation and uranium-plutonium tail end storage, treatment and transportation of uranium-containing plutonium elements is improved.
The aim of the invention can be achieved by the following technical scheme:
the first object of the present invention is to provide a highly stable fissile nuclide security system consisting of 235 U、 239 Pu and gadolinium simple substance composition, wherein 235 U and 239 the mass ratio of Pu is 3:1 to 1: and 3, in order to calculate the actual situation, the density of the easily-cracked metal pellets changes along with the change of the uranium-plutonium mass ratio, and the mass weighting of the uranium-plutonium simple substance density is adopted.
Further, the relative mass range of the gadolinium simple substance is 235 U and 239 pu mass sum is 0.05% -0.5%.
Further, the method comprises the steps of, 235 u and 239 the mass ratio of Pu is selected from 3: 1. 1:1 or 1:3.
the second object of the invention is to provide a critical safety control method of uranium-plutonium solution system, which adds soluble neutron poison into the uranium-plutonium solution system in spent fuel post-treatment process system,
the soluble neutron poison is gadolinium nitrate.
Further, the uranium plutonium solution system includes uranyl nitrate and plutonium nitrate.
The components in the uranium plutonium solution system further comprise 235 U ion, 239 Pu ion, gadolinium ion and H 2 O。
The above further, the uranium plutonium solution system 235 U and 239 the mass ratio of Pu is 3:1 to 1:3.
the ratio of hydrogen atoms to uranium atoms in the uranium plutonium solution system is as follows: h/u=10 to 60.
The ratio of hydrogen atoms to uranium atoms in the uranium plutonium solution system is as follows: h/u=35.
The above further has a relative mass content of gadolinium of 235 U and 239 pu mass 0.05-0.5%.
The principle of the invention is as follows:
at the head end of fuel treatment, the treatment capacity of containers such as pulse extraction columns, solution storage tanks and the like can be greatly improved by using soluble neutron poison. The soluble neutron poison used in uranium plutonium solution systems is gadolinium nitrate and no boron-containing solution is used. The reason is that boron cannot be ensured to continuously exist according to a preset distribution state in the dissolving process of the spent fuel assembly; boron is soluble in 0.2-0.5 mol/L nitric acid, while cadmium, gadolinium, samarium and other rare earth elements are soluble in 1-3 mol/L nitric acid, and the soluble acidity range of the rare earth elements is more in line with the dissolution process of a post-treatment plant.
The critical safety control method for the gadolinium nitrate which is the uniform neutron poison has the advantages that the gadolinium nitrate and the material are uniformly mixed in the system, and the neutron absorption efficiency is high and the effect is good. The method has the defects that the poison is required to be specially removed at the tail end of the process, and whether the poison exists or not is required to be checked frequently, so that when the method is used for implementing critical safety control, the concentration of gadolinium nitrate is not too high so as not to influence a main process system, and the relative mass content of gadolinium is controlled to be in the range of 0.05-0.5% compared with the content of the fissionable materials (total amount) according to the results of earlier investigation and thermal experiments.
Compared with the prior art, the invention has the following beneficial effects:
1. according to the invention, critical safety control of uranium-plutonium solution system can be realized by only using one soluble neutron poison gadolinium nitrate, and the control system is simple and easy to industrialize.
2. The method limits the adding amount of the soluble neutron poison gadolinium nitrate, and has little influence on the main process link of the post-treatment.
3. The gadolinium nitrate which is a soluble neutron poison used in the invention is easy to obtain, has good stability and is beneficial to the industrialized popularization of the method.
4. The application range of the invention covers the critical control of post-treatment processes of spent fuel such as power stacks, high-temperature gas cooled stacks, MOX, fast stacks and the like, and the relative content range of U and Pu is wide.
5. The control method of the invention has passed the hot test verification to confirm the reliability.
Drawings
FIG. 1 is a diagram of a uranium plutonium metal system model of total water reflection;
FIG. 2 shows the effective multiplication factor of uranium plutonium metal systems at different levels of elemental gadolinium incorporation;
FIG. 3 is a diagram of a system model of a totally water-reflective cylindrical uranium plutonium solution;
figure 4 shows the effective proliferation factor of uranium plutonium solution systems at different H/U.
Detailed Description
The invention will now be described in detail with reference to the drawings and specific examples. The present embodiment is implemented on the premise of the technical scheme of the present invention, and a detailed implementation manner and a specific operation process are given, but the protection scope of the present invention is not limited to the following examples.
The first object of the present invention is to provide a highly stable fissile nuclide security system consisting of 235 U、 239 Pu and gadolinium simple substance composition, wherein 235 U and 239 the mass ratio of Pu is 3:1 to 1: and 3, in order to calculate the actual situation, the density of the easily-cracked metal pellets changes along with the change of the uranium-plutonium mass ratio, and the mass weighting of the uranium-plutonium simple substance density is adopted.
Further, the relative mass range of the gadolinium simple substance is 235 U and 239 pu mass sum is 0.05% -0.5%.
Further, the method comprises the steps of, 235 u and 239 the mass ratio of Pu is selected from 3: 1. 1:1 or 1:3.
the second object of the invention is to provide a critical safety control method of uranium-plutonium solution system, which adds soluble neutron poison into the uranium-plutonium solution system in spent fuel post-treatment process system,
the soluble neutron poison is gadolinium nitrate.
Further, the uranium plutonium solution system includes uranyl nitrate and plutonium nitrate.
The components in the uranium plutonium solution system further comprise 235 U ion, 239 Pu ion, gadolinium ion and H 2 O。
The above further, the uranium plutonium solution system 235 U and 239 the mass ratio of Pu is 3:1 to 1:3.
the ratio of hydrogen atoms to uranium atoms in the uranium plutonium solution system is as follows: h/u=10 to 60.
The ratio of hydrogen atoms to uranium atoms in the uranium plutonium solution system is as follows: h/u=35.
The above further has a relative mass content of gadolinium of 235 U and 239 pu mass 0.05-0.5%. Some embodiments of the present invention are described in detail below with reference to the accompanying drawings. The embodiments described below and features of the embodiments may be combined with each other without conflict.
Example 1
The embodiment provides a critical safety control method of uranium plutonium metal system, which comprises the following specific steps:
preparing a metal pellet with diameter of 5cm, wherein the metal pellet is made of 235 U and 239 pu, the mass ratio of which is 3: 1. 1:1 and 1:3, in order to calculate the actual situation, the density of the metal pellets changes along with the change of the uranium plutonium mass ratio, and the mass weighting of the uranium plutonium simple substance density is adopted;
the metal pellets are doped with gadolinium simple substance, and the relative mass share ranges from 0.05% to 0.5%;
a30 cm thick water layer is coated outside the metal pellets, a model schematic diagram is shown in fig. 1, and in order to conservatively consider a total water reflection model, which is the most serious case in critical safety analysis, water is generally not generated.
Calculating effective multiplication factors k of total-water-reflection metal pellets under different uranium and plutonium compositions and different gadolinium doping amounts eff . The calculation results are shown in Table 1 and FIG. 2.
TABLE 1 Total Water reflection Metal globules effective proliferation factor
From the calculation results, it can be seen that the system reactivity of the metal pellets followsThe mass of gadolinium incorporation was reduced by an increase of 75% 235 U and 25% 239 Pu component, effective proliferation factor k of pellet without gadolinium simple substance incorporation eff 0.91869 + -0.00072, the effective proliferation factor of the pellet becomes 0.86515 + -0.00065 after the metal gadolinium is doped with 0.5 percent of simple substance; for 50% 235 U and 50% 239 Pu component, effective proliferation factor k of pellet without gadolinium simple substance incorporation eff 1.00914 + -0.00078, the effective proliferation factor of the pellet becomes 0.95989 + -0.00070 after the metal gadolinium is doped with 0.5% of simple substance; for 25% 235 U and 75% 239 Pu component, effective proliferation factor k of pellet without gadolinium simple substance incorporation eff The effective proliferation factor of the pellets becomes 1.05492 +/-0.00073 after being doped with 0.5% of metal gadolinium in 1.09714 +/-0.00081.
Therefore, as the concentration of the simple substance gadolinium increases, the decrease rate of the effective multiplication factor of the system becomes slow, which may be due to the fact that the increase of the content of the simple substance gadolinium further improves the neutron reflection probability of the system, and the decrease rate of the effective multiplication factor becomes slow under the mutual competition and balance of the two mechanisms of neutron absorption and neutron reflection. Therefore, the concentration of the soluble neutron poison gadolinium nitrate is not preferably too high from the two viewpoints of the system effectiveness control efficiency and the influence on the post-treatment main process.
Example 2
A critical safety control method of uranium plutonium solution system comprises the following specific steps:
the metal system is adjusted to be a solution system, the influence of the moderator on the system reactivity is considered, the model is a cylinder, the radius is 10cm, the height is 20cm, and the schematic diagram of the model is shown in figure 3. The solution comprises the following components 235 U、 239 Pu and H 2 O, where 235 U and 239 pu mass ratio is 3:1, in order to guarantee the principle of single variable, the influence of nitrate ions is not considered in the critical safety analysis of the example. Setting the mass of gadolinium doped with soluble neutron poison into a cylindrical internal solution system 235 U and 239 pu mass 0.05%.
When the critical safety analysis of uranium plutonium solution system is actually carried out, the following empirical formula can be adopted to calculate the densities of the uranyl (VI) nitrate and the plutonium (IV) nitrate aqueous solution (the densities are key calculation inputs, the outputs are critical, namely keff, and the density value has a great influence on keff):
wherein: ρ is the solution density at T, g/cm 3
g/L for plutonium concentration at 25 ℃;
is the uranium concentration at 25 ℃, g/L;
the molar concentration of nitrate solution at 25 ℃ and mol/L;
t is the temperature, DEG C.
In this example, by adjusting the ratio of H/U, i.e. the ratio of hydrogen atoms to uranium atoms, to characterize the concentration and the slowing effect of the fissionable materials, the effective proliferation factor of the 0.05% w.t. soluble gadolinium solution system under different H/U conditions was calculated, and the calculation results are shown in table 2 and fig. 4 in detail.
TABLE 2 Total aqueous reflection solution column systems effective multiplication factors
From the calculation results, when in the solution system 235 The U atomic density is kept constant along with H atomsThe increase in sub-density, the effective multiplication factor of the system exhibits the characteristic of increasing followed by decreasing, because the slowing effect of the system is gradually remarkable, 235 u and 239 fast neutron path H released by Pu fission 2 After O is slowed down, the energy is reduced to thermal neutrons, and uranium and plutonium are absorbed to carry out the next fission, so that the system reactivity is increased along with the increase of H/U value, and for the case of gadolinium doping, the solution cylinder system is optimally slowed down at about 30H/U, and the effective multiplication factor of the system is maximized and is 0.52309 +/-0.00075; for the case of no gadolinium doping, the solution cylinder system achieves optimal slowing at about 35H/U, and the effective proliferation factor of the system reaches the maximum, which is 0.57648 +/-0.0077. The effective multiplication factor of the cylindrical solution system then tends to decrease with further increases in H/U values due to excessive H 2 The slowing of the operon by O has little effect, namely H 2 The absorption effect of O on thermal neutrons is obviously enhanced, so that the effective multiplication factor of the system is reduced.
In the super-slowing stage, the decrease rate of the effective multiplication factor of the gadolinium-doped solution cylinder system is obviously higher than that of the gadolinium-free system because of the existence of Gd, so that the gadolinium-doped solution cylinder system passes through H 2 The thermal neutron absorption probability after O is slowed is increased, resulting in a rear section k eff The rate of descent increases.
The previous description of the embodiments is provided to facilitate a person of ordinary skill in the art in order to make and use the present invention. It will be apparent to those skilled in the art that various modifications can be readily made to these embodiments and the generic principles described herein may be applied to other embodiments without the use of the inventive faculty. Therefore, the present invention is not limited to the above-described embodiments, and those skilled in the art, based on the present disclosure, should make improvements and modifications without departing from the scope of the present invention.

Claims (10)

1. A high-stability fissionable nuclide safety system is characterized by comprising 235 U、 239 Pu and gadolinium simple substance composition, wherein 235 U and 239 the mass ratio of Pu is 3:1 to 1:3.
2. the high stability fissile nuclide security system of claim 1 wherein the relative mass range of the elemental gadolinium is 235 U and 239 pu mass sum is 0.05% -0.5%.
3. A highly stable, fissile nuclear safety system as claimed in claim 1, 235 u and 239 the mass ratio of Pu is selected from 3: 1. 1:1 or 1:3.
4. a critical safety control method of uranium-plutonium solution system is characterized in that soluble neutron poison is added into the uranium-plutonium solution system in spent fuel post-treatment process system,
the soluble neutron poison is gadolinium nitrate.
5. A method of critical security control of a uranium plutonium solution system according to claim 4, characterised in that the uranium plutonium solution system includes uranyl nitrate and plutonium nitrate.
6. A critical safety control method of uranium plutonium solution system according to claim 5, characterized in that components in the uranium plutonium solution system include 235 U ion, 239 Pu ion, gadolinium ion and H 2 O。
7. A critical security control method of uranium-plutonium solution system according to claim 6, characterised in that in the uranium-plutonium solution system 235 U and 239 the mass ratio of Pu is 3:1 to 1:3.
8. a critical safety control method of a uranium-plutonium solution system according to claim 6, wherein the ratio of hydrogen atoms to uranium atoms in the uranium-plutonium solution system is: h/u=10 to 60.
9. A critical safety control method of a uranium-plutonium solution system according to claim 8, characterized in that the ratio of hydrogen atoms to uranium atoms in the uranium-plutonium solution system is: h/u=35.
10. A critical safety control method of uranium plutonium solution system according to claim 6, characterized in that the relative mass content of gadolinium is 235 U and 239 pu mass 0.05-0.5%.
CN202311105250.7A 2023-08-30 2023-08-30 Uranium plutonium solution system critical safety control method Pending CN117219301A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN202311105250.7A CN117219301A (en) 2023-08-30 2023-08-30 Uranium plutonium solution system critical safety control method

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN202311105250.7A CN117219301A (en) 2023-08-30 2023-08-30 Uranium plutonium solution system critical safety control method

Publications (1)

Publication Number Publication Date
CN117219301A true CN117219301A (en) 2023-12-12

Family

ID=89043457

Family Applications (1)

Application Number Title Priority Date Filing Date
CN202311105250.7A Pending CN117219301A (en) 2023-08-30 2023-08-30 Uranium plutonium solution system critical safety control method

Country Status (1)

Country Link
CN (1) CN117219301A (en)

Similar Documents

Publication Publication Date Title
Frybortova Recommended strategy and limitations of burnable absorbers used in VVER fuel assemblies
Boczar et al. Thorium fuel-cycle studies for CANDU reactors
Ergen et al. The aircraft reactor experiment—physics
Khrais et al. Neutronic analysis of VVER-1000 fuel assembly with different types of burnable absorbers using Monte-Carlo code Serpent
Hassan et al. Investigation of using U-233 in thorium base instead of conventional fuel in Russian PWR by SERPENT Code
Insulander Björk et al. Study of thorium-plutonium fuel for possible operating cycle extension in PWRs
CN117219301A (en) Uranium plutonium solution system critical safety control method
Ovi et al. Neutronic analysis of VVER-1000 MOX fuel assembly with burnable absorber Gadolinia and Erbia
Nishimura et al. Preliminary core calculation on reactivity compensation for SiC matrix fuel compact HTTR with Erbium burnable poison and Plutonium fissile material
Kloosterman Multiple recycling of plutonium in advanced PWRs
Savitsky et al. The calculation of the campaign of reactor RITM-200
Galahom Analyze the effect of void fraction on the main operating parameters of the VVER-1200
JP7447046B2 (en) Operation method of light water reactor uranium fuel assembly and nuclear fuel cycle
Shimizu et al. Evaluation of the Applicability of Plutonium Transmuted From Minor Actinides by Fusion Reactor as Fertile Fuel in Boiling Water Reactor
Renteria del Toro et al. Loading pattern determination for 50% MOX and 50% UO 2 iPOWER reactor for initial cycle
Galahom et al. Design boiling water reactor core model using MCNPX for studying the burnable poisons and the axial enrichment fuel effect on the neutronic characteristics
da Silva et al. Neutronic evaluation of CANDU-6 core using reprocessed fuels
Volkov et al. Reactivity Runaway Reduction When Using Enriched Uranium in a Lead Fast Reactor
Yamamoto et al. Mechanisms of positive temperature reactivity coefficients of dilute plutonium solutions
Yu Reactor Theory
Demazière Reactor physics calculations on MOX fuel in Boiling water reactors (BWRs)
Duhamel et al. Criticality calculation codes validation: Experimental needs for low-moderated MOX media
Fuchs et al. The possibilities for the operation of a natural uranium breeder reactor without fuel element preparation
Debrue et al. Plutonium Recycle Studies for the SENA PWR Reactor
Chapin Nuclear analysis on the enrichment of PWR fuel in a fusion hybrid reactor

Legal Events

Date Code Title Description
PB01 Publication
PB01 Publication
SE01 Entry into force of request for substantive examination
SE01 Entry into force of request for substantive examination