High-entropy structure tritium breeding agent ceramic and preparation method thereof

Abstract

The invention relates to the technical field of nuclear energy materials, and discloses a high-entropy structure tritium breeder ceramic and a preparation method thereof, and the chemical formula of the high-entropy structure tritium breeder ceramic is Li < 2 > (Zr < 0.2 > Ti < 0.2 > Hf < 0.2 > Nb < 0.2 > Ta < 0.2 >) O < 3 >. The preparation method comprises the following steps: weighing LiOH.H2O powder, TiO2 powder, ZrO2 powder, HfO2 powder, Nb2O5 powder and Ta2O5 powder as raw materials according to a chemical formula; ball-milling and mixing the weighed raw materials to obtain mixed powder; calcining the mixed powder to obtain calcined powder; and putting the calcined powder into a mold, carrying out spark plasma sintering, and annealing to obtain a finished product. The preparation method is simple, and the prepared tritium breeding agent ceramic with the high-entropy structure can effectively inhibit lithium loss in a high-temperature working condition environment; sPS sintering is adopted in the preparation process, so that the obtained tritium breeding agent ceramic with the high-entropy structure is small in grain size, and tritium release is facilitated.

Description

Technical Field

[0001] The present invention relates to the technical field of nuclear energy materials, and particularly to a high-entropy structure tritium breeder ceramic and a preparation method thereof. Background Art

[0002] With the rapid development of human society and economy, the demand for energy is becoming increasingly urgent. Nuclear fusion energy is considered an ideal clean energy due to its safety, cleanliness, and high efficiency, and has received much attention in recent years. The development of nuclear fusion energy is of great significance to the sustainable development of human society. Tritium, as one of the main fuels of nuclear fusion energy, is scarce in nature and needs to be produced by bombarding tritium breeders (lithium-containing substances) with high-energy neutrons. Tritium breeders are the key to achieving "tritium self-sufficiency" in the tritium breeding blanket of a nuclear fusion reactor.

[0003] Lithium titanate (Li2TiO3) has low activation, excellent chemical stability, and good low-temperature tritium release performance, and is considered one of the most promising solid tritium breeding materials. However, the lithium density of Li2TiO3 is lower than that of lithium metasilicate, which seriously affects its tritium production capacity. A lithium-rich design can increase the lithium density of the tritium breeder, thereby improving the tritium breeding efficiency. Some researchers have successfully prepared lithium-rich Li4SiO4-0.3Li2O composite ceramics by sol-gel combined with the wet method; in addition, lithium-rich Li2TiO3-Li4SiO4 composite ceramics have been prepared by the metal organic solution method at 900 °C; other researchers have obtained lithium-rich Li 2+x TiO 3+y ceramics by calcining with the alkoxide method in an atmosphere of 5% H2-He at 1073K. Although the lithium-rich design can increase the lithium density of the tritium breeder, the lithium loss is serious under long-term high-temperature working conditions, which will still lead to a decrease in the tritium breeding efficiency. At the same time, the lost lithium diffuses from the tritium breeding blanket to the pipeline, blocking and corroding the pipeline, thereby affecting the normal operation of the reactor. Therefore, although the lithium-rich design can increase the lithium density of the tritium breeder, no solution has been given for the essence of lithium volatilization. Research shows that the main reason for lithium loss is that the residual Li2O and Li2CO3 in Li2TiO3 react to form a high-vapor-pressure product LiOH under high-temperature steam conditions, and LiOH will promote the mass transfer process of lithium in a high-temperature environment, accelerating lithium loss. Therefore, it is crucial to inhibit the lithium loss of tritium breeder ceramics under high-temperature working conditions. In nuclear fusion reactors, in order to inhibit the lithium loss of tritium breeders, existing technologies use means such as material modification (such as nanostructure design and composite material preparation), surface treatment (loading catalytically active elements), optimizing the preparation process (such as the sol-gel method), improving irradiation behavior research, and developing new fluid tritium breeders to improve the stability of lithium and the tritium release efficiency, but these methods still face problems such as complex preparation processes, high costs, and poor compatibility with the actual application environment.

[0004] To solve the above technical problems, a high-entropy structured tritium breeder ceramic and a preparation method thereof are urgently needed. Summary of the Invention

[0005] Aiming at the deficiencies of the above-mentioned existing technologies, the present invention aims to provide a high-entropy structured tritium breeder ceramic and a preparation method thereof, and obtain a high-entropy structured tritium breeder ceramic Li2(HE)O3 with good high-temperature lithium stability. By introducing high-entropy components at the B site of Li2TiO3, the diffusion of lithium at the A site is reduced, the generation of LiOH under high-temperature conditions is hindered, and lithium loss is inhibited.

[0006] To achieve the above purpose, the present invention is implemented according to the following technical solutions:

[0007] A high-entropy structured tritium breeder ceramic, the chemical formula of the high-entropy structured tritium breeder ceramic is Li2(Zr 0.2 Ti 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3.

[0008] Specifically, the high-entropy structured tritium breeder ceramic Li2(Zr 0.2 Ti 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 is simply referred to as the high-entropy structured tritium breeder ceramic Li2(HE)O3.

[0009] The present invention also includes a preparation method of a high-entropy structured tritium breeder ceramic, including the following steps:

[0010] S1, Weigh LiOH·H2O powder, TiO2 powder, ZrO2 powder, HfO2 powder, Nb2O5 powder, and Ta2O5 powder as raw materials according to the chemical formula Li2(Zr 0.2 Ti 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3;

[0011] S2, Ball-mill and mix the above-mentioned weighed raw materials to obtain a mixed powder;

[0012] S3, Calcinate the mixed powder to obtain a calcined powder;

[0013] S4, Load the calcined powder into a mold, carry out spark plasma sintering and then annealing to obtain Li2(Zr 0.2 Ti 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 ceramic.

[0014] Specifically, it includes the following steps:

[0015] S1, Weigh LiOH·H2O powder (purity 98%), TiO2 powder (purity 99%), ZrO2 powder (purity 99.99%), HfO2 powder (purity 99%), Nb2O5 powder (purity 99.99%), and Ta2O5 powder (purity 99.99%) as raw materials according to a certain stoichiometric ratio;

[0016] S2, Pour the raw material powders in S1 into a ball milling tank, add a certain proportion of zirconia ball milling balls and alcohol, then place it in a planetary ball mill for ball milling. The ball-milled and uniformly mixed powders are dried and sieved to obtain mixed powders;

[0017] S3, Place the mixed powders in S2 in a box-type muffle furnace for calcination to obtain calcined powders;

[0018] S4, Load the calcined powders in S3 into a graphite mold, place it in an SPS (spark plasma sintering) furnace for sintering and then annealing to obtain Li2(HE)O3 ceramics.

[0019] Preferably, in step S1, the purity of LiOH·H2O powder is 98%, the purity of TiO2 powder is 99%, the purity of ZrO2 powder is 99.99%, the purity of HfO2 powder is 99%, the purity of Nb2O5 powder is 99.99%, and the purity of Ta2O5 powder is 99.99%;

[0020] The LiOH·H2O powder, TiO2 powder, ZrO2 powder, HfO2 powder, Nb2O5 powder, and Ta2O5 powder are weighed according to a molar ratio of 20:2:2:2:1:1.

[0021] Preferably, in step S2, the ball-to-material ratio is (3 - 5):1, the ball milling speed is 200 - 300 r / min, and the ball milling time is 4 - 12 h.

[0022] Preferably, in step S3, the calcination temperature is 700 - 1200 °C; insulation is carried out at the calcination temperature, and the insulation time is 4 - 6 h.

[0023] Preferably, in step S3, the calcination program is: from room temperature, the temperature is raised to 200 °C at a heating rate of 2 °C / min; then the temperature is raised to the calcination temperature at a heating rate of 5 °C / min and insulation is carried out at the calcination temperature. After the insulation ends, the temperature is lowered to 500 °C at a rate of 5 °C / min, and then it is cooled with the furnace.

[0024] Specifically, step S3 uses a box-type muffle furnace for calcination to remove surface crystal water, promote particle growth, and reduce the surface energy of the powder.

[0025] Preferably, in the step S4, the sintering procedure of the spark plasma sintering process: under the condition that the pressure is 30-50 MPa, it is heated from room temperature to 600 °C at a rate of 145 °C / min, and then heated to 1150-1500 °C at a rate of 50 °C / min; at a temperature of 1150-1500 °C, it is vacuum-insulated for 10-30 min, and then cooled with the furnace.

[0026] The spark plasma sintering process is carried out in a vacuum environment, specifically, the heating process, the heat preservation process, and the cooling process are all in a vacuum environment.

[0027] Preferably, in the step S4, the annealing temperature of the annealing process is 700-900 °C; heat preservation is carried out at the annealing temperature, and the heat preservation time is 4-6 h.

[0028] Specifically, the step S4 is annealed in a box-type muffle furnace; the mold used is a graphite mold.

[0029] Principle of action:

[0030] The present invention creatively applies the high-entropy structure to the tritium breeder ceramic to obtain the high-entropy structure tritium breeder ceramic Li2(HE)O3 of the present invention.

[0031] High-entropy ceramics are single-phase solid solution materials formed by the random distribution of five or more cations with equal (near) molar amounts at the same lattice sites. In the high-entropy solid solution, due to the different atomic radii of each high-entropy component, serious lattice distortion is caused inside the material, thus having an important impact on its mechanical, thermal, and electrical properties. Through the diffusion behavior of the Co-Cr-Fe-Mn-Ni high-entropy alloy, it is found that the fluctuation of the lattice potential energy is positively correlated with the number of constituent elements in the matrix. The more serious the lattice distortion, the greater the fluctuation of the lattice potential energy, and the more obvious the atomic traps and atomic potentials are generated, so that the system has a higher activation energy and a more stable component structure. In addition, for the high-entropy A2B2O7 type high-level radioactive waste solidification mechanism, compared with the ternary A2B2O7, the low oxygen vacancy concentration and higher lattice potential energy of the high-entropy A2B2O7 inhibit the migration and diffusion of A-site cations. According to the Arrhenius curve of the conductivity, it can be seen that the diffusion activation energy of the high-entropy oxide is higher and the carrier concentration is smaller, indicating that the diffusion rate of the A-site cations is slower. In the present invention, high-entropy components are introduced at the B-site of Li2TiO3 to reduce the diffusion of lithium at the A-site, hinder the formation of LiOH under high-temperature conditions, and inhibit lithium loss.

[0032] The high-entropy structured tritium breeder ceramic Li2(HE)O3 of the present invention can effectively inhibit lithium loss in a high-temperature working environment. By introducing high-entropy metal elements, the lattice distortion of the material is increased. The more severe the lattice distortion, the greater the lattice potential energy fluctuation, and the more obvious the atomic traps and atomic potentials generated, so that the system has a higher activation energy and a more stable component structure; the high-entropy low oxygen vacancy concentration and higher lattice potential energy inhibit the migration and diffusion of lithium ions; the diffusion activation energy of high-entropy oxides is higher and the carrier concentration is smaller, so the lithium ion diffusion rate is slower.

[0033] The high-entropy structured tritium breeder ceramic Li2(HE)O3 obtained by SPS sintering has small grain size, which is helpful for tritium release. The spark plasma sintering (SPS) technology can realize rapid densification of samples at a lower sintering temperature by using pulsed current. At the same time, applying pressure helps the particles to rearrange and plastically deform, reducing the particle gap and further promoting its densification. The rapid heating of SPS makes the high-temperature residence time of the material extremely short, restricting grain growth; at the same time, the synergistic effect of pulsed current and pressure can reduce the grain boundary energy and inhibit grain boundary migration, thus hindering grain growth, making the grains smaller and the grain boundary specific surface area larger, and the diffusion barrier of tritium at the grain boundary is much lower than that in the grains. Therefore, small grains are helpful for tritium diffusion.

[0034] Beneficial effects:

[0035] The preparation method of the present invention is simple. The obtained high-entropy structured tritium breeder ceramic can effectively inhibit lithium loss in a high-temperature working environment; SPS sintering is used in the preparation process, so that the obtained high-entropy structured tritium breeder ceramic Li2(HE)O3 has small grain size, which is helpful for tritium release; the high-entropy design of the B site increases the lattice complexity, hinders the diffusion of lithium at the A site under high-temperature conditions, effectively avoids the generation of LiOH, and thus inhibits lithium loss. The preparation process is simple, the cost is low, and it is convenient for large-scale production. Description of the drawings

[0036] Figure 1 XRD patterns of the high-entropy structured tritium breeder ceramics Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 prepared in Examples 1 to 6;

[0037] Figure 2 EDS energy spectrum of the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 prepared in Example 2;

[0038] Figure 3 Atomic percentage contents of each element in the EDS spectrum of the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 prepared in Example 2;

[0039] Figure 4 SEM image of the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 prepared in Example 1 (Figure a in Figure 4 ) and SEM image of the high-entropy Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 ceramic prepared by pressureless sintering in Comparative Example 3 (Figure b in Figure 4 );

[0040] Figure 5 Ceramic grain size distribution diagram of the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 prepared in Example 1 (Figure a in Figure 5 ) and ceramic grain size distribution diagram of the high-entropy Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 ceramic prepared by pressureless sintering in Comparative Example 3 (Figure b in Figure 5 );

[0041] Figure 6 Curves of the relative density and densification rate of the sample versus temperature during SPS sintering in Example 2 (Figure a in Figure 6 ) and curves of the relative density of samples at different sintering temperatures in Example 1 (curve corresponding to 1300 °C), Example 2 (curve corresponding to 1400 °C), Example 3 (curve corresponding to 1150 °C), and Example 5 (curve corresponding to 1200 °C) versus holding time (Figure b in Figure 6 );

[0042] Figure 7 For Li2(Ti 0.2 Zr 0.2 Hf0.2 Nb 0.2 Ta 0.2 )O3 ceramic and Li2TiO3 ceramic samples at 900 °C, with a single heat preservation time of 4 h, the change curve of lithium loss rate with the number of thermal cycles. Detailed implementation mode

[0043] The following takes specific examples to further elaborate on the present invention in detail. It should be understood that the specific examples described herein are only used to explain the present invention and are not used to limit the present invention.

[0044] For all raw materials of the present invention, there is no special limitation on their purity. The present invention preferably uses industrial pure or conventional purity used in the art.

[0045] For the devices used in the present invention, those without special limitations are all the commonly used devices in the art.

[0046] The names, models and manufacturers of the experimental equipment used in the present invention are shown in Table 1.

[0047] Table 1 Main instrument and equipment

[0048]

[0049]

[0050] The specific implementation mode is shown in the following examples:

[0051] Example 1

[0052] A preparation method of a high-entropy structure tritium breeder ceramic, comprising the following steps:

[0053] (1) Using LiOH·H2O (98%), TiO2 (99%), ZrO2 (99.99%), HfO2 (99%), Nb2O5 (99.99%), Ta2O5 (99.99%) powder as raw materials, weighing according to the molar ratio of 20:2:2:2:1:1, and then placing them in a ball milling tank, adding an appropriate amount of anhydrous ethanol to make them fully mixed; according to the ball-to-material ratio of 4:1, adding zirconia ball milling balls with a diameter of 6 mm to the ball milling tank, and then immediately sealing the ball milling tank with plastic wrap.

[0054] (2) Fixing the sealed ball milling tank in a planetary ball mill, setting the ball milling speed to 200 r / min and the ball milling time to 4 h; placing the ball milled slurry in an oven, with a drying temperature of 60 °C and a drying time of 24 h.

[0055] (3) Weigh a number of dried powders and place them in a crucible, then calcine them in a box-type muffle furnace. Heat from room temperature to 200 °C at a rate of 2 °C / min, then heat to 1200 °C at a rate of 5 °C / min and hold for 4 h. Immediately cool to 500 °C at a rate of 5 °C / min and then cool with the furnace; Take out a number of pre-calcined powders, place them in a mortar and grind until there is no graininess, then sieve them through a 200-mesh sieve, and then dry and store them.

[0056] (4) Take 4.5 g of dried powder and pour it into a graphite mold, then place it in an SPS furnace for sintering; The sintering procedure is to heat from room temperature to 600 °C at a rate of 145 °C / min, then heat to 1300 °C at a rate of 50 °C / min, hold in a vacuum environment for 30 min, with a pressure of 50 MPa, and then immediately cool with the furnace.

[0057] (5) Anneal the sintered sample in a box-type muffle furnace. The annealing procedure is to heat to 200 °C at a rate of 2 °C / min, then heat to 900 °C at a rate of 5 °C / min and hold for 4 h. Immediately cool to 500 °C at a rate of 5 °C / min and then cool with the furnace to obtain the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 bulk.

[0058] For the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 bulk obtained in this example, polish both sides successively with 240-mesh, 600-mesh, 1200-mesh, 2300-mesh, 3000-mesh, 4000-mesh, and 8000-mesh diamond sandpapers until the thickness is 1 - 3 mm for testing.

[0059] Example 2

[0060] A preparation method of a high-entropy structured tritium breeder ceramic, comprising the following steps:

[0061] (1) Using LiOH·H2O (98%), TiO2 (99%), ZrO2 (99.99%), HfO2 (99%), Nb2O5 (99.99%), Ta2O5 (99.99%) powders as raw materials, weigh them according to a molar ratio of 20:2:2:2:1:1, then place them in a ball milling tank, add an appropriate amount of absolute ethanol to make them fully mixed; According to a ball-to-material ratio of 5:1, add zirconia ball milling balls with a diameter of 6 mm to the ball milling tank, and then immediately seal the ball milling tank with plastic wrap.

[0062] (2) Fix the sealed ball milling jar in a planetary ball mill, set the ball milling speed to 300 r / min, and the ball milling time to 12 h; place the ball milled slurry in an oven, with a drying temperature of 60 °C and a drying time of 24 h.

[0063] (3) Weigh a certain amount of the dried powder and place it in a crucible, then calcine it in a box-type muffle furnace. Heat from room temperature to 200 °C at a rate of 2 °C / min, then heat to 1200 °C at a rate of 5 °C / min and hold for 6 h. Immediately cool to 500 °C at a rate of 5 °C / min and cool with the furnace; take out a certain amount of the pre-calcined powder, grind it in a mortar until there is no particle feeling, then sieve it through a 200-mesh sieve, and then dry and store it.

[0064] (4) Pour 4.5 g of the dried powder into a graphite mold and place it in an SPS furnace for sintering; the sintering process is as follows: heat from room temperature to 600 °C at a rate of 145 °C / min, then heat to 1400 °C at a rate of 50 °C / min, hold in a vacuum environment for 30 min, with a pressure of 50 MPa; immediately cool with the furnace.

[0065] (5) Anneal the sintered sample in a box-type muffle furnace. The annealing process is to heat to 200 °C at a rate of 2 °C / min, then heat to 700 °C at a rate of 5 °C / min and hold for 6 h, then cool to 500 °C at a rate of 5 °C / min and cool with the furnace to obtain the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 bulk.

[0066] For the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 bulk obtained in this example, polish both sides successively with 240-mesh, 600-mesh, 1200-mesh, 2300-mesh, 3000-mesh, 4000-mesh, and 8000-mesh diamond sandpapers until the thickness is 1 - 3 mm for testing.

[0067] Example 3

[0068] A preparation method of a high-entropy structured tritium breeder ceramic, comprising the following steps:

[0069] (1) Using LiOH·H2O (98%), TiO2 (99%), ZrO2 (99.99%), HfO2 (99%), Nb2O5 (99.99%), Ta2O5 (99.99%) powders as raw materials, weigh them according to a molar ratio of 20:2:2:2:1:1. Then place them in a ball milling tank, add an appropriate amount of absolute ethanol to make them fully mixed. According to a ball-to-material ratio of 4:1, add zirconia ball milling balls with a diameter of 6 mm to the ball milling tank, and then immediately seal the ball milling tank with plastic wrap.

[0070] (2) Fix the sealed ball milling tank in a planetary ball mill, set the ball milling speed to 200 r / min, and the ball milling time to 4 h. Place the ball milled slurry in a drying oven, with a drying temperature of 60 °C and a drying time of 24 h.

[0071] (3) Weigh a certain amount of the dried powder and place it in a crucible, and then place it in a box-type muffle furnace for calcination. Heat from room temperature to 200 °C at a rate of 2 °C / min, then heat to 800 °C at a rate of 5 °C / min and hold for 4 h. Immediately cool to 500 °C at a rate of 5 °C / min and then cool with the furnace. Take out a certain amount of the pre-calcined powder, grind it in a mortar until there is no granular feeling, then sieve it through a 200-mesh sieve, and then dry and store it.

[0072] (4) Take 4.5 g of the dried powder and pour it into a graphite mold, and place it in an SPS furnace for sintering. The sintering procedure is to heat from room temperature to 600 °C at a rate of 145 °C / min, then heat to 1150 °C at a rate of 50 °C / min, hold for 10 min in a vacuum environment with a pressure of 30 MPa. Immediately cool with the furnace.

[0073] (5) Anneal the sintered sample in a box-type muffle furnace. The annealing procedure is to heat to 200 °C at a rate of 2 °C / min, then heat to 800 °C at a rate of 5 °C / min and hold for 6 h, then cool to 500 °C at a rate of 5 °C / min and then cool with the furnace to obtain a high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 bulk.

[0074] For the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 bulk obtained in this example, polish both sides with 240-mesh, 600-mesh, 1200-mesh, 2300-mesh, 3000-mesh, 4000-mesh, and 8000-mesh diamond sandpapers in sequence until the thickness is 1 - 3 mm for testing.

[0075] Example 4

[0076] A preparation method of a high-entropy structured tritium breeder ceramic, comprising the following steps:

[0077] (1) Using LiOH·H2O (98%), TiO2 (99%), ZrO2 (99.99%), HfO2 (99%), Nb2O5 (99.99%), Ta2O5 (99.99%) powders as raw materials, weighing according to a molar ratio of 20:2:2:2:1:1, then placing them in a ball milling tank, adding an appropriate amount of absolute ethanol to make them fully mixed; according to a ball-to-material ratio of 4:1, adding zirconia ball milling balls with a diameter of 6 mm to the ball milling tank, and then immediately sealing the ball milling tank with plastic wrap.

[0078] (2) Fixing the sealed ball milling tank in a planetary ball mill, setting the ball milling speed to 200 r / min and the ball milling time to 4 h; placing the ball milled slurry in a drying oven, with a drying temperature of 60 °C and a drying time of 24 h.

[0079] (3) Weighing a number of dried powders and placing them in a crucible, and calcining them in a box-type muffle furnace, heating from room temperature to 200 °C at a rate of 2 °C / min, then heating to 700 °C at a rate of 5 °C / min and holding for 4 h, then cooling to 500 °C at a rate of 5 °C / min and then cooling with the furnace; taking out a number of pre-calcined powders and grinding them in a mortar until there is no particle feeling, then sieving them through a 200-mesh sieve, and then drying and storing.

[0080] (4) Pouring 4.5 g of dried powder into a graphite mold and placing it in an SPS furnace for sintering; the sintering program is heating from room temperature to 600 °C at a rate of 145 °C / min, then heating to 1500 °C at a rate of 50 °C / min, holding for 20 min in a vacuum environment with a pressure of 50 MPa, and then cooling with the furnace.

[0081] (5) Annealing the sintered sample in a box-type muffle furnace, and the annealing program is heating to 200 °C at a rate of 2 °C / min, then heating to 800 °C at a rate of 5 °C / min and holding for 4 h, then cooling to 500 °C at a rate of 5 °C / min and then cooling with the furnace, to obtain a high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 bulk.

[0082] For the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2)The O3 bulk is polished on both sides with diamond sandpapers of 240 mesh, 600 mesh, 1200 mesh, 2300 mesh, 3000 mesh, 4000 mesh, and 8000 mesh in sequence until the thickness is 1 - 3 mm for testing.

[0083] Example 5

[0084] A preparation method of a high - entropy - structure tritium breeder ceramic, comprising the following steps:

[0085] (1) Using LiOH·H2O (98%), TiO2 (99%), ZrO2 (99.99%), HfO2 (99%), Nb2O5 (99.99%), Ta2O5 (99.99%) powders as raw materials, weighing according to a molar ratio of 20:2:2:2:1:1, then placing them in a ball - milling tank, adding an appropriate amount of absolute ethanol to make them fully mixed. According to a ball - to - material ratio of 3:1, zirconia ball - milling balls with a diameter of 6 mm are added to the ball - milling tank, and then the ball - milling tank is sealed with plastic wrap.

[0086] (2) Fix the sealed ball - milling tank in a planetary ball - mill, set the ball - milling speed to 250 r / min, and the ball - milling time to 6 h; place the ball - milled slurry in a drying oven, with a drying temperature of 60 °C and a drying time of 24 h.

[0087] (3) Weigh a certain amount of the dried powder and place it in a crucible, and calcine it in a box - type muffle furnace. Heat from room temperature to 200 °C at a rate of 2 °C / min, then heat to 1200 °C at a rate of 5 °C / min and hold for 4 h, then cool to 500 °C at a rate of 5 °C / min and cool with the furnace; take out a certain amount of the pre - calcined powder, grind it in a mortar until there is no particle feeling, then sieve it through a 200 - mesh sieve, and then dry and store it.

[0088] (4) Take 4.5 g of the dried powder and pour it into a graphite mold, and place it in an SPS furnace for sintering; the sintering procedure is to heat from room temperature to 600 °C at a rate of 145 °C / min, then heat to 1200 °C at a rate of 50 °C / min, hold for 30 min in a vacuum environment with a pressure of 50 MPa, and then cool with the furnace.

[0089] (5) Anneal the sintered sample in a box - type muffle furnace. The annealing procedure is to heat to 200 °C at a rate of 2 °C / min, then heat to 900 °C at a rate of 5 °C / min and hold for 4 h, then cool to 500 °C at a rate of 5 °C / min and then cool with the furnace to obtain the high - entropy - structure tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 bulk.

[0090] For the high - entropy - structure tritium breeder ceramic Li2(Ti obtained in this example0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 ) The O3 bulk is polished on both sides with 240-mesh, 600-mesh, 1200-mesh, 2300-mesh, 3000-mesh, 4000-mesh, and 8000-mesh diamond sandpapers in sequence until the thickness is 1 - 3 mm for detection.

[0091] Example 6

[0092] A preparation method of a high-entropy structured tritium breeder ceramic, comprising the following steps:

[0093] (1) Using LiOH·H2O (98%), TiO2 (99%), ZrO2 (99.99%), HfO2 (99%), Nb2O5 (99.99%), and Ta2O5 (99.99%) powders as raw materials, weighing them according to a molar ratio of 20:2:2:2:1:1, then placing them in a ball milling jar, adding an appropriate amount of absolute ethanol to make them fully mixed; adding zirconia ball milling balls with a diameter of 6 mm to the ball milling jar according to a ball-to-material ratio of 4:1, and then immediately sealing the ball milling jar with plastic wrap.

[0094] (2) Fix the sealed ball milling jar in a planetary ball mill, set the ball milling speed to 200 r / min, and the ball milling time to 12 h; place the ball milled slurry in a drying oven, with a drying temperature of 60 °C and a drying time of 24 h.

[0095] (3) Weigh a certain amount of the dried powder and place it in a crucible, and then calcine it in a box-type muffle furnace. Heat it from room temperature to 200 °C at a rate of 2 °C / min, then heat it to 700 °C at a rate of 5 °C / min and hold for 4 h, and then cool it to 500 °C at a rate of 5 °C / min and then cool it with the furnace; take out a certain amount of the pre-calcined powder and grind it in a mortar until there is no particle feeling, then sieve it through a 200-mesh sieve, and then dry and store it.

[0096] (4) Take 4.5 g of the dried powder and pour it into a graphite mold, and then sinter it in an SPS furnace; the sintering program is to heat it from room temperature to 600 °C at a rate of 145 °C / min, and then heat it to 1300 °C at a rate of 50 °C / min, hold it for 20 min in a vacuum environment, with a pressure of 50 MPa, and then cool it with the furnace.

[0097] (5) Anneal the sintered sample in a box-type muffle furnace. The annealing program is to heat it from room temperature to 200 °C at a rate of 2 °C / min, then heat it to 800 °C at a rate of 5 °C / min and hold for 4 h, and then cool it to 500 °C at a rate of 5 °C / min, and cool it with the furnace to obtain the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta0.2 ) O3 bulk.

[0098] For the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 ) O3 bulk, double-sided polish it to a thickness of 1 - 3 mm successively with 240-mesh, 600-mesh, 1200-mesh, 2300-mesh, 3000-mesh, 4000-mesh, and 8000-mesh diamond sandpapers for detection.

[0099] Comparative Example 1

[0100] (1) Using Li2CO3 (99.5%), TiO2 (99%), ZrO2 (99.99%), HfO2 (99%), Nb2O5 (99.99%), and Ta2O5 (99.99%) powders as raw materials, weigh them according to a molar ratio of 20:2:2:2:1:1, then place them in a ball milling jar, add an appropriate amount of absolute ethanol to make them fully mixed; according to a ball-to-material ratio of 4:1, add 6-mm diameter zirconia ball milling balls to the ball milling jar, and then immediately seal the ball milling jar with plastic wrap.

[0101] (2) Fix the sealed ball milling jar in a planetary ball mill, set the ball milling speed to 200 r / min, and the ball milling time to 4 h; place the ball milled slurry in a drying oven, with a drying temperature of 60 °C and a drying time of 24 h.

[0102] (3) Weigh a certain amount of the dried powder and place it in a crucible, and then place it in a box-type muffle furnace for calcination. Heat it from room temperature to 200 °C at a rate of 2 °C / min, then heat it to 1200 °C at a rate of 5 °C / min and hold for 4 h, then cool it to 500 °C at a rate of 5 °C / min and then cool it with the furnace; take out a certain amount of the pre-calcined powder, grind it in a mortar until there is no particle feeling, then sieve it through a 200-mesh sieve, and then dry and store it.

[0103] (4) Pour 4.5 g of the dried powder into a graphite mold and place it in an SPS furnace for sintering; the sintering program is to heat it from room temperature to 600 °C at a rate of 145 °C / min, then heat it to 1300 °C at a rate of 50 °C / min, hold it in a vacuum environment for 30 min, with a pressure of 50 MPa, and then immediately cool it with the furnace.

[0104] (5) Anneal the sintered sample in a box-type muffle furnace. The annealing program is to heat it to 200 °C at a rate of 2 °C / min, then heat it to 900 °C at a rate of 5 °C / min and hold for 4 h, then cool it to 500 °C at a rate of 5 °C / min and then cool it with the furnace to obtain Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta0.2 ) O3 ceramic block

[0105] For the Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 ) The O3 ceramic block was polished on both sides with 240-mesh, 600-mesh, 1200-mesh, 2300-mesh, 3000-mesh, 4000-mesh, and 8000-mesh diamond sandpapers until the thickness reached 1 - 3 mm for testing

[0106] Comparative Example 2

[0107] (1) Using Li2CO3 (99.5%), TiO2 (99%), ZrO2 (99.99%), HfO2 (99%), Nb2O5 (99.99%), and Ta2O5 (99.99%) powders as raw materials, weighed according to the molar ratio of 20:2:2:2:1:1, and then placed in a ball milling tank. An appropriate amount of absolute ethanol was added to make them fully mixed; according to the ball-to-material ratio of 4:1, zirconia ball milling balls with a diameter of 6 mm were added to the ball milling tank, and then the ball milling tank was sealed with plastic wrap

[0108] (2) The sealed ball milling tank was fixed in a planetary ball mill, the ball milling speed was set at 200 r / min, and the ball milling time was 4 h; the ball milled slurry was placed in a drying oven, the drying temperature was 60 °C, and the drying time was 24 h

[0109] (3) Weighed a certain amount of the dried powder and placed it in a crucible, and then placed it in a box-type muffle furnace for calcination. It was heated from room temperature to 200 °C at a rate of 2 °C / min, then heated to 700 °C at a rate of 5 °C / min and held for 4 h, and then cooled to 500 °C at a rate of 5 °C / min and then cooled with the furnace; took out a certain amount of the pre-calcined powder and ground it in a mortar until there was no particle feeling, then sieved it through a 200-mesh sieve, and then dried and stored

[0110] (4) Took 4.5 g of the dried powder and poured it into a graphite mold, and placed it in an SPS furnace for sintering; the sintering procedure was to heat from room temperature to 600 °C at a rate of 145 °C / min, then heat to 1300 °C at a rate of 50 °C / min, hold for 20 min in a vacuum environment with a pressure of 50 MPa, and then cool with the furnace

[0111] (5) The sintered sample was annealed in a box-type muffle furnace. The annealing procedure was to heat to 200 °C at a rate of 2 °C / min, then heat to 800 °C at a rate of 5 °C / min and hold for 4 h, and then cool to 500 °C at a rate of 5 °C / min and then cool with the furnace to obtain Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta0.2 ) O3 ceramic block

[0112] For the Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 ) O3 ceramic block was polished on both sides with 240-mesh, 600-mesh, 1200-mesh, 2300-mesh, 3000-mesh, 4000-mesh, and 8000-mesh diamond sandpapers in sequence until the thickness reached 1 - 3 mm for testing

[0113] Comparative Example 3

[0114] A method for pressureless sintering preparation of a tritium breeder ceramic, comprising the following steps

[0115] (1) Using LiOH·H2O (98%), TiO2 (99%), ZrO2 (99.99%), HfO2 (99%), Nb2O5 (99.99%), Ta2O5 (99.99%) powders as raw materials, weighing them according to a molar ratio of 20:2:2:2:1:1, then placing them in a ball milling jar, adding an appropriate amount of anhydrous ethanol to make them fully mixed; adding zirconia milling balls with a diameter of 6 mm to the ball milling jar according to a ball-to-material ratio of 4:1, and then immediately sealing the ball milling jar with plastic wrap

[0116] (2) Fixing the sealed ball milling jar in a planetary ball mill, setting the ball milling speed to 200 r / min and the ball milling time to 4 h; placing the ball milled slurry in a drying oven, with a drying temperature of 60 °C and a drying time of 24 h

[0117] (3) Weighing a number of dried powders and placing them in a crucible, and calcining them in a box-type muffle furnace. Heating from room temperature to 200 °C at a rate of 2 °C / min, then heating to 1200 °C at a rate of 5 °C / min and holding for 4 h, then immediately cooling to 500 °C at a rate of 5 °C / min and cooling with the furnace; taking out a number of pre-calcined powders, grinding them in a mortar until there is no particle feeling, sieving them through a 200-mesh sieve, and then drying and storing

[0118] (4) Taking 4.5 g of dried powder and loading it into a Φ20 mold, placing it in the center of a tablet press, closing the oil discharge valve, gradually applying pressure to 10 MPa by shaking the press handle, holding the pressure for 90 s to ensure that the powder is fully compacted, then slowly opening the oil discharge valve rod to release the pressure. Taking out the formed sample and placing it in a box-type muffle furnace for pressureless sintering, and the sintering procedure is heating from 2 °C / min to 200 °C, then heating to 1300 °C at a rate of 5 °C / min and holding for 4 h, then immediately cooling to 500 °C at a rate of 5 °C / min and cooling with the furnace

[0119] (5) Anneal the sample after pressureless sintering in a box-type muffle furnace. The annealing procedure is to raise the temperature to 200 °C at a rate of 2 °C / min, then raise the temperature to 900 °C at a rate of 5 °C / min and hold for 4 h, and then immediately cool to 500 °C at a rate of 5 °C / min and then cool with the furnace to obtain a high-entropy Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 ceramic bulk.

[0120] For the high-entropy Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 ceramic bulk obtained by annealing in this comparative example, polish both sides successively with 240-mesh, 600-mesh, 1200-mesh, 2300-mesh, 3000-mesh, 4000-mesh, and 8000-mesh diamond sandpapers until the thickness is 1 - 3 mm for testing.

[0121] Comparative Example 4

[0122] Li2TiO3 ceramic sample, and its preparation process is as follows:

[0123] (1) Weigh LiOH·H2O (98%) and TiO2 (99%) according to the chemical formula of Li2TiO3, then place them in a ball-milling jar, and add an appropriate amount of absolute ethanol to make them fully mixed; according to the ball-to-material ratio of 4:1, add zirconia ball-milling balls with a diameter of 6 mm to the ball-milling jar, and then immediately seal the ball-milling jar with plastic wrap.

[0124] (2) Fix the sealed ball-milling jar in a planetary ball mill, set the ball-milling speed to 200 r / min, and the ball-milling time to 4 h; place the ball-milled slurry in a drying oven, with a drying temperature of 60 °C and a drying time of 24 h.

[0125] (3) Weigh a certain amount of the dried powder and place it in a crucible, and put it into a box-type muffle furnace for calcination. Raise the temperature from room temperature to 200 °C at a rate of 2 °C / min, then raise the temperature to 1200 °C at a rate of 5 °C / min and hold for 4 h, and then immediately cool to 500 °C at a rate of 5 °C / min and then cool with the furnace; take out a certain amount of the pre-calcined powder and grind it in a mortar until there is no particle feeling, then sieve it through a 200-mesh sieve, and then dry and store it.

[0126] (4) Take 4.5 g of the dried powder and pour it into a graphite mold, and place it in an SPS furnace for sintering; the sintering procedure is to raise the temperature from room temperature to 600 °C at a rate of 145 °C / min, then raise the temperature to 1300 °C at a rate of 50 °C / min, hold for 30 min in a vacuum environment, with a pressure of 50 MPa, and then immediately cool with the furnace.

[0127] (5) Anneal the sintered sample in a box-type muffle furnace. The annealing procedure is to raise the temperature to 200 °C at a rate of 2 °C / min, then raise the temperature to 900 °C at a rate of 5 °C / min and hold for 4 h. Immediately afterwards, cool it to 500 °C at a rate of 5 °C / min and then cool it in the furnace to obtain Li2TiO3 bulk.

[0128] Experimental tests

[0129] Test the phase, structure, lithium loss rate, etc. of the ceramic samples obtained in Examples 1-6 and Comparative Examples 1-4. The results are as Figure 1-7 shown.

[0130] From Figure 1 the XRD analysis in, it shows that the diffraction peaks of the six groups of samples in Examples 1-6 (Examples 1 to 6 in the figure respectively represent the high-entropy structure tritium breeder ceramics Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3) are similar. Its characteristic diffraction peaks are basically consistent with the diffraction peaks of the monoclinic Li2TiO3 (PDF#33-0831) standard XRD spectrum, belonging to the C2 / c(15) space group. The shift of the main diffraction peak towards the small angle direction indicates that the multi-component solid solution in the high-entropy system causes serious lattice distortion.

[0131] From Figure 2 it can be seen that the components (Ti, Zr, Hf, Nb, Ta) of the high-entropy structure tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 prepared in Example 2 of the present invention are evenly distributed without obvious segregation.

[0132] Figure 3 The results show that the atomic contents of each element in the high-entropy structure tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 prepared in Example 2 of the present invention are not very different and are basically the same, meeting the near-equimolar ratio.

[0133] For Figure 4 the SEM image of the high-entropy structure tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 prepared in Example 1 in Figure 4Figure a) in and the SEM image of the high-entropy Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 ceramic ([Figure b) in Figure 4 Upon analyzing, it was found that for the high-entropy structure tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 prepared by SPS sintering in Example 1, the grains are more uniform and the size is much smaller than that of the sample prepared by pressureless sintering in Comparative Example 3.

[0134] From Figure 5 the grain size distribution, it can be seen that for the high-entropy structure tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 prepared by SPS sintering in Example 1, the average particle size is 10.79 μm, while for the high-entropy Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 ceramic prepared by pressureless sintering in Comparative Example 3, the average particle size is 22.75 μm.

[0135] From Figure 6 (a), it can be seen that during the process of preparing the high-entropy structure tritium breeder ceramic by SPS sintering in Example 2, the densification rate reaches the maximum value when the sintering temperature is near 1200 °C.

[0136] From Figure 6 (b), it can be seen that when the SPS sintering temperature is 1300 °C, the relative density of the high-entropy structure tritium breeder ceramic is the largest. In addition, when the sintering temperatures are 1150 °C (Example 3), 1200 °C (Example 5), 1300 °C (Example 1), and 1400 °C (Example 2) respectively, and the sintering time exceeds 10 min, the samples all obtain the maximum relative density and the densification is basically completed.

[0137] As Figure 7 shown:

[0138] "Li2(HE)O3 (LiOH·H2O, 200 r / min, 4 h, 1500 °C, 50 MPa)" in the figure represents the high-entropy structure tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb0.2 Ta 0.2 )O3;

[0139] In the figure, "Li2(HE)O3(LiOH·H2O, 200 r / min, 12 h, 1300 °C, 50 MPa)" represents the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3;

[0140] In the figure, "Li2(HE)O3(Li2CO3, 200 r / min, 4 h, 1300 °C, 50 MPa)" represents the Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 ceramic obtained in Comparative Example 2;

[0141] In the figure, "Li2(HE)O3(LiOH·H2O, 200 r / min, 4 h, 1300 °C, 50 MPa)" represents the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3.

[0142] In the figure, "Li2TiO3(LiOH·H2O, 200 r / min, 4 h, 1300 °C, 50 MPa)" represents the Li2TiO3 ceramic obtained in Comparative Example 4.

[0143] It can be seen from Figure 7 that the lithium loss rate of the high-entropy structured tritium breeder ceramic Li2(Ti 0.2 Zr 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 samples prepared in this invention is generally lower than that of Li2TiO3 in Comparative Example 4, but the advantage of the high-entropy tritium breeder weakens significantly with the increase of the number of thermal cycles.

[0144] The technical solution of the present invention is not limited to the limitations of the above specific embodiments. Any technical deformation made according to the technical solution of the present invention falls within the protection scope of the present invention.

Claims

1. A high-entropy structure tritium breeder ceramic, characterized in that: The chemical formula of the high-entropy structured tritium breeder ceramic is Li2(Zr 0.2 Ti 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3。 2. A preparation method of a high-entropy structure tritium breeder ceramic, characterized in that: including the following steps: S1. According to the chemical formula Li2(Zr 0.2 Ti 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3, weigh LiOH·H2O powder, TiO2 powder, ZrO2 powder, HfO2 powder, Nb2O5 powder, and Ta2O5 powder as raw materials; S2, ball-milling and mixing the above-mentioned weighed raw materials to obtain a mixed powder; S3, calcining the mixed powder to obtain a calcined powder; S4. Load the calcined powder into a mold, perform spark plasma sintering and then annealing to obtain Li2(Zr 0.2 Ti 0.2 Hf 0.2 Nb 0.2 Ta 0.2 )O3 ceramics.

3. The preparation method of a high-entropy structure tritium breeder ceramic according to claim 2, characterized in that: In the step S1, the purity of the LiOH·H2O powder is 98%, the purity of the TiO2 powder is 99%, the purity of the ZrO2 powder is 99.99%, the purity of the HfO2 powder is 99%, the purity of the Nb2O5 powder is 99.99%, and the purity of the Ta2O5 powder is 99.99%.

4. The preparation method of a high-entropy structure tritium breeder ceramic according to claim 2, characterized in that: In the step S1, the LiOH·H2O powder, TiO2 powder, ZrO2 powder, HfO2 powder, Nb2O5 powder, and Ta2O5 powder are weighed according to a molar ratio of 20:2:2:2:1:

1.

5. The preparation method of a high-entropy structure tritium breeder ceramic according to claim 2, characterized in that: In the step S2, the ball-to-material ratio is (3-5):1, the ball-milling speed is 200-300 r / min, and the ball-milling time is 4-12 h.

6. The preparation method of a high-entropy structured tritium breeder ceramic according to claim 2, characterized in that: In the step S3, the calcination temperature is 700-1200 °C; heat preservation is carried out at the calcination temperature, and the heat preservation time is 4-6 h.

7. The preparation method of a high-entropy structured tritium breeder ceramic according to claim 6, characterized in that: In the step S3, the calcination procedure is: rising from room temperature to 200 °C at a heating rate of 2 °C / min; then rising to the calcination temperature at a heating rate of 5 °C / min and carrying out heat preservation at the calcination temperature. After the heat preservation ends, cool down to 500 °C at a rate of 5 °C / min, and then cool with the furnace.

8. The preparation method of a high-entropy structure tritium breeder ceramic according to claim 2, characterized in that: In the step S4, the sintering procedure of the spark plasma sintering process: under the condition of a pressure of 30-50 MPa, rise from room temperature to 600 °C at a rate of 145 °C / min, and then rise to 1150-1500 °C at a rate of 50 °C / min; at a temperature of 1150-1500 °C, carry out vacuum heat preservation for 10-30 min, and then cool with the furnace.

9. The preparation method of a high-entropy structured tritium breeder ceramic according to claim 2, characterized in that: In the step S4, the annealing temperature of the annealing process is 700-900 °C; heat preservation is carried out at the annealing temperature, and the heat preservation time is 4-6 h.

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