CN103949159A - Separation method of radioisotope 14C - Google Patents
Separation method of radioisotope 14C Download PDFInfo
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- CN103949159A CN103949159A CN201410202914.6A CN201410202914A CN103949159A CN 103949159 A CN103949159 A CN 103949159A CN 201410202914 A CN201410202914 A CN 201410202914A CN 103949159 A CN103949159 A CN 103949159A
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Abstract
The invention provides a separation method of radioisotope 14C. The method comprises the following steps: firstly, introducing gas in chromatographic columns of a system, heating and activating, and removing H2O and air impurities out of the columns; then feeding a CO raw material gas in a rough separation system, carrying out circular separation for 4-8 processes between the two chromatographic columns, recycling one part of the CO raw material gas as a depleted gas by a storage tank, and feeding the other part of the CO raw material gas (serving as a pre-concentrated sample) into a concentration extraction system under the driving of a carrier gas; carrying out circular separation for 4-8 processes between chromatographic columns of the concentration extraction system, returning one part of the CO raw material gas (serving as depleted gas) to the rough separation system, and feeding the other part (serving as a concentrated sample) in a refining system; and finally, carrying out circular separation for 4-8 processes between the chromatographic columns of the refining system, returning one part of the raw material gas (serving as depleted gas) to the concentration extraction system, and feeding the other part (serving as abundant 14C) in a product gas storage tank. The method provided by the invention can obtain the 14CO product gas with 14C abundance being 95%. The method provided by the invention is simple in process, is simple and convenient to operate, is low in energy consumption, and is low in retention volume.
Description
Technical field
The invention belongs in Spent Radioactive graphite
14c processes the technical field of disposing, and is specifically related to a kind of radio isotope
14the separation method of C.
Background technology
The neutron activation reaction occurring in nuclear reactor running, comprises (n, γ) reaction, (n, p) reaction, (n, α) reaction etc., makes some nonradioactive isotopes in some structural material of reactor, cooling agent, especially graphite moderator etc., as
17o,
13c and
14n changes radionuclide into
14c.
14c is a kind of low energy beta radiator, and the half-life reaches 5730, and β decay is
14the β ray average energy discharging during N is 49.5keV, and highest energy 156keV, belongs to moderate toxicity.Due to
14the half-life of C is very long, easily in the interaction of bioprocess and soil and plant, moves, and mobility is extremely strong, with gas form (
14cO
2) exist
14c, reaches very soon balance after being sucked, and enter the mass part of bio-tissue by lung from air.
14be about 40 years the biological half-life of C,
14the accumulation of C in human body mainly causes because taking in contaminated food.Therefore, must be in graphite
14c tightens control or effectively removes, in order to avoid environmentally safe, constitutes a threat to.
The Spent Radioactive graphite drawing off due to reactor has that quantity is huge, activity is high, the fire-hazardous feature of high potential, it processes to dispose becomes a global difficult problem, not yet find a method being entirely satisfactory, current main processing mode has three kinds in the world: the one, and take that fixed bed or fluidized bed combustion chamber, laser burns is the burning mode of representative; The 2nd, steam pyrolysis (U.S.'s patent in 2003,6625248); The 3rd, cement solidification.The second way is in the laboratory research stage, and technical difficulty is large, and process is wayward.The third mode is that problem has been left for to offspring, and increase-volume is obvious, the long-range threat of environmentally safe formation.And first kind of way has the feature remarkable, technical feasibility is good, processing cost is cheap of holding that subtracts, become preferred manner, but current dispute has been possible discharge in a large number the rear formation of burning
14cO
2gas.If can not directly discharge, must be right
14cO
2gas is processed, and processing mode has two kinds: the one, utilize Ca (OH)
2after neutralization absorbs as CaCO
3be fixed up, cause increase-volume more than 8 times; The 2nd, utilize isotope separation technique separated
12c and
14c.Therefore, the isolation technics of carbon isotope and technological level become one of key technology of Spent Radioactive graphite treatment disposal.
The mode that Tokyo technical research institute adopts microwave discharge to combine with Chemical Exchange, take dibutyl amine-octane and diethylamine-octane as isotope switching architecture, intends using 20 years, in the 1600t graphite that Japanese CalderHall type reactor decommissioning is produced
14c reclaims, unstripped gas CO sample introduction flow 284L/min,
14the initial abundance 5.1 * 10 of C
-7, dilution gas after three-stage cascade is processed
14c abundance 1.2 * 10
-12, system
14c hold-up 0.014mol.Japan NGK company has developed variation fluidization, with CO
2and H
2the form of O reclaims
14c and tritium, intend carrying out the processing of East Sea I Magnox reactor barren rock China ink.Zurich, SUI ETH, between 2008-2009, adopts electron bombardment furnace to spend under pyrolytics at line drawing 1600 with atomic form
14c, will
14c mean concentration is 15
14c atom/gram sample separation be concentrated into 5.11 * 10
5individual
14c atom/gram.It is separated that Sweden Lund university has set up complete chemical process method between 2004-2010
14c sample, adopts ion exchange resin and inorganic, organic matter to carry out
14the extraction of C and washing, cause system
14the hold-up of C is larger.In a word, in order to solve
14the emission problem of C, various countries have carried out a large amount of
14c/
12c isotope separation technique research, is at present technically captured gradually, but expense is too high, is unfavorable for engineering application.
In China, the front-end technology research of useless graphite treatment is relatively more, carbon isotope separation, especially
14the separation of C is fewer with concentrated research.Chinese Radiation Protection Research Inst has carried out the incineration treatment technology research of Spent Radioactive graphite, and center group has carried out heavy water reactor power station
14generation-release of C and control measure research, Shanghai Chemical Research Inst simulates the cryogenic rectification process of carbon isotope.But these researchs are not yet applied to barren rock China ink after burning, through engineering approaches
14c/
12c isotopic separation.Along with the fast development of China's Nuclear Electricity and the passing of time, increasing Spent Radioactive graphite need to be processed disposal, therefore, and development new technologies and new technology, reduction radio isotope
14the separation costs of C is the active demand of useless graphite treatment disposal technology development.
Summary of the invention
The object of this invention is to provide a kind of radio isotope
14the separation method of C.
The principle of separation method of the present invention is to utilize
12cO with
14the difference that CO distributes between carrier gas mobile phase and the fixing phase of molecular sieve, makes adsorbate
12cO,
14cO is desorption from molecular sieve surface successively, reaches separated object, and separating effect can judge from flow-gas proportional counter and mass spectrometric monitored data.
Object of the present invention can be achieved through the following technical solutions:
A kind of radio isotope
14the separation method of C, comprises the following steps:
The activation of a, chromatographic column
By the chromatographic column ventilation body heat-activated of crude separation system, upgrading system and refining system, remove the H in chromatographic column
2o and air plankton;
B, crude separation stage
CO unstripped gas enters the crude separation system under liquid nitrogen cryogenics, at two cover chromatogram intercolumniations, circulates after a separated 4-8 flow process, and a part is reclaimed by storage tank as dilution gas, and another part enters upgrading system as preconcentration sample under the driving of carrier gas;
C, concentrate stage
The preconcentration sample of step b is entered to the upgrading system under liquid nitrogen cryogenics, at two cover chromatogram intercolumniations, circulate after a separated 4-8 flow process, a part is returned to crude separation system as dilution gas, and another part enters refining system as the sample that concentrates under the driving of carrier gas;
D, refining stage and product-collecting
The sample that concentrates of step c is entered to the refining system under liquid nitrogen cryogenics, at two cover chromatogram intercolumniations, circulate after a separated 4-8 flow process, a part is returned to upgrading system as dilution gas, and another part is as abundant
14c enters product air accumulator.
Described crude separation system comprises gas flow path, liquid nitrogen stream and chromatographic column, and gas flow path is formed by connecting by magnetic valve, stop valve, pipeline and elbow; Liquid nitrogen stream route low temperature valve, pipeline, joint and heat-insulation layer form; Column's length 50-70m, 2.25 inches of post external diameters, molecular sieve loading density is 0.7-0.8kg/L, after filling, coiling is helical disk tubulose, is immersed in low-temperature (low temperature) vessel.
Described upgrading system comprises gas flow path, liquid nitrogen stream and chromatographic column, and gas flow path is formed by connecting by disproportionation reactor, magnetic valve, stop valve, three-way connection, pipeline and elbow; Liquid nitrogen stream route low temperature valve, pipeline, joint and heat-insulation layer form; Column's length 40-60m, 1.0 inches of post external diameters, molecular sieve loading density is 0.6-0.7kg/L, after filling, coiling is helical disk tubulose, is immersed in low-temperature (low temperature) vessel.
Described refining system comprises gas flow path, liquid nitrogen stream and chromatographic column, and gas flow path is formed by connecting by disproportionation reactor, magnetic valve, stop valve, three-way connection, pipeline and elbow; Liquid nitrogen stream route low temperature valve, pipeline, joint and heat-insulation layer form; Column's length 30-50m, 0.375 inch of post external diameter, molecular sieve loading density is 0.6-0.7kg/L, after filling, coiling is helical disk tubulose, is immersed in low-temperature (low temperature) vessel.
Described disproportionation reactor is the copper tube of helical disk tubulose, external diameter 0.25-0.5 inch, filling Ru-Al
2o
3catalyst.
The sample introduction pressure of the CO unstripped gas described in step b is controlled at 0.3-0.4MPa.
Carrier gas described in step b, c, d is high-purity helium, and flow is 2-30L/min.
Radio isotope of the present invention
14the feature of the separation method of C is:
(1) compared with prior art, the invention provides that a kind of flow process is simple, easy and simple to handle, energy consumption is low, hold-up is little, it is abundant to obtain
14the method of C product.
(2) separation method cost is low, material loss is little, the chromatographic column life-span is long.The driving gas helium using can recycling, and the liquid nitrogen of filling can mutually shift and recycle between low-temperature (low temperature) vessel, and chromatographic column is loaded cheap 5A molecular sieve, and it is constant that the life-span reaches several years performance, can reuse by activating and regenerating.
(3) the method highly versatile.Although the method is for radio isotope
14the separation of C and designing, but its separation method is equally applicable to
3h,
39ar,
85the radioisotopic separation such as Kr is concentrated.
(4) the method scale is flexible.Adopt chromatographic column multi-stage cascade and disproportionation reactor, unpowered conveying between post and post, each separation phase is separate, can require and demand size according to the abundance of target product, increases or reduces cascade progression, zooms in or out column size parameter.
accompanying drawing explanation
Fig. 1 is radio isotope of the present invention
14the process chart of C separation.
In figure: 1. the chromatographic column II 11. disproportionation reactor III 12. disproportionation reactor IV 13. low-temperature (low temperature) vessel I 14. low-temperature (low temperature) vessel II 15. low-temperature (low temperature) vessel III 16. low-temperature (low temperature) vessel IV 17. low-temperature (low temperature) vessel V 18. low-temperature (low temperature) vessel VI 19. of chromatographic column I 10. refining systems of chromatographic column II 7. disproportionation reactor I 8. disproportionation reactor II 9. refining systems of chromatographic column I 6. upgrading systems of chromatographic column II 5. upgrading systems of the thick chromatographic column I 4. crude separation systems from system of high-purity He steel cylinder 2.CO unstripped gas storage tank 3.
14c product air accumulator, , 20. liquid nitrogen storage tanks, , 21. glove boxes, , 22. dilution gas collecting tanks, , LD-ZF. liquid nitrogen main valve, , LD1-1. low temperature valve, , LD1-2. low temperature valve, , LDT1-1-2. low temperature valve, , LDT1-2-1. low temperature valve, , LDG1-1. air bleeding valve, , LDG1-2. air bleeding valve, , V1-1-1. magnetic valve, , V1-1-2. magnetic valve, , V1-1-3. magnetic valve, , V1-1-4. magnetic valve, , V1-1-5. magnetic valve, , V1-1-6. magnetic valve, , V1-1-7. magnetic valve, , V1-1-8. magnetic valve, , V1-2-1. magnetic valve, , V1-2-2. magnetic valve, , V1-2-3. magnetic valve, , V1-2-4. magnetic valve, , V1-2-5. magnetic valve, , V1-2-6. magnetic valve, , V1-2-7. magnetic valve, , V1-2-8. magnetic valve, , S1-1-1. stop valve, , S1-1-2. stop valve, , S1-2-1. stop valve, , S1-2-2. stop valve, , V2-1-1. magnetic valve, , V2-1-2. magnetic valve, , V2-1-3. magnetic valve, , V2-1-4. magnetic valve, , V2-1-5. magnetic valve, , V2-1-6. magnetic valve, , V2-1-7. magnetic valve, , V2-1-8. magnetic valve, , V2-2-1. magnetic valve, , V2-2-2. magnetic valve, , V2-2-3. magnetic valve, , V2-2-4. magnetic valve, , V2-2-5. magnetic valve, , V2-2-6. magnetic valve, , V2-2-7. magnetic valve, , V2-2-8. magnetic valve, , S2-1-1. stop valve, , S2-1-2. stop valve, , S2-2-1. stop valve, , S2-2-2. stop valve, , LD2-1. low temperature valve, , LD2-2. low temperature valve, , LDT2-1-2. low temperature valve, , LDT2-2-1. low temperature valve, , LDG2-1. air bleeding valve, , LDG2-2. air bleeding valve, , V3-1-1. magnetic valve, , V3-1-2. magnetic valve, , V3-1-3. magnetic valve, , V3-1-4. magnetic valve, , V3-1-5. magnetic valve, , V3-1-6. magnetic valve, , V3-1-7. magnetic valve, , V3-1-8. magnetic valve, , V3-2-1. magnetic valve, , V3-2-2 is magnetic valve, , V3-2-3 is magnetic valve, , V3-2-4 is magnetic valve, , V3-2-5 is magnetic valve, , V3-2-6. magnetic valve, , V3-2-7. magnetic valve, , V3-2-8. magnetic valve, , S3-1-1. stop valve, , S3-1-2. stop valve, , S3-2-1. stop valve, , S3-2-2. stop valve, , LD3-1. low temperature valve, , LD3-2. low temperature valve, , LDT3-1-2. low temperature valve, , LDT3-2-1. low temperature valve, , LDG3-1. air bleeding valve, , LDG3-2. air bleeding valve, , T2-1-1. three-way connection, , T2-1-2. three-way connection, , T2-1-3. three-way connection, , T2-2-1. three-way connection, , T2-2-2. three-way connection, , T2-2-3. three-way connection, , T3-1-1. three-way connection, , T3-1-2. three-way connection, , T3-1-3. three-way connection, , T3-2-1. three-way connection, , T3-2-2. three-way connection, , T3-2-3. three-way connection.
The specific embodiment
Below in conjunction with the drawings and specific embodiments, content of the present invention is described in further detail.
Embodiment
A kind of radio isotope
14the separation method of C as shown in Figure 1, is by crude separation system, upgrading system, refining system, unstripped gas storage tank 2, liquid nitrogen storage 20, glove box 21, the three-stage cascade technique that low-temperature (low temperature) vessel I-VI and dilution gas collecting tank 22 forms, single cover column's length of every one-level is respectively 60,48,36m, and post external diameter is respectively 2.25,1.0,0.375 inches, in post, fill 5A molecular sieve, production capacity is annual output 40 Curie's abundance 95%
14cO gas, design parameter is in Table 1.
Table 1 radio isotope
14the separation parameter of C
Disproportionation reactor I-IV loads Ru-Al
2o
3logical hydrogen activation at the temperature of 873K after catalyst.Chromatographic column 3, chromatographic column 4, chromatographic column 5, chromatographic column 6, chromatographic column 9, chromatographic column 10 are heated simultaneously, lead to high-purity helium and activate, helium gas flow 1L/min activates 48h at the temperature of 530K.
Liquid nitrogen in liquid nitrogen storage 20 is filled with to the low-temperature (low temperature) vessel 13 at chromatographic column 3 places through liquid nitrogen main valve LD-ZF, low temperature valve LD1-1.CO unstripped gas from storage tank 2 out, enters chromatographic column 3 through magnetic valve V1-1-7 and stop valve S1-1-1
,sample introduction pressure is controlled at 0.3MPa, and carrier gas He from steel cylinder 1 out, enters crude separation system through magnetic valve V1-1-1 and magnetic valve V1-2-1.Chromatographic column 3 is carried out to the heating of temperature programming step by step, and liquid nitrogen is transferred to low-temperature (low temperature) vessel 14 from low-temperature (low temperature) vessel 13 through low temperature valve LDT1-1-2, liquid nitrogen utilizes liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD1-2 to supplement and fill with 14 after shifting.Take the lead in the CO gas of dilution of desorb under the driving of He, through stop valve S1-1-2, magnetic valve V1-2-5 and magnetic valve V1-2-6, enter dilution gas collecting tank 22; The CO gas concentrating of rear desorb, enters the chromatographic column 4 under liquid nitrogen cryogenics through stop valve S1-1-2, magnetic valve V1-1-2, magnetic valve V1-1-3 and stop valve S1-2-1; Chromatographic column 4 is carried out to the heating of temperature programming step by step, and liquid nitrogen is transferred to low-temperature (low temperature) vessel 13 from low-temperature (low temperature) vessel 14 through low temperature valve LDT1-2-1, liquid nitrogen utilizes liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD1-1 to supplement and fill with 13 after shifting.Take the lead in the CO gas of dilution of desorb under the driving of He, through stop valve S1-2-2, magnetic valve V1-1-5 and magnetic valve V1-1-6, enter dilution gas collecting tank 22; The CO gas concentrating of rear desorb, gets back to the chromatographic column 3 under liquid nitrogen cryogenics through stop valve S1-2-2, magnetic valve V1-2-2, magnetic valve V1-2-3 and stop valve S1-1-1; Again chromatographic column 3 is carried out to the heating of temperature programming step by step, the above-mentioned flow process of repetitive cycling 6 times, and separation process is carried out to on-line monitoring, respectively through stop valve S1-1-2, magnetic valve V1-1-2, magnetic valve V1-1-4 with sample through stop valve S1-2-2, magnetic valve V1-2-2, magnetic valve V1-2-4.After 6 flow processs of crude separation system,
14c abundance is from 10
-6concentrate to 0.1%.
Liquid nitrogen in liquid nitrogen storage 20 is filled with to the low-temperature (low temperature) vessel 15 at chromatographic column 5 places through liquid nitrogen main valve LD-ZF, low temperature valve LD2-1.Carrier gas He from steel cylinder 1 out, enters upgrading system through magnetic valve V2-1-1 and magnetic valve V2-2-1.From crude separation system out
14c abundance be 0.1% preconcentration sample under the driving of carrier gas, through magnetic valve V2-1-7 and stop valve S2-1-1, enter chromatographic column 5.Chromatographic column 5 is carried out to the heating of temperature programming step by step, and liquid nitrogen is transferred to low-temperature (low temperature) vessel 16 from low-temperature (low temperature) vessel 15 through low temperature valve LDT2-1-2, liquid nitrogen utilizes liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD2-2 to supplement and fill with 16 after shifting.Take the lead in the CO gas of dilution of desorb under the driving of He, through stop valve S2-1-2, magnetic valve V2-2-5 and magnetic valve V2-2-6, return to crude separation system, again as unstripped gas; The CO gas concentrating of rear desorb, enters the chromatographic column 6 under liquid nitrogen cryogenics through stop valve S2-1-2, magnetic valve V2-1-2, three-way connection T2-1-1, three-way connection T2-1-3, magnetic valve V2-1-3 and stop valve S2-2-1; Chromatographic column 6 is carried out to the heating of temperature programming step by step, and liquid nitrogen is transferred to low-temperature (low temperature) vessel 15 from low-temperature (low temperature) vessel 16 through low temperature valve LDT2-2-1, liquid nitrogen utilizes liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD2-1 to supplement and fill with 15 after shifting.Take the lead in the CO gas of dilution of desorb under the driving of He, through stop valve S2-2-2, magnetic valve V2-1-5 and magnetic valve V2-1-6, return to crude separation system, again as unstripped gas; The CO gas concentrating of rear desorb, gets back to the chromatographic column 5 under liquid nitrogen cryogenics through stop valve S2-2-2, magnetic valve V2-2-2, three-way connection T2-2-1, three-way connection T2-2-3, magnetic valve V2-2-3 and stop valve S2-1-1; Again chromatographic column 5 is carried out to the heating of temperature programming step by step, the above-mentioned flow process of repetitive cycling 5 times.Due to
14c
16the molecular weight of O is 30, so
12c
18o molecule with
14c
16o molecule is difficult to separation, if not
18o is transformed into
16o,
14the high abundance of C is only limited to 60% left and right, in order to obtain 95% abundance
14c product, must add isotope switch to remove
18o isotope, increases the disproportionated reaction of carbon isotope.In the 6th flow process, the CO gas concentrating of rear desorb, enters the chromatographic column 6 under liquid nitrogen cryogenics through stop valve S2-1-2, magnetic valve V2-1-2, three-way connection T2-1-1, disproportionation reactor 8, three-way connection T2-1-2, three-way connection T2-1-3, magnetic valve V2-1-3 and stop valve S2-2-1; Equally, the CO gas concentrating of rear desorb, gets back to the chromatographic column 5 under liquid nitrogen cryogenics through stop valve S2-2-2, magnetic valve V2-2-2, three-way connection T2-2-1, disproportionation reactor 7, three-way connection T2-2-2, three-way connection T2-2-3, magnetic valve V2-2-3 and stop valve S2-1-1.Separation process is carried out to on-line monitoring, through stop valve S2-1-2, magnetic valve V2-1-4 with through stop valve S2-2-2, magnetic valve V2-2-4, sample respectively.After 6 flow processs of upgrading system,
14c abundance concentrates to 20% from 0.1%.
Liquid nitrogen in liquid nitrogen storage 20 is filled with to the low-temperature (low temperature) vessel 17 at chromatographic column 9 places through liquid nitrogen main valve LD-ZF, low temperature valve LD3-1.Carrier gas He from steel cylinder 1 out, enters refining system through magnetic valve V3-1-1 and magnetic valve V3-2-1.From upgrading system out
14c abundance be 20% concentrate sample under the driving of carrier gas, through magnetic valve V3-1-7 and stop valve S3-1-1, enter chromatographic column 9.Chromatographic column 9 is carried out to the heating of temperature programming step by step, and liquid nitrogen is transferred to low-temperature (low temperature) vessel 18 from low-temperature (low temperature) vessel 17 through low temperature valve LDT3-1-2, liquid nitrogen utilizes liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD3-2 to supplement and fill with 18 after shifting.Take the lead in the CO gas of dilution of desorb under the driving of He, through stop valve S3-1-2, magnetic valve V3-2-5 and magnetic valve V3-2-6, return to upgrading system, again as unstripped gas; The CO gas concentrating of rear desorb, enters the chromatographic column 10 under liquid nitrogen cryogenics through stop valve S3-1-2, magnetic valve V3-1-2, three-way connection T3-1-1, three-way connection T3-1-3, magnetic valve V3-1-3 and stop valve S3-2-1; Chromatographic column 10 is carried out to the heating of temperature programming step by step, and liquid nitrogen is transferred to low-temperature (low temperature) vessel 17 from low-temperature (low temperature) vessel 18 through low temperature valve LDT3-2-1, liquid nitrogen utilizes liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD3-1 to supplement and fill with 17 after shifting.Take the lead in the CO gas of dilution of desorb under the driving of He, through stop valve S3-2-2, magnetic valve V3-1-5 and magnetic valve V3-1-6, return to upgrading system, again as unstripped gas; The CO gas concentrating of rear desorb, gets back to the chromatographic column 9 under liquid nitrogen cryogenics through stop valve S3-2-2, magnetic valve V3-2-2, three-way connection T3-2-1, three-way connection T3-2-3, magnetic valve V3-2-3 and stop valve S3-1-1; Again chromatographic column 9 is carried out to the heating of temperature programming step by step, the above-mentioned flow process of repetitive cycling 5 times.In order to obtain 95% abundance
14c product, the disproportionated reaction of increase carbon isotope.In the 6th flow process, the CO gas concentrating of rear desorb, enters product air accumulator 19 through stop valve S3-1-2, magnetic valve V3-1-2, three-way connection T3-1-1, disproportionation reactor 12, three-way connection T3-1-2; Equally, the CO gas concentrating of rear desorb, enters product air accumulator 19 through stop valve S3-2-2, magnetic valve V3-2-2, three-way connection T3-2-1, disproportionation reactor 11, three-way connection T3-2-2.Separation process is carried out to on-line monitoring, through stop valve S3-1-2, magnetic valve V3-1-4 with through stop valve S3-2-2, magnetic valve V3-2-4, sample respectively.After 6 flow processs of refining system,
14c abundance concentrates to 95% from 20%.For guaranteeing personnel's handling safety, the gas flow path of refining system and product air accumulator 19 are positioned at glove box 21.
Claims (7)
1. a radio isotope
14the separation method of C, is characterized in that, the method comprises the following steps:
A. the activation of chromatographic column
By the chromatographic column ventilation body heat-activated of crude separation system, upgrading system and refining system, remove the H in chromatographic column
2o and air plankton;
B. crude separation stage
CO unstripped gas enters the crude separation system under liquid nitrogen cryogenics, is circulating after a separated 4-8 flow process between two cover chromatographic columns, and a part is reclaimed by storage tank as dilution gas, and another part enters upgrading system as preconcentration sample under the driving of carrier gas;
C. concentrate stage
The preconcentration sample of step b is entered to the upgrading system under liquid nitrogen cryogenics, circulating after a separated 4-8 flow process between two cover chromatographic columns, a part is returned to crude separation system as dilution gas, and another part enters refining system as the sample that concentrates under the driving of carrier gas;
D. refining stage and product-collecting
The sample that concentrates of step c is entered to the refining system under liquid nitrogen cryogenics, circulating after a separated 4-8 flow process between two cover chromatographic columns, a part is returned to upgrading system as dilution gas, and another part is as abundant
14c enters product air accumulator.
2. radio isotope according to claim 1
14the separation method of C, is characterized in that: described crude separation system comprises gas flow path, liquid nitrogen stream and chromatographic column, and gas flow path is formed by connecting by magnetic valve, stop valve, pipeline and elbow; Liquid nitrogen stream route low temperature valve, pipeline, joint and heat-insulation layer form; Column's length 50-70m, 2.25 inches of post external diameters, molecular sieve loading density is 0.7-0.8kg/L, after filling, coiling is helical disk tubulose, is immersed in low-temperature (low temperature) vessel.
3. radio isotope according to claim 1
14the separation method of C, is characterized in that: described upgrading system comprises gas flow path, liquid nitrogen stream and chromatographic column, and gas flow path is formed by connecting by disproportionation reactor, magnetic valve, stop valve, three-way connection, pipeline and elbow; Liquid nitrogen stream route low temperature valve, pipeline, joint and heat-insulation layer form; Column's length 40-60m, 1.0 inches of post external diameters, molecular sieve loading density is 0.6-0.7kg/L, after filling, coiling is helical disk tubulose, is immersed in low-temperature (low temperature) vessel.
4. radio isotope according to claim 1
14the separation method of C, is characterized in that: described refining system comprises gas flow path, liquid nitrogen stream and chromatographic column, and gas flow path is formed by connecting by disproportionation reactor, magnetic valve, stop valve, three-way connection, pipeline and elbow; Liquid nitrogen stream route low temperature valve, pipeline, joint and heat-insulation layer form; Column's length 30-50m, 0.375 inch of post external diameter, molecular sieve loading density is 0.6-0.7kg/L, after filling, coiling is helical disk tubulose, is immersed in low-temperature (low temperature) vessel.
5. according to the radio isotope described in claim 3 or 4
14the separation method of C, is characterized in that: described disproportionation reactor is the copper tube of helical disk tubulose, external diameter 0.25-0.5 inch, filling Ru-Al
2o
3catalyst.
6. radio isotope according to claim 1
14the separation method of C, is characterized in that: the sample introduction pressure of the CO unstripped gas described in step b is controlled at 0.3-0.4MPa.
7. radio isotope according to claim 1
14the separation method of C, is characterized in that: the carrier gas described in step b, c is high-purity helium, and flow is 2-30L/min.
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| CN201410202914.6A CN103949159B (en) | 2014-05-15 | 2014-05-15 | A kind of radio isotope 14the separation method of C |
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|---|---|---|---|
| CN201410202914.6A CN103949159B (en) | 2014-05-15 | 2014-05-15 | A kind of radio isotope 14the separation method of C |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110465196A (en) * | 2019-08-16 | 2019-11-19 | 清华大学 | A kind of method of the separation carbon stable isotope of green high-efficient |
| CN110465197A (en) * | 2019-08-16 | 2019-11-19 | 清华大学 | A method of utilizing ionic liquid Carbon isotope separation |
| CN112557158A (en) * | 2021-02-28 | 2021-03-26 | 中国工程物理研究院核物理与化学研究所 | Separation, purification and collection device for xenon in air sample |
| CN112557157A (en) * | 2021-02-28 | 2021-03-26 | 中国工程物理研究院核物理与化学研究所 | Method for separating, purifying and collecting xenon in air sample based on specific device |
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| GB2024648A (en) * | 1978-07-05 | 1980-01-16 | Kakihana H | Chromatographic isotope separation process |
| EP0908226B1 (en) * | 1997-10-13 | 2006-02-22 | Taiyo Nippon Sanso Corporation | Process and apparatus for separation of stable isotope compound |
| CN1939839A (en) * | 2005-09-27 | 2007-04-04 | 上海化工研究院 | Purification for separating feed gas in stabilized isotope 13C by low-temperature CO rectifying method |
| CN101745315A (en) * | 2009-10-22 | 2010-06-23 | 上海化工研究院 | Process and device for rectifying and separating stable isotope 13C at low temperature by adopting CO |
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Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB2024648A (en) * | 1978-07-05 | 1980-01-16 | Kakihana H | Chromatographic isotope separation process |
| EP0908226B1 (en) * | 1997-10-13 | 2006-02-22 | Taiyo Nippon Sanso Corporation | Process and apparatus for separation of stable isotope compound |
| CN1939839A (en) * | 2005-09-27 | 2007-04-04 | 上海化工研究院 | Purification for separating feed gas in stabilized isotope 13C by low-temperature CO rectifying method |
| CN101745315A (en) * | 2009-10-22 | 2010-06-23 | 上海化工研究院 | Process and device for rectifying and separating stable isotope 13C at low temperature by adopting CO |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110465196A (en) * | 2019-08-16 | 2019-11-19 | 清华大学 | A kind of method of the separation carbon stable isotope of green high-efficient |
| CN110465197A (en) * | 2019-08-16 | 2019-11-19 | 清华大学 | A method of utilizing ionic liquid Carbon isotope separation |
| CN112557158A (en) * | 2021-02-28 | 2021-03-26 | 中国工程物理研究院核物理与化学研究所 | Separation, purification and collection device for xenon in air sample |
| CN112557157A (en) * | 2021-02-28 | 2021-03-26 | 中国工程物理研究院核物理与化学研究所 | Method for separating, purifying and collecting xenon in air sample based on specific device |
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| CN103949159B (en) | 2015-11-25 |
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