CN115595187A - Nuclear power station composite structure fuel and preparation method thereof - Google Patents
Nuclear power station composite structure fuel and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a composite structure fuel for a nuclear power station and a preparation method thereof, wherein the composite structure fuel for the nuclear power station is prepared from the following raw materials in percentage by mass: 30-70% of raw material A 1 The balance being raw material A 2 And a raw material B, and a raw material A 2 And the mass of the raw material B meets the following requirements: B/(A) 2 + B) =3-50%; the preparation method comprises the following steps: mixing materials, pressing and forming a core part, sintering in the first step, pressing and forming an outer layer, combining and sintering in the second step. The loading of uranium element or plutonium element of the fuel with the composite structure of the nuclear power station reaches 88-92 percent. The preparation method solves the problem of high sintering temperature, is beneficial to reducing sintering difficulty and realizing mass preparation, improves the oxidation resistance of the high-uranium or high-plutonium density fuel when contacting with cooling water, improves the interface combination condition of the core part and the outer layer of the composite structure fuel, and reduces interface thermal resistance.
Description
Technical Field
The invention relates to the technical field of preparation of composite structure fuel pellets, in particular to a composite structure fuel for a nuclear power station and a preparation method thereof.
Background
After an Accident of the fukushima nuclear power station occurs, manufacturing an Accident fault Tolerant Fuel (ATF) capable of bearing the Accident condition for a long time becomes a research focus of the nuclear power industry. ATFs must maintain or improve fuel performance under normal and transient operating conditions and during potential design base events (DBA) and over-design base events (BDBA). The high-uranium-density fuel pellet is beneficial to improving fuel consumption, increasing the fuel circulation length and reducing the volume of spent fuel, thereby effectively improving the safety and the economy of the nuclear power station. High uranium density fuel has a lower oxidation resistance when in contact with cooling water in a Light Water Reactor (LWR) system. In this case, the high uranium density fuel readily reacts with the coolant and loses its structural integrity, resulting in oxidation, shattering, washing and migration of the fuel pellets. Researchers now take a variety of approaches to improve, such as introducing dopants, adding secondary phases, coating protective layers, making composite structural pellets, etc., where making composite structural pellets is most promising for solving this problem.
The invention patent with the patent number of 201911325484.6 provides a UO 2 Composite UN-UO 2 According to the preparation method of the fuel pellet, the protective layer with oxidation resistance is arranged outside the pellet, but the shrinkage rate of the inner composite powder area is larger than that of the outer ring powder area in the sintering process, so that the interface bonding property inside the pellet of the composite structure is poor, the internal thermal resistance of the pellet is increased, and the operation safety of a nuclear power station is reduced. The invention patent with patent number 202210697559.9 provides a composite structure fuel and a preparation method thereof, which prepares composite fuel pellets with good interface bonding by a one-step sintering method, but needs higher sintering temperature.
Disclosure of Invention
The invention aims to solve the technical problem of providing a composite structure fuel for a nuclear power station and a preparation method thereof, aiming at the defects of the prior art.
The technical scheme adopted by the invention for solving the technical problem is as follows: a composite structure fuel for a nuclear power station is prepared from the following raw materials in percentage by mass: 30-70% of raw material A 1 The balance being raw material A 2 And a raw material B, and the raw material A 2 And the mass of the raw material B satisfies: B/(A) 2 + B) =3-50%; the raw material A 1 The raw material A 2 Are all UO respectively 2 Or PuO 2 The raw material B is UN, UC or U 3 Si 2 UCN, UCO, puC or PuN.
Preferably, the nuclear power plant composite structure fuel comprises a core part and an outer layer which are tightly combined, and the nuclear power plant composite structure fuel is a core part and UO which are pressed by high-uranium mixed powder 2 Outer layer of pressed powder, or core and PuO of pressed high plutonium powder blend 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: taking a raw material A 1 Mixing with liquid medium, ball milling, drying and sieving to obtain outer layer material; taking raw material A 2 Mixing with raw material B and liquid medium, ball milling, drying and sieving to obtain core raw material, wherein raw material A 1 Accounting for 30-70 percent of the total mass of the raw materials, wherein the raw material B and the raw material A 2 And the mass percentage B/(A) of the raw material B 2 + B) =3-50%; the raw material A 1 The raw material A 2 Are respectively all UO 2 Or PuO 2 The raw material B is UN, UC or U 3 Si 2 UCN, UCO, puC or PuN;
s2, core part press forming: pressing the core feedstock into a green columnar fuel core at 10-80 MPa;
s3, first-step sintering: sintering the green body of the fuel core part obtained in the step S2 at 500-1400 ℃ and 0-200 MPa to obtain the fuel core part;
s4, outer layer compression molding: pressing the outer layer raw material into a first outer layer green body under the pressure of 10-80 MPa;
s5, combining: placing the fuel core part obtained in the step S3 into the first outer layer green body obtained in the step S4, and pressing a second outer layer green body under the pressure of 10-80MPa to obtain a composite structure fuel assembly;
s6, sintering in the second step: and (3) sintering the composite structure fuel assembly obtained in the step (S5) at the temperature of 1000-1600 ℃ and under the pressure of 0-200 MPa to obtain the composite structure fuel.
Preferably, the feedstock A 1 The raw material A 2 And the raw material B is powder, and the raw material A 1 Particle size D50 of A1 = 0.3-170 μm, the raw material A 2 Particle size D50 of A2 = 0.3-170 μm, particle size D50 of the raw material B B 0.01 to 22 μm, and D50 B ＜D50 A1 ，D50 B ＜D50 A2 。
Preferably, the feedstock A 1 Particle size D50 of A1 = 1-100 μm, the raw material A 2 Particle size D50 of A2 = 1-100 μm, particle size D50 of the raw material B B 0.01 to 10 μm and D50 B ≤0.8D50 A1 ，D50 B ≤0.8D50 A2 。
Preferably, in the step S1, the liquid medium is ethanol or acetone, and the liquid medium and the raw material a are mixed 1 Mixing the liquid medium and the raw material A according to the mass ratio of 1 (3-7) 2 And the raw material B is mixed according to the mass ratio of 1 (3-7).
Preferably, in the step S1, the ball milling medium is silicon nitride, aluminum nitride or zirconium dioxide, the diameter of the milling ball is 4-8mm, and the ball-to-material ratio is (5-8): 1.
Preferably, the ball milling mode in the step S1 is roller ball milling, planetary ball milling or high energy ball milling.
Preferably, when the roller ball milling is selected, the rotating speed is 50-150r/min, and the ball milling time is 6-12 h.
Preferably, when the planetary ball milling is selected, the rotating speed is 150-250r/min, and the ball milling time is 4-6 h.
Preferably, when the high-energy ball milling is selected, the rotating speed is 150-250r/min, and the ball milling time is 4-6 h.
Preferably, in the step S1, the drying temperature is 40-80 ℃, and the drying time is 10-14h; the sieve is 80-120 meshes.
Preferably, in the step S2, the diameter of the core green compact is 6 to 13mm, and the height thereof is 8 to 24mm.
Preferably, in the steps S3 and S6, the sintering mode is at least one of pressureless sintering, hot-pressing sintering and field-assisted sintering, wherein the time of pressureless sintering and hot-pressing sintering is 1-2.5h, and the time of field-assisted sintering is 6-15min; the sintering atmosphere is vacuum, argon or helium.
Preferably, in the step S4, the first outer layer green compact is at least one of a tubular member, a block-shaped member, and a cylindrical member.
Preferably, in the step S5, the second outer layer green compact is at least one of a cylindrical member and a block member.
Preferably, in the step S5, the first outer layer green compact and the second outer layer green compact are combined into a hollow columnar outer layer, the inner diameter of which is 6-13 mm, the height of which is 8-24 mm, and the thickness of which is 1-3 mm.
The invention has the beneficial effects that:
the invention provides a composite structure fuel of a nuclear power station, wherein the mass of uranium element or plutonium element accounts for 88-92% of the total mass of the fuel, and the composite structure fuel is high in uranium or plutonium loading.
The invention provides a preparation method of a nuclear power station composite structure fuel, which solves the problem of high sintering temperature by pre-sintering a core part, and is beneficial to reducing sintering difficulty and preparing the fuel on a large scale; through the design of the core part, the outer layer and raw materials thereof, the oxidation resistance of the high-uranium or high-plutonium density fuel in contact with cooling water is improved, and the application of the nuclear fuel in a light water reactor is promoted; the preparation method of the two-step sintering improves the interface bonding condition of the core part and the outer layer in the composite structure fuel, reduces the interface thermal resistance of the composite structure fuel, and accordingly prepares the composite structure fuel of the nuclear power station, which has a good interface bonding effect and high uranium or plutonium loading.
Drawings
FIG. 1 is a schematic cross-sectional structural view of a composite structural fuel assembly according to some embodiments of the present invention;
FIG. 2 is a schematic cross-sectional structural view of a composite structural fuel assembly according to some embodiments of the present invention;
FIG. 3 is a schematic cross-sectional structural view of a composite structural fuel assembly according to some embodiments of the present invention.
Detailed Description
In order to clearly understand the technical features, objects and effects of the present invention, the present invention will be further described in detail with reference to the following embodiments, which are only used for explaining the present invention and are not to be construed as limiting the scope of the present invention.
A composite structure fuel for a nuclear power station is prepared from the following raw materials in percentage by mass: 30-70% of raw material A 1 The balance being raw material A 2 And a raw material B, and a raw material A 2 And the mass of the raw material B meets the following requirements: B/(A) 2 + B) =3-50%; starting materials A 1 Raw Material A 2 Are respectively all UO 2 Or PuO 2 Raw material B is UN, UC, U 3 Si 2 UCN, UCO, puC or PuN.
The composite structure fuel of the nuclear power station comprises a core part and an outer layer which are tightly combined, and the composite structure fuel of the nuclear power station is a core part and UO which are pressed by high-uranium mixed powder 2 Outer layer of pressed powder, or core and PuO of pressed high plutonium powder blend 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps:
s1, mixing materials: taking raw material A 1 Mixing with liquid medium according to the mass ratio of (3-7) to 1, ball-milling, drying at 40-80 ℃ for 10-14h, and sieving with 80-120 mesh sieve to obtain outer layer raw material; taking a raw material A 2 Mixing the raw material B with a liquid medium according to the mass ratio of (3-7) to 1, performing ball milling, drying at 40-80 ℃ for 10-14h, and sieving with a 80-120-mesh sieve to obtain a core raw material; wherein, the raw material A 1 Accounting for 30-70 percent of the total mass of the raw materials, wherein the raw material B and the raw material A 2 And the mass percentage B/(A) of the raw material B 2 +B)＝3-50％。
Starting materials A 1 The raw material A 2 Are respectively all UO 2 Or PuO 2 Raw material B is UN, UC, U 3 Si 2 UCN, UCO, puC or PuN. Starting materials A 1 Raw Material A 2 And raw material B are powder, raw material A 1 Particle size D50 of A1 = 0.3-170 μm, raw material A 2 Particle size D50 of A2 = 0.3-170 μm, particle size D50 of raw material B B =0.01 to 22 μm and D50 B ＜D50 A1 ，D50 B ＜D50 A2 . Preferably, the starting material A 1 Particle size D50 of A1 1-100 μm, raw material A 2 Particle size D50 of A2 = 1-100 μm, particle size D50 of raw material B B 0.01 to 10 μm and D50 B ≤0.8D50 A1 ，D50 B ≤0.8D50 A2 。
The liquid medium is ethanol or acetone. The ball milling medium is silicon nitride, aluminum nitride or zirconium dioxide, the diameter of the milling ball is 4-8mm, and the ball-to-material ratio is (5-8) to 1. The ball milling mode is roller ball milling, planetary ball milling or high-energy ball milling. When roller ball milling is selected, the rotating speed is 50-150r/min, and the ball milling time is 6-12 h; when planetary ball milling is selected, the rotating speed is 150-250r/min, and the ball milling time is 4-6 h; when high-energy ball milling is selected, the rotating speed is 150-250r/min, and the ball milling time is 4-6 h.
S2, core part press forming: pressing the core raw material into a columnar fuel core green compact under 10-80MPa, wherein the diameter of the columnar fuel core green compact is 6-13 mm, and the height of the columnar fuel core green compact is 8-24 mm.
S3, first-step sintering: sintering the green compact of the fuel core part obtained in the step S2 at 500-1400 ℃ and 0-200 MPa to obtain the fuel core part; the sintering mode is at least one of pressureless sintering, hot-pressing sintering and field-assisted sintering, wherein the pressureless sintering time and the hot-pressing sintering time are 1-2.5h, and the field-assisted sintering time is 6-15min; the sintering atmosphere is vacuum, argon or helium.
S4, outer layer compression molding: pressing the outer layer raw material into a first outer layer green body under the pressure of 10-80 MPa; the first outer layer green compact is at least one of a tubular member, a block member, and a cylindrical member.
S5, combining: and (4) placing the fuel core part obtained in the step (S3) into the first outer layer green body obtained in the step (S4), and pressing a second outer layer green body under the pressure of 10-80MPa to obtain the composite structure fuel assembly. Wherein, the second outer layer green compact is at least one of a cylindrical component and a block component. The first outer layer green compact and the second outer layer green compact are combined into a hollow columnar outer layer, the inner diameter of the outer layer is 6-13 mm, the height of the outer layer is 8-24 mm, and the thickness of the outer layer is 1-3 mm.
S6, sintering in the second step: and sintering the composite structure fuel assembly obtained in the step S5 at 1000-1600 ℃ and 0-200 MPa to obtain the composite structure fuel. The sintering mode is at least one of pressureless sintering, hot-pressing sintering and field-assisted sintering, wherein the pressureless sintering time and the hot-pressing sintering time are 1-2.5h, and the field-assisted sintering time is 6-15min; the sintering atmosphere is vacuum, argon or helium.
The invention provides a composite structure fuel of a nuclear power station, wherein the mass of uranium element or plutonium element accounts for 88-92% of the total mass of the fuel, and the composite structure fuel is high in uranium or plutonium loading.
The invention provides a preparation method of a composite structure fuel of a nuclear power station, which takes a raw material A 1 Preparing a core from raw material A 2 The outer layer is prepared from the raw material B, so that the oxidation resistance of the high-uranium-density fuel in contact with cooling water is improved, and on one hand, the outer layer of the fuel can be used as a protective layer to prevent the cooling water from directly contacting and reacting with the raw material B of the core part; on the other hand, when the core is the uniformly dispersed raw material A 1 When the raw material B is blended, the outer layer is broken, and then the raw material A 1 The reaction of the raw material B and water can be delayed or weakened, so that the application of the nuclear fuel in a light water reactor is promoted.
In addition, the nuclear power station composite structure fuel is prepared by a two-step sintering method, the interface bonding condition of the core part and the outer layer in the fuel is improved, the thermal resistance is increased due to the fact that the thermal conductivity of air is lower than that of the composite material, if gaps exist at the interface, the thermal resistance is increased, the bonding strength of the core part and the outer layer is improved, the gaps at the interface can be reduced, and the scattering phenomenon caused by the gaps encountered by phonons in the transmission process is reduced, so that the interface thermal resistance is reduced, and the thermal conductivity of the composite structure fuel is improved. Compared with a one-step sintering preparation method, the core of the composite structure fuel is pre-sintered, so that the sintering temperature is reduced, the sintering difficulty is reduced, and the mass preparation is realized.
The following is illustrated by specific examples:
examples 1 to 1
As shown in fig. 1, the composite structure fuel for the nuclear power plant is prepared from the following raw materials in percentage by mass: 50% of raw material A 1 48.5% of raw material A 2 And 1.5% of raw material B, raw material A 1 And raw material A 2 Are all UO 2 And raw material B is UN.
The composite structure fuel of the nuclear power station comprises a core part and an outer layer which are tightly combined, and the composite structure fuel of the nuclear power station is a core part and a UO (urea) which are pressed by high-uranium mixed powder 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: 50% of UO with a particle size of 1 μm is taken 2 Mixing with absolute ethyl alcohol according to a mass ratio of 5 2 And 1.5% UN with the particle size of 0.01 mu m and absolute ethyl alcohol are mixed according to the mass ratio of 5.
S2, core part press forming: the core feedstock was pressed at 50MPa to a green cylindrical fuel core with a diameter of 7.90mm and a height of 14.00mm.
S3, first-step sintering: and (3) carrying out field-assisted sintering on the green fuel core part obtained in the step (S2) for 6min at 500 ℃ and 30MPa in a helium atmosphere to obtain the fuel core part 200a.
S4, outer layer compression molding: the outer layer raw material was pressed under a pressure of 50MPa into a first outer layer green compact comprising a round tube 110a having an inner diameter of 7.90mm, an outer diameter of 10.00mm and a height of 16.00mm and a round block 120a having a diameter of 7.90mm and a thickness of 1.00mm, the round block 120a being used to close the bottom end of the round tube 110 a.
S5, combining: and (4) placing the fuel core obtained in the step (S3) into the first outer layer green compact obtained in the step (S4), and pressing to obtain a second outer layer green compact under the pressure of 50MPa to obtain the composite structure fuel assembly. The second outer layer green compact is a round block 130a used for sealing the top end of the round tube 110a, the diameter of the round block is 7.90mm, the thickness of the round block is 1.00mm, and the first outer layer green compact and the second outer layer green compact are combined into a hollow columnar outer layer 100a.
S6, sintering in the second step: and (4) carrying out field-assisted sintering on the composite structure fuel assembly obtained in the step (S5) for 6min at 1000 ℃ and 30MPa in helium atmosphere to obtain the composite structure fuel.
This example prepares UN-UO 2 The core part is composed of UO 2 The ratio of the measured pellet density to the theoretical pellet density is calculated to obtain the pellet densityThe density reaches 98%, and the interface between the core and the outer layer is tightly combined.
Examples 1 to 2
As shown in fig. 1, the composite structure fuel for the nuclear power plant is prepared from the following raw materials in percentage by mass: 30% of raw material A 1 35% of raw material A 2 And 35% of raw material B, raw material A 1 And raw material A 2 Are all UO 2 The raw material B is UC.
The composite structure fuel of the nuclear power station comprises a core part and an outer layer which are tightly combined, and the composite structure fuel of the nuclear power station is a core part and a UO (urea) which are pressed by high-uranium mixed powder 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: 30% of UO with particle size of 100 μm 2 Mixing with anhydrous ethanol according to the mass ratio of 3 2 And 35% of UC with the particle size of 10 microns is mixed with absolute ethyl alcohol according to the mass ratio of 3.
S2, core part press forming: the core feedstock was pressed at 10MPa to a green cylindrical fuel core with a diameter of 6.00mm and a height of 8.00mm.
S3, first-step sintering: and (3) carrying out field-assisted sintering on the green fuel core part obtained in the step (S2) at 1400 ℃ and 150MPa for 15min in an argon atmosphere to obtain the fuel core part 200a.
S4, outer layer compression molding: the outer layer raw material is pressed into a first outer layer green body under the pressure of 10MPa, and the first outer layer green body comprises a circular tube 110a with the inner diameter of 6.00mm, the outer diameter of 10.00mm and the height of 10.00mm and a round block 120a with the diameter of 6.00mm and the thickness of 1.00mm, wherein the round block 110a is used for closing the bottom end of the circular tube 110 a.
S5, combining: and (4) placing the fuel core part obtained in the step (S3) into the first outer layer green body obtained in the step (S4), and pressing a second outer layer green body under the pressure of 10MPa to obtain the composite structure fuel assembly. The second outer layer green compact is a round block 130a used for sealing the top end of the round tube 110a, the diameter of the round block is 6.00mm, the thickness of the round block is 1.00mm, and the first outer layer green compact and the second outer layer green compact are combined into the hollow columnar outer layer 100a.
S6, sintering in the second step: and (3) carrying out field-assisted sintering on the composite structure fuel assembly obtained in the step (S5) at 1600 ℃ and 150MPa for 15min in an argon atmosphere to obtain the composite structure fuel.
This example prepares UC-UO 2 The core part is composed of UO 2 The density of the wrapped composite structure fuel pellet can reach 98 percent by calculating the ratio of the actually measured pellet density to the theoretical pellet density, and the interface of the core and the outer layer is tightly combined.
Examples 1 to 3
As shown in fig. 1, the composite structure fuel for the nuclear power plant is prepared from the following raw materials in percentage by mass: 70% of raw material A 1 22.5% of raw material A 2 And 7.5% of raw material B, raw material A 1 And raw material A 2 Are all UO 2 And the raw material B is UCN.
The composite structure fuel of the nuclear power station comprises a core part and an outer layer which are tightly combined, and the composite structure fuel of the nuclear power station is a core part and UO which are pressed by high-uranium mixed powder 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: taking 70% UO with particle size of 10 μm 2 Mixing with acetone at a mass ratio of 7 2 And 7.5% of UCN with the particle size of 4 mu m is mixed with acetone according to the mass ratio of 7.
S2, core part press forming: the core feedstock was pressed at 80MPa to a green cylindrical fuel core with a diameter of 13.00mm and a height of 18.00mm.
S3, first-step sintering: and (3) carrying out field-assisted sintering on the green fuel core part obtained in the step (S2) at 1400 ℃ and 200MPa for 9min in an argon atmosphere to obtain the fuel core part 200a.
S4, outer layer compression molding: the outer layer raw material was pressed under a pressure of 80MPa into a first outer layer green compact comprising a round tube 110a having an inner diameter of 13.00mm, an outer diameter of 15.00mm and a height of 24.00mm and a round block 120a having a diameter of 13.00mm and a thickness of 3.00mm, the round block 110a being used to close the bottom end of the round tube 110 a.
S5, combining: and (4) placing the fuel core part obtained in the step (S3) into the first outer layer green body obtained in the step (S4), and pressing a second outer layer green body under the pressure of 80MPa to obtain the composite structure fuel assembly. The second outer layer green compact is a round block 130a for closing the top end of the round tube 110a, the diameter of the round block is 13.00mm, the thickness of the round block is 3.00mm, and the first outer layer green compact and the second outer layer green compact are combined into the hollow columnar outer layer 100a.
S6, sintering in the second step: and (4) carrying out field-assisted sintering on the composite structure fuel assembly obtained in the step (S5) at 1200 ℃ and 200MPa for 9min in the presence of argon to obtain the composite structure fuel.
This example prepares UCN-UO 2 The core part is composed of UO 2 The density of the wrapped composite structure fuel pellet can reach 98 percent by calculating the ratio of the measured pellet density to the theoretical pellet density, and the interface of the core and the outer layer is tightly combined.
Example 2-1
As shown in fig. 2, the composite structure fuel for the nuclear power plant is prepared from the following raw materials in percentage by mass: 60% of raw material A 1 24% of raw material A 2 And 16% of raw material B, raw material A 1 And raw material A 2 Are all UO 2 The raw material B is UCO.
The composite structure fuel of the nuclear power station comprises a core part and an outer layer which are tightly combined, and the composite structure fuel of the nuclear power station is a core part and UO which are pressed by high-uranium mixed powder 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: 60% of UO with particle size of 1 μm 2 Mixing with acetone according to a mass ratio of 4 2 And 16% of UCO with the particle size of 0.01 mu m is mixed with acetone according to the mass ratio of 4.
S2, core part press forming: the core feedstock was pressed at 20MPa to a green cylindrical fuel core with a diameter of 9.00mm and a height of 20.00mm.
S3, first-step sintering: and (3) carrying out hot-pressing sintering on the green fuel core part obtained in the step (S2) for 1h at 600 ℃ and 100MPa in a helium atmosphere to obtain a fuel core part 200b.
S4, outer layer compression molding: the outer layer raw material was pressed under a pressure of 20MPa into a first outer layer green compact, which was a cylinder 110b with an inner diameter of 9.00mm, an outer diameter of 11.00mm and a height of 11.00 mm.
S5, combining: and (4) placing the fuel core obtained in the step (S3) into the first outer layer green compact obtained in the step (S4), and pressing to obtain a second outer layer green compact under the pressure of 20MPa to obtain the composite structure fuel assembly. Wherein the second outer layer green compact is a cylinder 120b having an inner diameter of 9.00mm, an outer diameter of 11.00mm and a height of 11.00mm, and the first outer layer green compact and the second outer layer green compact are combined into a hollow columnar outer layer 100b.
S6, sintering in the second step: and (4) carrying out hot-pressing sintering on the composite structure fuel assembly obtained in the step (S5) for 1h at 1200 ℃ and 100MPa in helium to obtain the composite structure fuel.
This example prepares UCO-UO 2 The core part is composed of UO 2 The density of the wrapped composite structure fuel pellet can reach 98 percent by calculating the ratio of the actually measured pellet density to the theoretical pellet density, and the interface of the core and the outer layer is tightly combined.
Examples 2 to 2
As shown in fig. 2, the composite structure fuel for the nuclear power plant is prepared from the following raw materials in percentage by mass: 40% of raw material A 1 54% of raw material A 2 And 6% of raw material B, raw material A 1 And raw material A 2 Are all UO 2 The raw material B is U 3 Si 2 。
The composite structure fuel of the nuclear power station comprises a core part and an outer layer which are tightly combined, and the composite structure fuel of the nuclear power station is a core part and a UO (urea) which are pressed by high-uranium mixed powder 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: taking 40% UO with particle diameter of 0.3 μm 2 Mixing with acetone according to a mass ratio of 6 2 And 6% of U having a particle diameter of 0.01 μm 3 Si 2 Mixing with acetone according to a mass ratio of 6.
S2, core part press forming: the core raw material was pressed at 30MPa to give a green columnar fuel core having a diameter of 10.00mm and a height of 16.00mm.
S3, first-step sintering: and (3) carrying out hot-pressing sintering on the green fuel core part obtained in the step (S2) for 2h at 700 ℃ and 120MPa in a helium atmosphere to obtain the fuel core part 200b.
S4, outer layer compression molding: the outer layer raw material was pressed under a pressure of 30MPa into a first outer layer green compact, which was a cylinder 110b having an inner diameter of 10.00mm, an outer diameter of 12.00mm, and a height of 10.00 mm.
S5, combining: and (4) placing the fuel core part obtained in the step (S3) into the first outer layer green body obtained in the step (S4), and pressing a second outer layer green body under the pressure of 20MPa to obtain the composite structure fuel assembly. Wherein the second outer layer green compact is a cylinder 120b having an inner diameter of 10.00mm, an outer diameter of 12.00mm and a height of 10.00mm, and the first outer layer green compact and the second outer layer green compact are combined into a hollow columnar outer layer 100b.
S6, sintering in the second step: and (4) carrying out hot-pressing sintering on the composite structure fuel assembly obtained in the step (S5) for 2 hours at 1400 ℃ and 80MPa in the atmosphere of helium to obtain the composite structure fuel.
Prepared to U in this example 3 Si 2 -UO 2 The core part is composed of UO 2 The density of the wrapped composite structure fuel pellet can reach 98 percent by calculating the ratio of the measured pellet density to the theoretical pellet density, and the interface of the core and the outer layer is tightly combined.
Examples 2 to 3
As shown in fig. 2, the composite structure fuel for the nuclear power plant is prepared from the following raw materials in percentage by mass: 55% of raw material A 1 31.5% of raw material A 2 And 13.5% of raw material B, raw material A 1 And raw material A 2 Are all PuO 2 And the raw material B is PuC.
The fuel with the composite structure for the nuclear power plant comprises a core part and an outer layer which are tightly combined, and the fuel with the composite structure for the nuclear power plant is a core part and PuO (PuO) which are pressed by high plutonium mixed powder 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: taking 55% PuO with particle size of 170 μm 2 Mixing with acetone at a mass ratio of 5.5 2 And 13.5% of PuC with the particle size of 22 mu m is mixed with acetone according to the mass ratio of 5.5.
S2, core part press forming: the core feedstock was pressed at 70MPa to a green cylindrical fuel core with a diameter of 7.00mm and a height of 18.00mm.
S3, first-step sintering: and (3) carrying out hot-pressing sintering on the green fuel core part obtained in the step (S2) for 2.5h at 800 ℃ and 180MPa in a sintering atmosphere of helium to obtain the fuel core part 200b.
S4, outer layer compression molding: the outer layer raw material was pressed under a pressure of 70MPa into a first outer layer green compact, which was a cylinder 110b having an inner diameter of 7.00mm, an outer diameter of 9.00mm and a height of 12.00 mm.
S5, combining: and (4) placing the fuel core part obtained in the step (S3) into the first outer layer green body obtained in the step (S4), and pressing a second outer layer green body under the pressure of 70MPa to obtain the composite structure fuel assembly. Wherein the second outer layer green compact is a cylinder 120b having an inner diameter of 7.00mm, an outer diameter of 9.00mm and a height of 12.00mm, and the first outer layer green compact and the second outer layer green compact are combined into a hollow columnar outer layer 100b.
S6, sintering in the second step: and (3) carrying out hot-pressing sintering on the composite structure fuel assembly obtained in the step (S5) for 2.5h at 1450 ℃ and 180MPa in a helium atmosphere to obtain the composite structure fuel.
PuC-PuO prepared in this example 2 The core is made of PuO 2 The density of the wrapped composite structure fuel pellet can reach 98 percent by calculating the ratio of the actually measured pellet density to the theoretical pellet density, and the interface of the core and the outer layer is tightly combined.
Example 3-1
As shown in fig. 3, the composite structure fuel for the nuclear power plant is prepared from the following raw materials in percentage by mass: 45% of raw material A 1 44% of raw material A 2 And 11% of raw material B, raw material A 1 And raw material A 2 Are all PuO 2 And the raw material B is PuN.
The composite structure fuel of the nuclear power station comprises a core part and an outer layer which are tightly combined, and the composite structure fuel of the nuclear power station is a core part and PuO (Puo) which are formed by pressing high plutonium mixed powder 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: taking 45% of PuO with the particle size of 150 mu m 2 Mixing with acetone according to the mass ratio of 3.5 2 And 11% of PuN with the particle size of 15 mu m and acetone are mixed according to the mass ratio of 3.5To the outer layer material and the core material.
S2, core part press forming: the core feedstock was pressed at 60MPa to a green cylindrical fuel core with a diameter of 12.00mm and a height of 22.00mm.
S3, first-step sintering: and (3) sintering the green fuel core part obtained in the step (S2) at 900 ℃ and 0MPa in a vacuum pressureless mode for 1.5h to obtain the fuel core part 200c.
S4, outer layer compression molding: the outer layer feedstock was pressed at a pressure of 60MPa into a first outer layer green body which was a cylinder 110c having an inner diameter of 12.00mm, an outer diameter of 15.00mm and a height of 24.00 mm.
S5, combining: and (4) placing the fuel core obtained in the step (S3) into the first outer layer green compact obtained in the step (S4), and pressing to obtain a second outer layer green compact under the pressure of 60MPa to obtain the composite structure fuel assembly. The second outer layer green compact is a round block 120c for closing the cylinder 110c, the diameter of the round block is 12.00mm, the thickness of the round block is 1.00mm, and the first outer layer green compact and the second outer layer green compact are combined into a hollow columnar outer layer 100c.
S6, sintering in the second step: and (4) sintering the composite structure fuel assembly obtained in the step (S5) at 1500 ℃ and 0MPa in a vacuum pressureless mode for 1.5h, wherein the sintering atmosphere is helium gas, and thus obtaining the composite structure fuel.
PuN-PuO prepared in this example 2 The core part is made of PuO 2 The density of the wrapped composite structure fuel pellet can reach 98 percent by calculating the ratio of the measured pellet density to the theoretical pellet density, and the interface of the core and the outer layer is tightly combined.
Example 3-2
As shown in fig. 3, the composite structure fuel for the nuclear power plant is prepared from the following raw materials in percentage by mass: 65% of raw material A 1 20% of raw material A 2 And 15% of raw material B, raw material A 1 And raw material A 2 Are all PuO 2 And the raw material B is PuN.
The composite structure fuel of the nuclear power station comprises a core part and an outer layer which are tightly combined, and the composite structure fuel of the nuclear power station is a core part and PuO (Puo) which are formed by pressing high plutonium mixed powder 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: taking 65% of PuO with the particle size of 80 mu m 2 Mixing with acetone according to the mass ratio of 3 2 And 15% of PuN with the particle size of 8 microns is mixed with acetone according to the mass ratio of 3.
S2, core part press forming: the core feedstock was pressed at 30MPa to a green cylindrical fuel core with a diameter of 8.00mm and a height of 20.00mm.
S3, first-step sintering: and (3) sintering the green fuel core obtained in the step (S2) at 1000 ℃ and 0MPa in a vacuum pressureless manner for 1h to obtain a fuel core 200c.
S4, outer layer compression molding: the outer layer raw material was pressed under a pressure of 30MPa into a first outer layer green compact which was a cylinder 110c having an inner diameter of 8.00mm, an outer diameter of 11.00mm and a height of 24.00 mm.
S5, combining: and (4) placing the fuel core part obtained in the step (S3) into the first outer layer green body obtained in the step (S4), and pressing a second outer layer green body under the pressure of 60MPa to obtain the composite structure fuel assembly. Wherein the second outer layer green compact is a round block 120c for closing the cylinder 110c, the diameter of which is 8.00mm, and the thickness of which is 2.00mm, and the first outer layer green compact and the second outer layer green compact are combined into a hollow columnar outer layer 100c.
S6, sintering in the second step: and (4) sintering the composite structure fuel assembly obtained in the step (S5) at 1300 ℃ and 0MPa in a vacuum pressureless mode for 1h, wherein the sintering atmosphere is helium gas, and thus obtaining the composite structure fuel.
PuN-PuO prepared in this example 2 The core part is made of PuO 2 The density of the wrapped composite structure fuel pellet can reach 98 percent by calculating the ratio of the actually measured pellet density to the theoretical pellet density, and the interface of the core and the outer layer is tightly combined.
Examples 3 to 3
As is further shown in figure 3 of the drawings,a composite structure fuel for a nuclear power station is prepared from the following raw materials in percentage by mass: 70% of raw material A 1 20% of raw material A 2 And 10% of raw material B, raw material A 1 And raw material A 2 Are all PuO 2 And the raw material B is PuC.
The composite structure fuel of the nuclear power station comprises a core part and an outer layer which are tightly combined, and the composite structure fuel of the nuclear power station is a core part and PuO (Puo) which are formed by pressing high plutonium mixed powder 2 The powder is pressed into an outer layer and is sintered in two steps.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: taking 70% of PuO with the particle size of 100 mu m 2 Mixing with absolute ethyl alcohol according to a mass ratio of 7 2 Mixing 10% of PuC with the particle size of 10 microns with absolute ethyl alcohol according to the mass ratio of 7.
S2, core part press forming: the core feedstock was pressed at 50MPa to a green cylindrical fuel core with a diameter of 8.00mm and a height of 16.00mm.
S3, first-step sintering: and (3) carrying out vacuum pressureless sintering on the green fuel core part obtained in the step (S2) at 800 ℃ and 0MPa for 2.5h to obtain the fuel core part 200c.
S4, outer layer compression molding: the outer layer feedstock was pressed at a pressure of 50MPa into a first outer layer green compact which was a cylinder 110c having an inner diameter of 8.00mm, an outer diameter of 11.00mm and a height of 22.00mm.
S5, combining: and (4) placing the fuel core obtained in the step (S3) into the first outer layer green compact obtained in the step (S4), and pressing to obtain a second outer layer green compact under the pressure of 50MPa to obtain the composite structure fuel assembly. Wherein the second outer layer green compact is a round block 120c for closing the cylinder 110c, the diameter of which is 8.00mm, and the thickness of which is 3.00mm, and the first outer layer green compact and the second outer layer green compact are combined into a hollow columnar outer layer 100c.
S6, sintering in the second step: and (3) sintering the composite structure fuel assembly obtained in the step (S5) at 1600 ℃ and 0MPa in a vacuum pressureless mode for 2.5h, wherein the sintering atmosphere is helium gas, and thus obtaining the composite structure fuel.
PuC-PuO prepared in this example 2 The core is made of PuO 2 The density of the wrapped composite structure fuel pellet can reach 98 percent by calculating the ratio of the actually measured pellet density to the theoretical pellet density, and the interface of the core and the outer layer is tightly combined.
Comparative examples 1-1
As shown in fig. 1, the composite structure fuel for the nuclear power plant is prepared from the following raw materials in percentage by mass: 50% of raw material A 1 48.5% of raw material A 2 And 1.5% of raw material B, raw material A 1 And raw material A 2 Are all UO 2 And raw material B is UN.
The composite structure fuel of the nuclear power station comprises a core part and an outer layer which are tightly combined, and the composite structure fuel of the nuclear power station is a core part and UO which are pressed by high-uranium mixed powder 2 The outer layer pressed by the powder is formed by one-step sintering.
The preparation method of the composite structure fuel for the nuclear power station comprises the following steps of:
s1, mixing materials: 50% of UO with a particle size of 1 μm is taken 2 Mixing with absolute ethyl alcohol according to a mass ratio of 5 2 And mixing 1.5% of UN with the particle size of 0.01 mu m and absolute ethyl alcohol according to the mass ratio of 5.
S2, core part press forming: the core feedstock was pressed at 50MPa to a green cylindrical fuel core with a diameter of 7.90mm and a height of 14.00mm.
S3, outer layer compression molding: the outer layer raw material is pressed into an outer layer green body under the pressure of 50MPa, and the outer layer green body comprises a round pipe 110a with the inner diameter of 7.90mm, the outer diameter of 10.00mm and the height of 16.00mm, a round block 120a and a round block 130a with the diameter of 7.90mm and the thickness of 1.00mm, wherein the round block 120a and the round block 130a are used for sealing two ends of the round pipe 110a, and the round pipe 110a, the round block 120a and the round block 130a are combined into a hollow columnar outer layer 100a.
S4, combining: and (3) placing the green fuel core obtained in the step (S2) into the green outer layer obtained in the step (S3) to obtain the composite structure fuel assembly.
S5, sintering: and (4) carrying out field-assisted sintering on the composite structure fuel assembly obtained in the step (S4) for 6min at 1700 ℃ and 30MPa in helium atmosphere to obtain the composite structure fuel.
Preparation of this comparative example gave UN-UO 2 The core part is composed of UO 2 The density of the wrapped composite structure fuel pellet reaches 97 percent and the interface of the core and the outer layer is tightly combined by calculating the ratio of the actually measured pellet density to the theoretical pellet density.
Compared with the preparation method of the embodiment 1-1, the comparative example 1-1-1 prepares the composite structure fuel by one-step sintering after combining the core green body and the outer layer green body, the density of the composite structure fuel is similar to that of the composite structure fuel of the invention, but the sintering temperature reaches 1700 ℃, and the temperature of one-step sintering is usually 1700-1800 ℃.
The first step sintering temperature in the two-step sintering method is 500-1400 ℃, and the second step sintering temperature is 1000-1600 ℃, so that the sintering temperature is obviously reduced compared with the one-step sintering method. In addition, tests show that the density of the composite structure fuel is reduced by about 15% when the sintering temperature is reduced by 200 ℃, and the influence of the temperature on the density is large. In addition, the density of the fuel pellet reaches the standard when being more than 95 percent, if the temperature of one-step sintering is reduced, the density of the fuel with the composite structure does not reach the standard, which is also one of the reasons that the sintering temperature is difficult to reduce, but the invention can ensure that the density of the fuel pellet reaches the standard when the sintering temperature is reduced.
In conclusion, the core part of the fuel with the composite structure of the nuclear power station is pre-sintered, so that the problem of high sintering temperature is solved, and the sintering difficulty is reduced and the mass preparation is facilitated; through the design of the core part, the outer layer and the raw materials thereof, the oxidation resistance of the high-uranium or high-plutonium density fuel in contact with cooling water is improved, and the application of the nuclear fuel in a light water reactor is promoted; the preparation method of the two-step sintering improves the interface bonding condition of the core part and the outer layer in the composite structure fuel, reduces the interface thermal resistance of the composite structure fuel, and accordingly prepares the composite structure fuel of the nuclear power station, which has a good interface bonding effect and high uranium or plutonium loading.
The above description is only an embodiment of the present invention, and not intended to limit the scope of the present invention, and all modifications of equivalent structures and equivalent processes, which are made by the present specification, or directly or indirectly applied to other related technical fields, are included in the scope of the present invention.
Claims (17)
1. The composite structure fuel for the nuclear power station is characterized by being prepared from the following raw materials in percentage by mass: 30-70% of raw material A 1 The balance being raw material A 2 And a raw material B, and the raw material A 2 And the mass of the raw material B satisfies the following conditions: B/(A) 2 +B)＝3-50％；
The raw material A 1 The raw material A 2 Are respectively all UO 2 Or PuO 2 The raw material B is UN, UC or U 3 Si 2 UCN, UCO, puC or PuN.
2. The nuclear power plant composite structure fuel according to claim 1, comprising a tightly bonded core and skin, and the nuclear power plant composite structure fuel is a core and UO pressed from high uranium mixed powder 2 Outer layer of pressed powder, or core and PuO of pressed high plutonium powder blend 2 The powder is pressed into an outer layer and is sintered in two steps.
3. A method for preparing a composite structure fuel of a nuclear power plant as claimed in claim 1, wherein the method comprises the following steps:
s1, mixing materials: taking a raw material A 1 Mixing with liquid medium, ball milling, drying and sieving to obtain outer layer material; taking a raw material A 2 Mixing with raw material B and liquid medium, ball milling, drying and sieving to obtain core raw material, wherein raw material A 1 Accounting for 30-70 percent of the total mass of the raw materials, wherein the raw material B and the raw material A 2 And the mass percentage B/(A) of the raw material B 2 + B) =3-50%; the raw material A 1 The raw material A 2 Are all UO respectively 2 Or PuO 2 The raw material B is UN, UC or U 3 Si 2 UCN, UCO, puC or PuN;
s2, core part press forming: pressing the core raw material into a columnar fuel core green body under 10-80 MPa;
s3, first-step sintering: sintering the green body of the fuel core part obtained in the step S2 at 500-1400 ℃ and 0-200 MPa to obtain the fuel core part;
s4, outer layer compression molding: pressing the outer layer raw material into a first outer layer green body under the pressure of 10-80 MPa;
s5, combining: placing the fuel core part obtained in the step S3 into the first outer layer green body obtained in the step S4, and pressing a second outer layer green body under the pressure of 10-80MPa to obtain a composite structure fuel assembly;
s6, sintering in the second step: and (3) sintering the composite structure fuel assembly obtained in the step (S5) at the temperature of 1000-1600 ℃ and under the pressure of 0-200 MPa to obtain the composite structure fuel.
4. Method for producing a fuel for a nuclear power plant composite structure according to claim 3, characterized in that the raw material A is 1 The raw material A 2 And the raw material B is powder, and the raw material A 1 Particle size D50 of A1 = 0.3-170 μm, the raw material A 2 Particle size D50 of A2 = 0.3-170 μm, particle size D50 of the raw material B B =0.01 to 22 μm and D50 B ＜D50 A1 ，D50 B ＜D50 A2 。
5. Method for producing a fuel for a nuclear power plant composite structure according to claim 4, characterized in that the raw material A is 1 Particle size D50 of A1 = 1-100 μm, the raw material A 2 Particle size D50 of A2 = 1-100 μm, particle size D50 of the raw material B B ＝0.01～10μm，And D50 B ≤0.8D50 A1 ，D50 B ≤0.8D50 A2 。
6. The method for preparing the composite structural fuel of the nuclear power plant as claimed in claim 3, wherein in the step S1, the liquid medium is ethanol or acetone, and the liquid medium and the raw material A are mixed 1 Mixing the liquid medium and the raw material A according to the mass ratio of 1 (3-7) 2 And the raw material B is mixed according to the mass ratio of 1 (3-7).
7. The preparation method of the composite structure fuel of the nuclear power plant as claimed in claim 3, wherein in the step S1, the ball milling medium is silicon nitride, aluminum nitride or zirconium dioxide, the diameter of a milling ball is 4-8mm, and the ball-to-material ratio is (5-8): 1.
8. The preparation method of the fuel with the composite structure in the nuclear power plant according to claim 3, wherein the ball milling in the step S1 is roller ball milling, planetary ball milling or high-energy ball milling.
9. The preparation method of the composite structure fuel of the nuclear power plant as recited in claim 8, wherein the rotation speed is 50-150r/min and the ball milling time is 6-12 h when the roller ball milling is selected.
10. The preparation method of the composite structure fuel of the nuclear power plant as recited in claim 8, wherein the rotation speed is 150-250r/min and the ball milling time is 4-6 h when planetary ball milling is selected.
11. The preparation method of the nuclear power plant composite structure fuel as recited in claim 8, wherein the high energy ball milling is selected, the rotation speed is 150-250r/min, and the ball milling time is 4-6 h.
12. The preparation method of the composite structure fuel of the nuclear power plant as claimed in claim 3, wherein in the step S1, the drying temperature is 40-80 ℃, and the drying time is 10-14h; the sieve is 80-120 meshes.
13. The method for preparing a composite structural fuel of a nuclear power plant as recited in claim 3, wherein, in the step S2, the core green compact has a diameter of 6 to 13mm and a height of 8 to 24mm.
14. The method for preparing the composite structural fuel of the nuclear power plant as recited in claim 3, wherein in the steps S3 and S6, the sintering mode is at least one of pressureless sintering, hot-pressing sintering and field-assisted sintering, wherein the pressureless sintering and hot-pressing sintering time is 1-2.5 hours, and the field-assisted sintering time is 6-15min; the sintering atmosphere is vacuum, argon or helium.
15. The method for preparing a composite structural fuel of a nuclear power plant as recited in claim 3, wherein in the step S4, the first outer layer green compact is at least one of a tubular member, a block-shaped member, and a cylindrical member.
16. The method for preparing a composite structural fuel of a nuclear power plant as recited in claim 3, wherein in the step S5, the second outer layer green compact is at least one of a cylindrical member and a block member.
17. The method for preparing the composite structure fuel of the nuclear power plant as recited in claim 3, wherein in the step S5, the first outer layer green compact and the second outer layer green compact are combined into a hollow columnar outer layer having an inner diameter of 6 to 13mm, a height of 8 to 24mm, and a thickness of 1 to 3mm.
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