CN101866701B - A new method for preparing radionuclide 98Tc - Google Patents
A new method for preparing radionuclide 98Tc Download PDFInfo
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- CN101866701B CN101866701B CN2010101743569A CN201010174356A CN101866701B CN 101866701 B CN101866701 B CN 101866701B CN 2010101743569 A CN2010101743569 A CN 2010101743569A CN 201010174356 A CN201010174356 A CN 201010174356A CN 101866701 B CN101866701 B CN 101866701B
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- 238000000034 method Methods 0.000 title claims abstract description 38
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims abstract description 111
- 239000003957 anion exchange resin Substances 0.000 claims abstract description 22
- 238000002360 preparation method Methods 0.000 claims abstract description 14
- 238000005406 washing Methods 0.000 claims description 59
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 28
- 239000012153 distilled water Substances 0.000 claims description 25
- 230000002285 radioactive effect Effects 0.000 claims description 18
- 239000011347 resin Substances 0.000 claims description 16
- 229920005989 resin Polymers 0.000 claims description 16
- 238000010828 elution Methods 0.000 claims description 11
- 238000005349 anion exchange Methods 0.000 claims description 10
- 230000007704 transition Effects 0.000 claims description 9
- 238000004090 dissolution Methods 0.000 claims description 8
- 238000010438 heat treatment Methods 0.000 claims description 7
- 230000007935 neutral effect Effects 0.000 claims description 6
- 230000001351 cycling effect Effects 0.000 claims description 5
- 238000012545 processing Methods 0.000 claims description 5
- 238000004140 cleaning Methods 0.000 claims description 3
- 238000001704 evaporation Methods 0.000 claims description 3
- 230000008020 evaporation Effects 0.000 claims description 3
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 2
- IXCSERBJSXMMFS-UHFFFAOYSA-N hydrogen chloride Substances Cl.Cl IXCSERBJSXMMFS-UHFFFAOYSA-N 0.000 claims description 2
- 239000002245 particle Substances 0.000 claims description 2
- 238000012216 screening Methods 0.000 claims description 2
- 238000000926 separation method Methods 0.000 abstract description 13
- 229910052750 molybdenum Inorganic materials 0.000 abstract description 12
- 239000012535 impurity Substances 0.000 abstract description 4
- 238000011017 operating method Methods 0.000 abstract 1
- 239000000243 solution Substances 0.000 description 28
- 229910052713 technetium Inorganic materials 0.000 description 11
- 229910052739 hydrogen Inorganic materials 0.000 description 9
- 238000011084 recovery Methods 0.000 description 8
- 238000004088 simulation Methods 0.000 description 8
- 238000002835 absorbance Methods 0.000 description 7
- 238000001228 spectrum Methods 0.000 description 7
- 238000012360 testing method Methods 0.000 description 7
- SOIFLUNRINLCBN-UHFFFAOYSA-N ammonium thiocyanate Chemical compound [NH4+].[S-]C#N SOIFLUNRINLCBN-UHFFFAOYSA-N 0.000 description 4
- 238000011978 dissolution method Methods 0.000 description 4
- LBDSXVIYZYSRII-BJUDXGSMSA-N helion Chemical compound [3He+2] LBDSXVIYZYSRII-BJUDXGSMSA-N 0.000 description 4
- 230000000155 isotopic effect Effects 0.000 description 4
- 239000011259 mixed solution Substances 0.000 description 4
- 239000000523 sample Substances 0.000 description 4
- GKLVYJBZJHMRIY-UHFFFAOYSA-N technetium atom Chemical compound [Tc] GKLVYJBZJHMRIY-UHFFFAOYSA-N 0.000 description 4
- 235000011114 ammonium hydroxide Nutrition 0.000 description 3
- 229910052804 chromium Inorganic materials 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 229910052742 iron Inorganic materials 0.000 description 3
- 229910052748 manganese Inorganic materials 0.000 description 3
- 229910052751 metal Inorganic materials 0.000 description 3
- 239000002184 metal Substances 0.000 description 3
- 238000000746 purification Methods 0.000 description 3
- 229910052710 silicon Inorganic materials 0.000 description 3
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 239000003513 alkali Substances 0.000 description 2
- 238000005341 cation exchange Methods 0.000 description 2
- 238000004587 chromatography analysis Methods 0.000 description 2
- 238000000975 co-precipitation Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 238000009616 inductively coupled plasma Methods 0.000 description 2
- 238000001095 inductively coupled plasma mass spectrometry Methods 0.000 description 2
- 239000006166 lysate Substances 0.000 description 2
- 229910052749 magnesium Inorganic materials 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- 238000000638 solvent extraction Methods 0.000 description 2
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- QZPSXPBJTPJTSZ-UHFFFAOYSA-N aqua regia Chemical compound Cl.O[N+]([O-])=O QZPSXPBJTPJTSZ-UHFFFAOYSA-N 0.000 description 1
- 239000012496 blank sample Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
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- 238000004880 explosion Methods 0.000 description 1
- GPRLSGONYQIRFK-UHFFFAOYSA-N hydron Chemical group [H+] GPRLSGONYQIRFK-UHFFFAOYSA-N 0.000 description 1
- 238000005342 ion exchange Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 150000001455 metallic ions Chemical class 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000002808 molecular sieve Substances 0.000 description 1
- 230000003472 neutralizing effect Effects 0.000 description 1
- 238000007747 plating Methods 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- ZNNZYHKDIALBAK-UHFFFAOYSA-M potassium thiocyanate Chemical compound [K+].[S-]C#N ZNNZYHKDIALBAK-UHFFFAOYSA-M 0.000 description 1
- 238000001612 separation test Methods 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 1
- 238000004544 sputter deposition Methods 0.000 description 1
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Abstract
本发明公开了一种新的制取放射性核素98TC的方法，其主要的技术特点是，经氘核(2H)辐照的Mo靶用市售H2O2溶解，用NaOH将溶解后的Mo、TC转换成Na2MoO4和Na2TCO4，且使溶液的碱度维持在10％左右；在Mo与98Tc的分离过程中，含98TC的Na2MoO4溶液上Dowex-1阴离子交换树脂柱后，先用重量浓度9.5～10.5％的NaOH淋洗，将溶液中的Mo洗下来，之后分别用1.5～2.5mol/L的HCl淋洗和2～3mol/L的HNO3淋洗，将其他杂质洗下来，最后用交换柱体积5.0～8.0倍浓度为7.0～8.0mol/L的HNO3淋洗，得到高纯度的含98Tc的Na2TcO4溶液。采用本发明制取的98Tc，其Mo/Tc原子比小于1％；Tc的放射性核纯度大于99.9％，且制取方法操作程序简单，安全性好。
The present invention discloses a new method for preparing radionuclide 98 TC. Its main technical feature is that the Mo target irradiated by deuteron ( 2 H) is dissolved with commercially available H 2 O 2 , and NaOH is used to dissolve the Mo target. The final Mo and TC are converted to Na 2 MoO 4 and Na 2 TCO 4 , and the alkalinity of the solution is maintained at about 10%; during the separation process of Mo and 98 Tc, the Na 2 MoO 4 solution containing 98 TC is -1 After the anion exchange resin column, rinse with NaOH with a weight concentration of 9.5-10.5% to wash off the Mo in the solution, and then rinse with 1.5-2.5mol/L HCl and 2-3mol/L HNO 3 Rinse to wash off other impurities, and finally rinse with 5.0-8.0 times the volume of the exchange column with HNO 3 at a concentration of 7.0-8.0 mol/L to obtain a high-purity Na 2 TcO 4 solution containing 98 Tc. The Mo/Tc atomic ratio of the 98 Tc prepared by the invention is less than 1%; the radionuclear purity of Tc is greater than 99.9%, and the preparation method has simple operating procedures and good safety.
Description
Technical field
The present invention relates to the isotope technology field, more specifically, relate to a kind of through d nuclear (
2H) irradiation
98The Mo target is produced radioactive nuclide
98The method of Tc.
Background technology
98Tc is the longest a kind of nucleic of half life period in the isotope of Tc, reaches 4.2 * 10
6A.
98Tc does not exist at occurring in nature, only in type nuclear activities such as nuclear explosion, could produce.Therefore,
98Tc can be used for the having a nuclear test analysis again of data also can be used for the geochemistry and the researching nuclein migration of technetium.
98Tc generally produces through accelerator.Produce with accelerator
98Tc, the method for prior art mainly adopt proton (
1H) and helion (
3He) bombardment metal M o.Bibliographical information is arranged with the 22MeV proton (
1H) bombardment Mo target obtains about 10 μ g's
98Tc, and the isotopic abundance that has provided Tc form (
95Tc :～0.5%,
97Tc:56.0%,
98Tc:17.3%,
99But do not have concrete experimentation Tc:26.7%).Other bibliographical information is arranged with the 23MeV helion (
3He) and the 19MeV helion (
3He) bombardment Mo target has only been studied the excitation energy that helion bombards the Mo target.
Produce with accelerator
98Tc relates to the preparation of Mo target, the irradiation of Mo target, the dissolving and the technology such as Mo separates with the radiochemistry of Tc of irradiation Mo target.The wherein preparation of Mo target adopts that generally electrochemical plating, vacuum sputtering, Mo sheet mounting method, Mo plate are directly processed etc.The dissolving of irradiation Mo target mainly contains aqua regia dissolution method, red fuming nitric acid (RFNA) or the concentrated sulphuric acid, 10% NaOH (or 1mol/L NaOH) and 30%H
2O
2Solution heating for dissolving method, ammoniacal liquor and 30%H
2O
2Mixed solution dissolution method etc.The concentrated acid dissolution method is operated more loaded down with trivial details owing to need to add a large amount of alkali neutralizing acids; Ammoniacal liquor and 30%H
2O
2The mixed solution dissolution method because dissolving back alkalescence is on the low side, need adds alkali and make solution become strong basicity, operates also more loaded down with trivial details.10% NaOH (or 1mol/LNaOH) and 30%H
2O
2Solution heating for dissolving method, course of dissolution not only need heating, and dissolution velocity is fast inadequately, effect is also general.The radiochemistry separation method of Mo is many, and Al is arranged
2O
3Chromatography, anion exchange resins exchange process, Fe (OH)
3Coprecipitation, solvent extraction or several method are used in combination etc.To from a few gram Mo, isolate trace (～μ g level)
98Tc, it is very difficult adopting conventional method, does not also reach the requirement of separation and purification.Co-precipitation and solvent extraction complex operation, the recovery of Tc is not high; Al
2O
3The chromatography operation is also more loaded down with trivial details, Al
2O
3Also difficulty of processing, and be prone to cause the leakage of Mo to wear etc.There is bibliographical information to pass through reactor
98Mo (n, γ)
99The Tc reacted
99Tc is in its reacted
99In the process of Tc, adopt cation exchange column and anion-exchange column to combine to carry out separating of Mo and Tc, Co, Ag, this separation method is first with ammoniacal liquor and 30%H
2O
2Mixed solution dissolving irradiation Mo target, excessive H is removed in water-bath
2O
2, at first go up the Hydrogen cation exchange column after sample is water-soluble, use water wash; Leacheate is gone up anion-exchange column again, with washing, with potassium oxalate-KOH solution Mo drip washing is got off then earlier, and ammonium thiocyanate drip washing Tc is adopted in washing at last again.This method has been used the twice ion exchange column, operates more loaded down with trivial detailsly, and has adopted ammonium thiocyanate drip washing Tc, and elution volume is big (about 400-500mL) also, and there is certain danger in need with the ammonium thiocyanate heating and decomposition in last solution; In last result, do not provide related data (atomic ratio that comprises Mo/Tc) yet.
Summary of the invention
Produce radioactive nuclide to prior art
98The present situation of Tc, the object of the invention aim to provide a kind of d nuclear (
2H) irradiation bombardment Mo target produce the Tc/Mo atomic ratio less than 1%, radionuclide purity is greater than 99.9%
98Tc (contains
95Tc,
97Tc with
99The isotope of Tc such as Tc) new method overcomes prior art simultaneously and separates problems such as complex operation, leacheate volume that Mo, Tc exist are big, poor stability.
The radioactive nuclide of producing provided by the invention
98The method of Tc mainly may further comprise the steps:
(1) Mo target preparation: with the dimensioned Mo target sheet of Mo plate according to the accelerator target holder;
(2) Mo target irradiation: employing d nuclear (
2H) irradiation bombardment Mo target, placement is no less than 270 days entering dissolution process behind the irradiation;
(3) irradiation Mo target dissolving: use commercially available H
2O
2Dissolving irradiation Mo target, H
2O
2Consumption by 2.5～5.0mL/gMo, fully the dissolving back adds the NaOH of weight concentration 9.5～10.5%, converts Mo, Tc after the dissolving to Na
2MoO
4And Na
2TcO
4, the consumption of NaOH is by 5.0～8.0mL/gMo, and the basicity of solution maintains 9.5～10.5%;
(4) Mo with
98Tc separates: Dowex-1 anion-exchange resin column on the irradiation Mo target solution, and the Mo detection limit in NaOH drip washing to the leacheate of use weight concentration 9.5～10.5% is zero, removes NaOH with distilled water drip washing; Using 10.0～12.5 times of exchange column volumes, concentration afterwards respectively is the HCl drip washing of 1.5～2.5mol/L, and 8.0～10.0 times of exchange column volumes, concentration are the HNO of 2～3mol/L
3Drip washing; The HNO that to use 5.0～8.0 times of concentration of exchange column volume at last be 7.0～8.0mol/L
3Drip washing is contained
98The Na of Tc
2TcO
4Solution.
On the basis of such scheme, can further take following technical measures: will contain
98The Na of Tc
2TcO
4The solution heating evaporation is removed HNO
3, remove remaining HNO with HCl more afterwards
3, add dissolved in distilled water at last, obtain the higher Na of purity
2TcO
4Solution.
With d nuclear (
2H) irradiation Mo target preparation
98Tc can adopt enrichment
98The Mo target also can adopt natural Mo target, but because enrichment
98The Mo target is very expensive, for
98The development and production cost of Tc is too high.Given this, the present invention adopts natural Mo target preparation
98Tc.Natural Mo target mainly contains
94Mo,
95Mo,
96Mo,
97Mo,
98Mo,
99Mo with
100Isotopes such as Mo also contain elements such as micro Mg, Mn, Cr, Fe, Si in addition, with d nuclear (
2H) the natural Mo target of irradiation mainly take place (d, 2n), (d n) waits nuclear reaction, and the Tc coordination have the long half-lift of generation main:
95Tc (T
1/2=61d), by
95Mo (d, 2n)
95Tc,
94Mo (d, n)
95Tc produces;
97Tc (T
1/2=91.4d), by
97Mo (d, 2n)
97Tc,
96Mo (d, n)
97Tc produces;
98Tc (T
1/2=4.2 * 10
6A), by
98Mo (d, 2n)
98Tc,
97Mo (d, n)
98Tc produces.
Therefore, how the natural Mo target of irradiation is separated through radiochemistry and remove a large amount of Mo (gram magnitude) and non-material and trace put such as Mg, Mn, Cr, Fe, Si on a small quantity
95Zr,
95,96Nb,
94,95,97,103Radioimpurity radioactive impurities such as Ru, obtain the Tc/Mo atomic ratio less than 1% microgram magnitude, radionuclide purity is greater than 99.9%
98Tc (contains
95Tc,
97Tc with
99The isotope of Tc such as Tc), be to adopt natural Mo target preparation
98The technological difficulties of Tc.Technique scheme of the present invention has solved this technical matters well.
At the above-mentioned radioactive nuclide of producing
98In the scheme of TC, said Dowex-1 anion-exchange resin column preferably adopts the Dowex-1 anion-exchange column after handling transition.The Dowex-1 anion-exchange column was meant on the Dowex-1 resin and used distilled water, HCl, distilled water, HNO successively behind the anion-exchange resin column said transition
3, distilled water drip washing, use the NaOH drip washing of weight concentration 9.5～10.5% afterwards again, maintain 9.5～10.5% Dowex-1 anion-exchange resin column through the basicity of repeatedly drip washing process resin.In Dowex-1 anion-exchange resin column processing procedure transition, preferably use HCl, distilled water, HNO successively
3, distilled water carries out cycling elution, cycle index is no less than 3 times, it is neutral that drip washing to leacheate is.In the cycling elution process, the rate of flow in rinse of each link preferably is controlled at 0.4～0.6mL/min scope.Transition the Dowex-1 anion-exchange resin column, the Dowex-1 resin through cleaning, oven dry, grind and the screening processing, and was selected the Dowex-1 resin of particle diameter in 80～120 order scopes for use before last anion-exchange column.
At the above-mentioned radioactive nuclide of producing
98In the scheme of Tc, use commercially available H
2O
2Dissolving irradiation Mo target preferably adopts on a small quantity repeatedly dissolution mechanism, uses commercially available H at least
2O
2Dissolving irradiation Mo target 2 times, H
2O
2The each dissolving of consumption should be in 0.5～1.0mL/gMo scope, and total consumption is 2.5～5.0mL/gMo; On the irradiation Mo target solution behind the Dowex-1 anion-exchange resin column NaOH of operating weight concentration 9.5～10.5% carry out drip washing, rate of flow in rinse should be controlled at 0.4～0.6mL/min scope.
Highly purified in order to prepare
98Tc, inventor have improved the dissolving method of Mo, and in the detachment process of Mo and Tc, only adopt the Dowex-1 anion-exchange resin column, have improved the ELUTION METHOD of Mo and Tc in this course, last resulting containing
98The volume of Tc solution also reduces (60-100mL) greatly, and final separation and purification obtains
98Tc, its Mo/Tc atomic ratio is less than 1%, and radionuclide purity is greater than 99.9%.Producing
98In the prior art of Tc, tool the inventor know, also nobody obtains the Mo/Tc atomic ratio less than 1% before the present invention accomplishes
98Tc, and preparation method running program of the present invention is simple, good operation safety.
Prepare highly purified
98Tc, irradiation, the dissolving of irradiation Mo target that relates to preparation, the Mo target of Mo target separates with the radiochemistry of irradiation Mo target etc.In the preparation of Mo target, consider factors such as complexity and cost, compared the quality of several method, the present invention adopts highly purified Mo plate (99.99%) directly to process irradiation Mo target.The dissolving of irradiation Mo target, the inventor finds in experimentation, uses commercially available H separately
2O
2(the about 30%H of weight concentration
2O
2) dissolving Mo is than with 10% NaOH (or 1mol/L NaOH) and commercially available H
2O
2The mixed solution dissolution velocity is fast, effective and need not heat, so the present invention has adopted the first commercially available H that uses
2O
2Dissolving Mo, Mo, Tc after back NaOH with weight concentration about 10% will dissolve convert to and separate needed Na
2MoO
4And Na
2TcO
4Pattern.The radiochemistry of irradiation Mo target is separated, in high-purity
98Be most important link in the preparation process of Tc, the inventor according to analyze, the actual conditions of simulated experiment, improved the method for drip washing Mo and drip washing Tc, only adopted the Dowex-1 anion-exchange resin column to obtain needed microgram magnitude with regard to separation and purification
98Tc, the Mo/Tc atomic ratio is less than 1%, and radionuclide purity (contains greater than 99.9%
95Tc,
97Tc with
99The isotope of Tc such as Tc).Basic skills of the present invention is after first NaOH with q.s gets off Mo drip washing, then to use HCl, HNO again
3The non-materials and a spot of of putting such as a spot of Mo that drip washing is not got off and the Mg of trace, Mn, Cr, Fe, Si
95Zr,
95,96Nb,
94,95,97,103Radioimpurity radioactive impurity drip washing such as Ru are got off, and needed
98Tc (contains
95Tc,
97Tc with
99The isotope of Tc such as Tc) still stays on the Dowex-1 anion-exchange resin column, at last with the HNO of the about 7.5mol/L of weight concentration
3Drip washing Na
2 98TcO
4Thereby, the HNO of assurance high concentration
3Do not contain other metallic ion and radioimpurity radioactive impurity in the leacheate, obtain highly purified Tc.In the radiochemistry detachment process of irradiation Mo target of the present invention, do not adopt ammonium thiocyanate drip washing Tc, improved the security of preparation high-purity Tc.
Description of drawings
Accompanying drawing 1, accompanying drawing 2 are gamma spectrums of sample.
Can find out that from the gamma spectrum of accompanying drawing 1 and accompanying drawing 2 energy spectrum region has only
95mTc,
97The characteristic power spectrum of Tc does not have the power spectrum of other nucleic, explains to have obtained highly purified containing
98The Na of Tc
2TcO
4Solution.
Embodiment:
1.Mo the preparation of target
The highly purified Mo plate of buying (99.99%) is processed into the target sheet that meets dimensional requirement according to the requirement of accelerator target holder.Processed 4 Mo targets here altogether, 1 is used to do simulation test, and 1 is used for
99Tc
mRecovery test, other 2 are used for the irradiation target.
2.Mo the irradiation of target
Employing d nuclear (
2H) irradiation bombardment Mo target, " cooling " (are promptly placed a period of time, are no less than 270 days, so that let short-decayed nucleic decay) after a period of time and carry out the radiochemistry separation of irradiation target.
The situation such as the table 1 of 2 Mo target sheet irradiation.
The irradiation situation of table 1Mo target
3. the separation of simulation Mo target
Because irradiation Mo target has hot, should not directly carry out the experiments such as dissolving, separation of irradiation Mo target, so need carry out earlier " cold test " before irradiation Mo target separates carrying out, promptly simulate earlier the Mo target dissolving, simulation Mo target separation and
99Tc
mRecovery test etc.
1) dissolving of simulation Mo target
Improved dissolving method is adopted in the dissolving of Mo, promptly directly uses 30%H
2O
2Dissolving Mo need not heat in the course of dissolution.
(1) dissolving of Mo sheet
The thick Mo sheet of the heavy 1-5mm of 3g is cut into small pieces (3mm * 3mm), add weight concentration 30%H 5 times by each 0.5mL/gMo score
2O
2The Mo sheet is dissolved, and course of dissolution does not need heating.Add the MoO of the NaOH of weight concentration 10% after the dissolving again with dissolving
3Convert Na to
2MoO
4, the NaOH use amount, needed whole Na before last Dowex-1 anion-exchange resin column by 8.0mL/gMo
2MoO
4The basicity of solution maintains about 10%.
(2) dissolving of simulation Mo target
To simulate Mo target sheet and be fixed in the dissolving tank, adopt the method for above-mentioned (1), add weight concentration 30%H 5 times by each 0.5mL/gMo score
2O
2Simulation Mo target sheet is dissolved, add the MoO of the NaOH of weight concentration 10% after the dissolving again dissolving
3Convert Na to
2MoO
4, the NaOH use amount is by 8.0mL/gMo, Na
2MoO
4The basicity of solution maintains about 10%, and the meltage of Mo is controlled at about 3g.
2) Mo separates
As previously mentioned, (100 ± 20 orders, φ 1.0 * 20.0cm) carry out separating of Tc and Mo etc. to adopt the Dowex-1 anion-exchange resin column.
(1) processing of Dowex-1 resin
After the cleaning of Dowex-1 resin, oven dry is ground with muller, uses the molecular sieve sub-sieve again, and it is subsequent use to get 100 ± 20 purpose Dowex-1 resins.
With anion-exchange column on above-mentioned 100 ± 20 purpose Dowex-1 resins.Elder generation is cleaned with distilled water, uses the HCl drip washing 100-150mL of 6mol/L then, and is with distilled water that the HCl flush away is extremely neutral, uses the HNO of 3mol/L again
3Drip washing 100-150mL, with distilled water with HNO
3Flush away is to neutral.Repeat above-mentioned steps 3 times, flow speed control is at 0.5mL/min.
(2) transition of Dowex-1 resin
With 10% NaOH drip washing, the about 500mL of elution volume maintains about 10% the basicity of resin with above-mentioned treated Dowex-1 resin.
(3) separation of Mo
The Na that will contain 6g Mo
2MoO
4Solution (its basicity maintains about 10%) is gone up the Dowex-1 anion-exchange resin column after transition, uses 10% NaOH drip washing then, flow speed control about 0.5mL/min, its elution volume and content such as table 2.The content of Mo is used metric measurement.
Metric measurement Mo: sample thief is diluted with water to 25mL in the 50mL volumetric flask, adds 2.5mLHNO
3(HNO
3Drip 0.5%KMnO before using
4Solution is to showing stable light red); The KSCN solution and the 2.5mL 10%SnCl that add 5mL 25% again
2Solution shakes up, and is diluted with water to 50mL, places 15min, surveys absorbance in the 430nm place with the 1cm cuvette.
Table 210%NaOH elution volume and Mo content
Last table accumulative total Mo total content is 5.7889g, and the recovery is 96.5%.In order to guarantee that as far as possible the Dowex-1 anion-exchange resin column does not contain Mo, when drip washing 1000mL, absorbance is under 0 the situation, again drip washing 200mL10%NaOH solution.
After 10%NaOH drip washing was intact, with distilled water that the NaOH flush away is extremely neutral, its leacheate absorbance was 0; Use the HCl drip washing 120-150mL of 2mol/L then, its leacheate absorbance is 0; Use the HNO of 3mol/L again
3Drip washing 100-120mL, its leacheate absorbance also is 0; At last with distilled water with HNO
3Flush away to leacheate is neutral, and its leacheate absorbance is 0.HCl leacheate, HNO
3The absorbance of leacheate and distilled water leacheate is 0 all, explains that their leacheate does not contain Mo.In addition, HNO
3Leacheate carries out ICP (inductively coupled plasma) after treatment and analyzes (detectability ppm level), its content consistent with blank sample (＜0.1ppm), this shows HNO
3The content that leacheate does not contain Mo or Mo seldom.
Above-mentioned experimental result shows that 10% NaOH solution can be with Na
2MoO
4Fully drip washing is got off, thereby guarantee in drip washing thereafter
99Do not contain Na in the Tc sample
2MoO
4
3)
99Tc
mRecovery test
99Tc
mRecovery test and simulation Mo target in the separation test of Mo identical, unique different be at Na
2MoO
4The Na that adds 7.5mCi on the solution before the anion-exchange column
2 99Tc
mO
4Upper prop again behind the solution.
In the detachment process of simulation Mo target, NaOH, the HCl of 2mol/L and the HNO of 3mol/L through 10%
3After the drip washing, leacheate does not detect radioactivity, this explanation:
(1) 10% NaOH can not be with Na
2 99Tc
mO
4Drip washing is got off;
(2) HCl of 2mol/L can not be with Na
2 99Tc
mO
4Drip washing is got off;
(3) HNO of 3mol/L
3Can not be with Na
2 99Tc
mO
4Drip washing is got off.
Need to prove the HNO of 3mol/L especially
3Generally can the drip washing from the anion-exchange column of most metal example be got off, here earlier with the HNO of low concentration
3The HNO of high concentration is used in (3mol/L) drip washing again
3(7.5mol/L) drip washing Na
2 99Tc
mO
4Thereby, the HNO of assurance high concentration
3Do not contain other metal example in the leacheate, obtain highly purified Tc.
At HNO with 3mol/L
3After drip washing is intact, use the HNO of 7.5mol/L instead
3Drip washing 60-100mL is until Na
2 99Tc
mO
4Drip washing is got off fully.Use the Na of 7.5mCi simultaneously
2 99Tc
mO
4Make object of reference, calculate
99Tc
mThe recovery, its recovery＞99%.
4. the separation of irradiation Mo target
The dissolving of irradiation Mo target with separate fully with to simulate the Mo target the same.
1) dissolving of irradiation Mo target
Heavy 122.9g before No. 1 target dissolving, the heavy 119.6g in dissolving back, meltage is 3.3g; Heavy 119.0g before No. 2 target dissolvings, the heavy 116.2g in dissolving back, meltage is 2.8g, merges lysate, contains Mo 6.1g, the about 40mL of volume, control solution basicity is about 10%.
2) separation of irradiation Mo target
With the Dowex-1 anion-exchange resin column after transition on the above-mentioned merging lysate, use 10% NaOH drip washing then, flow speed control is about 0.5mL/min, and the NaOH elution volume is 1200mL; Then with the drip washing of about 100mL distilled water; Use the HCl drip washing of 150mL 2mol/L again; Then use the HNO of 120mL 3mol/L again
3Drip washing; Use the HNO of 7.5mol/L at last
3Drip washing 100mL is contained
98The Na of Tc
2TcO
4Solution.
Contain
98The Na of Tc
2TcO
4Solution evaporation is removed HNO
3After, add 2～3 HCl again and remove remaining HNO
3, add the 2mL dissolved in distilled water at last, contained
98The Na of Tc
2TcO
4Solution.The solution that takes a morsel is processed the source, surveys gamma spectrum; Analyze the isotopics of technetium with inductively coupled plasma mass spectrometry meter (ICP-MS).Each isotopic abundance composition of technetium sees that table 3, the content of Tc are 5.5 μ g, and its gamma spectrum is as depicted in figs. 1 and 2.
The isotopic abundance of table 3 technetium is formed
Claims (9)
1. new radioactive nuclide of producing
98T
CMethod, it is characterized in that mainly comprising following process:
(1) Mo target preparation: with the dimensioned Mo target sheet of Mo plate according to the accelerator target holder;
(2) Mo target irradiation: with d nuclear (
2H) irradiation bombardment Mo target, placement is no less than 270 days entering dissolution process behind the irradiation;
(3) irradiation Mo target dissolving: use commercially available H
2O
2Dissolving irradiation Mo target, H
2O
2Consumption by 2.5～5.0mL/gMo, fully the dissolving back adds the NaOH of weight concentration 9.5～10.5%, with Mo, the T after the dissolving
CConvert Na to
2MoO
4And Na
2T
CO
4, the consumption of NaOH is by 5.0～8.0mL/gMo, and the basicity of solution maintains 9.5～10.5%;
(4) Mo with
98Tc separates: contain
98T
CNa
2MoO
4Dowex-1 anion-exchange resin column on the solution, the Mo content in NaOH drip washing to the leacheate of use weight concentration 9.5～10.5% is zero, removes NaOH with distilled water drip washing; Using 10.0～12.5 times of exchange column volumes, concentration afterwards respectively is the HCl drip washing of 1.5～2.5mol/L, and 8.0～10.0 times of exchange column volumes, concentration are the HNO of 2～3mol/L
3Drip washing; The HNO that to use 5.0～8.0 times of concentration of exchange column volume at last be 7.0～8.0mol/L
3Drip washing is contained
98The Na of Tc
2TcO
4Solution.
2. the radioactive nuclide of producing according to claim 1
98T
CMethod, it is characterized in that containing
98The Na of Tc
2TcO
4The solution heating evaporation is removed HNO
3, remove remaining HNO with HCl more afterwards
3, add dissolved in distilled water at last, obtain the Na of 0.1～0.2 times of exchange column volume
2 98TcO
4Solution.
3. the radioactive nuclide of producing according to claim 2
98T
CMethod, it is characterized in that said Dowex-1 anion-exchange resin column is the Dowex-1 anion-exchange resin column after handling through transition, said processing transition is behind anion-exchange column on the Dowex-1 resin, uses distilled water, HCl, distilled water, HNO successively
3, distilled water drip washing, use the NaOH drip washing of weight concentration 9.5～10.5% afterwards again, make the basicity of resin maintain 9.5～10.5%.
4. the radioactive nuclide of producing according to claim 3
98T
CMethod, it is characterized in that the Dowex-1 resin is for through cleaning, oven dry, grinding and screening is handled particle diameter at 80～120 purpose Dowex-1 resins.
5. the radioactive nuclide of producing according to claim 2
98T
CMethod, it is characterized in that on the Dowex-1 resin using HCl, distilled water, HNO successively behind the anion-exchange column
3, the distilled water cycling elution, cycle index is no less than 3 times, and the distilled water drip washing in the cycling elution, it is neutral that drip washing to leacheate is.
6. the radioactive nuclide of producing according to claim 5
98T
CMethod, it is characterized in that using successively HCl, distilled water, HNO
3, distilled water carries out cycling elution, rate of flow in rinse is controlled at 0.4～0.6mL/min.
7. according to the described radioactive nuclide of producing of one of claim 1 to 6
98T
CMethod, it is characterized in that irradiation Mo target uses commercially available H
2O
2At least dissolve H 2 times
2O
2Each consumption is 0.5～1.0mL/gMo, and total consumption is 2.5～5.0mL/gMo.
8. according to the described radioactive nuclide of producing of one of claim 1 to 6
98T
CMethod, it is characterized in that the Dowex-1 anion-exchange resin column is with the NaOH drip washing of weight concentration 9.5～10.5% on the irradiation Mo target solution, its rate of flow in rinse is controlled at 0.4～0.6mL/min.
9. the radioactive nuclide of producing according to claim 7
98T
CMethod, it is characterized in that the Dowex-1 anion-exchange resin column is with the NaOH drip washing of weight concentration 9.5～10.5% on the irradiation Mo target solution, its rate of flow in rinse is controlled at 0.4～0.6mL/min.
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| KR20140050597A (en) * | 2011-04-10 | 2014-04-29 | 더 거버너스 오브 더 유니버시티 오브 앨버타 | Production of technetium from a molybdenum metal target |
| DE102011002265B4 (en) * | 2011-04-26 | 2012-12-06 | Technische Universität München | Process for the preparation of starting material for a technetium generator |
| EP4216680A1 (en) * | 2012-04-27 | 2023-07-26 | Triumf Inc. | Processes, systems, and apparatus for cyclotron production of technetium-99m |
| BR112017014717B1 (en) * | 2015-02-09 | 2022-05-31 | Framatome Gmbh | Radionuclide generation system |
| CN110335697B (en) * | 2019-07-11 | 2020-09-29 | 四川大学 | A kind of preparation method of high abundance 98Tc |
| EP3828899B1 (en) * | 2019-11-29 | 2022-01-05 | Ion Beam Applications | A method for producing ac-225 from ra-226 |
| CN111482452B (en) * | 2020-04-03 | 2022-05-10 | 武汉工程大学 | Gradient leaching technology for residual leaching agent of weathering crust leaching type rare earth ore |
| CN111621645A (en) * | 2020-06-09 | 2020-09-04 | 西安迈斯拓扑科技有限公司 | Irradiation from accelerator100Mo production99mRecovery from Tc process effluent100Method for Mo |
| CN113173595B (en) * | 2021-03-30 | 2023-09-15 | 广东回旋医药科技股份有限公司 | Cyclotron preparation 68 Purification method of Ga crude product |
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| US5729821A (en) * | 1996-12-10 | 1998-03-17 | Lockheed Martin Energy Research Coirporation | Concentration of perrhenate and pertechnetate solutions |
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