CN109765093B - Hydrogen isotope concentration system suitable for environmental level - Google Patents

Hydrogen isotope concentration system suitable for environmental level Download PDF

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Publication number
CN109765093B
CN109765093B CN201910219843.3A CN201910219843A CN109765093B CN 109765093 B CN109765093 B CN 109765093B CN 201910219843 A CN201910219843 A CN 201910219843A CN 109765093 B CN109765093 B CN 109765093B
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ceramic tube
inner cavity
hydrogen isotope
tube
quartz glass
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CN109765093A (en
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孟丹
陈志林
杜阳
谢云
周银行
王伟娟
王和义
杨勇
余卫国
谭昭怡
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Institute of Nuclear Physics and Chemistry China Academy of Engineering Physics
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Institute of Nuclear Physics and Chemistry China Academy of Engineering Physics
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Abstract

The invention discloses a hydrogen isotope concentration system suitable for environmental levels. The gas to be measured enters the system and is divided into two paths, one path enters the bottom of a ceramic tube arranged in the quartz glass tube through an Ar gas cylinder, and the other path directly enters the middle of the ceramic tube. After a certain time of reaction, two paths of gases from the ceramic tube and the quartz glass tube sequentially pass through the hygrothermograph and the flowmeter and are respectively connected with the dew point meter and the measuring module for relevant measurement. The system adopts a proton conductive ceramic tube to electrolyze HTO/HDO steam at high temperature to realize concentration of low-concentration hydrogen isotopes (HT/HD), and realizes measurement of the low-concentration hydrogen isotopes through a measurement module. The hydrogen isotope concentration system suitable for the environmental level can not only ensure the effective concentration of low-concentration hydrogen isotopes in a workplace, but also purify and collect samples in a certain time, and has the advantages of stability, reliability and high concentration and collection efficiency.

Description

Hydrogen isotope concentration system suitable for environmental level
Technical Field
The invention belongs to the technical field of radiation protection and environmental protection, and particularly relates to a hydrogen isotope concentration system suitable for environmental level.
Background
The low concentration tritium exists in the surrounding environment of tritium-related places such as nuclear power station, tritium target production, neutron generator production and the like (which is far lower than Bq/m 3 Magnitude). These tritium exists mainly in the form of HTO and HT, and about 60 days at normal temperature, normal pressure and normal humidity, half of HT is converted into HTO, while the inhalation hazard of HTO is 1.0X10 of gaseous tritium 4 Multiple times, therefore the hazards of HTO cannot be ignored. However, the sensitivity of the ionization chamber tritium detector at home and abroad is generally 10 at present 5 Bq/m 3 About, much higher than tritium concentrations in most tritium operation site environments. From the radiation protection point of view, the method is particularly important for enrichment and measurement of low-concentration tritium in the environment of tritium-related places.
At present, a sampling method for tritium in a tritium-related place environment is mainly a bubbling method, namely, radioactive gas bubbles when passing through a gas washing bottle with distilled water, and HTO in an air sample exchanges isotopes with water. However, the sensitivity of this method is generally (1-5) Bq/m 3 The measurement of low tritium concentrations in the environment cannot be satisfied.
Disclosure of Invention
The invention aims to provide a hydrogen isotope concentration system suitable for environmental level.
The invention relates to a hydrogen isotope concentration system suitable for environmental level, which is characterized in that: the hydrogen isotope concentration system is divided into two paths through a gas sampling pipeline, one path passes through an argon bottle and a hygrothermograph I, then passes through a flange plate to enter the upper part of an inner cavity of a ceramic tube, flows out of the inner cavity of the ceramic tube after reaction, and flows out of the inner cavity of the ceramic tube through a cooling coil I, a hygrothermograph II, a flowmeter I, a valve I, a measuring instrument and a pump I in sequence; the other path of the water vapor passes through the flange plate and enters the bottom of the inner cavity of the ceramic tube after passing through the hygrothermograph IV and the water vapor bottle, flows out of the inner cavity of the quartz glass tube after reacting, and flows out of the cooling coil II, the hygrothermograph III, the flowmeter II, the valve II, the dew point meter and the pump II in sequence;
the ceramic tube is nested in the quartz glass tube, one ends of the quartz glass tube and the ceramic tube are closed ends, the other ends of the quartz glass tube and the ceramic tube are open ends, and the open ends are sealed by adopting a flange plate to form an inner cavity of the ceramic tube and an inner cavity of the quartz glass tube positioned between the ceramic tube and the quartz glass tube; 4 pipelines are distributed on the flange plate, one sample injection pipeline extends into the upper part of the inner cavity of the ceramic tube, one sample injection pipeline extends into the bottom of the inner cavity of the ceramic tube, one gas outlet pipeline extends out of the upper part of the inner cavity of the ceramic tube, and one gas outlet pipeline extends out of the inner cavity of the quartz glass tube;
the quartz glass tube is wrapped with an electric furnace.
The ceramic tube is a proton conductive ceramic tube.
The cooling coil I and the cooling coil II are one of air cooling coils or air cooling coils.
The electric furnace is a programmed heating electric furnace, and the heating range is room temperature to 1100 ℃.
The pump I and the pump II are vacuum pumps.
The measuring instrument is one of an ionization chamber, a proportional counter tube or a chromatograph.
The connecting pipeline of the hydrogen isotope concentration system adopts a stainless steel pipeline with the thickness of 1/8inch or 1/4 inch.
The valve I and the valve II are one of manual valves, semi-manual valves or automatic valves with automatic temperature early warning.
The hydrogen isotope concentration system suitable for the environmental level adopts the electrochemical principle, introduces tritium-containing gas into a ceramic tube, ionizes the hydrogen isotope-containing gas at a certain temperature, and ionizes the tritium gas (HT/HD) and oxygen (O) 2 ) Respectively diffusing the tritium-containing gas into two stages of ceramic tubes under the action of electrodes, and then carrying out enrichment collection to further realize separation and enrichment of HT/HD in the tritium-containing gas.
The hydrogen isotope concentration system suitable for the environmental level adopts the proton conductive ceramic tube to ionize the hydrogen isotope gas, and by changing the material proportion of the proton conductive ceramic tube, not only HT/HD can be enriched in different atmospheres, but also the separation of the hydrogen isotopes can be carried out at different temperatures, and the hydrogen isotope concentration system can also be used for purifying tritium-containing gas.
The hydrogen isotope concentration system suitable for the environmental level adopts the temperature programming electric furnace, can uniformly and effectively heat the ceramic tube in advance, and can record the heating curve in the ceramic tube in real time, so that a user can select any temperature section for experimental measurement according to own needs.
The hydrogen isotope concentration system suitable for the environmental level is provided with the cooling coil after the high-temperature electric furnace, so that the gas coming out of the high-temperature ceramic tube can be effectively cooled, and the measuring instrument and meter at the rear end can be effectively protected.
The hydrogen isotope concentration system suitable for the environmental level is provided with the valve at the front end of the measuring instrument, so that the valve can be freely controlled according to the readings of the front-end hygrothermograph and the flowmeter, and the damage to the rear-end testing and measuring instrument caused by the overhigh gas temperature is avoided.
The hydrogen isotope concentration system suitable for the environmental level solves the problem of measuring low-concentration hydrogen isotopes, particularly solves the problem of measuring low-concentration hydrogen isotopes in the environment of a tritium-related place, meets the requirements of enriching and measuring the low-concentration hydrogen isotopes in the environment of the tritium-related place (nuclear power plant, tritium target production, neutron generator production and the like), and is suitable for enriching the low-concentration hydrogen isotopes in the related workplace and concentrating and collecting the low-concentration tritium in the surrounding environment of the related production places such as the nuclear power plant, the tritium target production, the neutron generator and the like.
Drawings
FIG. 1 is a schematic diagram of a hydrogen isotope enrichment system adapted for environmental levels in accordance with the present invention;
in the figure: 1. the device comprises a gas sampling pipeline 2, an argon gas bottle 3, a hygrothermograph I4, a water vapor bottle 5, a flange 6, an electric furnace 7, a quartz glass tube 8, a ceramic tube 9, a cooling coil I10, a cooling coil II 11, a hygrothermograph II 12, a hygrothermograph III 13, a flowmeter I14, a flowmeter II 15, a valve I16, a valve II 17, a measuring instrument 18, a dew point meter 19, a pump I20, a pump II 21 and a hygrothermograph IV.
Detailed Description
The invention will be described in further detail with reference to the accompanying drawings and specific examples.
In fig. 1, the hydrogen isotope concentration system of the invention is divided into two paths through a gas sampling pipeline 1, one path passes through an argon bottle 2 and a hygrothermograph I3, then passes through a flange 5, enters the upper part of the inner cavity of a ceramic tube 8, flows out of the inner cavity of the ceramic tube 8 after reaction, and then flows out of the inner cavity of the ceramic tube through a cooling coil I9, a hygrothermograph II 11, a flowmeter I13, a valve I15, a measuring instrument 17 and a pump I19 in sequence; the other path of the water vapor passes through the flange 5 to enter the bottom of the inner cavity of the ceramic tube 8 after passing through the hygrothermograph IV 21 and the water vapor bottle 4, flows out of the inner cavity of the quartz glass tube 7 after reacting, and flows out of the cooling coil II 10, the hygrothermograph III 12, the flowmeter II 14, the valve II 16, the dew-point meter 18 and the pump II 20 in sequence;
the ceramic tube 8 is nested in the quartz glass tube 7, one ends of the quartz glass tube 7 and the ceramic tube 8 are closed ends, the other ends are open ends, and the open ends are sealed by adopting the flange 5 to form an inner cavity of the ceramic tube 8 and an inner cavity of the quartz glass tube 7 positioned between the ceramic tube 8 and the quartz glass tube 7; 4 pipelines are distributed on the flange plate 5, one sample injection pipeline extends into the upper part of the inner cavity of the ceramic tube 8, one sample injection pipeline extends into the bottom of the inner cavity of the ceramic tube 8, one gas outlet pipeline extends out of the upper part of the inner cavity of the ceramic tube 8, and one gas outlet pipeline extends out of the inner cavity of the quartz glass tube 7;
the quartz glass tube 7 is externally wrapped with an electric furnace 6.
The ceramic tube 8 is a proton conductive ceramic tube.
The cooling coil I9 and the cooling coil II 10 are one of air cooling coils or air cooling coils.
The electric furnace 6 is a programmed heating electric furnace, and the heating range is room temperature to 1100 ℃.
Pump I19 and pump II 20 are vacuum pumps.
The meter 17 is one of an ionization chamber, a proportional counter, or a chromatograph.
The connecting pipeline of the hydrogen isotope concentration system adopts a stainless steel pipeline with the thickness of 1/8inch or 1/4 inch.
The valve I15 and the valve II 16 are one of manual valves, semi-manual valves or automatic valves with automatic temperature early warning.
Example 1
The ceramic tube used in this example was indium doped CaZrO 3 A base ceramic tube. The ceramic tube can react in the temperature range of 600-900 ℃ and can effectively electrolyze and concentrate hydrogen isotope gas.
The cooling coil I9 and the cooling coil II 10 in this embodiment are air cooling coils.
The electric furnace 6 in the embodiment is a self-made temperature programming electric furnace with the temperature range of room temperature to 1100 ℃.
The pumps I19 and II 20 in this embodiment are small vacuum pumps.
The measuring instrument 17 in this embodiment is a proportional counter tube, and the proportional counter tube has higher sensitivity, can measure in the range of extremely low tritium concentration (several Bq), and improves the detection sensitivity of the instrument.
All the pipes in this embodiment are hard-wired using 1/8inch stainless steel pipes.
In the embodiment, the valve I15 and the valve II 16 are manual one-way valves, and the air flow speed is manually controlled, so that the stability of flow speed control of the system is improved; meanwhile, the manual valve is adopted, so that data can be acquired at any time period and any temperature, and the convenience of operation is improved; the adoption of the single valve effectively avoids the reverse flow of the gas at the rear end into the measuring system at the front end, influences the accuracy of measurement, and further improves the reliability and stability of the hydrogen isotope concentration system.
In the embodiment, the HTO in the environment of a certain experiment place is subjected to 120h concentration treatment at 600 ℃,700 ℃ and 900 ℃ by adopting the materials and the equipment, and the concentration efficiencies are 110, 150 and 560 respectively.
The cooling coil in this embodiment may be an air-cooled coil, the measuring instrument may be an ionization chamber or a chromatograph, the hydrogen isotope concentration pipeline may be a stainless steel pipeline of 1/4inch, and the valves I15 and II 16 may be semi-manual valves or automatic valves with automatic temperature pre-warning. The same or similar concentration results can be obtained with any of the alternative devices or materials described above.
The present invention is not limited to the above-described embodiments, and various modifications are possible within the scope of the present invention without inventive work by those skilled in the art from the above-described concepts.

Claims (7)

1. A hydrogen isotope enrichment system adapted for use at an environmental level, characterized by:
the hydrogen isotope concentration system is divided into two paths through a gas sampling pipeline (1), one path passes through an argon bottle (2) and a hygrothermograph I (3) and then passes through a flange plate (5) to enter the upper part of an inner cavity of a ceramic tube (8), after reaction, flows out of the inner cavity of the ceramic tube (8), and then flows out of a cooling coil I (9), a hygrothermograph II (11), a flowmeter I (13), a valve I (15), a measuring instrument (17) and a pump I (19) in sequence; the other path of the water vapor enters the bottom of the inner cavity of the ceramic tube (8) through the flange (5) after passing through the hygrothermograph IV (21) and the water vapor bottle (4), flows out of the inner cavity of the quartz glass tube (7) after reacting, and flows out of the cooling coil II (10), the hygrothermograph III (12), the flowmeter II (14), the valve II (16), the dew point meter (18) and the pump II (20) in sequence;
the ceramic tube (8) is nested in the quartz glass tube (7), one ends of the quartz glass tube (7) and the ceramic tube (8) are closed ends, the other ends are open ends, and the open ends are sealed by adopting the flange plate (5) to form an inner cavity of the ceramic tube (8) and an inner cavity of the quartz glass tube (7) positioned between the ceramic tube (8) and the quartz glass tube (7); 4 pipelines are distributed on the flange plate (5), one sample injection pipeline extends into the upper part of the inner cavity of the ceramic tube (8), one sample injection pipeline extends into the bottom of the inner cavity of the ceramic tube (8), one gas outlet pipeline extends out of the upper part of the inner cavity of the ceramic tube (8), and one gas outlet pipeline extends out of the inner cavity of the quartz glass tube (7);
the quartz glass tube (7) is externally wrapped with an electric furnace (6);
the ceramic tube (8) is a proton conductive ceramic tube.
2. The hydrogen isotope concentration system adapted for use at ambient levels in accordance with claim 1 wherein: the cooling coil I (9) and the cooling coil II (10) are one of air cooling coils or air cooling coils.
3. The hydrogen isotope concentration system adapted for use at ambient levels in accordance with claim 1 wherein: the electric furnace (6) is a programmed heating electric furnace, and the heating range is room temperature to 1100 ℃.
4. The hydrogen isotope concentration system adapted for use at ambient levels in accordance with claim 1 wherein: the pump I (19) and the pump II (20) are vacuum pumps.
5. The hydrogen isotope concentration system adapted for use at ambient levels in accordance with claim 1 wherein: the measuring instrument (17) is one of an ionization chamber, a proportional counter tube or a chromatograph.
6. The hydrogen isotope concentration system adapted for use at ambient levels in accordance with claim 1 wherein: the connecting pipeline of the hydrogen isotope concentration system adopts a stainless steel pipeline with the thickness of 1/8inch or 1/4 inch.
7. The hydrogen isotope concentration system adapted for use at ambient levels in accordance with claim 1 wherein: the valve I (15) and the valve II (16) are one of a manual valve, a semi-manual valve and an automatic valve with automatic temperature early warning.
CN201910219843.3A 2019-03-22 2019-03-22 Hydrogen isotope concentration system suitable for environmental level Active CN109765093B (en)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN103728163A (en) * 2014-01-16 2014-04-16 中国工程物理研究院核物理与化学研究所 Fast sampling system for full tritium in gas
CN106018003A (en) * 2016-05-20 2016-10-12 中国科学院上海应用物理研究所 Sampling device and measurement method for multi-form tritium in atmosphere around nuclear facility
CN106886042A (en) * 2017-04-17 2017-06-23 中国工程物理研究院核物理与化学研究所 Tritium accumulation sampling system in a kind of air

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN103728163A (en) * 2014-01-16 2014-04-16 中国工程物理研究院核物理与化学研究所 Fast sampling system for full tritium in gas
CN106018003A (en) * 2016-05-20 2016-10-12 中国科学院上海应用物理研究所 Sampling device and measurement method for multi-form tritium in atmosphere around nuclear facility
CN106886042A (en) * 2017-04-17 2017-06-23 中国工程物理研究院核物理与化学研究所 Tritium accumulation sampling system in a kind of air

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