CN109991647B - Application method of radioactive xenon rapid high-sensitivity detection device - Google Patents
Application method of radioactive xenon rapid high-sensitivity detection device Download PDFInfo
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Abstract
The invention relates to the field of radioactive gas analysis, in particular to a quick high-sensitivity radioactive xenon detection device which is formed by matching a radon daughter filter, a needle valve, an air compressor, a buffer tank, an air source processor, a compressed air flowmeter, a pressure sensor, a mass flow controller, a dew point meter, a hollow fiber membrane, an adjusting valve, a flowmeter, an impurity removal column, a lead shielding chamber, an integrated adsorption/measurement sample box and an HPGe detector. The invention realizes the on-site rapid and high-sensitivity detection of radioactive xenon, the radon daughter filter effectively removes radon daughter and dust, and the self-cleaning function is realized.
Description
Technical Field
The invention relates to the field of radioactive gas analysis, and meets the requirements of on-site rapid and high-sensitivity measurement of activity and concentration of radioactive xenon.
Background
In the field of nuclear safety monitoring, a high-sensitivity field rapid detection technology is required to be adopted to detect radioactive nuclides in the surrounding environment of a nuclear facility so as to ensure the safety of the nuclear facility and provide a basis for radiation protection, safety evaluation and environmental impact evaluation of the nuclear facility. Real-time detection of radioactive gases and aerosols is the most sensitive and rapid means. However, due to the very high temperatures within these nuclear facilities, there are limitations to nonradioactive gas tracer detection, low survival rates, difficult to determine release volumes and release times, increased environmental background, and the inability to have repeated detections. The radioactive aerosol may reach the outside of the container through the leak path later than the radioactive gas, which is more easily monitored for leaks. Therefore, the method is a more direct and effective method for detecting the radioactive gas released by fission of the closed-structure container, and can make up for the defects of the existing methods such as chemical tracing leakage detection, plutonium aerosol detection and the like.
Radioactive xenon isotope133Xe、135The Xe has high fission yield, moderate half-life, high characteristic gamma ray emission probability and low environmental background, and is an ideal monitoring object. The existing radioactive inert gas detection is divided into two types: one is a rapid measurement system, which is mainly used for nuclear power station environment monitoring, and the detection limit of instruments is more than 104Bq/m3The instrument adopts a direct sampling measurement mode, other enrichment means are not basically adopted except that partial instruments pressurize gas, and most of the instruments adopt plastic scintillators to carry out total beta measurement and cannot carry out nuclide resolution. However, in the drainUnder the condition of low rate, the detection of radioactive gas is easily influenced by environmental radioactivity due to the diffusion and dilution effects of air on radioactive nuclide, so that the detection limit is higher, and therefore, the instrument is not suitable for early warning of gas leakage or leakage detection under the condition of low leakage rate. The other type of instrument is a high-sensitivity radioactive gas measurement system which is suitable for on-site observation scenes, adopts a more complicated process flow of multi-stage adsorption-purification-laboratory low-background gamma energy spectrum measurement, has very high detection sensitivity and is suitable for field observation scenes, and has a very high detection sensitivity133Xe and135the minimum detectable activity concentration of Xe is about 1mBq/m, respectively3、 60mBq/m3But the acquisition/analysis periods are all greater than 20 hours. Such systems are not suitable for direct measurement in the field due to their long analysis period. However, the rapid and high-sensitivity detection technology can timely find and early warn leakage, and can meet the requirement of nuclear safety monitoring. The device realizes the rapid and high-sensitivity field detection of the radioactive xenon isotope, and makes up for the defects of the system.
The literature comparison and analysis shows that the device research and the manufacturer with the same structure as the invention have no literature report.
Disclosure of Invention
The invention realizes the on-site rapid and high-sensitivity detection of radioactive xenon, the radon daughter filter effectively removes radon daughter and dust, and the self-cleaning function is realized
The invention relates to a quick high-sensitivity radioactive xenon detection device which is formed by matching a radon filter, a needle valve, an air compressor, a buffer tank, an air source processor, a compressed air flowmeter, a pressure sensor, a mass flow controller, a dew point meter, a hollow fiber membrane, an adjusting valve, a flowmeter, an impurity removal column, a lead shielding chamber, an integrated adsorption/measurement sample box and an HPGe detector.
The function realization mode of the invention is as follows: (1) the radon daughter filter removes dust and radon daughter in gas, adopts glass fiber filter paper with lateral openings, vertical placement and smoothness, and realizes the self-cleaning function. (2) The air compressor pumps out the gas and pressurizes. (3) Combined use of buffer tank, gas source processor, hollow fiber membrane and impurity removal column for removing CO2Water, CO and most of the nitrogen and oxygen gases. (4) The compressed air flowmeter, the pressure sensor, the dew point meter and the flowmeter respectively measure parameters such as sampling flow, gas pressure, dew point, flow after the membrane and the like. (5) The integrated adsorption/measurement sample box realizes ultralow temperature adsorption of gas and is used as a sample container, the gas inlet pipeline and the gas outlet pipeline are connected with an adsorption column, and the adsorption column is made of a thin-wall copper pipe and is filled with a carbon molecular sieve adsorbent. (6) The impurity removal column is filled with regenerated zeolite molecular sieve adsorbent for deep impurity removal. (7) HPGe detectors with lead shielded chambers measure the activity of radioactive xenon in the sample box. (8) A heat exchanger wound by a thin-wall copper pipe is assembled in the buffer tank, and the tail gas refrigerated by the sample box is fully utilized to accelerate the condensation of water in the gas in the buffer tank.
The device has the following innovation points: firstly, the device realizes the on-site rapid and high-sensitivity detection of radioactive xenon; the radon daughter filter effectively removes radon daughter and dust, and realizes the self-cleaning function; the buffer tank makes full use of the low-temperature cooling gas at the rear end, and the condensation of water is accelerated; fourthly, the hollow fiber membrane module with optimized combination can efficiently remove impurity gases such as water, CO2 and the like and most of nitrogen and oxygen gases; sixthly, the integrated adsorption/measurement sample box is used for efficiently enriching xenon and has field detection conditions.
Drawings
FIG. 1 is a schematic view of the structural connection of the present invention;
in fig. 1: the radon daughter filter is 1, the needle valve is 2, the air compressor is 3, the buffer tank is 4, the air source processor is 5, the compressed air flowmeter is 6, the pressure sensor is 7, the mass flow controller is 8, the dew point meter is 9, the hollow fiber membrane is 10, the regulating valve is 11, the flowmeter is 12, the impurity removing column is 13, the lead shielding chamber is 14, the integrated adsorption/measurement sample box is 15, and the HPGe detector is 16.
Detailed Description
A quick high-sensitivity radioactive xenon detection device is formed by matching a radon daughter filter 1, a needle valve 2, an air compressor 3, a buffer tank 4, an air source processor 5, a compressed air flowmeter 6, a pressure sensor 7, a mass flow controller 8, a dew point meter 9, a hollow fiber membrane 10, an adjusting valve 11, a flowmeter 12, an impurity removal column 13, a lead shielding chamber 14, an integrated adsorption/measurement sample box 15 and an HPGe detector 16.
The device comprises a radon filter, an air compressor, a buffer tank, an air source processor, a compressed air flowmeter, a mass flow controller, a pressure sensor, a dew point meter, a hollow fiber membrane, an adjusting valve, a flowmeter, an impurity removal column, an integrated adsorption/measurement sample box, a lead shielding chamber and an HPGe detector; the gas inlet pipeline and the gas outlet pipeline are connected with an adsorption column, the adsorption column is made of a thin-wall copper pipe and is filled with a carbon molecular sieve adsorbent, the impurity removal column is filled with a regenerated zeolite molecular sieve adsorbent, and a heat exchanger wound by the copper pipe is assembled in the buffer tank; the hollow fiber membrane is made of polyimide membrane or xenon special separation membrane, and the connection mode is three membranes connected in series.
The radon daughter filter 1, the buffer tank 4, the impurity removal column 13 and the lead shielding chamber 14 are processed by stainless steel.
The needle valve 2, the air source processor 5, the compressed air flowmeter 6, the pressure sensor 7, the mass flow controller 8, the dew-point meter 9, the hollow fiber membrane 10, the regulating valve 11 and the flowmeter 12 are standardized modules.
The integrated adsorption/measurement sample cartridge 15 is processed using stainless steel and red copper.
As shown in figure 1, the device consists of a radon filter 1, a needle valve 2, an air compressor 3, a buffer tank 4, an air source processor 5, a compressed air flowmeter 6, a pressure sensor 7, a mass flow controller 8, a dew point meter 9, a hollow fiber membrane 10, a regulating valve 11, a flowmeter 12, an impurity removal column 13, a lead shielding chamber 14, an integrated adsorption/measurement sample box 15 and an HPGe detector 16.
Fifth, best mode of carrying out the invention
The gas circuit is assembled and connected according to fig. 1, and the size of the lead shielding chamber 13 depends on the size of the integrated adsorption/measurement sample box 15 and the HPGe detector 15; the hollow fiber membrane 10 is made of polyimide, or xenon special separation membrane, and the connection mode is three membranes in series connection. The integrated adsorption/measurement sample box 15 adopts liquid nitrogen to refrigerate the adsorption column in the box, and the refrigerating time is not less than 40 min. After the refrigeration is finished, the air compressor 3 is started, the needle valve 2 is adjusted, and the flow of the compressed air flow meter 6 is not more than 100L-And min, adjusting the regulating valve 11 to ensure that the indication value of the pressure sensor 7 is less than 700kPa and the indication value of the flow meter 12 is not more than 1/3 of the indication value of the compressed air flow meter 6. Controlling the sampling time to ensure that the volume of the sampled gas is not less than 2m3. After sampling is finished, the HPGe detector 16 is started to measure the activity of the radioactive xenon in the integrated adsorption/measurement sample box 15, and the measurement duration depends on the statistical fluctuation of the full energy peak count of the concerned nuclide. After the measurement is finished, the system is closed, and the radioactive xenon activity concentration is calculated according to the formula (1).
In the formula, Nb is the background count of the energy region of the nuclide of interest;
λ -decay constant of the nuclear species of interest, s-1;
ε -detection efficiency, cps/Bq;
pγ-emission probability of a characteristic gamma-ray of a nuclide of interest;
l-volume flow rate for sample collection, m 3/s;
eta-recovery of xenon by the device;
ts-sample collection duration, s;
t1sample measurement duration, s.
The xenon recovery rate eta of the device to the xenon is obtained by desorption integration adsorption/measurement of an adsorption column in the sample box 15, and by adopting the chromatographic analysis to analyze the xenon concentration of the desorbed gas and then according to the formula (2).
Wherein V (Xe) — the volume of pure xenon in the enriched sample gas, mL;
r (Xe) -concentration of xenon in air, 0.087mL/m 3;
va-gas sample volume, m 3.
The invention relates to a quick and high-sensitivity detection device for radioactive xenon on site, which adopts a radon filter, a buffer tank, a gas source processor, a hollow fiber membrane and an impurity removal column to efficiently remove impurity gas components such as radon, water, CO2 and the like; carrying out high-efficiency adsorption enrichment on xenon by adopting an adsorption column refrigerated by liquid nitrogen; the activity and concentration of radioactive xenon are measured in situ by using a low background HPGe detector. The device realizes the rapid and high-sensitivity field measurement of the radioactive xenon, can be used for nuclear leakage detection and radiation protection monitoring, and can also be used for nuclear emergency monitoring.
The main technical parameters or indexes of the invention are as follows: sampling volume: 2m 3; sampling time length: 20 min; measuring time length: 10 min; MDC: 0.5Bq/m3(135 Xe); 5Bq/m3(133 Xe). The invention has the innovation points that: the main innovation points of the design of the quick and high-sensitivity detection device for the radioactive xenon field are as follows: the device realizes the on-site rapid and high-sensitivity detection of radioactive xenon; the radon daughter filter effectively removes radon daughter and dust, and realizes the self-cleaning function; the buffer tank fully utilizes the low-temperature cooling gas at the rear end, and the condensation of water is accelerated; the hollow fiber membrane module with optimized combination can efficiently remove impurity gases such as water, CO2 and the like and most of nitrogen and oxygen gases; the integrated adsorption/measurement sample box is highly efficient in enriching xenon and has field detection conditions.
The invention adopts a radon filter, a buffer tank, a gas source processor, a hollow fiber membrane and an impurity removal column to efficiently remove impurity gas components such as radon, water, CO2 and the like, adopts an adsorption column cooled by liquid nitrogen to efficiently adsorb and enrich xenon, adopts a low-background HPGe detector to measure the activity concentration of radioactive xenon on site, and realizes the rapid and high-sensitivity on-site measurement of the radioactive xenon.
Claims (1)
1. An application method of a quick high-sensitivity detection device for radioactive xenon comprises sequentially matching a radon daughter filter, a needle valve, an air compressor, a buffer tank, an air source processor, a compressed air flowmeter, a pressure sensor, a mass flow controller, a dew point meter, a hollow fiber membrane, an adjusting valve, a flowmeter, an impurity removal column, a lead shielding chamber, an integrated adsorption/measurement sample box and an HPGe detector; the method is characterized in that: the radon daughter filter is provided with a hole in the side direction and is vertically placed, and smooth glass fiber filter paper is arranged in the radon daughter filter; a heat exchanger wound by a thin-wall copper pipe is assembled in the buffer tank, and the condensation of water in the gas in the buffer tank is accelerated by fully utilizing the tail gas refrigerated by the sample box; the sample box adopts liquid nitrogen to refrigerate an adsorption column in the box, a gas inlet pipeline and a gas outlet pipeline are connected with the adsorption column, and the adsorption column is made of a thin-wall copper pipe and is filled with a carbon molecular sieve adsorbent; the application method of the device for detecting the radioactive xenon rapidly and with high sensitivity comprises the following steps:
the integrated adsorption/measurement sample box adopts liquid nitrogen to refrigerate an adsorption column in the box, the refrigerating time is not less than 40min, after the refrigeration is finished, an air compressor is started, a needle valve is adjusted, the flow of a compressed air flowmeter is not more than 100L/min, an adjusting valve is adjusted, the indication value of a pressure sensor is smaller than 700kPa, the indication value of a flowmeter is not more than 1/3 of the indication value of the compressed air flowmeter, and the sampling time is controlled so that the volume of the sampled gas is not less than 2m3After sampling is finished, an HPGe detector is started to measure the activity of radioactive xenon in the integrated adsorption/measurement sample box, the measurement duration depends on the statistical fluctuation of the total energy peak count of the concerned nuclide, the device is closed after the measurement is finished, and the activity concentration of the radioactive xenon is calculated according to the formula (1):
in equation (1): n is a radical ofγ-background counts of nuclear energy regions of interest; λ -decay constant of the nuclear species of interest, s-1(ii) a ε -detection efficiency, cps/Bq; p is a radical ofγ-emission probability of a characteristic gamma-ray of a nuclide of interest; l-volume flow rate of sample collection, m3S; eta-recovery of xenon by the device; t is ts-sample collection duration, s; t is t1-sample measurement duration, s; and (3) carrying out desorption integrated adsorption/measurement on an adsorption column in the sample box, analyzing the concentration of the xenon in the desorbed gas by adopting chromatography, and then calculating according to a formula (2) to obtain the recovery rate eta of the device to the xenon:
in equation (2): v (Xe) -the volume of pure xenon in the enriched sample gas, mL; r (Xe) -concentration of xenon in air, 0.087mL/m3;VaGas sampling volume, m3。
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