CN1312117A - Pd-103 seed medicine and its prepn - Google Patents
Pd-103 seed medicine and its prepn Download PDFInfo
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- CN1312117A CN1312117A CN 01105243 CN01105243A CN1312117A CN 1312117 A CN1312117 A CN 1312117A CN 01105243 CN01105243 CN 01105243 CN 01105243 A CN01105243 A CN 01105243A CN 1312117 A CN1312117 A CN 1312117A
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Abstract
The present invention relates to a seed preparation technology of palladium-103, including preparation of rhodium target, solvation of rhodium target, separation of rhodium and palladium, chemical plating and solder-sealing particle with palladium-103 in titanium tube; firstly, electroplating a layer of alloy on the target holder; using alternating current to electrolyze rhodium and palladium; using Dowex 1X8 chlorine anion-exchange resin, hydrochloric acid and ammonia and ammonium chloride mixed shower washing agent to separate rhodium and palladium; its chemical plating technology uses ammonia, ammonium chloride and sodium hypothosphite as main components of plating liquor and uses silver and copper or gold as carrier. Said invention also provides a palladium-103 seed medicine and a metal rod cover-coated with palladium-103 and solder-sealed in titanium tube.
Description
The present invention relates to radiopharmaceutical that is used for interventional therapy and preparation method thereof, be specifically related to Pd-103 seed medicine and preparation method thereof.
Close-range treatment is pressed close to medical radionuclide exactly or is implanted canceration position, a kind of therapy of kill cancer cell.Its advantage is: radioactive dosage concentrates on cancerous issue, and surrounding tissue is subjected to less or avoids radiation.It is divided into temporary implantation and permanent implanted two kinds of methods.Permanent implanted is that permanent the planting in the canceration position of used radioactive source do not taken out, and temporary implantation radioactive source implantation certain hour needs to take out.The nucleic that close-range treatment is commonly used has Ir-192, Au-198, Y-169, Pd-103 and I-125 etc.Pd-103 and I-125 are used for permanent implanted.
Many documents have been made report extensively and profoundly to the curative effect that Pd-103 and I-125 are used for treatment of solid tumors such as carcinoma of prostate.Ling et al. uses linear quaternary model to compare the curative effect of I-125 and Pd-103 on the radiobiological basis of theory, conclusion is: on the basis of clinical practice dosage, Pd-103 breeds rapidly to killing that the tumor cell effect is better than I-125, and I-125 preponderates in the slower tumor of treatment propagation.The animal experiment of Nag et al. studies show that simultaneously: the carcinoma of Pd-103 treatment differentiation is more effective.Therefore based on above-mentioned and other some achievements in research, I-125 is commonly used to treat early stage tumor (Gleason score 2-6) and Pd-103 is expected to be used for middle and advanced stage tumor (Gleason score＞6).
The production of nucleic Pd-103 has two kinds of methods: reactor production and accelerator production.Reactor is produced palladium-103 and had many deficiencies: Pd-103 is by producing with the long-pending target of the richness of neutron bombardment Pd-102 in nuclear reactor, therefore not resembling accelerator can produce DNAcarrier free Pd-103, nuclear reactor production contains other palladium isotope material nucleic, as Pd-102, Pd-109, Pd-111 etc.; The ratio degree of Pd-103 is regulated difficulty; There is the X ray that has shielded Pd-103 mental retardation in a large amount of stable palladiums.Therefore producing Pd-103 with accelerator is the effective way that obtains medical Pd-103.
The technology that accelerator is produced Pd-103 has a lot of documents once to carry out reporting (W.M.Garrison, J.L.Hamilton, U.S.atomic Energy Commission, UCRL-1067 (1950) etc.), that the most successful is preparation method (John L.Carden, Jr, the Tucker of John L.Carden, Ga.U.S.A.Patent.1995,5405309.).Its preparation method divides two parts:
(1) preparation of carrier-free palladium-103: the metal rhodium about 2 grams is electroplated onto on (copper) target holder, as the target of preparation palladium-103.With the charged ion bombardment rhodium target of suitable energy, the size of energy will be controlled at palladium-103 generation and not have other palladium nucleic generations.The rhodium target of irradiation at its surperficial mechanical punching, is coated the corrosive material of anti-nitric acid then on target holder.With nitric acid (copper) target, remove the rhodium target through hole portion etching off rhodium target low layer.Rhodium target water flushing back was fused under 700 ℃ 90 minutes with 30 gram sodium bisulfate.Treat that fused mass cooling back adds the hydrochloric acid of 20ml 1M, stir, make its dissolving, filter.In filtrate, add the silver nitrate of a certain amount of Palladous chloride. and a small amount of 0.1M, filter.
Realize separating of palladium-103 and rhodium with the ion exchange column chromatography method.Ion exchange resin is the cl anion resin, and volume is 30ml.Eluent is respectively: 0.03M HCl, 4M HCl and strong aqua ammonia.Obtain the ammonia solution of the palladium-103 of carrier-free adding at last.
(2) seed preparation: adding additive ammonium chloride and nicotiamide in above-mentioned leacheate, is 0.875mm with the direct current electrode position technology of routine in length, and diameter is plating one deck palladium-103 and a palladic coating on the high purity graphite granule of 0.575mm.Its activity can be regulated between 0.5mCi and 300mCi.With ASTMB265-78, the secondary titanium is 0.7mm for the material internal diameter, and 4.425mm is long, the titanium pipe of wall thickness 0.05mm.Make the cup end-blocking of titanium pipe with same standard.With two graphite granules and lead rod (lead rod places between the graphite granule) the titanium pipe of packing into, two cup end-blockings get up with laser and titanium sealing of tube, make seed.Its structure as shown in Figure 1.
This method and corresponding seed preparation technology have been applied to commercially produce, but still have very big defective.Key issue in the preparation of carrier-free palladium-103 and seed does not solve.The weak point of its invention is:
(1) conventional scorification method is adopted in the dissolving of rhodium target.The non-rhodium of putting of scorification method dissolving is practical, but for radioactive rhodium target, high-temperature melting easily causes the radioactivity volatilization, and Producer and environment are worked the mischief, and fuses simultaneously to be unfavorable for automation mechanized operation.
(2) adopt mechanical punching, nitric acid corroding method that the rhodium target is taken off from the copper holder, lost a part of palladium-103.
(3) separation of palladium-103-rhodium employing strong aqua ammonia is an eluent, and elution efficiency is low, and specific activity is low.
(4) seed inside is that three parts constitute, complicated process of preparation, and the each several part of packing into by hand is easy to make mistakes, and influences the yield rate of seed.
(5) with electroplating technology palladium plating-103 on carbon rod of routine,, make the distributing homogeneity of palladium-103 relatively poor, distribute thereby influence its dosage field because carbon rod out-of-flatness in surface own and electroplating current stability are difficult to control.
The preparation method that the purpose of this invention is to provide a kind of new Pd-103 seed medicine, prepare key technical problem in the carrier-free palladium-103 to solve accelerator, improve the technology of preparing of seed, for the preparation of Pd-103 seed provides cover method effectively, reliably and easily.
The present invention provides a kind of Pd-103 seed medicine simultaneously.
The preparation method that Pd-103 seed medicine is new is realized by the following step:
(1) (for example: molybdenum tungsten etc.) goes up plating one deck alloy at target holder (copper).
(2) with electroplating technology rhodium plating target on the molybdenum and tungsten alloy layer of routine, the wide 10mm of rhodium target, 100mm is long, and 5mm is thick.
(3) with the proton of 10Mev-22Mev, with the rhodium target be six degree angles bombardment rhodium targets, beam intensity is 200 μ A-400 μ A.Wherein the palladium-103 that produces with the proton bombardment of 17Mev, beam intensity 200 μ A is maximum.
(4) with alternating current power supply electrolysis rhodium target, electrolyte is the hydrochloric acid of 6M, and electric current density is 0.4-1.0A/cm
2With 0.5A/cm
2Be the best, fragment rate has only 3%.
(5) add an amount of Palladous chloride. in the solution after electrolysis, to regulate the specific activity of palladium-103.The amount of Palladous chloride. is decided according to prepared seed amount, the amount of every added Palladous chloride. carrier of seed at 5 μ g between the 500 μ g.Filter electrolyte.
The Palladous chloride. addition should have the plating speed of the chemical plating utilized, the uniformity of coating, the uniformity of intergranular dosage, is unlikely to too thick again, too much absorbs the low energy X ray that palladium-103 decay is emitted.The effect of Palladous chloride. shows as: can reduce the loss of radioactive palladium-103 in separation process as carrier; Quicken the molecular plating of palladium-103; Make palladium-103 even in the surperficial plating of silver rod, a bonding seed dosage field distribution evenly; Make intergranular plating dosage even.
(6) with ion exchange column chromatography method separate palladium-103.Ion exchange resin is Dowex (Cl
-) 1 * 8 anion exchange resin.The high 10cm of ion exchange column, internal diameter 1.5cm.Electrolyte is added ion exchange column.With 0.03M HCl, 8M HCl and NH
4Cl+NH
3(1: 1) is eluent drip washing successively, obtains uclear purity at last and be 98.5% palladium-103 ammonia solution.
(7) molecular plating is a mother solution with above-mentioned palladic ammonia solution, add ammonia and ammonium chloride and stablize plating bath, and with the hypophosphites Reducing agent, chemical palladium-plating on goldc grains, silver granuel or shot copper.The length of silver granuel or shot copper is 3mm, and diameter is 0.5mm.
(8) the titanium pipe that adopts Britain GOOGFELLOW company to provide is provided seed: the external diameter of pipe: 0.51mm.Internal diameter: 0.35mm.Wall thickness: 0.08mm.Purity: 99.6%.Length: 4.8mm.Will be through the silver (copper, gold) of the molecular plating grain titanium pipe of packing into, with laser welding technology sealing two ends.The profile of seed is seen Fig. 2.
The positive progressive effect of patent of the present invention is as follows:
(1) (for example: molybdenum tungsten etc.), when electrolysis rhodium target, can play the protection target holder and not be corroded on target holder, electroplates one deck alloy.Solve the target that accelerator prepares palladium-103 and prepared problem.
(2) avoided important disadvantages such as high-temperature melting method radioactivity volatilization with electrolysis tech electrolysis rhodium target, electrolysis tech can be realized automation mechanized operation simultaneously, and fragment rate is low under suitable electric current density condition, the response rate height of palladium-103.Electrolysis tech has solved accelerator and has prepared palladium-103 rhodium target indissoluble problem.
(3) ion exchange column chromatography method separate rhodium palladium: with ammonium chloride and ammonia as eluent elution efficiency height (95%), and volume ratio activity height, 75% the palladium-103 of having an appointment in the leacheate of first 10ml drenches, and the eluent of 50ml can drench 95% palladium-103.Conventional extraction extraction efficiency low (three extractions only can extract 66.6% palladium-103).John L.Carden is that the elution efficiency of eluent 100ml is about about 70% with the strong aqua ammonia, and first 10ml only can drench the palladium-103 about 30%.
(4) ammonia and ammonium chloride are the composition of molecular plating plating bath, need not to remove.Only need activity, adjust its specific activity and get final product according to the palladium that will plate-103.
(5) adopt chemical plating plating palladium-103 method on silver (copper) rod simple, the response rate height of palladium-103.Intergranular activity is even, seed yield rate height, and chemical plating has unique selectivity to palladium, and other radionuclide impurity of trace can not advance the palladium layer with palladium one plating in the plating bath, i.e. Zhi Bei nucleus of the seed purity height.
(6) seed inside be one long for 3mm, diameter is silver (copper) rod of 0.5mm, it is that the carrier of palladium-103 can be detected by X ray again.The internal structure of seed has three original parts only to change some into, has simplified the preparation technology of seed.
Further specify the present invention below in conjunction with drawings and Examples.
Fig. 1 is existing Pd-103 seed section of structure.
Fig. 2 is a Pd-103 seed section of structure of the present invention.
1-titanium tube wall 2-top seal
3-palladium-103 graphite carrier 4-lead rod
Silver (copper) carrier of 5-titanium shell 6-palladium-103
(1) rhodium target preparation
(for example: molybdenum tungsten etc.), thickness is 20mm to plate one deck alloy in the copper holder.The rhodium layer of plating thick 10mm, wide 10mm, long 100mm is made target on alloy-layer.Rhodium plating target electroplate liquid is formed: sulfamic acid rhodium (2-4g/L); Sulfamic acid (20-30g/L); Copper sulfate (600mg/L); Plumbi nitras (500mg/L); Temperature 35-55 ℃; Cathode-current density 0.5-1A/d
2M; Anode material: platinum filament or plate.The content of rhodium should be controlled at about 2-4g/L, if be lower than 2g/L, the tarnish of coating gray.As chelating agent, its content should not be lower than 20g/L to sulfamic acid in plating bath.It can increase cathodic polarization, makes that coating is careful, smooth, flawless.During too high levels, then cathode efficiency descends, and macula lutea or vaporific in vain appears in coating, and content is crossed when hanging down, and then coating is coarse.Copper sulfate is brightener, can make the coating crystallization careful, level and smooth, bright.Its consumption maximum is no more than 0.8g/L.Otherwise crackle appears in the coating embrittlement.Temperature generally is controlled at about 40 ℃, is lower than 20 ℃, and coating is brightless.Electric current density generally is controlled at 0.5-1A/d
2Between the m.Electric current density is too low, the coating tarnish.
With the proton stream bombardment rhodium target of 17MeV, 200 μ A, proton beam and rhodium target are six degree angles.With the cooling of the target after the bombardment two days.
(2) rhodium target dissolving and with the separating of palladium-103
Target is placed electrolysis unit, the rhodium target is contacted with electrolyte.Electrolyte is the hydrochloric acid of 6M, and electric current density is 0.5A/cm
2, electrolysis up to the dissolving of rhodium target fully.
Add an amount of Palladous chloride. and silver nitrate in electrolyte, vibration is filtered.The high 10cm of ion exchange column fills Dowex 1 * 8 (Cl in the internal diameter 1.5cm, post
-) anion exchange resin, resin 6M salt acid pre-pickling.Filtrate is added ion exchange column.The lessivation of ion exchange column is: 0.03M hydrochloric acid 100ml drip washing, and flow velocity is 4ml/min.;
8M hydrochloric acid drip washing 100ml, flow velocity is the same;
Residual hydrochloric acid in the post is removed in deionized water 30ml drip washing;
With the mixing eluent drip washing of ammonium chloride and ammonia (1: 1), flow velocity is the same, drip washing 50ml.
(3) molecular plating prepares 3mm length, and diameter is the silver granuel of 0.5mm.Regulating the specific activity of leacheate, is main component preparation plating bath with ammonia, ammonium chloride and sodium hypophosphite, and the pH value of plating bath is 10.Molecular plating is about 1 hour under 35 ℃ of temperature.
(4) the seed preparation will be plated good silver (copper) grain and be used washing with acetone, dry up.In the titanium pipe with the long 4.8mm that packs into, with laser with the two ends sealing.
Claims (10)
1. the seed technology of preparing of a palladium-103 comprises the preparation of rhodium target; The dissolving of rhodium target; The palladic separation of rhodium; Particulate chemical plating; The granule of band palladium-103 is welded in the titanium pipe; It is characterized in that with Dowex1 * 8 cl anion exchanger resins be the isolating exchanger resin of ion exchange column chromatography; With hydrochloric acid and ammonia and ammonium chloride mixing eluent respectively as rhodium and palladic eluent.
2. the seed technology of preparing of a palladium-103 comprises the preparation of rhodium target; The dissolving of rhodium target; The palladic separation of rhodium; Particulate chemical plating; The granule of band palladium-103 is welded in the titanium pipe; It is characterized in that on target holder, electroplating one deck alloy before the rhodium plating palladium.
3. according to the seed technology of preparing of claim 2, it is characterized in that alloy is a molybdenum and tungsten alloy.
4. according to the seed technology of preparing of claim 2, wherein use alternating current electrolysis rhodium palladium.
5. according to the seed technology of preparing of claim 4, wherein electric current density is 0.4A/cm
2To 1.0A/cm
2
6. according to the seed technology of preparing of claim 5, wherein electric current density is 0.5A/cm
2
7. according to the seed technology of preparing of claim 2, wherein the palladium rhodium separates the separation method that adopts in the claim 1 seed technology of preparing, is the isolating exchanger resin of ion exchange column chromatography with Dowex 1 * 8 cl anion exchanger resin; With hydrochloric acid and ammonia and ammonium chloride mixing eluent respectively as rhodium and palladic eluent.
8. according to the seed technology of preparing of claim 2, it is characterized in that chemical plating is the carrier of palladium-103 with silver, copper or gold; With electroless plating technology plating palladium-103; Electroless plating technology is main solution composition with ammonia, ammonium chloride and sodium hypophosphite.
9. Pd-103 seed medicine is characterized in that the metal bar of a plating palladium-103 of the inner sealing of titanium pipe.
10. according to the seed medicine of right 9, wherein metal bar refers to silver, copper, goldc grains.
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|---|---|---|---|
| CNB011052430A CN1169581C (en) | 2001-01-18 | 2001-01-18 | Pd-103 seed medicine and its prepn |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNB011052430A CN1169581C (en) | 2001-01-18 | 2001-01-18 | Pd-103 seed medicine and its prepn |
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| CN1312117A true CN1312117A (en) | 2001-09-12 |
| CN1169581C CN1169581C (en) | 2004-10-06 |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101880873A (en) * | 2010-06-30 | 2010-11-10 | 中国原子能科学研究院 | 103Preparation process of Pd sealed seed source core |
| CN102382994A (en) * | 2011-07-18 | 2012-03-21 | 原子高科股份有限公司 | Radioactivity68Preparation method of Ge solution |
| CN105152948A (en) * | 2015-10-08 | 2015-12-16 | 宝健（北京）生物技术有限公司 | Technology for preparing gamma-aminobutyric acid from quinoa |
| CN117059296A (en) * | 2023-09-27 | 2023-11-14 | 原子高科股份有限公司 | Preparation method and application of palladium-103 |
-
2001
- 2001-01-18 CN CNB011052430A patent/CN1169581C/en not_active Expired - Fee Related
Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101880873A (en) * | 2010-06-30 | 2010-11-10 | 中国原子能科学研究院 | 103Preparation process of Pd sealed seed source core |
| CN101880873B (en) * | 2010-06-30 | 2011-12-07 | 原子高科股份有限公司 | Preparation process of 103Pd sealed seed source core |
| CN102382994A (en) * | 2011-07-18 | 2012-03-21 | 原子高科股份有限公司 | Radioactivity68Preparation method of Ge solution |
| CN102382994B (en) * | 2011-07-18 | 2013-08-14 | 原子高科股份有限公司 | Radioactivity68Preparation method of Ge solution |
| CN105152948A (en) * | 2015-10-08 | 2015-12-16 | 宝健（北京）生物技术有限公司 | Technology for preparing gamma-aminobutyric acid from quinoa |
| CN117059296A (en) * | 2023-09-27 | 2023-11-14 | 原子高科股份有限公司 | Preparation method and application of palladium-103 |
| CN117059296B (en) * | 2023-09-27 | 2024-02-06 | 原子高科股份有限公司 | Preparation method and application of palladium-103 |
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| Publication number | Publication date |
|---|---|
| CN1169581C (en) | 2004-10-06 |
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