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CN-121975523-A - High-energy-resolution garnet aluminate scintillation material and preparation method and application thereof

CN121975523ACN 121975523 ACN121975523 ACN 121975523ACN-121975523-A

Abstract

The invention provides a high-energy-resolution garnet aluminate scintillation material, a preparation method and application thereof, which are characterized In that the scintillation material is doped with transition metal elements, the chemical formula of the scintillation material is RE 3‑x‑a‑z Ce x A a M z Al 5‑y D y O 12 , wherein x is more than or equal to 0 and less than or equal to 0.03,0, y is more than or equal to 0.4, z is more than or equal to 0.1, a is more than or equal to 0 and less than or equal to 0.06, the rare earth elements RE are selected from at least one of Gd, lu, Y, la, D is selected from at least one of Ga, in and Sc, A is selected from at least one of Li, mg, ca, K, na, cr, mn, fe, co, ni, yb, nd, and M is selected from at least one of Ag, cd and Pd. By accurately regulating and controlling the doping of the twelve-sided physique, the type and the concentration of defects in crystals are directionally regulated and controlled, and the non-radiation loss is reduced, so that the prior performance bottleneck is broken through on the premise of keeping high light output, the light output is obviously improved, and the energy resolution is greatly optimized.

Inventors

  • DING DONGZHOU
  • Fan Qinzheng
  • ZHAO SHUWEN
  • ZHENG XIANG
  • Zhang Aochen
  • XUE ZHONGJUN
  • Shi Gun

Assignees

  • 中国科学院上海硅酸盐研究所

Dates

Publication Date
20260505
Application Date
20260128

Claims (10)

  1. 1. A high-energy resolution garnet aluminate scintillation material is characterized in that the scintillation material is doped with transition metal elements, RE 3-x-a-z Ce x A a M z Al 5-y D y O 12 , wherein x is more than or equal to 0 and less than or equal to 0.03,0, y is more than or equal to 0 and less than or equal to 2.4, z is more than or equal to 0 and less than or equal to 0.1, a is more than or equal to 0 and less than or equal to 0.06, and the rare earth elements RE are selected from at least one of Gd, lu, Y, la; the D is selected from at least one of Ga, in and Sc; The A is at least one selected from Li, mg, ca, K, na, cr, mn, fe, co, ni, yb, nd; And M is at least one selected from Ag, cd and Pd.
  2. 2. The high energy resolution garnet aluminate scintillation material according to claim 1, wherein 0.00001 +.z +.0.05.
  3. 3. The high energy resolution garnet aluminate scintillation material according to claim 1, wherein 0.001< x is less than or equal to 0.03.
  4. 4. The high energy resolution garnet aluminate scintillation material according to claim 1, wherein 0.001< a +.0.05.
  5. 5. The high energy resolution garnet aluminate scintillation material of claim 1, wherein the garnet aluminate scintillation material is a high energy resolution garnet Dan Gouxing aluminate scintillation polycrystalline powder, a high energy resolution garnet Dan Gouxing aluminate scintillation ceramic or a high energy resolution garnet Dan Gouxing aluminate scintillation single crystal.
  6. 6. A method for preparing the high energy resolution garnet aluminate scintillation material of any one of claims 1 to 4, wherein the high energy resolution garnet aluminate scintillation material is a high energy resolution garnet Dan Gouxing aluminate scintillation polycrystalline powder, and the method comprises the steps of: (1) Weighing CeO 2 、Al 2 O 3 , RE oxide, D oxide, M oxide and A oxide as raw materials according to the chemical formula of the high-energy-resolution garnet Dan Gouxing aluminate scintillation polycrystalline powder, and mixing to obtain mixed powder; (2) And carrying out solid phase reaction on the mixed powder to obtain the high-energy-resolution garnet Dan Gouxing aluminate scintillation polycrystalline powder, wherein the temperature of the solid phase reaction is 1200-1800 ℃ and the time is 5-200 hours.
  7. 7. A method for preparing the high energy resolution garnet aluminate scintillation material according to any one of claims 1 to 4, wherein the high energy resolution garnet aluminate scintillation material is transition element doped garnet Dan Gouxing aluminate scintillation ceramic, and the method comprises the following steps: (1) Weighing CeO 2 、Al 2 O 3 , RE oxide, D oxide, M oxide and A oxide as raw materials according to the chemical formula of the high-energy-resolution garnet Dan Gouxing aluminate scintillation polycrystalline powder, and mixing to obtain mixed powder; (2) And preparing a green body from the mixed powder, and sintering to obtain the high-energy-resolution garnet Dan Gouxing aluminate scintillating ceramic.
  8. 8. The preparation method of the green body according to claim 7, wherein the forming mode of the green body comprises one of dry press forming and cold isostatic press forming, wherein the pressure of the dry press forming is 10-35 MPa, and the pressure of the cold isostatic press forming is 100-500 MPa; The sintering mode is one of pressureless sintering, hot-pressed sintering and vacuum sintering, wherein the pressureless sintering temperature is 1200-1800 ℃ and the time is 5-200 hours.
  9. 9. A method for preparing a high energy resolution garnet aluminate scintillation material, which is characterized by being used for preparing the garnet Dan Gouxing aluminate scintillation material as claimed in any one of claims 1 to 4, wherein the high energy resolution garnet aluminate scintillation material is transition element doped garnet Dan Gouxing aluminate scintillation single crystal, and the preparation method comprises the following steps: (1) Weighing CeO 2 、Al 2 O 3 , RE oxide, D oxide, M oxide and A oxide as raw materials according to the chemical formula of the high-energy-resolution garnet Dan Gouxing aluminate scintillation polycrystalline powder, and mixing to obtain mixed powder; (2) The mixed powder is melted by heating, and the growth of single crystals is started, wherein the growth method of single crystals comprises one of a pulling method, a crucible descending method, a temperature gradient method, a heat exchange method, a kyropoulos method, a top seed crystal method, a fluxing agent crystal growth method and a micro-downdraw method, and the heating mode is resistance heating, electromagnetic induction heating or light heating.
  10. 10. Use of the high energy resolution garnet aluminate scintillation material of any one of claims 1-5 in high energy physics, space physics, industrial nondestructive inspection, security inspection, mineral and oil well exploration, nuclear medicine imaging (X-CT, TOF-PET).

Description

High-energy-resolution garnet aluminate scintillation material and preparation method and application thereof Technical Field The invention relates to the field of scintillation materials, in particular to a high-energy-resolution garnet aluminate scintillation material, and a preparation method and application thereof. Background The inorganic scintillating material is used as an energy conversion carrier of high-energy rays (X rays, gamma rays) and particles (protons, neutrons and the like), can realize the accurate detection of nuclear radiation physical parameters by being coupled with photoelectric conversion devices (such as photodiodes and silicon photomultiplier tubes), and has irreplaceable functions in the fields of high-energy physics, nuclear medicine imaging (such as TOF-PET and X-CT), industrial nondestructive inspection, safety inspection, mineral and oil well exploration and the like. The energy resolution of the scintillation material is required to be extremely high in core application scenes such as nuclear medicine imaging and industrial nondestructive inspection, the energy resolution directly determines the distinguishing capability of the detection system on different energy rays, and the energy resolution is a core index affecting detection precision and application value. Cerium doped gadolinium aluminum gallate (Gd 3(Al,Ga)5O12: ce, GAGG: ce for short) scintillation crystal was first discovered in 2012 by Japanese academy Kei K, and by virtue of the design advantage of "band gap engineering", it has been recognized as an inorganic oxide scintillation crystal with optimal comprehensive performance so far. The crystal has the advantages of high density (6.63 g/cm 3), large effective atomic number (59), rapid luminescence attenuation (fast component about 90 ns), no deliquescence and the like, the luminescence mechanism of the crystal depends on 5 d-4 f transition of Ce 3+, the light output can reach 48000-58000 ph/MeV, the crystal is obviously superior to the scintillation crystal such as the traditional BGO, naI: tl and the like, and the GAGG: ce crystal also has the outstanding characteristics of higher light yield, better energy resolution and the like compared with the cerium doped lutetium silicate (LSO: ce) crystal which is widely applied in the current ionizing radiation detector, so the crystal is focused in the fields of particle physical fronts such as dark matter detection, nondestructive detection, nuclear safety, nuclear medicine imaging and the like, and becomes a preferable material for replacing the traditional scintillation crystal. However, with the continuous improvement of the detection precision requirements of various application fields, the energy resolution defect of the GAGG-Ce crystal is gradually highlighted, namely the energy resolution of the existing GAGG-Ce crystal under the excitation of 662 keV gamma rays is usually 7%, so that the energy resolution is difficult to adapt to the precise detection requirements in practical application, and the practical energy resolution is obviously inferior to a theoretical value, thereby becoming a key problem for restricting the further popularization and application of the energy resolution. In the field of nuclear medicine imaging, a TOF-PET technology needs to distinguish scattered photons from effective photons through the energy resolution capability of a scintillation material, the defect of energy resolution is insufficient to reduce the rejection efficiency of the scattered photons, image artifacts are further increased, the recognition accuracy of tumor focuses is affected, missed diagnosis or misdiagnosis can be possibly caused, in industrial nondestructive inspection, the defect detection aiming at key parts such as turbine blades of an aeroengine, a high-pressure container and the like is poor in energy resolution, ray response signals of defects (such as pores, cracks and inclusions) of different materials are overlapped, the defect type and size cannot be accurately judged, the potential safety hazards of equipment operation are buried, in a safety inspection scene, the simultaneous detection of various contraband products (such as explosives and radioactive substances) is faced, the defect ray signals of different substances are difficult to distinguish due to the defect of energy resolution, false report or false report is easy to occur, and the safety inspection efficiency is reduced. The source of poor energy resolution of GAGG: ce is mainly caused by nonlinear response of Ce to energy and uneven luminescence of crystals: the effect of non-uniformity of crystal luminescence on energy resolution results from non-uniformity of Ce 3+ luminescence center distribution, which may lead to local fluctuations of the light output signal. Such fluctuations reduce photon collection efficiency, increase energy spectrum peak width, and limit energy resolution. Non-uniformities are mainly caused by crystal struct