CN113176603B - Device for continuously measuring low-level radioactive nuclide in liquid effluent - Google Patents

Device for continuously measuring low-level radioactive nuclide in liquid effluent Download PDF

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CN113176603B
CN113176603B CN202110305259.7A CN202110305259A CN113176603B CN 113176603 B CN113176603 B CN 113176603B CN 202110305259 A CN202110305259 A CN 202110305259A CN 113176603 B CN113176603 B CN 113176603B
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wave
container
optical fiber
shifting
particles
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CN113176603A (en
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李群
夏斌元
熊忠华
任忠国
许清华
褚胜男
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Institute of Materials of CAEP
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    • GPHYSICS
    • G01MEASURING; TESTING
    • G01TMEASUREMENT OF NUCLEAR OR X-RADIATION
    • G01T1/00Measuring X-radiation, gamma radiation, corpuscular radiation, or cosmic radiation
    • G01T1/16Measuring radiation intensity
    • G01T1/167Measuring radioactive content of objects, e.g. contamination
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01TMEASUREMENT OF NUCLEAR OR X-RADIATION
    • G01T1/00Measuring X-radiation, gamma radiation, corpuscular radiation, or cosmic radiation
    • G01T1/16Measuring radiation intensity
    • G01T1/20Measuring radiation intensity with scintillation detectors
    • G01T1/2012Measuring radiation intensity with scintillation detectors using stimulable phosphors, e.g. stimulable phosphor sheets
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01TMEASUREMENT OF NUCLEAR OR X-RADIATION
    • G01T1/00Measuring X-radiation, gamma radiation, corpuscular radiation, or cosmic radiation
    • G01T1/16Measuring radiation intensity
    • G01T1/20Measuring radiation intensity with scintillation detectors
    • G01T1/202Measuring radiation intensity with scintillation detectors the detector being a crystal

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  • Health & Medical Sciences (AREA)
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  • Crystallography & Structural Chemistry (AREA)
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Abstract

The invention provides a device for continuously measuring low-level radioactive nuclide in liquid effluent, which comprises a container, a wave-shift optical fiber array and solid scintillation particles, wherein the wave-shift optical fiber array and the solid scintillation particles are arranged in the container; the container comprises a container body and a side panel which are detachably connected, and the container formed after the container body and the side panel are connected is of a hollow cylindrical structure; a liquid inlet and a liquid outlet are respectively arranged on the container main body and the side panel; two end faces of the container body are provided with optical fiber holes which correspond in position and are equal in distance; and each wave-shifting optical fiber of the wave-shifting optical fiber array respectively penetrates into the optical fiber holes corresponding to the two end faces of the container main body, and the end face of each wave-shifting optical fiber is flush with the two end faces of the container main body. The invention arranges the wave-shift optical fiber array in the container, which is equivalent to opening a transportation channel for the scintillation fluorescence of the solid scintillation particles in the container, can effectively increase the detection volume of the container, and improve the lower limit of the device for detecting the radionuclide in the liquid effluent.

Description

Device for continuously measuring low-level radioactive nuclide in liquid effluent
Technical Field
The invention relates to the technical field of continuous measurement of radionuclides, in particular to a device for continuously measuring low-level radionuclides in liquid effluents.
Background
The mainstream design idea at present is to utilize solid scintillator particles to realize continuous measurement of radionuclide in liquid effluent, generally grind water-insoluble scintillators such as calcium fluoride and the like to obtain particles of dozens to hundreds of micrometers (the effect within the particle size range is currently acknowledged to be the best), then put the particles into a disc-shaped or circular tube-shaped transparent container, and couple photomultiplier tubes (PMT) at two sides of the disc or two sides of the wall of the circular tube to perform coincidence measurement.
In the existing design, the radionuclide in the liquid effluent deposits energy in the scintillator particles, the scintillator fluoresces through the excitation-de-excitation process, the generated fluorescence is transmitted inside the container, and the fluorescence reaching both sides is detected by the PMT through coincidence measurement, but the design has fatal defects: under the working state, the inside of the container is a mixture of scintillator particles and liquid, namely a non-uniform medium, the transmission of light in the mixture does not satisfy the Lambert beer law, namely the light cannot be transmitted linearly, so that the light can be reflected and refracted among different media in the transmission process, and the transmission distance of fluorescence is greatly influenced.
This defect can lead to the following phenomena: the fluorescence generated in the central area of the container is seriously attenuated in the process of transmitting to two sides (coupling with PMT), so that the PMT signal is extremely small or no signal is generated; secondly, when the two side areas of the container are close, the generated fluorescence generates larger signals in the PMT at the near side, but the difficulty of transmitting the fluorescence from one side to the other side is higher, so that the PMT at the other side is difficult to generate signals.
The phenomenon determines that the thickness of the container (the distance between two sides coupled with the PMT) cannot be too thick, and the side area of the container cannot be too large (the side area of the container cannot be larger than the area of a photocathode of the PMT under the condition of direct coupling), so that the volume of the container is greatly limited, and performance parameters such as the detection lower limit of the device on the radioactive nuclide in liquid effluent and the like are influenced.
Disclosure of Invention
The invention aims to provide a device for continuously measuring low-level radioactive nuclides in liquid effluent, so as to solve the problem that the transmission problem of fluorescence inside a container limits the volume of the container in the prior art.
The invention provides a device for continuously measuring low-level radioactive nuclide in liquid effluent, which comprises a container, a wave-shift optical fiber array and solid scintillation particles, wherein the wave-shift optical fiber array and the solid scintillation particles are arranged in the container; the scintillation fluorescence peak wavelength of the solid scintillation particles is matched with the wave-shift optical fiber absorption wavelength in the wave-shift optical fiber array;
the container comprises a container body and a side panel which are detachably connected, and the container formed after the container body and the side panel are connected is of a hollow cylindrical structure; a liquid inlet and a liquid outlet are respectively arranged on the container main body and the side panel; two end faces of the container body are provided with optical fiber holes which correspond in position and are equal in distance;
each wave-shifting optical fiber of the wave-shifting optical fiber array penetrates into the optical fiber holes corresponding to the two end faces of the container main body respectively, the end face of each wave-shifting optical fiber is flush with the two end faces of the container main body, and the two end faces of the container main body are used for coupling the photomultiplier during coincidence measurement; and the wave-shift optical fiber array is provided with gaps through the space of the optical fiber holes, and the gaps of the wave-shift optical fiber array are used for filling solid scintillation particles when coincidence measurement is carried out.
In some embodiments, each wave shifting fiber of the wave shifting fiber array is a Y-11 type wave shifting fiber; the solid scintillation particles are calcium fluoride scintillation crystal particles.
Further, the wavelength of the Y-11 type wave shifting fiber is converted to 430nm → 470nm, that is, the Y-11 type wave shifting fiber is used for absorbing photons with the wavelength of 430nm from the side surface, then converting the absorbed photons with the wavelength of 430nm to photons with the wavelength of 470nm, and guiding the photons with the wavelength of 470nm meeting the total reflection condition to two end surfaces of the fiber.
Further, the calcium fluoride scintillation crystal particles are spherical.
Furthermore, the particle size range of the calcium fluoride scintillation crystal particles is 50-150 mu m.
In some embodiments, each wave shifting fiber of the wave shifting fiber array is an O-2 type wave shifting fiber; the solid scintillation particles are GAGG scintillation crystal particles.
Further, the wavelength of the O-2 type wave-shifting fiber is converted to 525nm → 550nm, that is, the O-2 type wave-shifting fiber is used for absorbing photons with the wavelength of 525nm from the side surface, then converting the absorbed photons with the wavelength of 525nm into photons with the wavelength of 550nm, and transmitting the photons with the wavelength of 550nm meeting the total reflection condition to two end surfaces of the fiber.
Further, the GAGG scintillation crystal particles are spherical.
Furthermore, the particle size range of the GAGG scintillation crystal particles is 50-150 mu m.
Preferably, the container formed when the container body and the side panels are connected has a hollow cylindrical structure.
Preferably, the container body and the side panels are detachably connected by screws.
Preferably, the container is made of non-transparent polytetrafluoroethylene.
In summary, due to the adoption of the technical scheme, the invention has the beneficial effects that:
1. the invention arranges the wave-shift optical fiber array in the container, which is equivalent to opening a transportation channel for the scintillation fluorescence of the solid scintillation particles in the container, and the distance between the two ends of the container is not limited by the fluorescence transmission distance any more, thus effectively increasing the detection volume of the container and further improving the lower limit of the device for detecting the radionuclide in the liquid effluent.
2. The invention adopts spheroidized solid crystal particles, and can furthest improve the detection capability of the device.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings in the embodiments will be briefly described below, it should be understood that the following drawings only illustrate some embodiments of the present invention, and therefore should not be considered as limiting the scope, and for those skilled in the art, other related drawings can be obtained according to the drawings without inventive efforts.
Fig. 1 is a schematic structural view of a container according to an embodiment of the present invention.
Fig. 2 is a schematic view of the structure of the optical fiber holes on the two end surfaces of the container body according to the embodiment of the invention.
Fig. 3 is a schematic structural diagram of an apparatus for continuous measurement of low-level radionuclides in a liquid effluent in accordance with an embodiment of the present invention.
Fig. 4 is a schematic diagram of the operation of the apparatus according to the embodiment of the present invention.
Reference numerals are as follows: 10-container, 11-container body, 12-side panel, 13-optical fiber hole, 14-liquid inlet, 15-liquid outlet and 20-wave shift optical fiber array.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are some, but not all, embodiments of the present invention. The components of embodiments of the present invention generally described and illustrated in the figures herein may be arranged and designed in a wide variety of different configurations.
Thus, the following detailed description of the embodiments of the present invention, presented in the figures, is not intended to limit the scope of the invention, as claimed, but is merely representative of selected embodiments of the invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Examples
As shown in fig. 1-3, the present embodiment proposes an apparatus for continuous measurement of low level radionuclides in liquid effluents, comprising a container 10, and a wave-shifting fiber array 20 and solid scintillating particles (not shown) disposed in the container 10; the peak wavelength of the scintillation fluorescence of the solid scintillation particles is matched with the absorption wavelength of the wave-shift optical fiber in the wave-shift optical fiber array 20;
the container 10 comprises a container body 11 and a side panel 12 which are detachably connected, and the container 10 formed after the container body 11 and the side panel 12 are connected is of a hollow cylindrical structure; a liquid inlet 14 and a liquid outlet 15 are respectively arranged on the container main body 11 and the side panel 12; two end faces of the container body 11 are provided with optical fiber holes 13 which correspond in position and are equal in distance;
each wave-shifting optical fiber of the wave-shifting optical fiber array 20 respectively penetrates into the optical fiber holes 13 corresponding to the two end faces of the container body 11, the end face of each wave-shifting optical fiber is flush with the two end faces of the container body 11, and the two end faces of the container body 11 are used for coupling a photomultiplier during coincidence measurement; and the wave-shift optical fiber array 20 is provided with gaps through the space of the optical fiber holes 13, and the gaps of the wave-shift optical fiber array 20 are used for filling solid scintillation particles when coincidence measurement is carried out.
The device carries out coincidence measurement in the following way:
(1) compared with the transparent glass or plastic container 10 commonly used in the prior art, the container 10 of the present embodiment is made of non-transparent polytetrafluoroethylene, and is made into a hollow cylindrical structure, preferably a hollow cylindrical structure, or a hollow prismatic structure;
(2) the container 10 is cut from the inner sides of the left and right end faces at a vertical height 2/3 of the side face to obtain the container main body 11 and the side panels 12 which are exposed inside, as shown in fig. 2;
(3) the container body 11 and the side panels 12 are detachably connected by screws for subsequent installation and filling with solid scintillation particles, as shown in fig. 2;
(4) a liquid inlet 14 and a liquid outlet 15 are respectively arranged on the container main body 11 and the side panel 12 to fill and drain liquid in the container 10, and the liquid inlet 14 and the liquid outlet 15 are preferably opposite to each other on the container 10;
(5) the two end surfaces of the container body 11 are provided with optical fiber holes 13 which are corresponding in position and equal in distance, and the arrangement modes are 'staggered in equal distance', as shown in fig. 2;
(6) respectively penetrating a plurality of wave-shifting optical fibers into optical fiber holes 13 corresponding to two end faces of the container body 11, enabling the end face of each wave-shifting optical fiber to be flush with the two end faces of the container body 11, and polishing and grinding the flush end face, so that the plurality of wave-shifting optical fibers form a wave-shifting optical fiber array 20, and enabling the wave-shifting optical fiber array 20 to have gaps through the space of the optical fiber holes 13;
(7) when coincidence measurement is carried out, the side panel 12 is opened, solid scintillation particles are filled in the container main body 11 and are filled in the gap of the wave-shift optical fiber array 20, then the side panel 12 is connected with the container main body 11 in a matching mode, and then photomultiplier tubes are coupled to two end faces of the container main body 11 to carry out coincidence measurement. As shown in fig. 4, the wave-shift fiber is a fiber that can enter light from the side, photons of a certain wavelength are absorbed by the wave-shift fiber when reaching the end face of the wave-shift fiber, then a core layer inside the wave-shift fiber generates photons of another wavelength, and the exit angles are random, if the exit angles satisfy total reflection, the photons can be transmitted inside the wave-shift fiber, and thus the photons are detected by the photomultiplier tubes at both ends.
From the above, the design features of the present invention are: the wave-shift optical fiber array 20 is arranged in the container 10, which is equivalent to opening a transportation channel for the scintillation fluorescence of the solid scintillation particles in the container 10, as shown in fig. 4, the distance between two ends of the container 10 is no longer limited by the fluorescence transmission distance, so that the detection volume of the container 10 can be effectively increased, and the lower limit of the device for detecting the radionuclide in the liquid effluent is improved.
In some embodiments, Y-11 type waveshifting fiber + calcium fluoride scintillation crystal particles are used: that is, each wave-shift optical fiber of the wave-shift optical fiber array 20 is a Y-11 type wave-shift optical fiber, the solid scintillation particles are calcium fluoride scintillation crystal particles, and through the Y-11 type wave-shift optical fiber, the scintillation fluorescence peak wavelength of the calcium fluoride scintillation crystal particles is matched with the absorption wavelength of the Y-11 type wave-shift optical fiber; the wavelength of the Y-11 type wave shifting optical fiber is converted into 430nm → 470nm, namely, the Y-11 type wave shifting optical fiber is used for absorbing photons with the wavelength of 430nm (namely, photons from calcium fluoride scintillation fluorescence) from the side surface, then converting the absorbed photons with the wavelength of 430nm into photons with the wavelength of 470nm, and transmitting the photons with the wavelength of 470nm meeting the total reflection condition to two end surfaces of the optical fiber.
For calcium fluoride scintillation crystal particles, the calcium fluoride scintillation crystal particles obtained by grinding are irregular fragments, and pores among the calcium fluoride scintillation crystal particles in a stacking state are uneven, so that on one hand, the flow resistance of liquid is increased, and on the other hand, radioactive nuclides in liquid need to reach the calcium fluoride scintillation crystal particles and deposit energy, and need to firstly pass through a liquid medium with a certain thickness, and in a region with larger pores, the nuclides need to pass through a thicker medium, so that the energy of the nuclides deposited in the liquid is increased, and the energy of the nuclides deposited in the calcium fluoride scintillation crystal particles is reduced, thereby affecting the detection capability of the device. Therefore, calcium fluoride scintillation crystal particles can be spheroidized, namely the calcium fluoride scintillation crystal particles are changed into spherical particles through high-temperature melting, gaps among the regular spherical particles are uniform, and the gaps among the particles can be changed by regulating and controlling the radius of the spherical particles, so that the detection capability of the device is improved to the maximum extent, and generally, the particle size range of the calcium fluoride scintillation crystal particles is 50-150 mu m.
In some embodiments, (8) O-2 type wave shifting fiber + GAGG scintillation crystal particles are employed: that is, each wave-shifting optical fiber of the wave-shifting optical fiber array 20 is an O-2 type wave-shifting optical fiber, the solid scintillation particles are GAGG scintillation crystal particles, and through the O-2 type wave-shifting optical fiber, the scintillation fluorescence peak wavelength of the GAGG scintillation crystal particles is matched with the absorption wavelength of the O-2 type wave-shifting optical fiber; the wavelength of the O-2 type wave shifting optical fiber is converted into 525nm → 550nm, namely the O-2 type wave shifting optical fiber is used for absorbing photons with the wavelength of 525nm (namely photons from GAGG crystal scintillation fluorescence) from the side surface, then converting the absorbed photons with the wavelength of 525nm into photons with the wavelength of 550nm, and transmitting the photons with the wavelength of 550nm meeting the total reflection condition to two end surfaces of the optical fiber; through the wavelength conversion of the O-2 type wave-shifting optical fiber, the scintillation fluorescence peak wavelength of the GAGG crystal is matched with the absorption wavelength of the optical fiber.
The GAGG scintillation crystal (cerium-doped gadolinium aluminum gallium garnet crystal) is the crystal with the highest light output in the existing known oxide scintillation crystal, has the advantages of high energy resolution, no self-radiation, no deliquescence and the like, and has the luminous efficiency 2 times that of calcium fluoride, so that the GAGG scintillation crystal can be used for continuously measuring low-level radionuclides in liquid. Like the calcium fluoride scintillation crystal particles, the GAGG scintillation crystal particles obtained by grinding are irregular fragments, and pores among the GAGG scintillation crystal particles in a stacking state are uneven, so that on one hand, the flow resistance of liquid is increased, and on the other hand, radioactive nuclides in liquid need to reach the GAGG scintillation crystal particles and deposit energy, the nuclides need to pass through a liquid medium with a certain thickness in a region with larger pores, and the nuclides need to pass through a thicker liquid medium, so that the energy of the nuclides deposited in the liquid is increased, and the energy of the nuclides deposited in the GAGG scintillation crystal particles is reduced, thereby affecting the detection capability of the device. From this, can spheroidize the GAGG scintillation crystal granule, promptly the GAGG scintillation crystal granule becomes the spheroid through high temperature melting, and the gap is even unanimous between the regular spheroid granule, and the accessible is regulated and control the spheroid granule radius and is changed the gap between the granule to furthest promotes device detectivity, generally, the particle size scope of GAGG scintillation crystal granule is 50 ~ 150 mu m.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims (8)

1. An apparatus for continuous measurement of low level radionuclides in a liquid effluent, comprising a container (10), and a wave-shifting fiber array (20) and solid scintillating particles disposed in the container (10); the scintillation fluorescence peak wavelength of the solid scintillation particles is matched with the wave-shift optical fiber absorption wavelength in the wave-shift optical fiber array (20);
the container (10) comprises a container body (11) and a side panel (12) which are detachably connected, and the container (10) formed after the container body (11) and the side panel (12) are connected is of a hollow cylindrical structure; a liquid inlet (14) is formed in the container main body (11), and a liquid outlet (15) is formed in the side panel (12); two end faces of the container body (11) are provided with optical fiber holes (13) which correspond in position and are equal in distance;
each wave-shifting optical fiber of the wave-shifting optical fiber array (20) respectively penetrates into the optical fiber holes (13) corresponding to the two end faces of the container body (11), the end face of each wave-shifting optical fiber is flush with the two end faces of the container body (11), and the two end faces of the container body (11) are used for coupling a photomultiplier during coincidence measurement; and the wave-shift optical fiber array (20) is provided with gaps through the spacing of the optical fiber holes (13), and the gaps of the wave-shift optical fiber array (20) are used for filling solid scintillation particles when coincidence measurement is carried out; the solid scintillation particles are spherical.
2. The device for the continuous measurement of low levels of radionuclides in a liquid effluent according to claim 1, wherein each wave-shifting fiber of the wave-shifting fiber array (20) is a Y-11 type wave-shifting fiber; the solid scintillation particles are calcium fluoride scintillation crystal particles.
3. The apparatus according to claim 2, wherein said Y-11 type wavelength shifting fiber is used to absorb photons with 430nm → 470nm from the side, then convert absorbed photons with 430nm wavelength to photons with 470nm wavelength, and conduct photons with 470nm wavelength satisfying the total reflection condition to both end faces of the fiber.
4. The device for continuous measurement of low levels of radionuclides in a liquid effluent of claim 2 or 3, wherein the calcium fluoride scintillation crystal particles have a particle size in the range of 50-150 μm.
5. The device for the continuous measurement of low levels of radionuclides in a liquid effluent according to claim 1, wherein each wave-shifting fiber of the wave-shifting fiber array (20) is an O-2 type wave-shifting fiber; the solid scintillation particles are GAGG scintillation crystal particles.
6. The apparatus for the continuous measurement of low level radionuclides in a liquid effluent of claim 5 wherein said O-2 type wavelength shifting fiber is configured to absorb photons of 525nm → 550nm from the side, then convert the absorbed photons of 525nm into photons of 550nm, and conduct the photons of 550nm satisfying the total reflection condition to both end faces of the fiber.
7. The apparatus according to claim 5 or 6, wherein the GAGG scintillation crystal particles have a size in the range of 50-150 μm.
8. The device for the continuous measurement of low levels of radionuclides in a liquid effluent of claim 1, wherein the container (10) formed when the container body (11) and side panel (12) are connected is a hollow cylindrical structure.
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