Radiation protection and detection device

Abstract

The application relates to an irradiation protection and detection device and belongs to the technical field of irradiation protection and detection. The material of the irradiation protection and detection device comprises Lu2O3-based transparent ceramic, the chemical general formula of the Lu2O3-based transparent ceramic is (Lu 1‑x M x )2O3, wherein M comprises at least one of Mg, Ca, Sr or Ba; 0.01<=x<=0.05. Since the Lu2O3-based transparent ceramic has high light transmittance, high shielding efficiency and linear attenuation coefficient for high-energy rays (such as gamma rays), under irradiation, the Lu2O3-based transparent ceramic can appear high-contrast and reversible irradiation-induced discoloration in the visible light region, can realize integrated and visualized irradiation protection and detection, has excellent irradiation resistance stability, can be used for a long time, and thus can realize the integration of the irradiation protection function and the irradiation detection function of the device, can effectively simplify the device structure and optimize the device performance.

Description

Technical Field

[0001] This application relates to the field of radiation protection and detection technology, and particularly to a radiation protection and detection device. Background Technology

[0002] With the rapid development of nuclear energy technology, medical imaging equipment, and space exploration engineering, the requirements for the stability and functionality of materials in high-energy radiation environments have significantly increased. Existing radiation protection and detection systems often employ a composite structure of radiation protection devices and radiation detection devices, such as lead glass or tungsten alloy shielding layers combined with scintillation crystals or semiconductor detectors. This structure is not only heavy, complex, and difficult to manufacture, but also prone to problems such as interface damage, optical attenuation, and shortened lifespan under strong radiation conditions.

[0003] Therefore, how to simplify the structure and improve the performance of radiation protection and detection devices is of great research value. Summary of the Invention

[0004] To address the shortcomings of existing technologies, this application provides an irradiation protection and detection device to effectively improve the problems of complex structure and insufficient performance of existing irradiation protection and detection devices.

[0005] This application provides an irradiation protection and detection device, the material of which includes Lu2O3-based transparent ceramic. The general chemical formula of Lu2O3-based transparent ceramic is (Lu... 1-x M x )2O3, wherein M includes at least one of Mg, Ca, Sr or Ba; 0.01≤x≤0.05.

[0006] In the aforementioned technical solution, the radiation protection and detection device designed in this application incorporates Lu2O3-based transparent ceramic. This Lu2O3-based transparent ceramic possesses high light transmittance while exhibiting high shielding efficiency and a high linear attenuation coefficient against high-energy radiation (such as gamma rays, neutrons, and X-rays). Under radiation, it displays high-contrast, reversible radiochromic changes in the visible light region, enabling the recording or display of radiation events. This achieves integrated, visualized radiation protection and detection, and also demonstrates excellent radiation resistance stability, allowing for long-term cyclic use. Using this Lu2O3-based transparent ceramic to fabricate radiation protection and detection devices integrates radiation protection and detection functions, effectively simplifying device structure and optimizing device performance. It has significant scientific value and broad application prospects in fields such as nuclear safety monitoring, medical imaging detection, space radiation monitoring, and high-energy particle physics experiments.

[0007] Among them, the general chemical formula of Lu2O3-based transparent ceramics is designed as (Lu 1-x M xIntroducing divalent Mg, Ca, Sr, or Ba ions into high-density, wide-bandgap transparent Lu₂O₃ ceramics provides strong absorption cross-sections and high mass density, enabling high-energy radiation protection and imparting excellent radiation resistance. When irradiated by high-energy rays (such as gamma rays, neutrons, and X-rays), the doped Mg, Ca, Sr, or Ba divalent ions can induce controllable oxygen vacancies (V₂O₃) through localized charge compensation. O The formation of optically active defect centers causes a decrease in the transmittance of the visible light region and a darkening of the color. When exposed to visible or infrared light, the optically active defect centers are eliminated, and the transparency is restored, thus exhibiting reversible radiation-induced color change and self-healing properties.

[0008] In some implementations, 0.01 ≤ x ≤ 0.03.

[0009] In the above technical solution, by adjusting the range of doping amount, the number of defect energies formed in the Lu2O3 lattice can be adjusted accordingly, thereby improving the irradiation response speed and radiochromic contrast, and improving the detection accuracy of the device; in addition, it is also beneficial to reduce the damage to the integrity of the Lu2O3 crystal, and to balance and maintain the high transmittance and high radiation shielding efficiency of the device.

[0010] In some embodiments, the Lu2O3-based transparent ceramic is also doped with Yb. 3+ Ce 3+ Gd 3+ Ta 5+ or Zr 4+ At least one of them.

[0011] In the above technical solution, by further doping with Yb 3+ Ce 3+ Gd 3+ These rare-earth activated ions are doped into the Lu2O3 lattice, effectively improving the irradiation response intensity and response speed of the device with minimal impact on transparency; further doping with Ta... 5+ or Zr 4+ These high-valence cations can enter the Lu2O3 lattice through cation substitution, and synergistically construct a "multi-level defect energy level system" with the original M ions. This allows for the regulation of the density, position, and distribution of defect energy levels, effectively improving the radiation protection performance, transparency, and structural and performance stability of the device.

[0012] In some embodiments, the preparation method of Lu2O3-based transparent ceramics includes the following steps: Lu2O3 and M-containing 2+The dopants are mixed and pressed into green blanks, and then subjected to cold isostatic pressing, sintering and hot isostatic pressing to obtain Lu2O3-based transparent ceramics; wherein the dopants include MCO3 or MO.

[0013] In the above technical solution, this application first combines Lu2O3 and M-containing... 2+ The dopant mixing achieves uniform dispersion of the dopant in Lu2O3 (i.e., achieving M). 2+ The uniform dispersion of the dopant is pressed to form a uniform and dense green blank. Cold isostatic pressing is then performed to increase the density of the green blank and eliminate porosity and lamination defects inside the green blank. Sintering is then performed to achieve preliminary densification of the green blank and complete the solid solution and lattice fusion of the dopant. Finally, hot isostatic pressing is performed to eliminate the closed pores remaining after sintering, achieving near-full densification of the transparent ceramic and obtaining a high-density, uniformly doped Lu2O3-based transparent ceramic. This is beneficial for further improving the radiation protection performance, transparency, and radiation detection performance of integrated radiation protection and detection devices.

[0014] In some implementations, the pressure of the cold isostatic pressing process is 150 MPa to 250 MPa.

[0015] In the above technical solution, by controlling the pressure of cold isostatic pressing within a suitable range, it is beneficial to further improve the density of the blank and eliminate porosity and delamination defects inside the blank, thereby further improving the radiation protection performance, transparency and radiation detection performance of the device.

[0016] In some embodiments, the sintering temperature is 1700℃~1750℃ and the time is 5h~10h.

[0017] In the above technical solution, sintering temperature and time are within a suitable range, which is beneficial for achieving initial densification. Simultaneously, controlling the grain size within a suitable range is beneficial for matching the subsequent hot isostatic pressing step to effectively refine the grains. Furthermore, within this temperature and time range, M can be... 2+ Ions overcome the grain boundary barrier and diffuse into Lu₂O₃ through the lattice, forming a uniformly distributed Lu₂O₃. 3+ Vacancy defects can help further improve the radiation protection performance, transparency, and radiation detection performance of the device.

[0018] In some embodiments, hot isostatic pressing is carried out in an inert atmosphere at a temperature of 1600°C to 1700°C, a pressure of 180 MPa to 220 MPa, and a time of 2 to 6 hours.

[0019] In the above technical solution, by controlling the hot isostatic pressing process in an inert atmosphere and keeping the temperature, pressure and time within a suitable range, the density of transparent ceramics can be increased to 99.9%, the grain size can be maintained within a suitable range, and the lattice defects can be further stabilized and homogenized, which is conducive to further improving the radiation protection performance, transparency and radiation detection performance of the device.

[0020] In some embodiments, after the hot isostatic pressing step, an annealing treatment is further included, which is carried out in an oxygen-containing atmosphere at a temperature of 1350°C to 1450°C for 5 to 15 hours.

[0021] In the above technical solution, annealing is used to eliminate lattice stress and defects generated by sintering and hot isostatic pressing. By controlling the annealing process to be carried out in an oxygen-containing atmosphere and with the temperature and time within a suitable range, supplementary lattice oxygen can be introduced to suppress oxygen vacancy disorder, optimize defect energy levels, and effectively eliminate lattice stress and defects. This is beneficial to further improve the radiation protection performance, transparency, and radiation detection performance of the device.

[0022] In some embodiments, the method for preparing the green blank includes: According to the stoichiometric ratio of the general chemical formula, Lu2O3 powder and M-containing... 2+ The dopant powder is mixed and wet ball-milled to form a slurry; The slurry is dried, sieved, and molded to form a raw blank.

[0023] In the above technical solution, the use of wet ball milling combined with drying, sieving, and molding to form a blank is beneficial to the uniform dispersion of dopants in the Lu2O3 matrix, forming a uniform and dense blank, which is beneficial to further improve the radiation protection performance, transparency, and radiation detection performance of the device.

[0024] In some implementations, the wet ball milling time is 15h to 20h.

[0025] In the above technical solution, by controlling the wet ball milling time within a suitable range, it is beneficial to further improve the dispersion uniformity of the dopant in the Lu2O3 matrix, thereby further improving the radiation protection performance, transparency, and radiation detection performance of the device.

[0026] In some embodiments, the drying temperature is 60°C to 80°C.

[0027] In the above technical solution, by controlling the drying temperature within a suitable range, gentle drying helps to reduce powder agglomeration, thereby further improving the radiation protection performance, transparency, and radiation detection performance of the device.

[0028] In some implementations, the molding pressure is 10 MPa to 30 MPa.

[0029] In the above technical solution, by controlling the molding under lower pressure, the green blank can be given appropriate strength while reducing damage to the material structure.

[0030] In some embodiments, the Lu2O3-based transparent ceramic has a transmittance of ≥80% in the wavelength range of 400nm to 1200nm.

[0031] In the above technical solution, Lu2O3-based transparent ceramics have high transparency, which can ensure the high sensitivity and high accuracy of the device's irradiation detection performance, and can also be effectively used as an observation window to achieve visual protection and detection.

[0032] In some embodiments, when the thickness is 5 mm, Lu2O3-based transparent ceramics are used for 1.25 mgy 60 The shielding efficiency of Co gamma rays is ≥80%; and / or, after 1.25 mgy 60 After irradiation with Co gamma rays, the linear attenuation coefficient of Lu₂O₃-based transparent ceramics at a wavelength of 600 nm is >0.5 cm⁻¹. -1 .

[0033] In the above technical solution, Lu2O3-based transparent ceramics can achieve high shielding efficiency with a small thickness and have a high linear attenuation coefficient, indicating that they have excellent radiation protection performance. They are also conducive to the thinning and weight reduction of radiation protection and detection devices, and are more conducive to maintaining high transparency and high radiation detection performance.

[0034] In some embodiments, Lu2O3-based transparent ceramics are subjected to 1 mgy at a wavelength of 600 nm. 60 The contrast ratio of radiochromic changes before and after Co γ-ray irradiation is ≥60%.

[0035] In the above technical solution, Lu2O3-based transparent ceramics have high radiochromic contrast, indicating that they have high radiation response intensity, which is beneficial for the device to accurately record and interpret the visible light intensity of irradiation.

[0036] In some embodiments, Lu2O3-based transparent ceramics are subjected to 1 mgy 60 After being irradiated with Co γ-rays and then exposed to visible or infrared light, the transmittance of Lu2O3-based transparent ceramics at a wavelength of 400 nm is ≥75% when the irradiation time is ≥30 min.

[0037] In the above technical solution, Lu2O3-based transparent ceramics exhibit radiochromic changes after irradiation, and can regain transparency after irradiation with visible or infrared light, with a transmittance of ≥75%. This indicates that Lu2O3-based transparent ceramics can undergo reversible radiochromic changes and have excellent optical and structural stability. They do not suffer significant structural damage after irradiation with high-energy rays, which is beneficial for the long-term cyclic use of the device. Attached Figure Description

[0038] To more clearly illustrate the technical solutions of the embodiments of this application, the accompanying drawings used in the embodiments will be briefly introduced below. It should be understood that the following drawings only show some embodiments of this application and should not be regarded as a limitation of the scope. For those skilled in the art, other related drawings can be obtained based on these drawings without creative effort.

[0039] Figure 1 The image shows the XRD pattern of the Lu2O3-based transparent ceramic prepared in Example 1 of this application.

[0040] Figure 2 This is a transmittance curve of the Lu2O3-based transparent ceramic prepared in Example 1 of this application before and after γ-ray irradiation.

[0041] Figure 3 The Lu2O3-based transparent ceramic prepared in Example 1 of this application was subjected to 1.25 mgy 60 Attenuation curve of Co γ-ray irradiation.

[0042] Figure 4 The images show the optical properties of the Lu2O3-based transparent ceramic prepared in Example 1 of this application before and after γ-ray irradiation. Detailed Implementation

[0043] The following detailed description of embodiments of the radiation protection and detection device of this application is provided with appropriate reference to the accompanying drawings; however, unnecessary details may be omitted. For example, detailed descriptions of well-known matters and repetitive descriptions of practically identical structures may be omitted. This is to avoid unnecessarily lengthy descriptions and to facilitate understanding by those skilled in the art. Furthermore, the accompanying drawings and the following description are provided to enable those skilled in the art to fully understand this application and are not intended to limit the subject matter of the claims.

[0044] The "range" disclosed in this application is defined by a lower limit and an upper limit. A given range is defined by selecting a lower limit and an upper limit, which define the boundaries of a particular range. Ranges defined in this way can include or exclude endpoints and can be arbitrarily combined; that is, any lower limit can be combined with any upper limit to form a range. For example, if ranges of 60~120 and 80~110 are listed for a specific parameter, it is also expected that ranges of 60~110 and 80~120 are also included. Furthermore, if minimum range values ​​of 1 and 2 are listed, and if maximum range values ​​of 3, 4, and 5 are listed, then the following ranges are all expected: 1~3, 1~4, 1~5, 2~3, 2~4, and 2~5. In this application, unless otherwise stated, the numerical range "a~b" represents a shortened representation of any combination of real numbers between a and b, where a and b are real numbers. For example, the numerical range "0~5" indicates that all real numbers between "0~5" have been listed in this article; "0~5" is simply a shortened representation of these numerical combinations. Furthermore, when a parameter is stated as an integer ≥2, it is equivalent to disclosing that the parameter is, for example, an integer such as 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, etc.

[0045] Unless otherwise specified, all embodiments and optional embodiments of this application can be combined to form new technical solutions.

[0046] Existing radiation protection and detection systems often employ a composite structure of radiation protection devices and radiation detection devices, such as lead glass or tungsten alloy shielding layers combined with scintillation crystals or semiconductor detectors. This structure is not only heavy, complex, and difficult to manufacture, but also prone to problems such as interface damage, optical attenuation, and shortened lifespan under strong radiation conditions.

[0047] Although some studies have disclosed that using lanthanide and actinide metal oxides to prepare single crystals or rare earth ion-doped transparent ceramics can achieve radiation protection and detection to a certain extent, they usually have at least one of the following defects: (1) poor shielding efficiency against radiation, especially high-dose radiation, and low linear attenuation coefficient; (2) low contrast of radiochromic color change, slow response, and poor radiation dose monitoring effect; (3) poor radiation stability, which can easily lead to structural damage after irradiation and cannot be reused for a long time.

[0048] Therefore, existing materials cannot effectively integrate radiation protection and detection functions of the device, nor can they effectively simplify the device structure or optimize its performance.

[0049] Based on this, embodiments of this application provide an irradiation protection and detection device, the material of which includes Lu2O3-based transparent ceramic, the general chemical formula of which is (Lu2O3-based transparent ceramic is...). 1-x Mx )2O3, wherein M includes at least one of Mg, Ca, Sr or Ba; 0.01≤x≤0.05.

[0050] As an example, x can be any single value among 0.01, 0.02, 0.03, 0.04, and 0.05, or a range between any two values.

[0051] It is understood that the radiation protection and detection device referred to in this application refers to a single structural device that integrates radiation protection and radiation detection functions, rather than a structural combination of radiation protection devices and radiation detection devices.

[0052] The general chemical formula of the Lu2O3-based transparent ceramic designed in this application is (Lu2O3-based transparent ceramic). 1-x M x Lutene oxide (Lu₂O₃) is introduced into high-density, wide-bandgap transparent Lu₂O₃ ceramics by introducing divalent ions of Mg, Ca, Sr, or Ba. Lu₂O₃ is a high-density (approximately 9.42 g·cm⁻¹) ion. -3 Rare earth oxides with high atomic numbers (Z=71) exhibit significantly higher linear attenuation coefficients for gamma rays and neutrons than traditional lead glass and transparent ceramic systems such as YAG and Y2O3. Furthermore, due to its cubic C-type rare earth oxide crystal structure (space group Ia-3), it possesses high symmetry and low lattice defect density, enabling near-single-crystal-level optical transparency—combining high density, high atomic number, and high optical transparency. Moreover, Lu2O3 ceramics possess higher Vickers hardness (approximately 11 GPa~12 GPa), greater thermal shock resistance, and chemical stability than lead glass, and do not contain toxic elements, aligning with the future development direction of green radiation protection materials.

[0053] Introducing heterovalent dopant ions of Mg, Ca, Sr, and Ba into the Lu₂O₃ lattice can create localized charge imbalances, thereby introducing controlled oxygen vacancy defects (V₂O₃) into the oxygen sublattice. O These oxygen vacancies can act as electron-trapping centers, and under high-energy gamma-ray, X-ray, or beta-particle irradiation, they can be excited and occupied by electrons, producing F. + or F 2+ Color centers cause a red shift in the light absorption edge of the material or a change in the color of the visible region, exhibiting a radiochromic effect.

[0054] This process can be represented as: .

[0055] When bombarded by high-energy rays or particles, electrons are excited from the valence band to the conduction band and then captured by oxygen vacancy traps, forming localized defect states. This causes changes in the optical absorption spectrum, manifested as a decrease in transmittance or a deepening of color in the visible light region. Since the formed F-center absorption band is generally located in the 2.5 eV~3.2 eV (400 nm~500 nm) wavelength range, a noticeable color change effect from colorless to red can be observed by the human eye. When the material is exposed to ultraviolet or visible light, the trapped electrons are released, the color centers are eliminated, the lattice returns to an electrically neutral state, and the color fades, i.e., a photobleaching effect occurs. This reversible radiochromic behavior allows Lu2O3-based transparent ceramics to achieve optical recording and visual detection of irradiation dose through changes in transmittance or color.

[0056] Compared to existing integrated radiation shielding and detection materials, this Lu2O3-based transparent ceramic has the following advantages: (1) It has high shielding efficiency and linear attenuation coefficient for high-energy rays. It can achieve ≥80% gamma-ray shielding efficiency with a thickness of millimeters. It also has a certain absorption effect on thermal neutrons.

[0057] (2) It has high optical transmittance, which ensures that it does not affect imaging or signal transmission when used as a window or optical readout interface; (3) The contrast of radiochromic changes before and after high-energy ray irradiation is high, and the energy dose or particle event can be accurately detected through optical changes; (4) After being irradiated by high-energy rays, it can quickly recover its transparency under visible or infrared light, and has excellent radiation resistance, thermal shock resistance and chemical stability. The shielding efficiency does not decrease significantly under high-dose irradiation. It maintains optical and structural stability in high temperature, high-dose irradiation and corrosive atmosphere, and can be used for a long time.

[0058] Therefore, by designing radiation protection and detection devices using materials including this Lu2O3-based transparent ceramic, the radiation protection and detection functions of the devices can be effectively integrated. This can effectively simplify the device structure and optimize device performance, and has significant scientific significance and broad application prospects in fields such as nuclear energy safety monitoring, medical imaging detection, space radiation monitoring, and high-energy particle physics experiments.

[0059] In some embodiments, 0.01 ≤ x ≤ 0.03.

[0060] In some embodiments, the Lu2O3-based transparent ceramic is also doped with Yb. 3+ Ce 3+ Gd 3+ Ta 5+ or Zr 4+ At least one of them.

[0061] Among them, the general chemical formula of Lu2O3-based transparent ceramics is (Lu 1-x M x N y )2O3, wherein N includes at least one of Yb, Ce, Gd, Ta or Zr. Further, 0.01≤y≤0.1.

[0062] In some embodiments, the preparation method of Lu2O3-based transparent ceramics includes the following steps: Lu2O3 and M-containing 2+ The dopants are mixed and pressed into green blanks, and then subjected to cold isostatic pressing, sintering and hot isostatic pressing to obtain Lu2O3-based transparent ceramics; wherein the dopants include MCO3 or MO.

[0063] Understandably, MCO3 or MO corresponds to the carbonate or oxide of element M. Examples of dopants include CaCO3, CaO, BaCO3, SrO, etc.

[0064] In some embodiments, the method for preparing the green blank includes: According to the stoichiometric ratio of the general chemical formula, Lu2O3 powder and M-containing... 2+ The dopant powder is mixed and wet ball-milled to form a slurry; the slurry is dried, sieved, and molded to form a green blank.

[0065] As an example, the molar ratio of Lu2O3 powder to dopant powder can be 95:10, 99:2, etc.

[0066] Furthermore, the wet ball milling time is 15h to 20h. As an example, the wet ball milling time is any one value or any two values ​​among 15h, 16h, 17h, 18h, 19h, and 20h.

[0067] Understandably, in actual operation, the conditions of ball milling can be routinely adjusted according to the actual situation to ensure that the Lu2O3 powder and dopant powder are mixed evenly. For example, the ball milling medium can be zirconium dioxide (ZrO2), and the ball-to-material ratio can be controlled at 1:3 during the ball milling process, but is not limited to this; the dispersion solvent used for ball milling can be ethanol.

[0068] Furthermore, the drying temperature is 60°C to 80°C. As an example, the drying temperature is any one value or a range between any two values ​​of 60°C, 65°C, 70°C, 75°C, and 80°C.

[0069] Furthermore, the pressure used in molding is 10MPa to 30MPa. As an example, the pressure used in molding is any one value or any two values ​​between 10MPa, 15MPa, 20MPa, 25MPa, and 30MPa.

[0070] Molding refers to forming a blank by pressing it with a mold. Furthermore, a hardened stainless steel mold can be used to press the blank, but it is not limited to this.

[0071] In some embodiments, the pressure of the cold isostatic pressing process is 150 MPa to 250 MPa. As an example, the pressure of the cold isostatic pressing process is any one value or a range between any two values ​​of 150 MPa, 200 MPa, 220 MPa, and 250 MPa.

[0072] In some embodiments, the sintering temperature is 1700°C to 1750°C, and the time is 5h to 10h. As an example, the temperature is any one value or a range between any two values ​​among 1700°C, 1710°C, 1720°C, 1730°C, 1740°C, and 1750°C; the time is any one value or a range between any two values ​​among 5h, 6h, 7h, 8h, 9h, and 10h.

[0073] Furthermore, the sintering process is carried out in a vacuum atmosphere.

[0074] In some embodiments, hot isostatic pressing is carried out in an inert atmosphere at a temperature of 1600°C to 1700°C, a pressure of 180 MPa to 220 MPa, and a time of 2 to 6 hours.

[0075] As an example, the temperature is any one value or a range between any two values ​​among 1600℃, 1620℃, 1650℃, 1680℃, and 1700℃; the pressure is any one value or a range between any two values ​​among 180MPa, 190MPa, 200MPa, 210MPa, and 220MPa; and the time is any one value or a range between any two values ​​among 2h, 3h, 4h, 5h, and 6h.

[0076] Furthermore, the inert atmosphere can be argon.

[0077] In some embodiments, after the hot isostatic pressing step, the process further includes an annealing treatment, which is carried out in an oxygen-containing atmosphere at a temperature of 1350°C to 1450°C for 5 to 15 hours.

[0078] As an example, the temperature is any one value or the range between any two values ​​among 1350℃, 1380℃, 1400℃, 1420℃, and 1450℃; the time is any one value or the range between any two values ​​among 5h, 8h, 10h, 12h, and 15h.

[0079] Furthermore, the oxygen-containing atmosphere can be air.

[0080] In some embodiments, the method further includes: performing double-sided polishing on the annealed ceramic to meet optical testing requirements.

[0081] In some embodiments, the transmittance of Lu2O3-based transparent ceramics is ≥80% in the wavelength range of 400nm to 1200nm. As an example, the transmittance of Lu2O3-based transparent ceramics at a wavelength of 600nm is 82%, etc.

[0082] In some embodiments, when the thickness is 5 mm, Lu2O3-based transparent ceramics are used for 1.25 mgy 60 The shielding efficiency of Co gamma rays is ≥80%. As an example, when the thickness is 5 mm, Lu₂O₃-based transparent ceramics provide shielding efficiency against 1.25 mgy gamma rays. 60 The shielding efficiency of Co gamma rays is 86%, etc.

[0083] In this application, shielding efficiency refers to the percentage reduction in intensity of incident gamma rays after passing through the ceramic material, used to measure the material's ability to attenuate gamma rays. The shielding efficiency of Lu2O3-based transparent ceramics against gamma rays can be tested and calculated using conventional testing methods and equipment in the art. For example, a 5mm thick Lu2O3-based transparent ceramic is used... 60 A Co radiation source emits 1.25 mgy of gamma rays and is positioned 200 mm away from a ceramic sample. Without a sample, the incident gamma ray count rate I0 is measured. A 5 mm ceramic sample is placed coaxially between the source and detector, and the gamma ray count rate I after penetrating the sample is measured. Based on the Lambert-Beer law of gamma ray attenuation through matter, the shielding efficiency η = (I0) / (I0) I) / I0×100%.

[0084] In some embodiments, via 1.25MGy 60 After irradiation with Co gamma rays, the linear attenuation coefficient of Lu₂O₃-based transparent ceramics at a wavelength of 600 nm is >0.5 cm⁻¹. -1 As an example, via 1.25MGy 60 After irradiation with Co gamma rays, the linear attenuation coefficient of Lu₂O₃-based transparent ceramics at a wavelength of 600 nm is 0.57 cm⁻¹. -1 .

[0085] In this application, the linear attenuation coefficient refers to the probability of intensity attenuation of γ-rays propagating a unit distance in a material, which can be tested and calculated using conventional testing methods and equipment in the field.

[0086] In some embodiments, at a wavelength of 600 nm, Lu2O3-based transparent ceramics are subjected to 1 mgy 60 The radiochromic contrast before and after Co gamma ray irradiation is ≥60%. As an example, at a wavelength of 600 nm, Lu₂O₃-based transparent ceramics were irradiated with 1 mgy... 60 The contrast ratio of radiochromic changes before and after Co γ-ray irradiation was 80%.

[0087] In this application, the radiochromic contrast ratio is a quantitative indicator that measures the degree of change in the transmittance of a material before and after gamma ray irradiation. Its essence is the "light absorption difference rate caused by the generation of irradiation-induced color centers". The calculation formula for the radiochromic contrast ratio is as follows: ΔT=(T0-T1) / T0×100%, where T0 is the transmittance of the material before irradiation and T1 is the transmittance of the material after irradiation.

[0088] In some embodiments, Lu2O3-based transparent ceramics are subjected to 1 mgy 60 After being irradiated with Co γ-rays and then exposed to visible or infrared light, the transmittance of Lu2O3-based transparent ceramics at a wavelength of 600 nm is ≥75% when the irradiation time is ≥30 min.

[0089] Understandably, Lu2O3-based transparent ceramics were subjected to 1 mgy 60 After being irradiated with Co gamma rays, the transparent ceramic changes color, becomes darker, and its transmittance decreases. After being irradiated with visible light (wavelength 400nm~750nm) or infrared light (wavelength 800nm~1200nm) for a period of time, the sample color returns to transparency and the transmittance increases, which means that photobleaching has occurred.

[0090] To make the objectives, technical solutions, and advantages of the embodiments of this application clearer, the technical solutions in the embodiments of this application will be clearly and completely described below. Where specific conditions are not specified in the embodiments, conventional conditions or conditions recommended by the manufacturer shall apply. Reagents or instruments whose manufacturers are not specified are all conventional products that can be purchased commercially.

[0091] Example 1 This embodiment provides an irradiation protection and detection device, the preparation method of which includes the following steps: (1) According to chemical composition (Lu 0.99 Ca 0.01Weigh out Lu₂O₃ (99.99% purity) and CaO (99.99% purity) (molar ratio Lu₂O₃:CaO = 99:2), then add an appropriate amount of anhydrous ethanol, and add zirconia pellets at a pellet-to-material ratio of 1:3. Place the mixture in a ball mill jar and ball mill in both directions for 15 hours to obtain a mixed slurry. Then dry the slurry at 70℃ and pass it through a 200-mesh sieve. Finally, mold it at 20 MPa to form a green blank.

[0092] (2) The green blank is subjected to cold isostatic pressing at 200 MPa, and then sintered at 1730℃ for 7 h in a vacuum atmosphere to obtain a preliminary crystallized structure. Then it is subjected to hot isostatic pressing at 1650℃ and 196 MPa argon for 4 h to form a highly dense and transparent body.

[0093] (3) The high-density transparent body obtained in step (2) is annealed at 1400°C for 10 hours in an air atmosphere, and finally polished on both sides to a thickness of 2.5 mm to obtain radiation protection and detection device.

[0094] Example 2 This embodiment provides a radiation protection and detection device, the preparation method of which differs from that of Embodiment 1 in that: In step (1), according to the chemical composition (Lu 0.97 Ca 0.03 Weigh Lu2O3 (purity 99.99%) and CaO (purity 99.99%) (molar ratio Lu2O3:CaO = 97:6).

[0095] Example 3 This embodiment provides a radiation protection and detection device, the preparation method of which differs from that of Embodiment 1 in that: In step (1), according to the chemical composition (Lu 0.99 Sr 0.01 Weigh Lu2O3 (purity 99.99%) and SrO (purity 99.99%) (molar ratio Lu2O3:SrO = 99:2).

[0096] Example 4 This embodiment provides a radiation protection and detection device, the preparation method of which differs from that of Embodiment 1 in that: In step (3), both sides are polished to a thickness of 3mm.

[0097] Example 5 This embodiment provides a radiation protection and detection device, the preparation method of which differs from that of Embodiment 1 in that: (1) According to chemical composition (Lu 0.98 Ca 0.01 Yb 0.01Weigh Lu2O3 (purity 99.99%), CaO (purity 99.99%) and Yb2O3 (purity 99.99%) (molar ratio Lu2O3:CaO:Yb2O3=98:2:1).

[0098] Comparative Example 1 This comparative example provides a radiation protection and detection device, the preparation method of which differs from that of Example 1 in that: No CaO is added in step (1).

[0099] Table 1 shows some of the fabrication parameters of the radiation protection and detection devices in the examples and comparative examples.

[0100] Table 1. Some fabrication parameters of radiation protection and detection devices

[0101] Performance testing and results analysis The radiation protection and detection devices prepared in the examples and comparative examples were subjected to performance tests, and the test methods are as follows: (1) XRD The transparent ceramic sample was ground into powder and tested using an X-ray diffractometer.

[0102] (2) Light transmittance Using a Lambda UV-Vis-NIR spectrometer (750, PerkinElmer, USA) The transmittance of transparent ceramic samples was tested in the wavelength range of 200 nm to 1300 nm.

[0103] (3) Gamma-ray shielding efficiency The gamma-ray shielding effectiveness of the samples was evaluated using a comprehensive experimental platform employing β / γ detection. 60 A Co radiation source emitting 1.25 MeV gamma rays was positioned 200 mm from the ceramic sample. To obtain a collimated, narrow gamma-ray beam, a collimator with a 3 mm aperture was inserted between the radiation source and the ceramic sample. The gamma-ray detector was located behind the ceramic sample, and the entire measuring apparatus was surrounded by a 10 cm thick lead plate to cancel out scattered radiation and minimize external interference.

[0104] (4) Radiation-induced color contrast Using 1MGy 60 Co γ-rays were used to irradiate radiation protection and detection devices, and the transmittance before and after irradiation was measured at 600 nm.

[0105] The formula for calculating the radiation-induced color contrast ratio is as follows: ΔT = (T0 - T1) / T0 × 100%, where T0 is the transmittance of the material before irradiation and T1 is the transmittance of the material after irradiation.

[0106] Figure 1 The XRD pattern of the Lu2O3-based transparent ceramic prepared in Example 1 of this application is shown below. Figure 1 As can be seen from the data, the ceramic material has a good crystal state and no obvious impurity peaks, indicating that the doping with M... 2+ The crystal structure of the Lu2O3-based material was not significantly altered, resulting in high-purity transparent ceramics. It should be noted that due to the presence of M in the Lu2O3-based material... 2+ The doping level is very low, therefore (Lu 0.99 Ca 0.01 In the XRD pattern of Lu₂O₃, the diffraction peaks are basically in the same positions as those of pure Lu₂O₃, and there is no obvious peak shift.

[0107] Figure 2 This is a transmittance curve of the Lu2O3-based transparent ceramic prepared in Example 1 of this application before and after γ-ray irradiation. Figure 2 It can be seen that before irradiation, the material has a transmittance of up to 82% at a wavelength of 600 nm; it also exhibits high radiochromic contrast in the wavelength range of 400 nm to 750 nm, with a radiochromic contrast ΔT at a wavelength of 600 nm. 600 It can reach 80%.

[0108] Example 1 prepared Lu2O3-based transparent ceramics for 1.25MGy 60 The shielding efficiency of Co gamma rays is as high as 86%. Figure 3 The Lu2O3-based transparent ceramic prepared in Example 1 of this application was subjected to 1.25 mgy 60 The attenuation curve of Co γ-ray irradiation, from Figure 3 It can be seen that the linear attenuation coefficient of gamma rays in Lu2O3-based transparent ceramics is 0.57 cm⁻¹. -1 This is much larger than the 0.19 cm of existing leaded glass. -1 ~0.50cm -1 It has a linear attenuation coefficient, which means it has excellent radiation protection performance.

[0109] Figure 4 These are optical images of the Lu2O3-based transparent ceramic prepared in Example 1 of this application before and after γ-ray irradiation. Figure 4 As can be seen from this, Lu2O3-based transparent ceramics, after 1 mgy 60 After being irradiated with Co gamma rays, the color deepens; it can regain its transparency after being exposed to natural light for 30 minutes.

[0110] The embodiments described above are some, but not all, of the embodiments of this application. The detailed description of the embodiments of this application is not intended to limit the scope of the claimed application, but merely to illustrate selected embodiments. All other embodiments obtained by those skilled in the art based on the embodiments of this application without inventive effort are within the scope of protection of this application.

Claims

1. A radiation protection and detection device, characterized in that, The radiation protection and detection device is made of Lu2O3-based transparent ceramic, and the general chemical formula of the Lu2O3-based transparent ceramic is (Lu 1-x M x )2O3, wherein M includes at least one of Mg, Ca, Sr or Ba; 0.01≤x≤0.

05.

2. The radiation protection and detection device according to claim 1, characterized in that, 0.01≤x≤0.03。 3. The radiation protection and detection device according to claim 1, characterized in that, The Lu2O3-based transparent ceramic is also doped with Yb. 3+ Ce 3+ Gd 3+ Ta 5+ or Zr 4+ At least one of them.

4. The radiation protection and detection device according to claim 1, characterized in that, The preparation method of the Lu2O3-based transparent ceramic includes the following steps: Lu2O3 and M-containing 2+ The dopants are mixed and pressed into a green body, and then subjected to cold isostatic pressing, sintering and hot isostatic pressing in sequence to obtain the Lu2O3-based transparent ceramic. The dopant includes at least one of MCO3 or MO.

5. The radiation protection and detection device according to claim 4, characterized in that, The pressure of the cold isostatic pressing process is 150MPa~250MPa; And / or, the sintering treatment is performed at a temperature of 1700℃~1750℃ for 5h~10h; And / or, the hot isostatic pressing treatment is carried out in an inert atmosphere at a temperature of 1600℃~1700℃, a pressure of 180MPa~220MPa, and a time of 2h~6h. Optionally, after the hot isostatic pressing step, the process further includes an annealing treatment, which is carried out in an oxygen-containing atmosphere at a temperature of 1350℃~1450℃ for 5h~15h.

6. The radiation protection and detection device according to claim 4, characterized in that, The method for preparing the green body includes: mixing the Lu2O3 powder and M-containing powder according to the stoichiometric ratio of the general chemical formula. 2+ The dopant powder is mixed and wet ball-milled to form a slurry; The slurry is dried, sieved, and molded to form the raw blank; Optionally, the wet ball milling time is 15h~20h; Optionally, the drying temperature is 60°C to 80°C; Optionally, the molding pressure is 10MPa to 30MPa.

7. The radiation protection and detection device according to any one of claims 1 to 6, characterized in that, The Lu2O3-based transparent ceramic has a transmittance of ≥80% in the wavelength range of 400nm~1200nm.

8. The radiation protection and detection device according to any one of claims 1 to 6, characterized in that, When the thickness is 5 mm, the Lu2O3-based transparent ceramic has a strength of 1.25 mgy. 60 The shielding efficiency of Co gamma rays is ≥80%; And / or, via 1.25MGy 60 After irradiation with Co γ rays, the linear attenuation coefficient of the Lu2O3-based transparent ceramic at a wavelength of 600 nm is >0.5 cm⁻¹. -1 .

9. The radiation protection and detection device according to any one of claims 1 to 6, characterized in that, At a wavelength of 600 nm, the Lu2O3-based transparent ceramic was subjected to 1 mgy 60 The contrast ratio of radiochromic changes before and after Co γ-ray irradiation is ≥60%.

10. The radiation protection and detection device according to any one of claims 1 to 6, characterized in that, The Lu2O3-based transparent ceramic was subjected to a 1 mgy reaction. 60 After being irradiated with Co γ-rays and then exposed to visible or infrared light, the Lu2O3-based transparent ceramic exhibits a transmittance of ≥75% at a wavelength of 600nm when the irradiation time is ≥30min.

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