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CN-118206993-B - Preparation and application of scintillating ceramic powder @ silicon oxide aerogel composite luminescent material

CN118206993BCN 118206993 BCN118206993 BCN 118206993BCN-118206993-B

Abstract

The invention discloses a preparation method and application of a scintillating ceramic powder @ silicon oxide aerogel composite luminescent material, which comprises the steps of taking Tb 4 O 7 、Al(NO 3 ) 3 ·9H 2 O、Gd(NO 3 ) 3 ·6H 2 O、Ce(NO 3 ) 3 ·6H 2 O and citric acid as raw materials, adopting a sol-gel method to prepare the scintillating ceramic powder, mixing and stirring tetraethoxysilane, deionized water and ethanol, adding the scintillating ceramic powder, continuing stirring, adding ammonia water for catalysis, continuing stirring, transferring to a proper mold when approaching a gel state to form wet gel, soaking with ethanol, and then carrying out supercritical drying with ethanol to obtain the scintillating ceramic powder @ silicon oxide aerogel composite luminescent material. The scintillating ceramic powder@silicon oxide aerogel composite luminescent material prepared by the method has good luminescent performance and luminescent thermal stability, has high internal quantum yield, and can be applied to the fields of energy conservation, environmental protection, laser illumination and the like for military and civil use.

Inventors

  • REN HONGBO
  • ZHU JIAYI
  • BI YUTIE
  • GAO YAN
  • FENG JIE

Assignees

  • 西南科技大学

Dates

Publication Date
20260512
Application Date
20240318

Claims (9)

  1. 1. The preparation method of the scintillating ceramic powder@silicon oxide aerogel composite luminescent material is characterized by comprising the following steps of: Heating HNO 3 solution, adding rare earth oxide Tb 4 O 7 into HNO 3 solution, mixing and stirring to react to obtain colorless transparent solution; volatilizing the solution, adding deionized water for dissolution, repeating for 2-4 times, removing excessive HNO 3 until the pH of the solution is neutral, adding Al(NO 3 ) 3 ·9H 2 O、Gd(NO 3 ) 3 ·6H 2 O、Ce(NO 3 ) 3 ·6H 2 O and citric acid into the solution, stirring, and reacting to obtain light yellow gel, wherein the molar ratio of ,Al(NO 3 ) 3 ·9H 2 O、Gd(NO 3 ) 3 ·6H 2 O、Ce(NO 3 ) 3 ·6H 2 O、 citric acid to Tb 4 O 7 in the first step is 18-22:6-10:0.05-0.15:30-36:0.8-1.0; drying and grinding the light yellow gel into powder, and sintering at a high temperature to obtain the scintillating ceramic powder, wherein the high-temperature sintering method comprises the steps of heating to 550-650 ℃ at a heating rate of 5-15 ℃ per minute, preserving heat for 0.5-1.5 h, and then heating to 1400-1600 ℃ and preserving heat for 2-4 h; And step four, mixing and stirring tetraethoxysilane, deionized water and ethanol, adding scintillating ceramic powder, continuing stirring, adding ammonia water for catalysis, continuing stirring, transferring to a proper mold when the gel state is approached to form wet gel, soaking with ethanol, and then performing supercritical drying with ethanol to obtain the scintillating ceramic powder @ silicon oxide aerogel composite luminescent material.
  2. 2. The method for preparing the scintillating ceramic powder@silicon oxide aerogel composite luminescent material according to claim 1, wherein in the first step, the volume fraction of HNO 3 solution is 40-60%, and the temperature is heated to 80-100 ℃.
  3. 3. The method for preparing the scintillating ceramic powder@silicon oxide aerogel composite luminescent material according to claim 1, wherein in the first step, the volume-mass ratio of HNO 3 solution to Tb 4 O 7 is 20 mL:0.6-0.8 g, and the steps of mixing and stirring are carried out for 0.5-1.5 h.
  4. 4. The method for preparing the scintillating ceramic powder@silicon oxide aerogel composite luminescent material according to claim 1, wherein in the second step, stirring is carried out for 0.5-1.5 h, and the reaction is carried out for 3-4 h at 70-90 ℃.
  5. 5. The method for preparing the scintillating ceramic powder@silicon oxide aerogel composite luminescent material according to claim 1, wherein in the third step, the drying temperature is 130-170 ℃.
  6. 6. The method for preparing the scintillating ceramic powder@silicon oxide aerogel composite luminescent material according to claim 1, wherein in the fourth step, the concentration of ammonia water is 1.5-2.5 mol/L, and the volume ratio of tetraethoxysilane, deionized water, ethanol and ammonia water is 1:1:4:0.2-0.3.
  7. 7. The method for preparing the scintillating ceramic powder@silicon oxide aerogel composite luminescent material according to claim 1, wherein in the fourth step, the addition amount of the scintillating ceramic powder is 5% -20% of the total mass of the ethyl orthosilicate and the scintillating ceramic powder.
  8. 8. The method for preparing the scintillating ceramic powder@silicon oxide aerogel composite luminescent material according to claim 1, wherein in the fourth step, the mixture is mixed and stirred for 20-40 min, the stirring is continued for 0.5-1.5 h, and the ethanol soaking is performed for 20-28 h.
  9. 9. Use of a scintillating ceramic powder @ silica aerogel composite luminescent material prepared by a method according to any one of claims 1-8 in laser illumination.

Description

Preparation and application of scintillating ceramic powder @ silicon oxide aerogel composite luminescent material Technical Field The invention belongs to the technical field of preparation of silica aerogel, and particularly relates to preparation and application of a scintillating ceramic powder@silica aerogel composite luminescent material. Background Solid state lighting devices, represented by Light Emitting Diodes (LEDs), play an important role in the fields of home lighting, plant lighting, automotive lighting, and the like. However, the conventional LED chip element is limited by auger recombination, so that there are serious problems of light decay and unstable illumination light color, which greatly limit the application of the LED chip element in ultra-high brightness and ultra-high power illumination and display scenes. Therefore, laser illumination based on Laser Diodes (LD) has been attracting attention and has shown a broad market potential in the field of special illumination such as deep sea illumination, automotive illumination, medical illumination, and the like. On the one hand, the laser element is small in size, more beneficial to production and more power-saving. On the other hand, the laser excited fluorescent powder has high efficiency and does not have the phenomenon of 'efficiency roll-off'. However, the current method of obtaining white light by remotely exciting fluorescent material with blue light LD chip or near ultraviolet LD chip is affected by light saturation and light extraction, so that the improvement of luminous efficiency and color stability is limited. Disclosure of Invention It is an object of the present invention to address at least the above problems and/or disadvantages and to provide at least the advantages described below. To achieve these objects and other advantages and in accordance with the purpose of the invention, a method for preparing a scintillating ceramic powder @ silica aerogel composite luminescent material is provided, comprising the steps of: Heating HNO 3 solution, adding rare earth oxide Tb 4O7 into HNO 3 solution, mixing and stirring to react to obtain colorless transparent solution; Volatilizing the solution, adding deionized water for dissolution, repeating for 2-4 times, removing excessive HNO 3 until the pH of the solution is neutral, adding Al(NO3)3·9H2O、Gd(NO3)3·6H2O、Ce(NO3)3·6H2O and citric acid into the solution, stirring, and reacting to obtain light yellow gel; step three, drying and grinding the pale yellow gel into powder, and sintering at high temperature to obtain scintillating ceramic powder; And step four, mixing and stirring tetraethoxysilane, deionized water and ethanol, adding scintillating ceramic powder, continuing stirring, adding ammonia water for catalysis, continuing stirring, transferring to a proper mold when the gel state is approached to form wet gel, soaking with ethanol, and then performing supercritical drying with ethanol to obtain the scintillating ceramic powder @ silicon oxide aerogel composite luminescent material. Preferably, in the first step, the volume fraction of the HNO 3 solution is 40-60%, and the temperature is heated to 80-100 ℃. Preferably, in the first step, the volume-mass ratio of the HNO 3 solution to the Tb 4O7 is 20mL, 0.6-0.8 g, and the steps of mixing and stirring are performed for 0.5-1.5 h. Preferably, the molar ratio of ,Al(NO3)3·9H2O、Gd(NO3)3·6H2O、Ce(NO3)3·6H2O、 citric acid in the second step to Tb 4O7 in the first step is 18-22:6-10:0.05-0.15:30-36:0.8-1.0. Preferably, in the second step, stirring is carried out for 0.5-1.5 h, and the reaction is carried out for 3-4 h at 70-90 ℃. The method comprises the steps of heating to 550-650 ℃ at a heating rate of 5-15 ℃ per min, preserving heat for 0.5-1.5 h, and then heating to 1400-1600 ℃ and preserving heat for 2-4 h. Preferably, in the fourth step, the concentration of the ammonia water is 1.5-2.5 mol/L, and the volume ratio of the ethyl orthosilicate to the deionized water to the ethanol to the ammonia water is 1:1:4:0.2-0.3. Preferably, in the fourth step, the addition amount of the scintillating ceramic powder is 5% -20% of the total mass of the ethyl orthosilicate and the scintillating ceramic powder, wherein the mass=v Tetraethoxysilane (TEOS) *0.51,V Tetraethoxysilane (TEOS) of the ethyl orthosilicate is the volume (mL) of the ethyl orthosilicate. Preferably, in the fourth step, the materials are mixed and stirred for 20-40 min, continuously stirred for 0.5-1.5h, and soaked in ethanol for 20-28 h. Preferably, the step three further comprises the steps of pre-treating the gel before high-temperature sintering, wherein the specific method of pre-treating is to dissolve Eu 2O3 in nitric acid solution, then cut the light yellow gel into square blocks, add the square blocks into the solution, stir for 2-5 min, take out the square blocks for drying, place the square blocks in an ultrasonic suspension device, open an ultrasonic standin