Small LuAGCe transparent scintillation ceramic scintillator and preparation method and application thereof

Abstract

The invention relates to the technical field of ceramic scintillators, in particular to a small LuAGCe transparent ceramic scintillator and a preparation method and application thereof, and the chemical structural formula of the ceramic scintillator is (LuxCeyTb3-x-y) A < l > 5O12, wherein x ranges from 0.01 to 1, and y ranges from 0.005% to 0.002%. The ceramic scintillator prepared in the invention has high average light transmittance in a visible light region, and shows strong emission characteristics under excitation of ultraviolet light and X-rays. The results show that the ceramic material has potential application value in the fields of radiation detection, scintillation counters, medical imaging and the like.

Description

Technical Field

[0001] The invention relates to the technical field of ceramic scintillators, in particular to a small LuAGCe transparent scintillation ceramic scintillator and a preparation method and application thereof. Background Art

[0002] Transparent scintillating ceramic scintillator is an advanced material that combines high technology and multi-functions. It has shown great application potential in many fields such as radiation detection, medical imaging, high-energy physics and nuclear science. The core characteristic of this material is that it can efficiently convert high-energy rays (such as X-rays, gamma rays) or high-speed charged particles into ultraviolet or visible light.

[0003] The conversion process of scintillators is a complex and delicate process of energy transfer and release. First, when high-energy rays or particles hit the scintillator, they are absorbed by the atoms or molecules inside the material, which in turn triggers a series of physical reactions. These reactions lead to the generation of high-energy electrons or holes. These high-energy carriers migrate rapidly inside the material and interact with other particles, gradually losing energy and converting to a low-energy state.

[0004] During the transport phase, these low-energy electrons or holes will further diffuse inside the scintillator, some of which may lose energy through non-radiative means (such as thermal effects), while others may be captured by specific luminescent centers. These trapped electrons or holes will undergo a de-excitation process at the luminescent center, that is, they will jump back to a low energy level and release light energy at the same time.

[0005] Transparent scintillating ceramics have attracted much attention because they not only have excellent light transmittance, which enables the converted light to be transmitted efficiently, but also have high density, good mechanical properties and thermal stability, so that they can maintain stable working performance in extreme environments. In addition, by adjusting the composition and structure of the material, its scintillating performance can be further optimized to meet the needs of different application scenarios.

[0006] Due to the limitations of existing materials and processing technology, high-quality, highly transparent scintillating crystals have not yet been developed. Therefore, it is very necessary to study a small LuAGCe transparent scintillating ceramic scintillator. Summary of the invention

[0007] The object of the present invention is to provide a small LuAGCe transparent scintillating ceramic scintillator and a preparation method thereof, so as to solve the problems raised in the above background technology.

[0008] To achieve the above object, the present invention provides the following technical solutions:

[0009] A small LuAGCe transparent scintillation ceramic scintillator and a preparation method thereof, comprising:

[0010] The chemical structure of the ceramic scintillator is (Lu x Ce y Tb 3-x-y )Al5O 12 ;

[0011] Among them, x=0.01-1, y=0.005%-0.002%.

[0012] Optionally, the ceramic scintillator emits yellow fluorescence with a wavelength of 579 nm when excited by X-rays.

[0013] Optionally, the light transmittance of the ceramic scintillator is 75%.

[0014] According to another aspect of the present application, a method for preparing a small LuAGCe transparent scintillating ceramic scintillator is provided, comprising the following steps:

[0015] S1: Lu2O3, Al2O3, CeO2, Tb2O3 are weighed once according to the ratio and put into the ball mill. The ball milling medium is anhydrous ethanol and the ball milling time is 12h;

[0016] S2: drying the fully mixed powder slurry;

[0017] S3: sieving;

[0018] S4: calcination;

[0019] S5: dry pressing;

[0020] S6: cold isostatic pressing;

[0021] S7: sintering the ceramic green body in vacuum atmosphere;

[0022] S8: annealing treatment of the ceramic sample after vacuum sintering;

[0023] S9: The sample is mechanically double-sided polished and processed into a ceramic sheet of Φ1 mm and 0.5×0.5 mm.

[0024] Optionally, the molecular weights of the raw materials are Lu2O3: 398; CeO2: 172; Al2O3: 102; Tb2O3: 366.

[0025] Optionally, in step S7, the sintering temperature is: 1760-1860°C, and the sintering time is 10 hours.

[0026] Optionally, in step S8, the annealing is to anneal the ceramic sample in an oxidizing atmosphere at 1450° C. for 10 hours.

[0027] According to another aspect of the present application, there is provided an application of a small LuAGCe transparent scintillation ceramic scintillator in delayed detection of X-rays.

[0028] Compared with the prior art, the present invention has the following beneficial effects:

[0029] The ceramic scintillator prepared in the present invention has a high average transmittance in the visible light region and exhibits strong emission characteristics under both ultraviolet light and X-ray excitation. These results show that the ceramic material has potential application value in the fields of radiation detection, scintillation counters and medical imaging. BRIEF DESCRIPTION OF THE DRAWINGS

[0030] Figure 1 The transmittance curve of the LuAGCe transparent scintillating ceramic scintillator after different sintering times in Example 1 of the present invention;

[0031] Figure 2 The photoinduced emission spectra of the LuAGCe transparent scintillating ceramic scintillator before and after annealing in Example 1 of the present invention;

[0032] Figure 3 1 is the X-ray excitation emission spectrum of the LuAGCe transparent scintillating ceramic scintillator before and after annealing in Example 1 of the present invention. DETAILED DESCRIPTION

[0033] The following will be combined with the drawings in the embodiments of the present invention to clearly and completely describe the technical solutions in the embodiments of the present invention. The described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without creative work are within the scope of protection of the present invention.

[0034] A small LuAGCe transparent scintillating ceramic scintillator, the chemical structure of the ceramic scintillator is (Lu x Ce y Tb 3-x-y )Al5O 12 ;

[0035] Among them, the molecular weight of each raw material is:

[0036] Lu2O3:398; CeO2:172; Al2O3:102; Tb2O3:366;

[0037] x=0.01-1, y=0.005%-0.002%.

[0038] Embodiment 1:

[0039] x = 0.5; y = 0.01%; scintillator molecular formula: (Lu0.05 Ce 0.0001 Tb 2.4999 )Al5O 12

[0040] Preparation method:

[0041] (1) Mass calculation:

[0042] Based on molar percentage calculation, the raw materials for preparing 1 mol of scintillator are as follows:

[0043] Lu2O3: 0.025mol, mass: 0.025*398=9.95g;

[0044] CeO2: 0.0001 mol, mass: 0.0001*172=0.0172 g;

[0045] Al2O3: 2.5 mol, mass: 2.5*102=255 g;

[0046] Tb2O3: 1.24995 mol, mass: 1.24995*366=457.4817 g;

[0047] (2) Scintillator preparation:

[0048] 1: Weigh once according to the formula (Lu2O3, Al2O3, CeO2, Tb2O3) and put into the ball mill. The ball milling medium is anhydrous ethanol and the ball milling time is 12h;

[0049] 2: Dry the fully mixed powder slurry;

[0050] 3: sieve;

[0051] 4: Calcination;

[0052] 5: Dry pressing;

[0053] 6: Cold isostatic pressing;

[0054] 7: The ceramic blank is sintered in vacuum atmosphere at a temperature of 1760-1860°C and a sintering time of 10 hours;

[0055] 8: The vacuum sintered ceramic samples were annealed in an oxidizing atmosphere at 1450°C for 10 h;

[0056] 9: The sample is mechanically double-sided polished and processed into a ceramic sheet of Φ1mm, 0.5×0.5mm.

[0057] Embodiment 2:

[0058] x = 0.2; y = 0.05%; scintillator molecular formula: (Lu 0.2 Ce0.0005 Tb 2.7995 )Al5O 12 ;

[0059] Raw materials for preparing 1 mol of scintillator:

[0060] (1) Mass calculation:

[0061] Based on molar percentage calculation, the raw materials for preparing 1 mol of scintillator are as follows:

[0062] Lu2O3: 0.025mol, mass: 0.025*398=9.95g;

[0063] CeO2: 0.0001 mol, mass: 0.0001*172=0.0172 g;

[0064] Al2O3: 2.5 mol, mass: 2.5*102=255 g;

[0065] Tb2O3: 1.24995 mol, mass: 1.24995*366=457.4817 g;

[0066] (2) The scintillator preparation method is the same as that in Example 1.

[0067] Embodiment 3:

[0068] x = 0.8; y = 0.02%; scintillator molecular formula: (Lu 0.8 Ce 0.0002 Tb 2.1998 )Al5O 12 ;

[0069] Raw materials for preparing 1 mol of scintillator:

[0070] (1) Mass calculation:

[0071] Based on molar percentage calculation, the raw materials for preparing 1 mol of scintillator are as follows:

[0072] Lu2O3: 0.4 mol, mass: 0.4*398=159.2 g;

[0073] CeO2: 0.0002 mol, mass: 0.0002*172=0.0344 g;

[0074] Al2O3: 2.5 mol, mass: 2.5*102=255 g;

[0075] Tb2O3: 1.0999 mol, mass: 1.0999*366=402.5634;

[0076] (2) The scintillator preparation method is the same as that in Example 1.

[0077] Embodiment 4:

[0078] x value: 0.1; y value: 0.015%; scintillator molecular formula: (Lu 0.1 Ce 0.00015 Tb 2.89985 )Al5O 12 ; Raw materials for preparing 1 mol of scintillator:

[0079] (1) Mass calculation:

[0080] Lu2O3: mole: 0.0125mol; mass: 0.0125*398=5.0g;

[0081] CeO2: mole: 0.00015 mol; mass: 0.00015*172=0.026 g;

[0082] Al2O3: mole number: 2.5 mol; mass: 2.5*102=255 g;

[0083] Tb2O3: mole number: 1.28735mol; mass: 1.28735*366=470.1g;

[0084] (2) The scintillator preparation method is the same as that in Example 1.

[0085] Comparison data:

[0086] Experimental procedures and conditions

[0087] Raw material ratio: according to the predetermined molecular formula (Lu x Ce y Tb 3-x-y )Al5O 12 , calculate and accurately weigh each raw material;

[0088] Ball milling: Place the raw materials in a ball mill, use anhydrous ethanol as the medium, and ball mill for 12 hours to ensure uniform mixing;

[0089] Drying and sieving: Dry the milled slurry and sieve it to obtain uniform powder;

[0090] Calcination: Calcine the powder at an appropriate temperature to remove organic impurities and promote the reaction of raw materials;

[0091] Molding: The powder is made into the desired ceramic shape through dry pressing and cold isostatic pressing technology;

[0092] Sintering: Sintering ceramics at a high temperature of 1760-1860°C in a vacuum atmosphere to obtain a dense microstructure;

[0093] Annealing treatment: The sintered ceramic is annealed in an oxidizing atmosphere at 1450°C to further improve its properties;

[0094] Polishing: The ceramic samples were mechanically double-sided polished to prepare them for testing.

[0095] Experimental data

[0096] 1. Raw material ratio and molar mass (taking the preparation of 1 mol of scintillator as an example)

[0097] Lu2O3: xmol, mass = x*398g;

[0098] CeO2: y mol, mass = y*172g;

[0099] Tb2O3: (3-xy)mol, mass = (3-xy)*366g;

[0100] Al2O3: 2.5 mol, mass = 2.5*102 g;

[0101] 2. Transmittance data

[0102] Sample number: A (x = 0.5, y = 0.0001); Wavelength range: visible light region (400-700nm);

[0103] Average light transmittance: 75% (measured at 800nm ​​wavelength);

[0104] 3. Excitation emission spectrum data

[0105] Excitation source: ultraviolet light (wavelength 365nm);

[0106] Measuring range: 700nm;

[0107] Peak wavelength: 535nm;

[0108] Luminous intensity: 1200cd / m 2 (at peak wavelength);

[0109] 4. X-ray excitation emission spectrum data

[0110] X-ray source: CuKα (wavelength );

[0111] Measuring range: 832nm;

[0112] Peak wavelength: 535nm;

[0113] Luminous intensity: 800cd / m 2 ;

[0114] in conclusion

[0115] Through this experiment, we successfully prepared LuAGCe transparent scintillating ceramics with excellent transmittance and luminescence properties. The experimental data showed that the ceramics had a high average transmittance in the visible light region and exhibited strong emission characteristics under ultraviolet light and X-ray excitation. These results show that the ceramic material has potential application value in radiation detection, scintillation counters and medical imaging.

[0116] Specific examples are used in this article to illustrate the principles and implementation methods of the present invention. The above examples are only used to help understand the method and its core ideas of the present invention. The above is only a preferred implementation of the present invention. It should be pointed out that due to the limitations of textual expression, there are objectively infinite specific structures. For ordinary technicians in this technical field, without departing from the principles of the present invention, several improvements, modifications or changes can be made, and the above technical features can be combined in an appropriate manner. These improvements, modifications, changes or combinations, or the concept and technical solution of the invention are directly applied to other occasions without improvement, which should be regarded as the protection scope of the present invention.

Claims

1. A small LuAGCe transparent scintillating ceramic scintillator, characterized in that: include: The chemical structure of the ceramic scintillator is (Lu x Ce y Tb 3-x-y )Al5O 12 ; Among them, x=0.01-1, y=0.005%-0.002%.

2. According to claim 1, a small LuAGCe transparent scintillating ceramic scintillator is characterized by: The ceramic scintillator emits yellow fluorescence with a wavelength of 579 nm when excited by X-rays.

3. According to claim 1, a small LuAGCe transparent scintillating ceramic scintillator is characterized by: The light transmittance of the ceramic scintillator is 75%.

4. A small LuAGCe transparent scintillating ceramic scintillator and a preparation method thereof according to any one of claims 1 to 3, characterized in that: The steps include: S1: Lu2O3, Al2O3, CeO2, Tb2O3 are weighed once according to the ratio and put into the ball mill. The ball milling medium is anhydrous ethanol and the ball milling time is 12h; S2: drying the fully mixed powder slurry; S3: sieving; S4: calcination; S5: dry pressing; S6: cold isostatic pressing; S7: sintering the ceramic green body in vacuum atmosphere; S8: annealing treatment of the ceramic sample after vacuum sintering; S9: The sample is mechanically double-sided polished and processed into a ceramic sheet of Φ1 mm and 0.5×0.5 mm.

5. The method for preparing a small LuAGCe transparent scintillating ceramic scintillator according to claim 4, characterized in that: The molecular weights of the raw materials are Lu2O3: 398; CeO2: 172; Al2O3: 102; Tb2O3:

366.

6. The method for preparing a small LuAGCe transparent scintillating ceramic scintillator according to claim 4, characterized in that: In step S7, the sintering temperature is 1760-1860° C. and the sintering time is 10 hours.

7. The method for preparing a small LuAGCe transparent scintillating ceramic scintillator according to claim 4, characterized in that: In step S8, the annealing is to subject the ceramic sample to an annealing treatment in an oxidizing atmosphere at 1450° C. for 10 hours.

8. Use of the small LuAGCe transparent scintillating ceramic scintillator according to any one of claims 1 to 3, or the small LuAGCe transparent scintillating ceramic scintillator prepared according to the preparation method according to any one of claims 5 to 7 in delayed detection of X-rays.

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