CN111573687A - Neutron absorber material with high boron loading capacity - Google Patents

Neutron absorber material with high boron loading capacity Download PDF

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Publication number
CN111573687A
CN111573687A CN202010573534.9A CN202010573534A CN111573687A CN 111573687 A CN111573687 A CN 111573687A CN 202010573534 A CN202010573534 A CN 202010573534A CN 111573687 A CN111573687 A CN 111573687A
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neutron
absorber material
neutron absorber
high boron
boron loading
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陈向阳
卢俊强
郑轶雄
秦慧敏
张兆泉
范武刚
王晓娇
李聪
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Shanghai Institute of Ceramics of CAS
Shanghai Nuclear Engineering Research and Design Institute Co Ltd
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Shanghai Institute of Ceramics of CAS
Shanghai Nuclear Engineering Research and Design Institute Co Ltd
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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B35/00—Boron; Compounds thereof
    • C01B35/02—Boron; Borides
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B35/00—Boron; Compounds thereof
    • C01B35/02—Boron; Borides
    • C01B35/04—Metal borides

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  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Monitoring And Testing Of Nuclear Reactors (AREA)

Abstract

The invention discloses a neutron absorber material with high boron loading capacity, wherein the neutron absorber material is a multi-B compound, and the chemical formula of the multi-B compound is MBxWherein x is not less than 6, B is not less than 75% by mass, and M is Al, Mg, Si, Y, an element having a thermal neutron absorption cross section of not more than 1.5 Bayonine, or a mixture thereof. The neutron absorption material has the absorption value and the water corrosion resistance superior to those of the neutron absorption material B4C and ZrB2And the like, the B-containing absorber material is commonly used, so that the reactivity value of the neutron absorber and the safety of the shell under the condition of breakage are obviously improved.

Description

Neutron absorber material with high boron loading capacity
Technical Field
The invention relates to the technical field of neutron absorber materials, in particular to a neutron absorber material with high boron loading capacity.
Background
In the initial phase of the first charging or initial refueling cycle of the reactor, the initial residual reactivity of the core is high, and chemical compensation poisons, burnable poisons or control rods are required to control the residual reactivity.
For burnable poisons, the main function is represented in two aspects: the maximum fuel utilization rate is obtained, and the fuel circulation cost is reduced. The capability of the burnable poison for absorbing the excess neutrons is stably reduced along with the operation, so that the reactivity bound by the burnable poison is gradually and finally fully released in the burnup process; and secondly, the power distribution control capability can be well provided, and the optimal matching of the consumption of the burnable poison and the fuel burnup on the rate and the spatial relationship can be realized. The consumption of the B element is stably reduced and well matched with the fuel consumption, almost no penalty is remained, the consumption rate is always slowly reduced and widely applied, so that the burnable poison materials used for the pressurized water reactor core at home and abroad mainly comprise boron stainless steel, borosilicate glass and boron carbide-alumina (B)4C-Al2O3) And ZrB2. However, the above materials all have obvious disadvantages, mainly represented by the poor water corrosion resistance of the above materials, and the damage of the core block in the claddingIn which case it will be quickly eroded by the water and lose geometry. Therefore, the safety of the reactor core can be obviously improved by researching and developing a new material with stronger water corrosion resistance to replace the material. It is worth noting that ZrB is enriched for monolithic burnable poison absorbers2There is also a problem of high cost because of the price of the B material and the10The B enrichment degree is in an exponential growth trend, and the cost of the enriched B material is increased by several times to hundreds times compared with that of the natural B material, so that the research and development of the absorber material with higher boron loading capacity for replacing ZrB with high enrichment degree2Reduction of material pair10The requirement of B enrichment can significantly reduce material cost.
In summary, a novel neutron absorber material with high boron loading and good water corrosion resistance is developed to replace the currently common B-containing neutron absorber material (such as B)4C and ZrB2) Has important significance for improving the economy and the safety of the assembly.
Disclosure of Invention
The invention provides a neutron absorber material with high boron loading capacity, aiming at the problems of poor water corrosion resistance, high price and the like of the conventional neutron absorber material, and is characterized in that the material is a multi-B compound, has high boron loading capacity, and can realize long-period reactivity regulation and control, moderator negative temperature coefficient regulation or control of reactor operation power and reactor shutdown on the function.
The neutron absorber material with high boron loading capacity is a multi-B compound, and the chemical formula of the multi-B compound is MBxWherein x is not less than 6, the mass fraction of B is not less than 75%, M is Al, Mg, Si, Y elements and the mixture thereof with a thermal neutron absorption cross section not more than 1.5 Bayonin, and the reactivity value of the neutron absorber and the safety of the cladding under breakage can be obviously improved.
Preferably, the neutron absorber material can be used alone or in combination with the first mixed material as a burnable poison assembly absorber material for flattening the neutron fluence distribution in the reactor core and realizing long-period reactivity control and negative temperature coefficient control of the moderator.
Preferably, the neutron absorber material can be used alone or in combination with a second hybrid material as a control rod assembly absorber material for controlling reactor operating power and shutdown.
Preferably, the first mixed material contains B, Er, Gd or a mixture thereof, so that the sum of the thermal neutron absorption cross sections of other elements contained in the material is not more than 1.5 target en, and the first mixed material does not contain B, Er, Gd or a mixture thereof, so that the sum of the thermal neutron absorption cross sections of other elements contained in the material is not more than 5 target en.
Preferably, the second mixed material at least contains one or more of B, Gd, Dy, Tb, Tm, Sm, Eu, Ir, Lu, Ag, In, Cd, Nd and Hf elements.
Compared with the prior art, the invention has the following beneficial effects:
1. the invention provides a neutron absorbing material AlB with high boron loading capacity12B loading of 2.14g/cm3Is ZrB commonly used2Middle B load (1.17 g/cm)3) Approximately 2 times of the total amount of the burnable poison absorber material10The enrichment degree of B, thereby obviously reducing the material cost. Further, AlB12The thermal neutron (E is 0.0253eV) absorption cross section of the medium Al element is smaller than that of the Zr element, the reaction residual toxicity at the end of the service life is smaller, and the service life of the fuel assembly can be prolonged to a certain extent.
2. The invention provides a neutron absorbing material AlB with high boron loading capacity12The corrosion resistance of the alloy is obviously better than that of the alloy B4C and ZrB2. With AlB12The thermal conductivity of the material is about 38W/(m.K), which is obviously better than that of B4C (10.47-29.31W/(mK)) and ZrB2(23W/(m.K)) is advantageous for the absorber material to conduct away the heat generated during operation. The higher thermal conductivity and the better water corrosion resistance can obviously improve the safety of the reactor under the condition that the cladding tube is damaged.
Drawings
FIG. 1 is a schematic diagram of10ZrB of B linear density2And AlB12Relative price of (assuming price is 1) and10b, a schematic diagram of the linear density relationship;
FIG. 2 is a schematic diagram of the difference10The sales price of B-abundant boric acid;
FIG. 3 is B4C、AlB12And ZrB2And (5) testing the water corrosion resistance of the core block.
Detailed Description
The invention will be further illustrated with reference to specific examples.
Example one
The neutron absorber material with high boron loading capacity provided by the invention is a multi-B compound, and the chemical formula of the multi-B compound is MBxWherein x is not less than 6, B is not less than 75% by mass, M is Al, Mg, Si, Y, and other elements and mixtures thereof with thermal neutron absorption cross section not more than 1.5 Bayonine, which can improve the reactivity value of neutron absorber and the safety of cladding under damage, and is obviously superior to enriched ZrB2The price advantage of (c). Preferably, the neutron-absorber material with high boron loading is AlB12The cost of the B-containing material is mainly determined by the boric acid as the raw material, and the price of the boric acid is equal to that of the boric acid10The abundance of B is shown in FIG. 2, assuming that the inner diameter of the monolithic burnable poison coating is 7.6mm, the thickness is 6.75m, and the density of the coating is 80%, the difference is calculated10AlB of B line density12And ZrB2As required10After B abundance, AlB can be deduced12And ZrB2Price of and10b the relationship of linear density, as shown in FIG. 110When the linear density of B is more than 0.5mg/cm, ZrB is enriched2Price ratio of AlB12Several times to hundreds times more expensive.
The neutron absorber material can be used independently or in combination with the first mixed material, is used as an absorber material in a burnable poison assembly, is used for flattening the neutron fluence distribution of a reactor core and realizing long-period reactivity regulation and negative temperature coefficient regulation of a moderator, the first mixed material contains B, Er, Gd or a mixture thereof, the sum of the thermal neutron absorption cross sections of other elements contained in the material is not more than 1.5 target en, and the first mixed material does not contain B, Er, Gd or a mixture thereof, the sum of the thermal neutron absorption cross sections of the other elements contained in the material is not more than 5 target en; the neutron absorber material can be used independently or matched with a second mixed material to be used as an absorber material In the control rod assembly and used for controlling the operating power of the reactor and stopping the reactor, and the second mixed material at least contains one or more of B, Gd, Dy, Tb, Tm, Sm, Eu, Ir, Lu, Ag, In, Cd, Nd and Hf elements; when the neutron absorber material is matched with other absorber materials for use, the mass fraction of the neutron absorber material is between 10% and 90%.
Example two
The neutron absorber material with high boron loading capacity provided by the invention is a multi-B compound, and the chemical formula of the multi-B compound is MBxWherein x is not less than 6, B is not less than 75% by mass, M is Al, Mg, Si, Y, and other elements and mixtures thereof with thermal neutron absorption cross section not more than 1.5 Bayonine, which can improve the reactivity value of neutron absorber and the safety of cladding under damage, and is obviously superior to ZrB2Preferably, the high boron loading neutron absorbing material may be AlB12When AlB is12、ZrB2When the core block has the same density of 80 percent, AlB is corroded in water at the temperature of 360 +/-2 ℃ for 100 hours12And ZrB2The amount of the lost substance per unit volume of the two pellets was 1.9210 × 10-5mol and 7.0210 × 10-5mol, compared to ZrB2，AlB12The water corrosion resistance of the composite material is improved by 3.7 times.
The neutron absorber material can be used independently or in combination with the first mixed material, is used as an absorber material in a burnable poison assembly, is used for flattening the neutron fluence distribution of a reactor core and realizing long-period reactivity regulation and negative temperature coefficient regulation of a moderator, the first mixed material contains B, Er, Gd or a mixture thereof, the sum of the thermal neutron absorption cross sections of other elements contained in the material is not more than 1.5 target en, and the first mixed material does not contain B, Er, Gd or a mixture thereof, the sum of the thermal neutron absorption cross sections of the other elements contained in the material is not more than 5 target en; the neutron absorber material can be used independently or matched with a second mixed material to be used as an absorber material In the control rod assembly and used for controlling the operating power of the reactor and stopping the reactor, and the second mixed material at least contains one or more of B, Gd, Dy, Tb, Tm, Sm, Eu, Ir, Lu, Ag, In, Cd, Nd and Hf elements; when the neutron absorber material is matched with other absorber materials for use, the mass fraction of the neutron absorber material is between 10% and 90%.
EXAMPLE III
The neutron absorber material with high boron loading capacity provided by the invention is a multi-B compound, and the chemical formula of the multi-B compound is MBxWherein x is not less than 6, B is not less than 75% by mass, M is Al, Mg, Si, Y, and other elements and mixtures thereof with thermal neutron absorption cross section not more than 1.5 Bayonin, which can improve the reactivity value of neutron absorber and the safety of cladding under breakage, and is obviously superior to B4C, preferably, the high boron loading neutron absorbing material may be AlB12When AlB is12、B4When the C core block has the same density of 80 percent, AlB is corroded in water at the temperature of 360 +/-2 ℃ for 100 hours12And B4The molar mass loss of the C two pellets per unit volume is 1.9210 × 10-5mol sum 110 × 10-4mol, compared with B4C，AlB12The water corrosion resistance of the alloy is respectively improved by 5.2 times.
The neutron absorber material can be used independently or in combination with the first mixed material, is used as an absorber material in a burnable poison assembly, is used for flattening the neutron fluence distribution of a reactor core and realizing long-period reactivity regulation and negative temperature coefficient regulation of a moderator, the first mixed material contains B, Er, Gd or a mixture thereof, the sum of the thermal neutron absorption cross sections of other elements contained in the material is not more than 1.5 target en, and the first mixed material does not contain B, Er, Gd or a mixture thereof, the sum of the thermal neutron absorption cross sections of the other elements contained in the material is not more than 5 target en; the neutron absorber material can be used independently or matched with a second mixed material to be used as an absorber material In the control rod assembly and used for controlling the operating power of the reactor and stopping the reactor, and the second mixed material at least contains one or more of B, Gd, Dy, Tb, Tm, Sm, Eu, Ir, Lu, Ag, In, Cd, Nd and Hf elements; when the neutron absorber material is matched with other absorber materials for use, the mass fraction of the neutron absorber material is between 10% and 90%.
The embodiments 1 to 3 clearly show that the neutron absorber material with high boron loading capacity is more common than the neutron absorber material with high boron loading capacity at present in the aspects of economy and water corrosion resistanceZrB2And B4C has obvious advantages and can be reduced in the whole burnable poison absorber material10The enrichment degree of B, thereby obviously reducing the material cost, and in addition, the AlB12The thermal neutron (E is 0.0253eV) absorption cross section of the medium Al element is smaller than that of the Zr element, the reaction residual toxicity at the end of the service life is smaller, and the service life of the fuel assembly can be prolonged to a certain extent; the corrosion resistance and the thermal conductivity are obviously better than those of B4C and ZrB2The heat generated in the operation process can be led out by the absorber material. The higher thermal conductivity and the better water corrosion resistance can obviously improve the safety of the reactor under the condition that the cladding tube is damaged.
The foregoing shows and describes the general principles and features of the present invention. It will be understood by those skilled in the art that the present invention is not limited to the embodiments described above, which are merely illustrative of the principles of the present invention, but that various changes and modifications may be made without departing from the spirit and scope of the invention, which is defined by the appended claims and their equivalents.

Claims (5)

1. A neutron absorber material with high boron loading capacity, characterized in that the neutron absorber material is a polyB compound, the chemical formula of which is MBxWherein x is not less than 6, the mass fraction of B is not less than 75%, M is Al, Mg, Si, Y elements and the mixture thereof with a thermal neutron absorption cross section not more than 1.5 Bayonine, and the reactivity value of the neutron absorption material body and the safety of the cladding under damage can be improved.
2. The high boron loading neutron absorber material of claim 1, wherein the neutron absorber material can be used alone or in combination with a first hybrid material as a burnable poison assembly absorber material for flattening core neutron fluence distribution, achieving long-term reactivity control and moderator negative temperature coefficient control.
3. The high boron loading neutron absorber material of claim 1, wherein the neutron absorber material is used alone or in combination with a second hybrid material as a control rod assembly absorber material for controlling reactor operating power and shutdown.
4. The high boron loading neutron absorber material of claim 2, wherein the first hybrid material comprises B, Er, Gd, or mixtures thereof, such that the sum of thermal neutron absorption cross sections of other elements contained in the material does not exceed 1.5 target en, and wherein the first hybrid material does not comprise B, Er, Gd, or mixtures thereof, such that the sum of thermal neutron absorption cross sections of other elements contained in the material does not exceed 5 target en.
5. The high boron loading neutron absorber material of claim 3, wherein the second hybrid material contains at least one or more of the elements B, Gd, Dy, Tb, Tm, Sm, Eu, Ir, Lu, Ag, In, Cd, Nd, Hf.
CN202010573534.9A 2019-11-15 2020-06-22 Neutron absorber material with high boron loading capacity Pending CN111573687A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115386836A (en) * 2022-09-05 2022-11-25 上海核工程研究设计院有限公司 Burnable poison coating coated on surface of nuclear fuel pellet and application

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JPH04175700A (en) * 1990-11-08 1992-06-23 Power Reactor & Nuclear Fuel Dev Corp Boron compound neutron shielding material
CN1989262A (en) * 2004-04-22 2007-06-27 艾尔坎国际有限公司 Improved neutron absorption effectiveness for boron content aluminum materials
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115386836A (en) * 2022-09-05 2022-11-25 上海核工程研究设计院有限公司 Burnable poison coating coated on surface of nuclear fuel pellet and application
WO2024051678A1 (en) * 2022-09-05 2024-03-14 上海核工程研究设计院股份有限公司 Burnable poison coating and preparation method therefor, and nuclear fuel element

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