CN110648779A - Circulation loop for preparing I-125 by reactor irradiation - Google Patents

Circulation loop for preparing I-125 by reactor irradiation Download PDF

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Publication number
CN110648779A
CN110648779A CN201910597315.1A CN201910597315A CN110648779A CN 110648779 A CN110648779 A CN 110648779A CN 201910597315 A CN201910597315 A CN 201910597315A CN 110648779 A CN110648779 A CN 110648779A
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China
Prior art keywords
irradiation
loop
reactor
pipeline
bottle
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CN201910597315.1A
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于宁文
罗志福
邓新荣
向学琴
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China Institute of Atomic of Energy
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China Institute of Atomic of Energy
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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
    • G21G1/001—Recovery of specific isotopes from irradiated targets
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
    • G21G1/02—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes in nuclear reactors
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
    • G21G1/001—Recovery of specific isotopes from irradiated targets
    • G21G2001/0063—Iodine

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Plasma & Fusion (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)

Abstract

The invention discloses a circulation loop for preparing I-125 by reactor irradiation, which comprises a loop pipeline, an irradiation part, a recovery device, a gas barrier device, a raw material gas cylinder, a tail gas purification device and a molecular pump, wherein the irradiation part is arranged on the loop pipeline; an electromagnetic valve is arranged on the loop pipeline to control the node; the irradiation component, the recovery device, the gas blocking device, the raw material gas cylinder, the tail gas purification device and the molecular pump are all connected to the loop pipeline; the irradiation component is arranged in the stack part. The invention has the following beneficial effects: the invention controls the amount of the raw material gas filled in the irradiation bottle through the loop system, and can accurately control the preparation125I yield, to achieve on-heap production125The irradiation efficiency is high during the irradiation, the irradiation safety of the circulation loop is good, the radioactive pollution is less, and the radiation injury of operators is small. The input amount of the raw material target gas can be determined according to the demand of the yield, and continuous circulation and intermittent circulation can be carried out according to the demand of the yield.

Description

Circulation loop for preparing I-125 by reactor irradiation
Technical Field
The invention relates to the field of nuclear chemical industry, in particular to a circulation loop for preparing I-125 by reactor irradiation.
Background
125I is a long half-life (T)1/259.7d) releases low-energy gamma rays (27KeV, X-rays) by electron capture. Due to the fact that125Long half-life period of I, low energy of gamma ray and no beta-Radiation, widely used in clinical diagnosis of nuclear medicine, biomedical research and tumor brachytherapy (X-ray seed source). In particular in the recent years it has become possible,125the medical use of I-seed sources has developed very rapidly.125The I seed source can be used for the brachytherapy of various malignant tumors (head and neck, digestive system, chest, urinary system tumors and the like),125the tumor tissue is killed to the maximum extent by releasing the radioactive rays for a short time, and the normal tissue is not damaged or minimally damaged, so that the treatment aim is fulfilled. In the clinical field, the medicine is prepared by mixing the raw materials,125the therapeutic effect of the I particle source on malignant tumors is confirmed, and the I particle source is considered to be a safe and effective treatment technology with low complication rate.
With following125The medical application of I is becoming more and more extensive, domestic125The demand of I is in a rapidly growing situation. In the face of the greater domestic application demand, the existing125The efficiency of the production process is far from sufficient.
In view of the above, the present invention is particularly proposed.
Disclosure of Invention
Aiming at the defects in the prior art, the invention aims to provide a circulation loop for preparing I-125 by reactor irradiation, which can produce I-125 by the circulation loop and improve the production efficiency.
The technical scheme of the invention is as follows:
a circulation loop for preparing I-125 by reactor irradiation comprises a loop pipeline, an irradiation part, a recovery device, a gas blocking device, a raw material gas cylinder, a tail gas purification device and a molecular pump; an electromagnetic valve is arranged on the loop pipeline to control the node; the irradiation component, the recovery device, the gas blocking device, the raw material gas cylinder, the tail gas purification device and the molecular pump are all connected to the loop pipeline; the irradiation component is arranged in the stack part.
Further, the circulation loop of the reactor irradiation preparation I-125 is characterized in that the irradiation component comprises an irradiation bottle and an automatic control unit; the automatic control unit is arranged on a connecting pipeline of the irradiation bottle and the loop pipeline.
Further, in the above circulation loop for preparing I-125 by reactor irradiation, a plurality of irradiation bottles are connected in parallel, and each irradiation bottle corresponds to one automatic control unit.
Further, the circulation loop for preparing I-125 by reactor irradiation also comprises a diffusion bottle, wherein the diffusion bottle is arranged on a connecting pipeline of the irradiation bottle and the loop pipeline, and a lead shielding radiation protection sleeve is arranged outside the diffusion bottle.
Further, the recycling loop of the reactor irradiation preparation I-125 is characterized in that the recovery device comprises a plurality of collecting decay bottles connected in parallel.
Further, the reactor irradiation preparation I-125 circulation loop is characterized in that the tail gas purification device is a plurality of tail gas purification bottles connected in series.
Further, the vacuum degree of the loop pipeline reaches 10 to prepare the circulation loop of I-125 by reactor irradiation-6Pa or above.
Further, a loop of the reactor irradiation preparation I-125 is provided with a vacuum gauge, a vacuum pressure gauge and a pressure sensor.
Furthermore, the electromagnetic valve and the automatic control unit of the circulation loop of the reactor irradiation preparation I-125 are connected with the automatic control device in a control way.
The invention has the following beneficial effects:
1. the invention controls the amount of the raw material gas filled in the irradiation bottle through the loop system, and can accurately control the preparation125I yield, to achieve on-heap production125High irradiation efficiency in the time I, good irradiation safety of a circulation loop, less radioactive pollution and less radiation damage to operators
2. The input amount of the raw material target gas can be determined according to the demand of the yield, and continuous circulation or intermittent circulation can be carried out according to the demand of the yield.
3. The closed vacuum degree of the circulation loop can reach 10-6And the gas can be completely transferred safely and efficiently by more than Pa.
4. The circulation loop system adopts the modes of irradiation in the reactor and decay outside the reactor,greatly simplifies the structure of the inner part of the stack, and is easy to produce with large batch quantity and high purity125I。
5. The circulation loop system supports a plurality of irradiation bottles and collection decay bottles in parallel, conveniently125I throughput requirements regulate throughput.
6. The circulation loop system adopts automatic control, and operators can remotely and automatically control each electromagnetic valve by setting a program on the controller, thereby ensuring the radiation safety of the operators.
Drawings
FIG. 1 is irradiation124Xe production125And (I) nuclear reaction.
FIG. 2 is a schematic diagram of the structure of a circulation loop for preparing I-125 by reactor irradiation.
In the attached drawings, 1, an irradiation bottle; 2. an electromagnetic valve; 3. an overboard circulation main pipeline; 4. a pressure sensor; 5. a diffusion bottle; 6. a radiation protective jacket; 7. a choke tube; 8. an electromagnetic valve; 9. collecting decay bottles; 10. a radiation protective jacket; 11. a vacuum gauge; 12. an electromagnetic valve; 13. collecting decay bottles; 14. a radiation protective jacket; 15. an electromagnetic valve; 16. collecting decay bottles; 17. a radiation protective jacket; 18. an electromagnetic valve; 19. collecting decay bottles; 20. a radiation protective jacket; 21. an electromagnetic valve; 22. a gas cylinder; 23. a radiation protective jacket; 24. a tail gas purifying bottle; 25. a radiation protective jacket; 26. a tail gas purifying bottle; 27. a radiation protective jacket; 28. a valve; 29. a raw material gas cylinder; 30. a vacuum pressure gauge; 31. a valve; 32. a molecular pump; 33. an electromagnetic valve; 34. an electromagnetic valve; 35. an actuator; 36. a controller; 37. an irradiation bottle; 38. and (5) irradiating the bottle.
Detailed Description
The invention is described in detail below with reference to the figures and examples.
Mass production125I can utilize reactor thermal neutron irradiation124Xe to obtain125Xe，125Xe decay to produce125I. The nuclear reaction is shown in FIG. 1.
There are also two types of secondary nuclear reactions during the irradiation preparation:
secondary nuclear reaction 1:125I(n，γ)126I(n，γ)127I
secondary nuclear reaction 2:125Xe(n，γ)126Xe(n，γ)127Xe
125i has a large thermal neutron section of 894b, and a certain amount of thermal neutrons are generated in the irradiation preparation process126I, produced by126I has strong gamma ray, energy 666KeV and beta+And beta－And (4) rays. In order to avoid the influence of impurities generated by the secondary nuclear reaction on the product quality, the irradiation needs to be carried out for a certain time125The Xe is transferred out of the stack and allowed to decay outside the stack to125I. Produced by simultaneous irradiation125Xe and126i has strong radioactive energy, and in order to reduce radiation damage to human bodies, a remote automatic control method is adopted to control the irradiation process of the operation circulation loop.
The loop method is to establish a circulation loop system on the reactor and adopt the mode of irradiation in the reactor and decay outside the reactor to produce and prepare125I. According to different reactor irradiation reaction time and yield and125the half-life of Xe, etc. has an influence on the quality of the product by filling the irradiation bottles in the reactor with a circulating loop124After Xe target gas is irradiated for a certain time, the irradiated gas (including Xe target gas) is circulated through a circulation loop125Xe、125I, etc.) recovering to the outside of the reactor in a recovery device waiting for decay, charging the target gas124The amount of Xe can be controlled according to the size of the yield. The target gas can be filled again or repeatedly according to the required quantity to carry out irradiation production preparation125I, the circulation loop can be used for production and preparation of intermittent and continuous circulation methods125I。
As shown in FIG. 2, the invention provides a circulation loop for preparing I-125 by reactor irradiation, which comprises a loop pipeline, an irradiation part, a recovery device, a gas blocking device, a raw material gas cylinder 29, a tail gas purification device and a molecular pump 32; an electromagnetic valve is arranged on the loop pipeline to control the node; the irradiation part, the recovery device, the gas blocking device, the raw material gas cylinder 29, the tail gas purification device and the molecular pump 32 are connected to the loop pipeline; the irradiation component is arranged in the stack part.
The circulation loop system of the invention can adopt the modes of in-pile irradiation and out-pile decay, greatly simplifies the in-pile structure, and is easy to produce large-batch high-purity products125I。
The irradiation part comprises an irradiation bottle (1, 37, 38) and an automatic control unit; the automatic control unit is arranged on a connecting pipeline of the irradiation bottle and the loop pipeline. The irradiation bottles are connected in parallel, and each irradiation bottle corresponds to one automatic control unit. A plurality of irradiation bottles can be arranged in a plurality of pore channels of the reactor, and the off-reactor treatment system in the continuous circulation production circulation loop of the plurality of irradiation bottles can be used for treating the gas in different irradiation bottles through control. The recovery apparatus comprises a plurality of collection decay vials connected in parallel. By a plurality of irradiation bottles and collection decay bottles connected in parallel, the system can be based on125I requirement of production quantity, production by batch or continuous process125I. The irradiation bottle 1 is arranged in the active area of the irradiation pore canal of the reactor core and is used for filling124The Xe target gas is irradiated and is led out by a connecting conduit to be connected with a main reactor external circulation pipeline 3 (the external part of the loop pipeline). Filled with irradiation bottles 1124After the Xe target gas is irradiated for a certain period of time, the automatic control unit (electromagnetic valve 2) is opened, and the irradiated gas (including the gas after irradiation)125Xe、125I gas, etc.). According to the requirements of yield as much as possible of irradiation and the requirements of irradiation conditions of different reactors, different materials can be selected according to different reactors to process and manufacture irradiation bottles, the selection of the material of the irradiation bottles in the pore canal of the active region of the reactor needs to consider that the material has good thermal neutron economy, smaller nuclear heating power and good heat release performance, the influence of basic particles in the active region and the effect of electromagnetic irradiation on the material structure of the irradiation bottles, the safety problem of corrosion in the pore canal of the active region of the reactor and good machining performance are also considered, and the materials such as zirconium Zr, aluminum Al, magnesium Mg and the like can be selected.
The irradiation bottle 1 is filled124After the irradiation of the Xe target gas is finished, the Xe target gas is collected into a recovery bottle through a loop, and the recovered irradiated gas mainly contains125Xe and125I，125xe emits gamma rays, with a maximum energy of 243KeV,125i emitted X-rays with a maximum energy of 35 KeV.
Irradiation production preparation built on reactor125The I automatically controlled circulation loop irradiation system fully utilizes the resource condition of the reactor, has good universality, and can determine the target gas according to the yield requirement124The input amount of Xe and the circulation loop irradiation system can be subjected to continuous circulation and intermittent circulation according to the requirement of yield.
In this embodiment, the circulation pipeline is made of stainless steel and titanium alloy material. The out-of-pile circulation loop is connected with the in-pile connection conduit to form an all-metal closed vacuum circulation loop system, and the vacuum circulation loop uses electromagnetic valves (8, 12, 15, 18, 21, 33 and 34) to carry out node control.
The circulation loop further comprises a diffusion bottle 5, wherein the diffusion bottle 5 is arranged on a connecting pipeline of the irradiation bottle (1, 37, 38) and the loop pipeline, and a lead shielding radiation protection sleeve 6 is arranged outside the diffusion bottle 5. Besides the diffusion bottle 5, the collection decay bottles (9, 13, 16, 19), the gas storage bottle 22, the tail gas purification bottles (24, 26) are also provided with lead radiation shielding protective sleeves (10, 14, 17, 20, 23, 25, 27). Needle-shaped diffusion bottle 5 for diffusion filling124Xe target gas, choke 7, is used to slow the gas flow rate. The irradiated gas can be collected in collecting decay bottles (9, 13, 16, 19) respectively, and a raw material gas bottle 29 (provided with a valve 28) is provided124Xe raw material target gas is filled into an irradiation bottle 1 for irradiation, and the circuit is abundant124Xe source target gas is stored in a gas cylinder 22 for recirculation, and a molecular pump 32 is used to evacuate the circulation loop system to a vacuum level of 10-6Pa above to ensure the safe and efficient complete transfer of the gas. In addition, for the sake of control, a valve 31 is provided upstream of the molecular pump 32.
The tail gas purification device is provided with a plurality of tail gas purification bottles (two in the embodiment) connected in series so as to meet the higher requirement of tail gas purification emission generated along with the increase of yield. In this embodiment, a plurality of stages of tail gas purification bottles (24, 26) connected in series are installed in front of the molecular pump 32 to ensure that the gas discharged by the molecular pump 32 meets the environmental protection requirement.
In this embodiment, the vacuum degree of the loop pipeline reaches 10-6Pa or above. And the loop pipeline is provided with a vacuum gauge 11, a vacuum pressure gauge 30 and a pressure sensor 4 so as to monitor the vacuum degree of the pipeline at any time. The circulation loop is an all-metal closed system, and the closed vacuum degree of the circulation loop can reach 10-6And the gas can be completely transferred safely and efficiently by more than Pa.
The electromagnetic valve and the automatic control unit are connected with the automatic control device in a control way. The automatic control is realized by an automatic control device (such as a PLC programmable logic digital operation system). The automation control means consist of a controller 36 and an actuator 35. By programming the controller 36 to be executed by the actuator 34 output, each solenoid valve can be automatically controlled to effect automatic control of the circulation loop.
When the electromagnetic valve is used, an operator can program each electromagnetic valve on the controller to realize automatic control. The vacuum pump 32 is started to open the valve 31, the electromagnetic valve of the control loop is opened, the tail gas is purified by the tail gas purifying bottles 24 and 26, and the vacuum degree of the pumped circulation loop system reaches 10-6Pa or above. And closing all the electromagnetic valves and the valve 31, opening the valve 28, the electromagnetic valves 33, 34 and 2 in sequence to charge the raw material gas into the irradiation bottle 1, and closing the electromagnetic valves 2, 34 and 33 to perform irradiation after reaching a limit value. After reaching the preset irradiation time, the electromagnetic valves 8 and 2 are opened in sequence to recover the irradiated gas (including125Xe and125I) and (4) putting the sample into a collecting decay bottle 9, closing the electromagnetic valve 8 and completing the first cyclic irradiation.
After the first circulation irradiation is finished, the valve 28, the electromagnetic valves 33, 34 and 2 are opened again to charge the raw gas into the irradiation bottle 1, the electromagnetic valves 2, 34 and 33 are closed to perform irradiation after the limit value is reached, and the electromagnetic valves 12 and 2 are opened in sequence to recover the irradiated gas (including the irradiated gas) after the preset irradiation time is reached125Xe and125I) and (6) entering a collecting decay bottle 13, closing the electromagnetic valve 12 and completing the second cycle irradiation.
Performing third and fourth cyclic irradiation according to the operation flow, wherein the irradiated gas (including125Xe and125I) are recovered into collection decay bottles 16, 19, respectively.
According to the requirement of production, a plurality of channels of the reactor are parallelly provided with irradiation bottles (such as 37 and 38), and the irradiation production is performed by the irradiation bottles in an alternating continuous circulating way125I。
After the cyclic irradiation is completed, all valves are closed and the collection decay vials (9, 16, 19) are removed and returned to the laboratory for further processing125And (I) purifying and recovering.
It will be apparent to those skilled in the art that various changes and modifications may be made in the present invention without departing from the spirit and scope of the invention. Thus, if such modifications and variations of the present invention fall within the scope of the claims of the present invention and their equivalents, the present invention is intended to include such modifications and variations.

Claims (9)

1. A circulation loop for preparing I-125 by reactor irradiation is characterized in that: comprises a loop pipeline, an irradiation component, a recovery device, a gas barrier device, a raw material gas cylinder, a tail gas purification device and a molecular pump; an electromagnetic valve is arranged on the loop pipeline to control the node; the irradiation component, the recovery device, the gas blocking device, the raw material gas cylinder, the tail gas purification device and the molecular pump are all connected to the loop pipeline; the irradiation component is arranged in the stack part.
2. The recirculation loop for reactor irradiation preparation I-125 of claim 1, wherein: the irradiation component comprises an irradiation bottle and an automatic control unit; the automatic control unit is arranged on a connecting pipeline of the irradiation bottle and the loop pipeline.
3. The recirculation loop of reactor irradiation preparation I-125 of claim 2, wherein: the irradiation bottles are connected in parallel, and each irradiation bottle corresponds to one automatic control unit.
4. The recirculation loop of reactor irradiation preparation I-125 of claim 2, wherein: still include the diffusion bottle, the diffusion bottle set up in irradiation bottle with the connecting pipeline of return circuit pipeline, the outside is provided with lead shielding radiation lag.
5. The recirculation loop for reactor irradiation preparation I-125 of claim 1, wherein: the recovery apparatus comprises a plurality of collection decay vials connected in parallel.
6. The recirculation loop for reactor irradiation preparation I-125 of claim 1, wherein: the tail gas purification device is a plurality of tail gas purification bottles connected in series.
7. The recirculation loop for reactor irradiation preparation I-125 of any of claims 1-6, wherein: the vacuum degree of the loop pipeline reaches 10-6Pa or above.
8. The recirculation loop for reactor irradiation preparation I-125 of any of claims 1-6, wherein: and a vacuum gauge, a vacuum pressure gauge and a pressure sensor are arranged on the loop pipeline.
9. The recirculation loop for reactor irradiation preparation I-125 of any of claims 2-6, wherein: the electromagnetic valve and the automatic control unit are connected with the automatic control device in a control mode.
CN201910597315.1A 2019-07-04 2019-07-04 Circulation loop for preparing I-125 by reactor irradiation Pending CN110648779A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111370154A (en) * 2020-03-23 2020-07-03 中国原子能科学研究院 Device for producing isotopes

Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1999041755A1 (en) * 1998-02-12 1999-08-19 Robert Robertson Method for making iodine-125 loaded substrates for use in radioactive sources
CN1571073A (en) * 2004-04-29 2005-01-26 北京原子高科核技术应用股份有限公司 Radioactivity125I preparation method and intermittent circulation loop device
CN202119274U (en) * 2011-06-17 2012-01-18 四平维克斯换热设备有限公司 Build-in heat exchanger for vertical type industrial furnace
CN104616713A (en) * 2015-01-26 2015-05-13 中国工程物理研究院核物理与化学研究所 Xenon target preparation device for reactor irradiation production of I-125 (iodine-125)
WO2015114424A1 (en) * 2014-01-31 2015-08-06 Istituto Nazionale Di Fisica Nucleare Method for producing beta emitting radiopharmaceuticals, and beta emitting radiopharmaceuticals thus obtained
CN106225092A (en) * 2016-07-18 2016-12-14 合肥美菱净化设备有限公司 A kind of silent dehumidifying machine
CN106898406A (en) * 2017-02-28 2017-06-27 中国核动力研究设计院 A kind of preparation method of radioactivity I125 and continuous circulation loop device
CN207731139U (en) * 2017-12-18 2018-08-14 中国原子能科学研究院 It is prepared for reactor125The intermittent cyclic circuit automation control device of I

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1999041755A1 (en) * 1998-02-12 1999-08-19 Robert Robertson Method for making iodine-125 loaded substrates for use in radioactive sources
CN1571073A (en) * 2004-04-29 2005-01-26 北京原子高科核技术应用股份有限公司 Radioactivity125I preparation method and intermittent circulation loop device
CN202119274U (en) * 2011-06-17 2012-01-18 四平维克斯换热设备有限公司 Build-in heat exchanger for vertical type industrial furnace
WO2015114424A1 (en) * 2014-01-31 2015-08-06 Istituto Nazionale Di Fisica Nucleare Method for producing beta emitting radiopharmaceuticals, and beta emitting radiopharmaceuticals thus obtained
CN104616713A (en) * 2015-01-26 2015-05-13 中国工程物理研究院核物理与化学研究所 Xenon target preparation device for reactor irradiation production of I-125 (iodine-125)
CN106225092A (en) * 2016-07-18 2016-12-14 合肥美菱净化设备有限公司 A kind of silent dehumidifying machine
CN106898406A (en) * 2017-02-28 2017-06-27 中国核动力研究设计院 A kind of preparation method of radioactivity I125 and continuous circulation loop device
CN207731139U (en) * 2017-12-18 2018-08-14 中国原子能科学研究院 It is prepared for reactor125The intermittent cyclic circuit automation control device of I

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111370154A (en) * 2020-03-23 2020-07-03 中国原子能科学研究院 Device for producing isotopes

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