CN103949159B - A kind of radio isotope 14the separation method of C - Google Patents
A kind of radio isotope 14the separation method of C Download PDFInfo
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- CN103949159B CN103949159B CN201410202914.6A CN201410202914A CN103949159B CN 103949159 B CN103949159 B CN 103949159B CN 201410202914 A CN201410202914 A CN 201410202914A CN 103949159 B CN103949159 B CN 103949159B
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Abstract
The invention provides a kind of radio isotope
14the separation method of C, the method comprises the following steps: first by the chromatographic column of system ventilation body heat-activated, remove the H in post
2o and air plankton; Then CO unstripped gas enters crude separation system, and between two cover chromatographic columns after a multi-cycle separation 4-8 flow process, 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; Between the chromatographic column of upgrading system after a multi-cycle separation 4-8 flow process, a part returns crude separation system as dilution gas, and another part enters refining system as the sample that concentrates; Last between the chromatographic column of refining system after a multi-cycle separation 4-8 flow process, a part ofly return upgrading system as dilution gas, another part is as abundant
14c enters product air accumulator.Method of the present invention is adopted to obtain
14c abundance is 95%
14cO gas product.Method flow of the present invention is simple, easy and simple to handle, energy consumption is low, hold-up is little.
Description
Technical field
The invention belongs in Spent Radioactive graphite
14the technical field that C process is disposed, is specifically related to a kind of radio isotope
14the separation method of C.
Background technology
The neutron activation reaction occurred 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 discharged during N is 49.5keV, and highest energy 156keV, belongs to moderate toxicity.Due to
14the half-life of C is very long, and easily move in the interaction of bioprocess and soil and plant, mobility is extremely strong, with gas form (
14cO
2) exist
14c, reaches balance very soon after being sucked, and enter the mass part of bio-tissue by lung from air.
14the biological half-life of C is about 40 years,
14mainly because taking in, contaminated food causes in the accumulation of C in human body.Therefore, must in graphite
14c tightens control or effectively removes, and constitutes a threat in order to avoid environmentally safe.
The Spent Radioactive graphite drawn off due to reactor has that substantial amounts, activity are high, the fire-hazardous feature of high potential, its process disposal becomes a global difficult problem, not yet find a method be entirely satisfactory, main processing ways current in the world has three kinds: one to be that to burn with fixed bed or fluidized bed combustion chamber, laser be the burning mode of representative; Two is steam pyrolysis (U.S.'s patent in 2003,6625248); Three is cement solidifications.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 offspring, and increase-volume is obvious, the long-range threat of environmentally safe formation.And first kind of way have subtract hold significantly, technical feasibility is good, processing cost is cheap feature, become preferred manner, but current dispute be possible discharge in a large number burn after formed
14cO
2gas.If can not directly discharge, must be right
14cO
2gas processes, and processing mode has two kinds: one to be utilize Ca (OH)
2as CaCO after neutralization absorbs
3be fixed up, cause increase-volume more than 8 times; Two is utilize isotope separation technique to be separated
12c and
14c.Therefore, the isolation technics of carbon isotope and technological level become one of key technology that Spent Radioactive graphite treatment disposes.
Tokyo technical research institute adopts the mode that combines with Chemical Exchange of microwave discharge, with dibutyl amine-octane with diethylamine-octane for isotope switching architecture, plan used for 20 years, in the 1600t graphite of Japanese CalderHall type reactor decommissioning generation
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 process
14c abundance 1.2 × 10
-12, system
14c hold-up 0.014mol.NGK company of Japan develops variation fluidization, with CO
2and H
2the form of O reclaims
14c and tritium, intend the process carrying out East Sea I Magnox reactor barren rock ink.Zurich, SUI ETH, between 2008-2009, adopts electron bombardment furnace with under atomic form On-line testing 1600 degree of pyrolytics
14c, will
14c mean concentration is 15
14c atom/gram sample separation be concentrated into 5.11 × 10
5individual
14c atom/gram.Lund university of Sweden establishes complete chemical process method and is separated 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 carry out a large amount of
14c/
12c isotope separation technique is studied, and technically captured gradually at present, but expense is too high, is unfavorable for engineer applied.
In China, the front-end technology research of useless graphite treatment is relatively more, carbon isotope separation, especially
14the separation of C with concentrated study fewer.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 and the control measure research of C, the cryogenic rectification process of Shanghai Chemical Research Inst to carbon isotope is simulated.But these researchs to be not yet applied to barren rock ink burn after, 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 needs to carry out process to be disposed, 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, utilizes
12cO with
14the difference that CO distributes between carrier gas phase and molecular sieve Stationary liquid, makes adsorbate
12cO,
14cO is successively from desorption molecular sieve surface, and reach the object of separation, separating effect can judge from flow-gas proportional counter and mass spectrometric Monitoring 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 of crude separation system, upgrading system and refining system ventilation body heat-activated, 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, and after two cover chromatogram intercolumniation multi-cycle separation 4-8 flow process, 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 the upgrading system under liquid nitrogen cryogenics, after two cover chromatogram intercolumniation multi-cycle separation 4-8 flow process, a part returns 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 the refining system under liquid nitrogen cryogenics, after two cover chromatogram intercolumniation multi-cycle separation 4-8 flow process, a part returns 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 are formed; Column's length 50-70m, post external diameter 2.25 inches, molecular sieve loading density is 0.7-0.8kg/L, and after filling, coiling is helically coil-like, 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 are formed; Column's length 40-60m, post external diameter 1.0 inches, molecular sieve loading density is 0.6-0.7kg/L, and after filling, coiling is helically coil-like, 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 are formed; Column's length 30-50m, post external diameter 0.375 inch, molecular sieve loading density is 0.6-0.7kg/L, and after filling, coiling is helically coil-like, 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 Stress control of the CO unstripped gas described in step b is at 0.3-0.4MPa.
Carrier gas described in step b, c 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 used can recycling, and the liquid nitrogen of filling mutually can shift and recycle between low-temperature (low temperature) vessel, and chromatographic column loads 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 concentrates.
(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, zooming in or out column size parameter.
Accompanying drawing explanation
Fig. 1 is radio isotope of the present invention
14the process chart that C is separated.
Diagram: 1. 2. High purity He cylinders CO feed gas storage tank (3) the coarse from the system of chromatographic column I4. Coarse separation system of chromatographic column II5. Strong system of chromatographic column I6. Strong system of chromatographic column II7. Disproportionation reactor I8. II9 disproportionation reactor. The refining system of chromatographic column I10 refining system of chromatographic column II11 disproportionation reactor III12. IV13 disproportionation reactor. The cryogenic vessels I14, cryogenic vessels II15. Cryogenic vessels III16. Cryogenic vessels IV17. Cryogenic vessels V18, cryogenic vessels VI19. < sup TranNum = "180" > and < / sup > C product storage tanks, liquid nitrogen storage tank 21. 22. The glove box depleted gas collecting cans of LD - ZF. Total nitrogen valve LD1-1. The cryogenic valve LD1-2. Cryogenic valve LDT1-1-2. Cryogenic valve LDT1-2-1. The cryogenic valve LDG1-1. The exhaust valve LDG1-2. The exhaust valve V1-1-1. The solenoid valve V1-1-2. Electromagnetic valve V1-1-3. Electromagnetic valve V1-1-4. Electromagnetic valve V1-1-5. Electromagnetic valve V1-1-6. Electromagnetic valve V1-1-7.Electromagnetic valve solenoid valve V1-1-8. V1-2-1. The solenoid valve V1-2-2. Electromagnetic valve V1-2-3. Electromagnetic valve V1-2-4. Electromagnetic valve V1-2-5. Electromagnetic valve V1-2-6. Electromagnetic valve V1-2-7. Electromagnetic valve V1-2-8. Electromagnetic valve S1-1-1. Stop valve S1-1-2. Cut-off valve S1-2-1. Stop valve S1-2-2. Cut-off valve V2-1-1. The solenoid valve V2-1-2. Electromagnetic valve V2-1-3. The solenoid valve V2-1-4. Electromagnetic valve V2-1-5. Electromagnetic valve V2-1-6. Electromagnetic valve V2-1-7. Electromagnetic valve V2-1-8. Electromagnetic valve V2-2-1. The solenoid valve V2-2-2. Electromagnetic valve V2-2-3. Electromagnetic valve V2-2-4. Electromagnetic valve V2-2-5. Electromagnetic valve V2-2-6. Electromagnetic valve V2-2-7. Electromagnetic valve V2-2-8. Electromagnetic valve S2-1-1. Stop valve S2-1-2. Cut-off valve S2-2-1. Stop valve S2-2-2. Cut-off valve LD2-1. The cryogenic valve LD2-2. Cryogenic valve LDT2-1-2. Cryogenic valve LDT2-2-1. The cryogenic valve LDG2-1. The exhaust valve LDG2-2. The exhaust valve V3-1-1. The solenoid valve V3-1-2. Electromagnetic valve V3-1-3. The solenoid valve V3-1-4. Solenoid valve V3-1-6. Electromagnetic valve V3-1-7. Electromagnetic valve V3-1-8. Electromagnetic valve V3-2-1. The solenoid valve V3-2-2 for electromagnetic valve V3-2-3 for electromagnetic valve V3 for electromagnetic valve V3-2-2-4-5 for electromagnetic valve V3-2-6. Electromagnetic valve V3-2-7. Electromagnetic valve V3-2-8. Electromagnetic valve S3-1-1. Stop valve S3-1-2. Cut-off valve S3-2-1. Stop valve S3-2-2. Cut-off valve LD3-1. The cryogenic valve LD3-2. Cryogenic valve LDT3-1-2. Cryogenic valve LDT3-2-1. The cryogenic valve LDG3-1. The exhaust valve LDG3-2. The exhaust valve T2-1-1. The tee joint T2-1-2. Tee joint T2-1-3. Tee joint T2-2-1. The tee joint T2-2-2. Tee joint T2-2-3 T3 tee joint - 1-1. The tee joint T3-1-2. Tee joint T3-1-3. The tee joint T3-2-1. The tee joint T3-2-2. Tee joint T3-2-3. The tee joint.
Detailed description of the invention
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 form, the list cover column's length of every one-level is respectively 60,48,36m, post external diameter is respectively 2.25,1.0,0.375 inches, fill 5A molecular sieve in post, production capacity is annual output 40 Curie 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 heated simultaneously, logical high-purity helium activates, helium gas flow 1L/min, activates 48h at the temperature of 530K.
Liquid nitrogen in liquid nitrogen storage 20 is filled the low-temperature (low temperature) vessel 13 at chromatographic column 3 place 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 Stress control is 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.Ramped heating schedule is step by step carried out to chromatographic column 3, 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 transfer after utilize liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD1-2 to 14 carry out supplement fill.Take the lead in the CO gas of dilution of desorb under the driving of He, enters dilution gas collecting tank 22 through stop valve S1-1-2, magnetic valve V1-2-5 and magnetic valve V1-2-6; The CO gas concentrated of rear desorb, the chromatographic column 4 under stop valve S1-1-2, magnetic valve V1-1-2, magnetic valve V1-1-3 and stop valve S1-2-1 enter liquid nitrogen cryogenics; Ramped heating schedule is step by step carried out to chromatographic column 4, 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 transfer after utilize liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD1-1 to 13 carry out supplement fill.Take the lead in the CO gas of dilution of desorb under the driving of He, enters dilution gas collecting tank 22 through stop valve S1-2-2, magnetic valve V1-1-5 and magnetic valve V1-1-6; The CO gas concentrated of rear desorb, the chromatographic column 3 under stop valve S1-2-2, magnetic valve V1-2-2, magnetic valve V1-2-3 and stop valve S1-1-1 get back to liquid nitrogen cryogenics; Again ramped heating schedule is step by step carried out to chromatographic column 3, the above-mentioned flow process of repetitive cycling 6 times, and on-line monitoring is carried out to separation process, 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 crude separation system 6 flow processs,
14c abundance is from 10
-6concentrate to 0.1%.
Liquid nitrogen in liquid nitrogen storage 20 is filled the low-temperature (low temperature) vessel 15 at chromatographic column 5 place 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 the preconcentration sample of 0.1% under the driving of carrier gas, enter chromatographic column 5 through magnetic valve V2-1-7 and stop valve S2-1-1.Ramped heating schedule is step by step carried out to chromatographic column 5, 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 transfer after utilize liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD2-2 to 16 carry out supplement fill.Take the lead in the CO gas of dilution of desorb under the driving of He, returns crude separation system, again as unstripped gas through stop valve S2-1-2, magnetic valve V2-2-5 and magnetic valve V2-2-6; The CO gas concentrated of rear desorb, the chromatographic column 6 under 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 enter liquid nitrogen cryogenics; Ramped heating schedule is step by step carried out to chromatographic column 6, 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 transfer after utilize liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD2-1 to 15 carry out supplement fill.Take the lead in the CO gas of dilution of desorb under the driving of He, returns crude separation system, again as unstripped gas through stop valve S2-2-2, magnetic valve V2-1-5 and magnetic valve V2-1-6; The CO gas concentrated of rear desorb, the chromatographic column 5 under 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 get back to liquid nitrogen cryogenics; Again ramped heating schedule is step by step carried out to chromatographic column 5, 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 be difficult to be separated, if not
18o is transformed into
16o, then
14the most high abundance of C is only limited to about 60%, in order to obtain 95% abundance
14c product, must add isotope switch to remove
18o isotope, namely increases the disproportionated reaction of carbon isotope.In the 6th flow process, the CO gas concentrated of rear desorb, the chromatographic column 6 under 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 enter liquid nitrogen cryogenics; Equally, the CO gas concentrated of rear desorb, the chromatographic column 5 under 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 get back to liquid nitrogen cryogenics.On-line monitoring is carried out to separation process, samples through stop valve S2-1-2, magnetic valve V2-1-4 with through stop valve S2-2-2, magnetic valve V2-2-4 respectively.After upgrading system 6 flow processs,
14c abundance concentrates to 20% from 0.1%.
Liquid nitrogen in liquid nitrogen storage 20 is filled the low-temperature (low temperature) vessel 17 at chromatographic column 9 place 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, enter chromatographic column 9 through magnetic valve V3-1-7 and stop valve S3-1-1.Ramped heating schedule is step by step carried out to chromatographic column 9, 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 transfer after utilize liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD3-2 to 18 carry out supplement fill.Take the lead in the CO gas of dilution of desorb under the driving of He, returns upgrading system, again as unstripped gas through stop valve S3-1-2, magnetic valve V3-2-5 and magnetic valve V3-2-6; The CO gas concentrated of rear desorb, the chromatographic column 10 under 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 enter liquid nitrogen cryogenics; Ramped heating schedule is step by step carried out to chromatographic column 10, 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 transfer after utilize liquid nitrogen storage 20, liquid nitrogen main valve LD-ZF, low temperature valve LD3-1 to 17 carry out supplement fill.Take the lead in the CO gas of dilution of desorb under the driving of He, returns upgrading system, again as unstripped gas through stop valve S3-2-2, magnetic valve V3-1-5 and magnetic valve V3-1-6; The CO gas concentrated of rear desorb, the chromatographic column 9 under 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 get back to liquid nitrogen cryogenics; Again ramped heating schedule is step by step carried out to chromatographic column 9, the above-mentioned flow process of repetitive cycling 5 times.In order to obtain 95% abundance
14c product, increases the disproportionated reaction of carbon isotope.In the 6th flow process, the CO gas concentrated 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 concentrated 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.On-line monitoring is carried out to separation process, samples through stop valve S3-1-2, magnetic valve V3-1-4 with through stop valve S3-2-2, magnetic valve V3-2-4 respectively.After refining system 6 flow processs,
14c abundance concentrates to 95% from 20%.For guaranteeing human users's safety, gas flow path and the product air accumulator 19 of refining system 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 of crude separation system, upgrading system and refining system ventilation body heat-activated, remove the H in chromatographic column
2o and air plankton;
B. the crude separation stage
CO unstripped gas enters the crude separation system under liquid nitrogen cryogenics, and between two cover chromatographic columns after a multi-cycle separation 4-8 flow process, 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. the concentrate stage
The preconcentration sample of step b is entered the upgrading system under liquid nitrogen cryogenics, between two cover chromatographic columns after a multi-cycle separation 4-8 flow process, a part returns 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 the refining system under liquid nitrogen cryogenics, between two cover chromatographic columns after a multi-cycle separation 4-8 flow process, a part returns 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 are formed; Column's length 50-70m, post external diameter 2.25 inches, molecular sieve loading density is 0.7-0.8kg/L, and after filling, coiling is helically coil-like, 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 are formed; Column's length 40-60m, post external diameter 1.0 inches, molecular sieve loading density is 0.6-0.7kg/L, and after filling, coiling is helically coil-like, 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 are formed; Column's length 30-50m, post external diameter 0.375 inch, molecular sieve loading density is 0.6-0.7kg/L, and after filling, coiling is helically coil-like, is immersed in low-temperature (low temperature) vessel.
5. the radio isotope according to 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 Stress control of the CO unstripped gas described in step b is 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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| 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 |
| CN112557158B (en) * | 2021-02-28 | 2021-05-28 | 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 |
| CN112557157B (en) * | 2021-02-28 | 2021-05-04 | 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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2014
- 2014-05-15 CN CN201410202914.6A patent/CN103949159B/en not_active Expired - Fee Related
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 |
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