A method for treating An 3+ With An 4+ Solidification method of sintered solidified body of radioactive mud

Abstract

The present invention belongs to the technical field of radioactive nuclear waste treatment, in particular to a method for treating an 3+ With An 4+ A method for solidifying a sintered solidified body of radioactive mud comprises a simulated radioactive mud base material powder containing a glass former and a solidified body material; the simulated radioactive mud base material powder containing the glass former comprises 40-100 wt% by mass of a simulated radioactive mud base material raw material powder and 0-60 wt% by mass of a silicate glass particle raw material powder; the solidified body material comprises 40 wt% by mass of simulated radioactive mud and 60 wt% by mass of a silicate glass particle powder, the simulated radioactive mud comprises 60-100 wt% by mass of the simulated radioactive mud base material powder and 0-40 wt% by mass of a radionuclide or simulated radionuclide; and the sintering process is adjusted by adjusting the formula composition of the silicate glass particles, the simulated radionuclides Nd2O3 and CeO2, and the simulated radioactive mud base material powder to achieve the purpose of rapidly treating the radioactive mud.

Description

Technical Field

[0001] The present invention belongs to the field of radioactive nuclear waste treatment technology and involves a method for treating An 3+ With An 4+ A method for solidifying a sintered solidified body of radioactive mud. Background Art

[0002] At present, the international disposal of radioactive waste usually involves first fixing the radionuclides stably in a matrix material to form a solid body, and then storing it in a disposal repository for long-term monitoring to prevent the release of radionuclides into the biosphere. This requires a high level of physical and chemical stability of the solid body.

[0003] The main solidification methods for different levels of radioactive waste are:

[0004] 1. Solidification methods for medium and low-level radioactive waste:

[0005] Cement solidification: It is the preferred method due to its early development, mature technology, wide application, simple operation, strong processing capacity, low investment and operating costs;

[0006] Asphalt solidification: Suitable for treating wet waste and powdered waste. Radioactive nuclides are evenly wrapped in asphalt through saponification reaction. It has the advantages of simple process, high volume reduction rate and low leaching rate.

[0007] 2. Solidification methods for medium- and high-level radioactive waste: mainly using glass solidification, ceramic solidification, and glass-ceramic solidification technologies; among them, glass solidification technology: radioactive waste liquid, waste and glass raw materials are mixed in a certain proportion, and then subjected to conventional heating, high-temperature melting and room-temperature cooling to form a glass body. The solidified body mainly includes borosilicate glass, aluminosilicate glass and phosphate glass; ceramic solidification (artificial rock solidification): high-temperature solid-phase reaction is used to make radioactive nuclides enter the lattice sites and lattice gaps of natural minerals or synthetic ceramic mineral phases, and after cooling, a multi-mineral phase is formed; glass-ceramic solidification: radioactive waste is combined with a specific glass substrate, and the ceramic crystal phase is precipitated from the glass body by changing the sintering process to form a solid solid body, which combines the advantages of glass solidification body and ceramic solidification body;

[0008] The sintering technologies for nuclear waste solidification mainly include traditional Joule sintering technology, spark plasma sintering technology and microwave sintering technology. Compared with conventional heating methods (such as electromagnetic induction, electrode, plasma, etc.), microwave heating is safer and more reliable, has stronger environmental adaptability, and has the characteristics of selective heating, fast temperature rise, short sintering time, timely control, sensitive response, strong penetration ability, high energy utilization and low waste. It has obvious advantages in improving material properties, improving microstructure, energy conservation and environmental protection.

[0009] However, there are currently no reports on related inventions regarding a process and method for rapidly fixing radioactive mud using microwave sintering technology. Therefore, the applicant proposes a method for curing a radioactive mud solidified body by microwave sintering to solve the above problem. Summary of the Invention

[0010] Based on this, it is necessary to provide a method for curing radioactive mud by microwave sintering technology, which can achieve rapid solidification of radioactive mud, so as to reduce the storage and processing time of radioactive waste, improve processing efficiency, and reduce environmental risks.

[0011] A method for treating An 3+ With An 4+ A sintered solidified body of radioactive mud, comprising a simulated radioactive mud base material powder containing a glass former and a solidified body material;

[0012] The simulated radioactive mud base material powder containing the glass former comprises 40-100 wt% of simulated radioactive mud base material raw material powder and 0-60 wt% of silicate glass particle raw material powder;

[0013] The solidified material comprises 40 wt% of simulated radioactive mud and 60 wt% of silicate glass particle powder, wherein the simulated radioactive mud comprises 60-100 wt% of simulated radioactive mud base material powder and 0-40 wt% of radioactive nuclides or simulated radioactive nuclides.

[0014] A method for preparing a microwave sintering solidified body for radioactive mud, comprising:

[0015] S100: preparing simulated radioactive mud base material raw material powder;

[0016] S200: preparing silicate glass particle raw material powder;

[0017] S300: preparing a simulated radioactive mud base material powder containing a glass former by mixing the simulated radioactive mud base material powder obtained in step S100 with the silicate glass particle powder obtained in step S200 in a ratio of 40-100 wt % to 0-60 wt % by mass;

[0018] S400: The simulated radioactive mud base material raw material powder obtained in step S100 and radioactive nuclides or simulated radioactive nuclides are mixed in a mass percentage ratio of 60-100 wt%:0-40 wt% to prepare simulated radioactive mud, and then the silicate glass particle raw material powder obtained in step S200 and the simulated radioactive mud are mixed in a mass percentage ratio of 60 wt%:40 wt% to prepare a solidified material.

[0019] Furthermore, the preparation of the simulated radioactive mud base material powder includes:

[0020] S101: Take the raw materials with mass percentages of CaCO319.81 wt%, Mg(OH)22.25 wt%, Na2CO343.28 wt%, Al(OH)315.21 wt%, Fe2O37.31 wt%, SiO25.52 wt%, Cr2O33.97 wt%, NiO 1.70 wt%, and MoO30.89 wt%;

[0021] S102: The raw materials in step S101 are mixed and stirred. The raw materials are placed in a flask and 150% of the total weight of the raw materials is added with anhydrous ethanol, and the mixture is mixed and stirred using a mechanical stirrer for 3-5 hours;

[0022] S103: drying the mixed raw materials in a constant temperature oven at 105° C. for 24 to 36 hours;

[0023] S104: The dried raw materials are ball-milled in a ball mill for 3 to 5 hours to prepare a uniformly mixed simulated radioactive mud matrix raw material powder.

[0024] Furthermore, the preparation of the raw material powder for silicate glass particles includes:

[0025] S201: taking the raw materials in mass percentages of SiO261.44 wt%, CaO11.20 wt%, Na2O7.90 wt%, BaO5.82 wt%, MgO5.82 wt%, Al2O34.78 wt%, and V2O52.64 wt%;

[0026] S202: Place the raw materials in a flask and add 150% of the total weight of the raw materials in anhydrous ethanol, and mix and stir using a mechanical stirrer for 3-5 hours;

[0027] S203: drying the mixed raw materials in a constant temperature oven at 105° C. for 24 to 36 hours;

[0028] S204: placing the dried raw material in a microwave muffle furnace for sintering at a temperature of 800° C., and keeping the sintering temperature at 800° C. for 40 min;

[0029] S205: placing the pre-sintered raw materials in a ball mill for 3 to 5 hours to obtain silicate glass particle powder;

[0030] S206: The ball-milled powder is passed through a 200-mesh sieve to obtain silicate glass particle powder with a particle size of 75 μm.

[0031] Furthermore, the step S300 further includes:

[0032] S301: Mixing, grinding, and drying a mixture of a simulated radioactive mud base material and silicate glass particle powder, and placing the dried mixture into a ball mill for 3 to 5 hours;

[0033] S302: Place the mixed powder in a microwave muffle furnace and heat it to 1000°C at a heating rate of 20°C / min, then heat it to 1100~1300°C at a heating rate of 10°C / min, keep it at the target temperature for 40 minutes, and then naturally cool it to room temperature to obtain a SiO2-Na2O-Al2O3 curing system material.

[0034] Furthermore, the step S400 further includes:

[0035] The radioactive nuclides or simulated radioactive nuclides in the simulated radioactive mud include Nd2O3 and CeO2. The Nd2O3 and CeO2 are mixed in a two-phase manner according to a mass percentage of 0 to 60 wt%, stirred, ground, dried and ball-milled to obtain the simulated radioactive mud.

[0036] Furthermore, the radioactive nuclides or simulated radioactive nuclides in the simulated radioactive mud include Nd2O3 and CeO2. The Nd2O3 and CeO2 are mixed in a two-phase manner at a mass percentage of 0 to 60 wt%, stirred, ground, dried and ball-milled to obtain the simulated radioactive mud.

[0037] Furthermore, the ball mill is a planetary ball mill.

[0038] Beneficial effects of the present invention:

[0039] 1. The present invention utilizes microwave sintering technology to adjust the formula composition of silicate glass particles, simulated radioactive nuclides Nd2O3 and CeO2, and simulated radioactive mud base material powder, and adjusts the sintering process to achieve the purpose of quickly treating radioactive mud. By combining X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS), high-resolution transmission electron microscopy-selected electron diffraction (HRTEM-SAED) and chemical stability testing for analysis, a SiO2-Na2O-Al2O3 silicate solidified body substrate is selected, and the formula composition of the glass solidified body or glass-ceramic solidified body for solidifying the radionuclides in the radioactive mud or simulating radionuclides and the microwave sintering process are used to prepare a SiO2-Na2O-Al2O3 silicate glass solidified body material with high efficiency in fixing radionuclides and silicate apatite (A I x A II10-x (BO4)6O2(A=Na, Ca and Nd)) glass ceramic solid body material;

[0040] 2. By using the SiO2-Na2O-Al2O3 silicate glass solidified body material of the present invention, Nd2O35 wt.% and CeO25 wt.%, Nd2O310 wt.% and CeO25 wt.%, Nd2O310 wt.% and CeO210wt.%, Nd2O315 wt.% and CeO25 wt.%, and Nd2O320 wt.% and CeO25 wt.% can be achieved at a sintering temperature of 1200°C. At the sintering temperature of 1300 ℃, the contents of Nd2O35wt.% and CeO25 wt.%, Nd2O35 wt.% and CeO210 wt.%, Nd2O310 wt.% and CeO25 wt.%, Nd2O310 wt.% and CeO210 wt.%, Nd2O310 wt.% and CeO215 wt.%, Nd2O315 wt.% and CeO25 wt.%, Nd2O315 wt.% and CeO210 wt.%, Nd2O315 wt.% and CeO215 wt.%, Nd2O315 wt.% and CeO220 wt.%, Nd2O320 wt.% and CeO25 wt.%, Nd2O320 wt.% and CeO210 wt.%, Nd2O320 wt.% and CeO215 wt.%, Nd2O320 wt.% and CeO220 wt.%, Nd2O320 wt.% and CeO225 wt.%, Nd2O325 wt.% and CeO25 wt.%, Nd2O325 wt.% and CeO210 wt.%, Nd2O325 wt.% and CeO215 wt.%, Nd2O325 wt.% and CeO220 wt.%, Nd2O325 wt.% and CeO225 wt.%, Nd2O325 wt.% and CeO230 wt.%, Nd2O330 wt.% and CeO25 wt.%, Nd2O330 wt.% and CeO210 wt.%, Nd2O330 wt.% and CeO215 wt.%, Nd2O330 wt.% and CeO220 wt.%, Nd2O330 wt.% and CeO225 wt.%, no other phases appeared in the glass solidified samples. At 1200 ℃, the glass solidified samples containing Nd2O35 wt.% and CeO210 wt.%, Nd2O310 wt.% and CeO210 wt.%, Nd2O315 wt.% and CeO215wt.% were mainly composed of Si4O 116- The main structural unit is sheet silicate group, Si4O 11 6- The total content of sheet silicate groups and SiO2 three-dimensional network structural units is 48%, 56% and 59% respectively. The Si4O in the glass solidified bodies containing Nd2O315 wt.% and CeO220 wt.%, Nd2O325 wt.% and CeO230 wt.%, and Nd2O330 wt.% and CeO225 wt.% at 1300 ℃ is 2.34%. 11 6- The total proportions of sheet silicate groups and SiO2 three-dimensional network structural units are 51%, 55% and 39% respectively. These solids all show good glass polymerization degree; XPS results show that some Ce 4+ Will be restored to Ce 3+ SEM-EDS results show that Si, Na, Ca, O, Ce, and Nd are uniformly distributed in the solidified body with no elemental enrichment. HRTEM-SAED results reveal the apparent disorder and amorphous diffraction rings of the amorphous structure. Therefore, the SiO2-Na2O-Al2O3 silicate glass solidified body can effectively immobilize the simulated radioactive mud containing the aforementioned Nd2O3 and CeO2 contents, while also exhibiting a high compatibility ratio and excellent glass polymerization degree. The normalized leaching rates (RLCe, RLNd, and RLSi) of Ce, Nd, and Si in deionized water at 90°C are less than 2.2×10 -6 g·m -2 ·d -1 , 1.5×10 -6 g·m -2 ·d -1 , 1.4×10 -6 g·m -2 ·d -1 The glass solidification body has good chemical stability and meets the requirements of nuclear industry (1×10 -2 g·m -2 ·d -1 ) expected requirements.

[0041] 3. Using the present invention, silica apatite (A I x A II 10-xIn the (BO4)6O2 (A = Na, Ca, Ce and Nd)) glass ceramic solidification material, the solidification treatment of simulated radioactive mud with Nd2O3 20 wt.% and CeO25 wt.%, Nd2O3 25 wt.% and CeO25 wt.% at a sintering temperature of 1100℃ and Nd2O3 25 wt.% and CeO25 wt.% at a sintering temperature of 1200℃ can be achieved. The crystalline phases appearing in the samples are (Ca, Na) x Nd 10-x (SiO4)6O2、Na 1-x Ce x+y Nd 9-y (SiO4)6O2 and Ca2Ce x Nd 8-x (SiO4)6O2 contains Nd and Ce Ca-silicon oxyapatite and Na-silicon oxyapatite phases, and the XRD spectrum results show a steamed bun peak. This sample is silicon oxyapatite (A I x A II 10-x (BO4)6O2 (A = Na, Ca, Ce and Nd)) glass-ceramic material; SEM-EDS results show that a large number of needle-tipped tubular structures appear on the surface of the solidified body of the simulated radioactive mud containing 25 wt.% Nd2O3 and 25 wt.% CeO2. Si, Na, Ca, O, Ce and Nd elements are obviously enriched on the needle-tipped tubular structures, and Al, Na, Si, O, and a small amount of Nd and Ce are distributed on the surface of the glass structure except the residual interface of the needle-tipped tubular structure; Na+ and some Nd + Occupy A I It forms a tetrahedral NaNd9(SiO4)6O2 crystal structure with the surrounding 9 oxygen atoms. 2+ Replacement mix in A I Na + and Nd 3+ , forming a decahedral Ca2Nd8(SiO4)6O2 crystal structure with the surrounding 7 oxygen atoms. XPS results show that some Ce 4+ Will be restored to Ce 3+ One case is to replace the Nd in AI and AII in NaNd9(SiO4)6O2 to form Na 1-x Ce x+y Nd 9-y (SiO4)6O2 crystal phase structure, another case is to replace Ca2Nd8(SiO4)6O2 in A II The Nd in the position forms Ca2Ce x Nd 8-x(SiO4)6O2 crystal phase structure, the remaining small amount of Nd and Ce elements are fixed in the SiO2-Na2O-Al2O3 glass phase, forming (A I x A II 10-x The (BO4)6O2 (A = Na, Ca, Ce, and Nd)) glass-ceramic solid has an extremely high solid solubility. The Nd and Ce elements are "confined" in the silicate apatite glass-ceramic structure, and the remaining Nd and Ce elements are fixed in the glass structure of the glass-ceramic material. This fixing mechanism provides a double layer of protection for the Nd and Ce elements, resulting in the normalized leaching rates (RLCe, RLNd, and RLSi) of Ce, Nd, and Si in a 90°C deionized water environment to be less than 2.0×10 -6 g·m -2 ·d -1 , 1.3×10 -6 g·m -2 ·d -1 and 1.2×10 -6 g·m -2 ·d -1 The glass ceramic solidification body has good chemical stability and meets the requirements of nuclear industry (1×10 -2 g·m -2 ·d -1 ) is expected. The glass solid has good chemical stability and meets the requirements of the nuclear industry (1×10 -2 g·m -2 ·d -1 ) expected requirements.

[0042] 4. The SiO2-Na2O-Al2O3 silicate glass solidified material prepared by the present invention has a certain effect on the An 3+ and An 4+ The simulated radioactive mud was fixed, and a part of the solidified body of the simulated radioactive mud with different Nd2O3 and CeO2 contents appeared a silicate glass material with CeO2 crystal phase precipitation, and Nd element enrichment appeared in the crystallization of CeO2. At the same time, (A I x A II 10-x Two solid forms of glass-ceramic materials in which (BO4)6O2 (A=Na, Ca, Ce and Nd)) ceramic crystal phase and CeO2 crystal phase precipitate and coexist. BRIEF DESCRIPTION OF THE DRAWINGS

[0043] Figure 1 The XRD spectra of the solidified bodies obtained in Examples 6-17, 33-35, 36 and 37 of the present invention at a sintering temperature of 1100° C. are shown;

[0044] Figure 2 The XRD spectra of the solidified bodies obtained at a sintering temperature of 1200° C. in Examples 18-24, 35, and 38-43 of the present invention are shown in FIG.

[0045] Figure 3 The XRD spectra of the solidified bodies obtained in Examples 25-32 and 44-68 of the present invention at a sintering temperature of 1300° C. are shown;

[0046] Figure 4 This is an SEM image of a silicate glass solidified material with CeO2 crystal phase precipitation obtained in Example 6-32 of the present invention;

[0047] Figure 5 The (A) obtained in Examples 33-35 of the present invention I x A II 10-x SEM-EDS images of glass-ceramic materials in which (BO4)6O2 (A = Na, Ca, Ce and Nd)) ceramic phase and CeO2 precipitated phase coexist;

[0048] Figure 6 (Ca, Na) prepared in Examples 36-38 of the present invention x Nd 10-x (SiO4)6O2、Na 1-x Ce x+y Nd 9-y (SiO4)6O2 and Ca2Ce x Nd 8-x SEM-EDS image of glass ceramic material with (SiO4)6O2 ceramic crystal phase. DETAILED DESCRIPTION

[0049] To facilitate understanding of the present invention, the present invention will be described more fully below with reference to the accompanying drawings. The accompanying drawings illustrate preferred embodiments of the present invention. However, the present invention may be implemented in many different forms and is not limited to the embodiments described herein. Rather, these embodiments are provided to provide a more thorough and comprehensive understanding of the present disclosure.

[0050] It should be noted that when an element is referred to as being "fixed to" another element, it may be directly attached to the other element or there may be an intermediate element. When an element is referred to as being "connected to" another element, it may be directly connected to the other element or there may be an intermediate element. The terms "vertical," "horizontal," "left," "right," and similar expressions used herein are for illustrative purposes only and do not represent the only implementation methods.

[0051] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one skilled in the art to which this invention pertains. The terms used herein are for the purpose of describing specific embodiments only and are not intended to limit the present invention. The term "and / or" as used herein includes any and all combinations of one or more of the associated listed items.

[0052] Example 1: A simulated radioactive mud base material powder containing a glass former, the simulated radioactive mud base material powder containing a glass former comprising a simulated radioactive mud base material raw material powder and a silicate glass particle raw material powder;

[0053] A method for preparing a simulated radioactive slurry base material powder containing a glass former, comprising:

[0054] S100: preparing simulated radioactive mud base material raw material powder;

[0055] S101: Take the raw materials with mass percentages of CaCO319.81 wt%, Mg(OH)22.25 wt%, Na2CO343.28 wt%, Al(OH)315.21 wt%, Fe2O37.31 wt%, SiO25.52 wt%, Cr2O33.97 wt%, NiO 1.70 wt%, and MoO30.89 wt%;

[0056] S102: The raw materials in step S101 are mixed and stirred. The raw materials are placed in a flask and 150% of the total weight of the raw materials is added with anhydrous ethanol, and the mixture is mixed and stirred using a mechanical stirrer for 3-5 hours;

[0057] S103: drying the mixed raw materials in a constant temperature oven at 105° C. for 24 to 36 hours;

[0058] S104: ball milling the dried raw materials in a ball mill for 3 to 5 hours to prepare a uniformly mixed simulated radioactive mud base material raw material powder;

[0059] S200: preparing silicate glass particle raw material powder;

[0060] S201: taking the raw materials in mass percentages of SiO261.44 wt%, CaO11.20 wt%, Na2O7.90 wt%, BaO5.82 wt%, MgO5.82 wt%, Al2O34.78 wt%, and V2O52.64 wt%;

[0061] S202: Place the raw materials in a flask and add 150% of the total weight of the raw materials in anhydrous ethanol, and mix and stir using a mechanical stirrer for 3-5 hours;

[0062] S203: drying the mixed raw materials in a constant temperature oven at 105° C. for 24 to 36 hours;

[0063] S204: placing the dried raw material in a microwave muffle furnace for sintering at a temperature of 800° C., and keeping the sintering temperature at 800° C. for 40 min;

[0064] S205: placing the pre-sintered raw materials in a ball mill for 3 to 5 hours to obtain silicate glass particle powder;

[0065] S206: Passing the ball-milled powder through a 200-mesh sieve to obtain silicate glass particle powder with a particle size of 75 μm;

[0066] S300: preparing a simulated radioactive mud base material powder containing a glass former by mixing the simulated radioactive mud base material powder obtained in step S100 and the silicate glass particle powder obtained in step S200 in a mass percentage ratio of 100 wt %:0 wt %, and recording the sample number as SG0;

[0067] S301: Mixing, grinding, and drying a mixture of a simulated radioactive mud base material and silicate glass particle powder, and placing the dried mixture into a ball mill for 3 to 5 hours;

[0068] S302: placing the mixed powder in a microwave muffle furnace and heating it to 1000°C at a heating rate of 20°C / min, then heating it to 1100 / 1200 / 1300°C at a heating rate of 10°C / min, and keeping it at the target temperature for 40 minutes, and then naturally cooling it to room temperature to prepare a SiO2-Na2O-Al2O3 curing system material;

[0069] Example 2:

[0070] The difference from the previous embodiment is that the simulated radioactive mud base material powder in step S300 and the silicate glass particle raw material powder obtained in step S200 are prepared in a ratio of 70 wt %:30 wt % to obtain a simulated radioactive mud base material powder containing a glass former, and the sample is numbered SG30.

[0071] Example 3:

[0072] The difference from the previous embodiment is that the simulated radioactive slurry base material powder in step S300 and the silicate glass particle raw material powder obtained in step S200 are prepared in a ratio of 60 wt %:40 wt % to obtain a simulated radioactive slurry base material powder containing glass formers. The sample is numbered SG40.

[0073] Example 4:

[0074] The difference from the previous embodiment is that the simulated radioactive mud base material powder in step S300 and the silicate glass particle raw material powder obtained in step S200 are mixed in a mass percentage ratio of 50 wt%:50 wt% to prepare a simulated radioactive mud base material powder containing glass formers, and the sample is numbered SG50.

[0075] Example 5:

[0076] The difference from the previous embodiment is that the simulated radioactive mud base material powder in step S300 and the silicate glass particle raw material powder obtained in step S200 are prepared in a ratio of 40 wt %:60 wt % to obtain a simulated radioactive mud base material powder containing glass formers, and the sample is numbered SG60.

[0077] The table of the simulated radioactive slurry base material powder containing glass formers prepared in Examples 1-5 is as follows:

[0078]

[0079] Example 6:

[0080] The difference from the previous embodiment is that a method for treating An 3+ With An 4+ The sintered solidified body of the radioactive mud comprises simulated radioactive mud base material powder containing glass formers, Nd2O3 and CeO2;

[0081] S400: Mixing the simulated radioactive mud base material powder obtained in Example 1 with Nd2O3 and CeO2 to prepare simulated radioactive mud;

[0082] S401: Nd2O3 and CeO2 in the simulated radioactive mud are mixed in a two-phase manner according to a mass percentage of 0 to 60 wt%, stirred, ground, dried and ball-milled to obtain the simulated radioactive mud; the simulated radioactive mud base material powder is mixed with the Nd2O3 and CeO2 raw materials, ground and dried, and the dried mixed powder is placed in a ball mill and ball-milled for 3 to 5 hours;

[0083] S402: drying the mixed raw materials in a constant temperature oven at 105° C. for 24 to 36 hours;

[0084] The mass percentage ratios of the simulated radioactive mud base material powder, Nd2O3 and CeO2 are as follows:

[0085]

[0086] A silicate glass solid material having CeO2 crystal phase precipitated is prepared by mixing 40 wt% of the simulated radioactive mud obtained in No. 1 and 60 wt% of the silicate glass particle powder obtained in step 200 of Example 1, and drying the mixture to obtain a mixed powder, which is recorded as sample number N5-C5. The mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, then to 1100°C at a heating rate of 10°C / min, and maintained at the target temperature for 40 minutes, followed by natural cooling to room temperature, to obtain a silicate glass solid material having CeO2 crystal phase precipitated.

[0087] Example 7:

[0088] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 2 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, and recorded as sample number N5-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0089] Example 8:

[0090] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 3 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0091] Example 9:

[0092] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 4 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C20; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0093] Example 10:

[0094] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 5 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C25; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0095] Example 11:

[0096] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 6 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N10-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0097] Example 12:

[0098] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 7 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N10-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0099] Example 13:

[0100] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 8 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, and recorded as sample numbers N10-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0101] Example 14:

[0102] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 9 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N10-C20; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0103] Example 15:

[0104] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 10 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N15-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0105] Example 16:

[0106] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 11 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N15-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0107] Example 17:

[0108] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 12 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N15-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0109] Example 18:

[0110] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 2 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, and recorded as sample number N5-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0111] Example 19:

[0112] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 3 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0113] Example 20:

[0114] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 4 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C20; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0115] Example 21:

[0116] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 5 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C25; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0117] Example 22:

[0118] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 8 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, which is recorded as sample number N10-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0119] Example 23:

[0120] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 9 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N10-C20; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0121] Example 24:

[0122] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 11 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N15-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0123] Example 25:

[0124] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 3 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0125] Example 26:

[0126] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 4 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C20; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0127] Example 27:

[0128] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 5 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C25; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0129] Example 28:

[0130] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 9 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N10-C20; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0131] Example 29:

[0132] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained according to No. 14 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N15-C25; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0133] Example 30:

[0134] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 20 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N20-C30; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0135] Example 31:

[0136] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 21 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N25-C35; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0137] Example 32:

[0138] The difference from the previous embodiment is that a silicate glass solid material with CeO2 crystal phase precipitated is obtained, and 40 wt% of the simulated radioactive mud obtained according to No. 33 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N30-C30; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a silicate glass solid material with CeO2 crystal phase precipitated.

[0139] Example 33:

[0140] The difference from the previous embodiment is that a I x A II 10-xA glass-ceramic material in which (SiO4)6O2 (A = Na, Ca, Ce and Nd)) ceramic crystal phase and CeO2 crystal phase precipitate coexisted was prepared by mixing 40 wt% of the simulated radioactive mud obtained in No. 12 and 60 wt% of the silicate glass particle powder obtained in Example 2, and obtaining a mixed powder by mixing and drying, which was recorded as sample number N15-C15; the mixed powder was placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain (A I x A II 10-x A glass-ceramic material in which (SiO4)6O2 (A = Na, Ca, Ce and Nd)) ceramic crystal phase and CeO2 crystal phase precipitate and coexist.

[0141] Example 34:

[0142] The difference from the previous embodiment is that a I x A II 10-x A glass-ceramic material in which (SiO4)6O2 (A = Na, Ca, Ce and Nd)) ceramic crystal phase and CeO2 crystal phase precipitate coexist is prepared. 40 wt% of the simulated radioactive mud obtained in No. 16 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, which is recorded as sample number N20-C10. The mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1100°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain (A I x A II 10-x A glass-ceramic material in which (SiO4)6O2 (A = Na, Ca, Ce and Nd)) ceramic crystal phase and CeO2 crystal phase precipitate and coexist.

[0143] Example 35:

[0144] The difference from the previous embodiment is that a I x A II 10-xA glass-ceramic material in which (SiO4)6O2 (A = Na, Ca, Ce and Nd)) ceramic crystal phase and CeO2 crystal phase precipitate coexist is prepared. 40 wt% of the simulated radioactive mud obtained in No. 16 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, which is recorded as sample number N20-C10. The mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain (A I x A II 10-x A glass-ceramic material in which (SiO4)6O2 (A = Na, Ca, Ce and Nd)) ceramic crystal phase and CeO2 crystal phase precipitate and coexist.

[0145] Example 36:

[0146] The difference from the previous embodiment is that a silicate (A I x A II 10-x (SiO4)6O2 (A = Na, Ca, Ce and Nd)) glass ceramic solidified body material, 40 wt% of the simulated radioactive mud obtained in No. 15 and 60 wt% of the silicate glass particle powder obtained in Example 2 were taken, mixed and dried to obtain a mixed powder, recorded as sample number N20-C5; the mixed powder was placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, then heated to 1100°C at a heating rate of 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain (Ca, Na) x Nd 10-x (SiO4)6O2、Na 1-x Ce x+y Nd 9-y (SiO4)6O2 and Ca2Ce x Nd 8-x Glass ceramic material with (SiO4)6O2 ceramic crystal phase.

[0147] Example 37:

[0148] The difference from the previous embodiment is that a silicate (A I x A II 10-x(SiO4)6O2 (A = Na, Ca, Ce and Nd)) glass ceramic solidified body material, 40 wt% of the simulated radioactive mud obtained in No. 21 and 60 wt% of the silicate glass particle powder obtained in Example 2 were taken, mixed and dried to obtain a mixed powder, recorded as sample number N25-C5; the mixed powder was placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, then heated to 1100°C at a heating rate of 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain (Ca, Na) x Nd 10-x (SiO4)6O2、Na 1-x Ce x+y Nd 9-y (SiO4)6O2 and Ca2Ce x Nd 8-x Glass ceramic material with (SiO4)6O2 ceramic crystal phase.

[0149] Example 38:

[0150] The difference from the previous embodiment is that a silicate (A I x A II 10-x (SiO4)6O2 (A = Na, Ca, Ce and Nd)) glass ceramic solidified body material, 40 wt% of the simulated radioactive mud obtained in No. 16 and 60 wt% of the silicate glass particle powder obtained in Example 2 were taken, mixed and dried to obtain a mixed powder, recorded as sample number N25-C5; the mixed powder was placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, then heated to 1200°C at a heating rate of 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain (Ca, Na) x Nd 10-x (SiO4)6O2、Na 1-x Ce x+y Nd 9-y (SiO4)6O2 and Ca2Ce x Nd 8-x Glass ceramic material with (SiO4)6O2 ceramic crystal phase.

[0151] Example 39:

[0152] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 1 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0153] Example 40:

[0154] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 6 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N10-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at a heating rate of 10°C / min, and maintained at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0155] Example 41:

[0156] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 7 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N10-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0157] Example 42:

[0158] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 10 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N15-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0159] Example 43:

[0160] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 15 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N20-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1200°C at a heating rate of 10°C / min, and maintained at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0161] Example 44:

[0162] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in Example 1 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N5-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0163] Example 45:

[0164] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 2 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, which is recorded as sample number N5-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0165] Example 46:

[0166] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 6 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N10-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and maintained at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0167] Example 47:

[0168] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 7 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N10-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0169] Example 48:

[0170] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 8 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, which is recorded as sample number N10-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0171] Example 49:

[0172] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 10 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N15-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0173] Example 50:

[0174] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 11 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N15-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0175] Example 51:

[0176] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 12 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N15-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0177] Example 52:

[0178] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 13 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N15-C20; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0179] Example 53:

[0180] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 15 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N20-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0181] Example 54:

[0182] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 16 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N20-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0183] Example 55:

[0184] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 17 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N20-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0185] Example 56:

[0186] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 18 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N20-C20; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0187] Example 57:

[0188] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 19 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N20-C25; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0189] Example 58:

[0190] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 21 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N25-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0191] Example 59:

[0192] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 22 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N25-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0193] Example 60:

[0194] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 23 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N25-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0195] Example 61:

[0196] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 24 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N25-C20; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0197] Example 62:

[0198] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 25 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N25-C25; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0199] Example 63:

[0200] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 26 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N25-C30; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0201] Example 64:

[0202] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 28 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N30-C5; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0203] Example 65:

[0204] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 29 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N30-C10; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0205] Example 66:

[0206] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 30 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N30-C15; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0207] Example 67:

[0208] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 31 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N30-C20; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0209] Example 68:

[0210] The difference from the previous embodiment is that a SiO2-Na2O-Al2O3 silicate glass solid material is obtained, and 40 wt% of the simulated radioactive mud obtained in No. 32 and 60 wt% of the silicate glass particle powder obtained in Example 2 are taken, mixed and dried to obtain a mixed powder, recorded as sample number N30-C25; the mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, and then heated to 1300°C at a heating rate of 10°C / min, and kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 silicate glass solid material.

[0211] The above embodiment is described below with reference to the accompanying drawings:

[0212] from Figure 1-Figure 3It can be seen that when the sintering temperatures are 1100°C, 1200°C and 1300°C respectively, by using the SiO2-Na2O-Al2O3 silicate glass solidified body material of the present invention, Nd2O35 wt.% and CeO25 wt.%, Nd2O310 wt.% and CeO25 wt.%, Nd2O310 wt.% and CeO210 wt.%, Nd2O315 wt.% and CeO25 wt.%, and Nd2O320 wt.% and CeO25 wt.% can be achieved at a sintering temperature of 1200°C. At the sintering temperature of 1300 ℃, the contents of Nd2O35 wt.% and CeO25 wt.%, Nd2O35 wt.% and CeO210 wt.%, Nd2O310 wt.% and CeO25 wt.%, Nd2O310 wt.% and CeO210 wt.%, Nd2O310 wt.% and CeO215 wt.%, Nd2O315 wt.% and CeO25 wt.%, Nd2O315 wt.% and CeO210 wt.%, Nd2O315 wt.% and CeO215 wt.%, Nd2O315 wt.% and CeO220 wt.%, Nd2O320 wt.% and CeO25 wt.%, Nd2O320 wt.% and CeO210 wt.%, Nd2O320 wt.% and CeO215 wt.%, Nd2O320 wt.% and CeO220 wt.%, Nd2O320 wt.% and CeO225 wt.%, Nd2O325 wt.% and CeO25 wt.%, Nd2O325 wt.% and CeO210 wt.%, Nd2O325 wt.% and CeO215 wt.%, Nd2O325 wt.% and CeO220 wt.%, Nd2O325 wt.% and CeO225 wt.%, Nd2O325 wt.% and CeO230 wt.%, Nd2O330 wt.% and CeO25 wt.%, Nd2O330 wt.% and CeO210 wt.%, Nd2O330 wt.% and CeO215 wt.%, Nd2O330 wt.% and CeO220 wt.%, and Nd2O330 wt.% and CeO225 wt.%. As can be seen from the figure, there is no obvious diffraction peak, and no other phases appear in the glass solidified body sample. At 1200 ℃, the glass solidified bodies containing Nd2O35 wt.% and CeO210 wt.%, Nd2O310 wt.% and CeO210 wt.%, and Nd2O315 wt.% and CeO215 wt.% are mainly composed of Si4O 11 6-The main structural unit is sheet silicate group, Si4O 11 6- The total content of sheet silicate groups and SiO2 three-dimensional network structural units is 48%, 56% and 59% respectively. The Si4O in the glass solidified bodies containing Nd2O315 wt.% and CeO220 wt.%, Nd2O325 wt.% and CeO230 wt.%, and Nd2O330 wt.% and CeO225 wt.% at 1300 ℃ is 2.34%. 11 6- The total proportions of sheet silicate groups and SiO2 three-dimensional network structural units are 51%, 55% and 39% respectively. These solids all show good glass polymerization degree; XPS results show that some Ce 4+ Will be restored to Ce 3+ ;

[0213] like Figure 4-Figure 6 The SEM-EDS results shown in the figure show that Si, Na, Ca, O, Ce, and Nd are uniformly distributed throughout the solidified structure with no elemental enrichment. HRTEM-SAED results reveal the apparent disorder and amorphous diffraction rings of the amorphous structure. Therefore, the SiO2-Na2O-Al2O3 silicate glass solidified structure can effectively immobilize simulated radioactive mud containing the aforementioned Nd2O3 and CeO2 contents, while also exhibiting a high compatibility ratio and excellent glass polymerization. The normalized leaching rates (RLCe, RLNd, and RLSi) of Ce, Nd, and Si in deionized water at 90°C are less than 2.2×10 -6 g·m -2 ·d -1 , 1.5×10 -6 g·m -2 ·d -1 , 1.4×10 -6 g·m -2 ·d -1 The glass solidification body has good chemical stability and meets the requirements of nuclear industry (1×10 -2 g·m -2 ·d -1 ) expected requirements.

[0214] The XRD spectrum also shows that silicate apatite (A I x A II 10-xIn the (BO4)6O2 (A = Na, Ca, Ce and Nd)) glass ceramic solidification material, the solidification treatment of simulated radioactive mud with Nd2O320 wt.% and CeO25 wt.%, Nd2O325 wt.% and CeO25 wt.% at a sintering temperature of 1100℃ and Nd2O325 wt.% and CeO25 wt.% at a sintering temperature of 1200℃ can be achieved. The crystal phase of (Ca,Na)xNd 10-x (SiO4)6O2、Na 1-x Ce x+y Nd 9-y (SiO4)6O2 and Ca2Ce x Nd 8-x (SiO4)6O2 contains Nd and Ce Ca-silicon oxyapatite and Na-silicon oxyapatite phases, and the XRD spectrum results show a steamed bun peak. This sample is silicon oxyapatite (A I x A II 10-x (BO4)6O2(A=Na, Ca, Ce and Nd)) glass-ceramic materials;

[0215] And as Figure 4-Figure 6 The SEM-EDS results shown in the figure show that a large number of needle-tipped tubular structures appear on the surface of the solidified body of the simulated radioactive mud containing 25 wt.% Nd2O3 and 25 wt.% CeO2. The elements Si, Na, Ca, O, Ce and Nd are obviously enriched on the needle-tipped tubular structures, and Al, Na, Si, O, and a small amount of Nd and Ce are distributed on the surface of the glass structure of the residual interface except the needle-tipped tubular structure; Na+ and part of Nd+ occupy A I It forms a tetrahedral NaNd9(SiO4)6O2 crystal structure with the surrounding 9 oxygen atoms. 2+ Replacement mix in A I Na + and Nd 3+ , forming a decahedral Ca2Nd8(SiO4)6O2 crystal structure with the surrounding 7 oxygen atoms. XPS results show that some Ce 4+ Will be restored to Ce 3+ , one case is to replace NaNd9(SiO4)6O2 in A I and A II Nd forms Na 1- x Ce x+y Nd 9-y (SiO4)6O2 crystal phase structure, another case is to replace Ca2Nd8(SiO4)6O2 in A II The Nd in the position forms Ca2Ce xNd 8-x (SiO4)6O2 crystal phase structure, the remaining small amount of Nd and Ce elements are fixed in the SiO2-Na2O-Al2O3 glass phase, forming (A I x A II 10-x The (BO4)6O2 (A = Na, Ca, Ce, and Nd)) glass-ceramic solid has an extremely high solid solubility. The Nd and Ce elements are "confined" in the silicate apatite glass-ceramic structure, and the remaining Nd and Ce elements are fixed in the glass structure of the glass-ceramic material. This fixing mechanism provides a double layer of protection for the Nd and Ce elements, resulting in the normalized leaching rates (RLCe, RLNd, and RLSi) of Ce, Nd, and Si in a 90°C deionized water environment to be less than 2.0×10 -6 g·m -2 ·d -1 , 1.3×10 -6 g·m -2 ·d -1 and 1.2×10 -6 g·m -2 ·d -1 The glass ceramic solidification body has good chemical stability and meets the requirements of nuclear industry (1×10 -2 g·m -2 ·d -1 ) expected requirements; the glass solidification body has good chemical stability and meets the requirements of nuclear industry (1×10 -2 g·m -2 ·d -1 ) expected requirements.

[0216] The ball mill in the above embodiment can be a planetary ball mill or other existing ball mills, and the simulated radioactive mud has the same chemical properties as An 3+ and An 4+ Similar radioactive mud or non-radioactive mud;

[0217] In the above examples: the raw materials used are all commercially available products and are AR analytical grade reagents;

[0218] In the above embodiment: the mass percentage ratio is to mix the ingredients according to the percentage of the total mass set manually;

[0219] In the above embodiments, the process parameters (drying temperature, ball milling time, etc.) in each step are within a range of values, and are applicable as long as the operation objectives are met.

[0220] The present invention is not limited to the above embodiments, and all embodiments described in the present invention can be implemented and have the above good effects.

[0221] The technical features of the above-mentioned embodiments can be combined arbitrarily. In order to make the description concise, not all possible combinations of the technical features in the above-mentioned embodiments are described. However, as long as there is no contradiction in the combination of these technical features, they should be considered to be within the scope of this specification.

[0222] The above-described embodiments merely represent several embodiments of the present invention. While the descriptions are relatively specific and detailed, they should not be construed as limiting the scope of the present invention. It should be noted that a person skilled in the art would be able to make various modifications and improvements without departing from the spirit of the present invention, all of which fall within the scope of protection of the present invention. Therefore, the scope of protection of the present invention shall be determined by the appended claims.

Claims

1. A method for treating An 3+ With An 4+ A method for solidifying a sintered solidified body of radioactive mud, characterized in that: include S100: preparing simulated radioactive mud base material raw material powder; S200: preparing silicate glass particle raw material powder; S300: preparing a simulated radioactive mud base material powder containing a glass former by mixing the simulated radioactive mud base material powder obtained in step S100 with the silicate glass particle powder obtained in step S200 in a ratio of 40-100 wt % to 0-60 wt % by mass; S400: preparing simulated radioactive mud by mixing the simulated radioactive mud base material powder obtained in step S100 with radionuclides or simulated radionuclides in a mass ratio of 60-100 wt%:0-40 wt% to obtain simulated radioactive mud, and then preparing a solidified material by mixing the silicate glass particle powder obtained in step S200 with the simulated radioactive mud in a mass ratio of 60 wt%:40 wt% to obtain a solidified material; The simulated radioactive mud is chemically similar to An 3+ and An 4+ Similar radioactive mud or non-radioactive mud; The steps of preparing silicate glass particle raw material powder include: S201: taking the raw materials in mass percentages of SiO261.44 wt%, CaO11.20 wt%, Na2O7.90 wt%, BaO5.82 wt%, MgO5.82 wt%, Al2O3 4.78 wt%, and V2O52.64 wt%; S202: Place the raw materials in a flask and add 150% of the total weight of the raw materials in anhydrous ethanol, and mix and stir using a mechanical stirrer for 3-5 hours; S203: drying the mixed raw materials in a constant temperature oven at 105° C. for 24 to 36 hours; S204: placing the dried raw material in a microwave muffle furnace for sintering at a temperature of 800° C., and keeping the sintering temperature at 800° C. for 40 min; S205: placing the pre-sintered raw materials in a ball mill for 3 to 5 hours to obtain silicate glass particle powder; S206: Passing the ball-milled powder through a 200-mesh sieve to obtain silicate glass particle powder with a particle size of 75 μm; The step S300 further includes: S301: Mixing, grinding, and drying a mixture of a simulated radioactive slurry base material raw material powder and a silicate glass particle raw material powder, and placing the dried mixed powder into a ball mill for 3 to 5 hours; S302: placing the mixed powder in a microwave muffle furnace and heating it to 1000°C at a heating rate of 20°C / min, then heating it to 1100-1300°C at a heating rate of 10°C / min, keeping it at the target temperature for 40 minutes, and then naturally cooling it to room temperature to obtain a SiO2-Na2O-Al2O3 curing system material; The step S400 further includes: S401: Mixing, grinding, and drying the simulated radioactive mud and silicate glass particle raw material powder, and then putting the dried mixed powder into a ball mill for 3-5 hours; S402: The mixed powder is placed in a microwave muffle furnace and heated to 1000°C at a heating rate of 20°C / min, then heated to 1200°C at a heating rate of 10°C / min, kept at the target temperature for 40 minutes, and then naturally cooled to room temperature to obtain a SiO2-Na2O-Al2O3 glass system solid body and a silicate apatite silicate glass ceramic solid body.

2. The method for treating An-containing 3+ With An 4+ A method for solidifying a sintered solidified body of radioactive mud, characterized in that: The preparation of the simulated radioactive mud base material raw material powder comprises: S101: Take the raw materials in the following mass percentages: CaCO3 19.81 wt%, Mg(OH)2 2.25 wt%, Na2CO3 43.28 wt%, Al(OH)3 15.21 wt%, Fe2O3 7.31 wt%, SiO2 5.52 wt%, Cr2O3 3.97 wt%, NiO 1.70 wt%, and MoO3 0.89 wt%; S102: The raw materials in step S101 are mixed and stirred. The raw materials are placed in a flask and 150% of the total weight of the raw materials is added with anhydrous ethanol, and the mixture is mixed and stirred using a mechanical stirrer for 3-5 hours; S103: drying the mixed raw materials in a constant temperature oven at 105° C. for 24 to 36 hours; S104: The dried raw materials are ball-milled in a ball mill for 3 to 5 hours to prepare a uniformly mixed simulated radioactive mud matrix raw material powder.

3. The method for treating An-containing 3+ With An 4+ A method for solidifying a sintered solidified body of radioactive mud, characterized in that: The radioactive nuclides or simulated radioactive nuclides in the simulated radioactive mud include Nd2O3 and CeO2, and the Nd2O3 and CeO2 are mixed in two phases according to a mass percentage of 0 to 60 wt%, stirred, ground, dried and ball milled to obtain the simulated radioactive mud.

4. The method for treating An-containing 3+ With An 4+ A method for solidifying a sintered solidified body of radioactive mud, characterized in that: The ball mill is a planetary ball mill.

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