US3914372A - Process for the preparation of labelled compounds - Google Patents

Process for the preparation of labelled compounds Download PDF

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Publication number
US3914372A
US3914372A US309030A US30903072A US3914372A US 3914372 A US3914372 A US 3914372A US 309030 A US309030 A US 309030A US 30903072 A US30903072 A US 30903072A US 3914372 A US3914372 A US 3914372A
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Prior art keywords
vial
tritium
gas
labelled
adsorbent
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US309030A
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English (en)
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Masaru Takagi
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Sinloihi Co Ltd
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Sinloihi Co Ltd
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Priority claimed from JP46094895A external-priority patent/JPS5122595B2/ja
Priority claimed from JP46098302A external-priority patent/JPS5128800B2/ja
Priority claimed from JP9799572A external-priority patent/JPS5112798B2/ja
Priority claimed from JP47097994A external-priority patent/JPS4955560A/ja
Priority claimed from JP9861672A external-priority patent/JPS4961593A/ja
Application filed by Sinloihi Co Ltd filed Critical Sinloihi Co Ltd
Priority to US05/577,130 priority Critical patent/US3986835A/en
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B08—CLEANING
    • B08B—CLEANING IN GENERAL; PREVENTION OF FOULING IN GENERAL
    • B08B15/00—Preventing escape of dirt or fumes from the area where they are produced; Collecting or removing dirt or fumes from that area
    • B08B15/02—Preventing escape of dirt or fumes from the area where they are produced; Collecting or removing dirt or fumes from that area using chambers or hoods covering the area
    • B08B15/023—Fume cabinets or cupboards, e.g. for laboratories
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/001—Decontamination of contaminated objects, apparatus, clothes, food; Preventing contamination thereof
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/50—Improvements relating to the production of bulk chemicals
    • Y02P20/582—Recycling of unreacted starting or intermediate materials

Definitions

  • a labelled compound is obtained by adsorbing and releasing a gaseous radioisotope under vacuum in a reaction system incorporated with vials containing adsorbents thereby to bring said gas into contact with a compound to be labelled and to recover the gas remaining in the system by ad sorbents or reacting agents, and removing a vial of products and a recovery vial of unreacted gases by sealing under vacuum.
  • the gaseous radioisotope used in said preparation of the labelled compound is itemized by applying the principle of adsorption and release and the removal by sealunder vacuum mentioned above to capillary apparatus connected with said gas ampoule and a plural of recovery vials.
  • FIG.I3 Flam U.S. Patent 0a. 21, 1975 Sheet 5 of5 3,914,372
  • the present invention relates to the preparation of a labelled compound and to the manipulation of a gaseous radioisotope in a double-sealed state.
  • Glass apparatus are used in general for sealing hermetically gaseous radioisotopes.
  • the conventional hoods the human body and environments would undoubtedly be contaminated by the leaking gaseous radioisotopes on breakdown of the glass apparatus. Accordingly, it is required that gaseous radioisotopes can be manipulated with use of an apparatus systern sealed under vacuum and also such an apparatus system can be handled in a hood sealed'hermetically.
  • Labelled compounds are extensively being utilized as a tracer in the various fields such as physics and chemistry, medical science, biology, pharmacology, biochemistry, and industries.
  • a gas exposure method includes enclosing a compound to be labelled and tritium gas within a container, allowing them to stand for a desired time and thereafter recovering tritium gas and producing a labelled compound.
  • improvements of the gas exposure method such as an electric discharge method, catalytic method, irradiation method of ultraviolet ray, and radiation method, and a ctalytic reduction method. It is well known that apparatus provided with Toeplers pump have hitherto been used for realizing these methods. However, such the prior art have the following disadvantages:
  • the attached instruments such as vacuum pump and exhaust pipes are contaminated by tritium.
  • a large-sized waste contaminated with tritium, such as disused apparatus, vacuum pump and other attached devices is generated.
  • the conventional method requires a large-sized hood because the appparatus to be used becomes large-sized.
  • tritium gas to be used as the preparation material of labelled compounds is economically advantageous to be purchased in an ampoule with large quantities.
  • tritium gas is manipulated in the form of several or several tens ampoules with small quantities separately. Therefore it is necessary to itemize the large quantities of tritium gas to the ampoules with small quantities.
  • the apparatus with the Toeplers pump have hitherto been utilized for the itemizing operation.
  • the method using such conventional apparatus has the disadvantages as in l) to 8) mentioned hereinbefore.
  • a treatment apparatus having high efficiency must be provided with to satisfy these systems.
  • such apparatus are difficult to set up or become large-sized and expensive.
  • the treatment apparatus having low efficiency when an accident happens, there is danger of the radioisotope gas with high concentration being diffused or scattered, as it is untreated, in and out of the laboratories. This is quite unsafe and therefore prohibited by laws.
  • the exhaust gas below tolerance limits must be discharged.
  • the gaseous radioisotope manipulating apparatus are usually operated in the glove box, hoods or drafts while ventilating the chamber directly or through treatment apparatus.
  • powdered substances often are scattered by the air pressure due to flowing of the gases.
  • Such substances therefore must be manipulated without operating the ventilation equipment.
  • weighing by even balance is effected without operating the ventilation equipment.
  • this is sometimes accompanied by a very dangerous aspect because the radioisotopes are gradually accumulated.
  • a main object of the present invention is to provide a system wherein gaseous radioisotopes can be safely manipulated with use of apparatus hermetically sealed under vacuum and particularly a double-closed system wherein such sealed apparatus can be also handled in a sealed chamber for increased safety.
  • Another object of the present invention is to provide a process for preparing safely and simply labelled compounds and apparatus to be used in carring out the same, which are applicable to the gas exposure method and its improvements such as electric discharge method, catalytic method, irradiation method of ultraviolet ray and radiation method or the catalytic reduction method, thereby overcoming all of the disadvantages of the prior art.
  • Another object of the present invention is to provide a method for itemizing safely and simply a definite amount of gaseous radioisotopes.
  • Still another object of the present invention is to provide a closed system for handling a gaseous radioisotope manipulating apparatus in a closed state and discharging gases below tolerance limits to the outdoors.
  • An aspect of the present invention is directed to a process for the preparation of a labelled compound which comprises communicating a vial containing a compound to be labelled with an adsorbent containing vial through a glass tube, said two vials each being provided with at least one opening for connection, or providing a vial containing a mixture of the compound to be labelled and adsorbent with openings for connection, breaking in vacuum an ampoule of gaseous radioisotope connected to any one of the openings of the said vials to diffuse the gaseous radioisotope into a confined zone, adsorbing the diffused gas by the adsorbent under cooling, removing the said ampoule by melt-sealing, thereafter releasing the adsorbed gas by allowing the adsorbent to stand at room temperature or at an elevated temperature to bring the said gas into contact with the compound to be labelled thereby to obtain the labelled compound, recovering then the gas remaining in the confined zone by again cooling the
  • the present invention includes the steps of providing an adsorbent or. reacting agent containing vial for recovering the said gas separately, recovering the gas remaining in the confined zone by cooling or heating the said adsorbent or reacting agent and then removing the recovery vial by melt-sealing.
  • the present invention may preferably include the step of communicating under vacuum a vial of a cleaning solvent with the labelled compound containing vial, establishing a temperature difference between these two vials to transfer the cleaning solvent thereby separating the labelled compound from unstable gaseous radioisotopes.
  • the catalytic reduction method includes steps of connecting a reaction vial containing compounds to be labelled and optionally a catalyst and solvent, a vial containing adsorbent for recovery of hydrogen, a vial containing adsorbent for recovery of tritium, a hydrogen gas ampoule and a tritium gas ampoule respectively to a glass tube, said vials and ampoules each being provided with at least one opening for connection and connected to the glass tube in such a way that one of said openings of the vials and ampoules each is communicated with the glass tube, breaking in vacuum said tritium gas ampoule to diffuse tritium gas into a confined zone, adsorbing the diffused gas by the adsorbent for tritium under cooling, removing the tritium gas ampoule by melt-sealing, thereafter releasing the adsorbed gas by allowing the adsorbent for tritium to stand at room temperature or an elevated temperature to bring the compounds to be labelled into catalytic reduction
  • the catalytic reduction method of the present invention is carried out by communicating in vacuum a solvent containing vial provided with a filter for recovery of the labelled compounds with the reaction vial, cooling the reaction vial to clean it with the solvent, and recovering the labelled compounds by the vial under cooling while removing the catalyst with the filter.
  • Apparatus to be used for conveniently carrying out the process according to the present invention comprises a combination of i) a vial of a cleaning solvent provided with openings for connection, ii) a vial of an adsorbent provided with openings for connection and a vial of a compound to be labelled provided with openings for connection, said two vials being communicated with each other by a glass tube, or a vial of a mixture of an adsorbent and compound to be labelled provided with openings for connection, and iii) another vial of an adsorbent or reacting agent provided with connecting openings for recovery of a gaseous ratioisotope.
  • These vials or apparatus are combined and connected with one another conveniently to carry out the process of the present invention.
  • apparatus to be used for earring out the catalytic reduction method according to the present invention comprises a combination of i) a reaction vial of a compound to be labelled and optionally a catalyst and solvent provided with openings for connection, ii) a mercury manometer, iii) a glass tube provided with openings for connection, iv) a vial of an adsorbent provided with connecting openings for recovery of tritium gas, v)a vial of an adsorbent provided with connecting openings for recovery of hydrogen gas, and vi) a vial of a cleaning solvent provided with a filter for recovery of labelled compounds.
  • These vials or apparatus are combined and connected with one another conveniently to carry out the catalytic reduction method according to the present invention.
  • Another aspect of the present invention being the itemizing process of the gaseous radioisotope used for the preparation of the labelled compounds, comprises connecting a radioisotope gas ampoule to an end of a capillary tube, communicating a plural of recovery vials for the radioisotope gas of which capacities may be the same or different respectively with the capillary tube, at least'one of said recovery vials containing an adsorbent, breaking in vacuum said radioisotope gas ampoules to diffuse the gas into a confined zone, adsorbing the diffused gas by cooling said adsorbent,
  • At least one of the plurality of recovery vials for tritium gas sealed in vacuum contains a reacting agent for converting tritium into tritiated water and is connected to the capillary tube in such a way that a breakable seal of the vial faces on the capillary tube.
  • Itemizing is attained by breaking in vacuum a tritium gas ampoule to diffuse the gas into a confined zone, subdividing and recovering the diffused gas depending on the capacities of the recovery vials, removing the recovery vials by melt-sealing separately, thereafter breaking the breakable seal of said reacting agent containing vial, allowing the reacting agent to stand at room temperature or an elevated temperature, and cooling another vial communicated with the bottom of said reacting agent containing vial or any one of said recovery vials as a vial for collecting a reaction product thereby to collect the tritium gas remaining in the zone as tritiated water.
  • a hood for the gaseous radioisotope manipulating apparatus comprises an operation box sealed hermetically under negative pressure containing the gaseous radioisotope manipulating apparatus therein, a ventilation box containing a treatment apparatus therein connected with said operation box, and a ventilation equipment connected with said ventilation box, said treatment apparatus being provided with means for recycling an escaping gaseous radioisotope containing fluid and means for recovering said gas, and said operation box being provided with a door leading to the upper part of the ventilation box.
  • the gaseous radioisotope manipulating apparatus can be handled without ventilating the operating box.
  • FIG. 1 is a schematic view showing the conventional apparatus for preparing labelled compounds with the use of the Toeplers pump.
  • FIGS. 2, 3, 4 and 5 each represents embodiments of apparatus to be used for carring out processes for the preparation of labelled compounds according to the present invention.
  • FIG. 6 represents a vial for cleaning solvents
  • FIG. 7 a vial for recovery of gaseous radioactive isotope
  • FIG. 8 and FIG. 9 either a reaction vial connected with a vial of an adsorbent through a glass tube.
  • the vials set forth in FIG. 6 to FIG. 9 illustrate another embodiment of apparatus to be used in combination for carring out the process according to the present invent1on.
  • FIG. 10 represents a reaction vial of a compound to be labelled
  • FIG. 11 a mercury manometer
  • FIG. 12 a connecting glass tube
  • FIG. 13 a vial of an adsorbent for recovery of tritium gas and hydrogen gas
  • FIG. 14 a-vial of a cleaning solvent, provided with a filter for removal of a catalyst for recovery of labelled compounds.
  • the vials set forth in FIG. 10 to FIG. 14 illustrate another embodiment of apparatus to be used in combination for carrying out the process of the present invention.
  • FIG. 15 represents an embodiment of an apparatus to be used for carring out a process for itemizing a gaseous radioisotope according to the present invention.
  • FIG. 16 represents a modification of the apparatus set forth in FIG. 15.
  • FIG. 17 represents a schematic sectional view of an embodiment of a hood for a gaseous radioisotope manipulating apparatus in a closed state according to the present invention.
  • a labelled compound can be safely and simply obtained by adsorbing and releasing a gaseous radioisotope under vacuum with use of a confined reaction system incorporated with vials containing an adsorbent thereby to bring said gas into contact with a compound to be labelled and to recover the gas remaining in the confined system by an adsorbent or reacting agent, and removing a vial of products and a recovery vial of unreacted radioisotope gas by meltsealing under vacuum.
  • the labelled compound is produced by communicating a vial containing a compound to be labelled provided with openings for connection to a vial containing an adsorbent provided with openings for connection through a glass tube, breaking in vacuum a radioisotope ampoule connected to any one of the openings of said vials to diffuse the gaseous radioisotope into a confined zone, adsorbing the diffused gas by cooling the adsorbent, removing said ampoule by meltsealing, thereafter releasing the adsorbed gas by allowing the adsorbent to stand at room temperature or an elevated temperature to bring said gas into contact with the compound to be labelled thereby to obtain labelled compounds, adsorbing an unreacted gas remaining in the confined zone by again cooling the adsorbent, removing the recovery vial of said gas by meltsealing, and removing the vial containing labelled compounds by melt-sealing.
  • the radioisotope particularly the gaseous radioisotopes exhibit behavior that is not in accordance with common sense in the radiation control.
  • the gaseous radioisotopes have been manipulated in the conventional methods and apparatus without such points being made clear.
  • the way that is at present conceived to be best is to manipulate the radioisotopes in a hermetically sealed apparatus system.
  • the present invention is conveniently practised in the hermetically sealed system.
  • the operation of opening a vial by breaking its breakable seal with a magnet is herein referred to as mere breaking and melt-sealing by a gas burner is referred to as mere melt-sealing".
  • All of vials with openings for connection and connecting tubes used in the present invention are made of glass and the portions heated to a temperature of 480C or more are made of quartz glass. Also, the portions used at a temperature below 480C are preferably made of usual hard glass.
  • the vials or tubes are connected by welding or by air-proof materials such as polyvinylchloride tubes.
  • Shapes and capacities of vials may be properly set up in accordance with the scale to be used.
  • openings for connection of vials and portions to be melt-sealed are glass tubes with outside diameter of 1cm or less and inside diameter of 2mm-5mm.
  • adsorbent used in the present invention examples include an active carbon, silicagel and alumina.
  • gaseous radioisotope is tritium
  • adsorbents such as titanium, zirconium, nickel, palladium, platinum, lithium, sodium, rubidium, cesium, calcium, strontium, erbium and uranium are also used.
  • reacting agents used for recovery of gaseous radioisotopes include copper oxide, platinum oxide and palladium oxide. These reacting agents are in general used to recover tritium as tritiated water which can be reused as the starting material.
  • the gaseous radioisotopes to be used include tritium, argon-3 7, krypton-85, gaseouss labelled compound-C- 14 and gaseous labelled compound S-35.
  • the vial for recovery of tritium is filled with a reacting agent capable of reacting with tritium, such as copper oxide instead of the adsorbent such as the active carbon and furthermore connected in vacuum with another empty vial.
  • a reacting agent capable of reacting with tritium such as copper oxide instead of the adsorbent such as the active carbon
  • tritiated water is produced by connecting the reacting agent containing vial with the adsorbent containing vial, communicating in vacuum said two vials with each other and collecting by said empty vial a reaction product obtained by heating the reacting agent as tritiated water.
  • the recovered tritiated water can be used as the starting material for the labelled compound.
  • another vial for recovery of the gaseous radioisotope is provided in addition to the vial filled with the adsorbent.
  • This is based on the following reason. There is need to reduce the volume of the confined zone as much as possible and increase the reaction gas pressure in order to raise a specific activity of the labelled compound and reaction efficiency. It may, therefore, be proposed to reduce the capacity of the adsorbent filled vial which is a part of the confined zone, but when the adsorbent filled vial is removed by melt-sealing to recover the gaseous radioisotope and stored at room temperature it is inevitable that the vial would be brought under pressure. Accordingly storing such a vial is attended with danger. For this reason it is preferred to provide an adsorbent or reacting agent filled vial for recovery of the gaseous radioisotope in addition to said vial.
  • the vial containing the labelled compound produced by the process of the present invention is communicated in vacuum with a vial containing a cleaning solvent.
  • the labelled compound is separated from unstable gaseous radioisotops by establishing a temperature difference between these two vials to transfer the cleaning solvent.
  • the compounds labelled in the reaction vial are always accompanied by volatile tritium compounds produced by decomposition and unstable tritium. From the point of control of radioactive contamination it is necessary to remove the unstable radioactive substances when the apparatus system is still hermetically sealed. For this reason the reaction vial after completion of reaction is connected to a vial containing a cleaning solvent which has an affinity for tritium.
  • the labelled compound can be safely removed from the system by repeating the heating and cooling to clean sufficiently the reaction vial.
  • the cleaning solvent used for this purpose is preferable one having a low boiling point and dissociative hydrogen, such as water and alcohols.
  • a reaction vial containing compounds to be labelled and optionally a catalyst and solvent, a vial of the adsorbent for recovery of hydrogen, a vial of the adsorbent for recovery of tritium, a hydrogen ampoule and a tritium gas ampoule respective are connected to a glass tube.
  • the vials each are provided with openings for connection and connected to the glass tube in such a way that openings are communicated with it.
  • the compound to be labelled is reacted with tritium and then hydrogen to obtain labelled compounds under a hermetically sealed system. An unreacted tritium and hydrogen each are recovered and separated, and thus the reaction vial containing the labelled compounds is removed by melt-sealing.
  • Toeplers pump 102 for transferring tritium gas is mounted in the center and connected to mercury chamber 104 with a poly-vinylchloride tube.
  • Tritium gas ampoule 101 provided with a magnet capable of breaking its breakable seal is mounted to the right of Toeplers pump, while a reaction vessel 103 with a desirable capacity is connected to the left.
  • Three-way cocks 105 and 108 are connected to the right and to the left respectively to discharge or introduce the air. After all the air is purged from the apparatus, the breakable seal is broken by a magnet to release tritium gas.
  • the gas is, then, transferred to a vial 103 containing a compound to be labelled by operating cock 106 and Toeplers pump 102.
  • a vial 103 containing a compound to be labelled by operating cock 106 and Toeplers pump 102.
  • three way cock 107 and Toeplers pump 102 are operated to transfer tritium gas into a recovery vial 109 which is then melt-sealed.
  • Manometer 110 is to measure tritium gas pressure.
  • the labelled compound is removed by introducing air from cock 108. It is required to effect all the operation mentioned above in a hood with high efficiency.
  • FIG. 2 and FIG. 3 Examples of the apparatus used for carrying out the process of the present invention are illustrated by FIG. 2 and FIG. 3.
  • Via] 1 provided with a breakable seal, containing an adsorbent is connected to vial 2 containing a compound to be labelled through a glass tube and an opening of any one of said two vials is connected with gaseous radioisotopes ampoule 3.
  • the connected portions are indicated in a dotted line.
  • the opening is provided with piece of iron 4 to break a breakable seal of the ampoule 3.
  • FIG. 4 A modification of the apparatus is shown in FIG. 4.
  • Vial 5 provided with openings for connection of a gaseous radioisotope ampoule and vacuum pump, and a breakable seal is filled with a mixture of an adsorbent and compound to be labelled.
  • Vial 1 containing the adsorbent is to recover the gaseous radioisotope.
  • Symbols A, B, C, D, E, F, G, H, I, and J each indicate portions to be melt-sealed.
  • FIG. 5 Examples of the apparatus used for carrying out the catalytic reduction method according to the present invention are illustrated by FIG. 5.
  • Reaction vial 6 containing a compound to be labelled, catalyst and solvent, tritium gas ampoule 9, hydrogen gas ampoule 10, an adsorbent containing vial 7 for recovery of hydrogen gas provided with a breakable seal and an adsorbent containing via] 8 for recovery of tritium gas provided with a breakable seal are connected to glass tube 12 respectively.
  • Mercury manometer 11 is connected to an end of glass tube 12 and a vacuum pump to the other end e.
  • Symbols K, L, M, N, O and P indicate portions to be melt-sealed.
  • Vial 11 provided with openings a and a is one for a cleaning solvent.
  • Vial 12 with openings b and b and a breakable seal provided with openings b and b is one for an adsorbent for recovery of a gaseous radioisotope.
  • vial 13 of a compound to be labelled provided with openings c and c is connected with vial 14 of an adsorbent provided with openings and c through a glass tube.
  • each of vials l3 and 14 is fitted with breakable seals having openings c and 6 Any one of openings 0 and c is connected to a gaseous radioisotope ampoule and the other to a vacuum pump. Vial 12 is to recover finally the unreacted gas remaining in the apparatus while vial 14 is a temporary rest-hous wherein the gas adsorbed once is released.
  • FIG. 9 a modification of the appartus set forth in FIG. 8 is illustrated by FIG. 9 wherein vial 15 of a compound to be labelled provided with openings d d., and d and breakable seals each having openings d, and d are communicated with vial 16 of an adsorbent having openings d through a glass tube.
  • alphabetical capital letters indicate portions to be melt-sealed and alphabetical small letters indicate openings for connecting with a vacuum pump and other vials. These vials or apparatus are connected with one another in a suitable combination to carry out the process of the present invention.
  • FIG. 10 to FIG. 14 examples of apparatus used for carrying out conveniently the catalytic reduction method are set forth in FIG. 10 to FIG. 14.
  • Symbol 17 is a reaction vial for filling a compund to be labelled, catalyst and solvent, symbol 18 a mercury manometer, symbol 19 a connecting glass tube, symbol 20 a vial for filling an adsorbent for recovery of tritium gas (the same vial as this being used for recovery of hydrogen gas), and symbol 22 a recovery vial of a labelled compound containing a solvent, provided with filter for removal of the catalyst.
  • Alphabetical letters indicated in drawings are as defined above.
  • a radioisotope concentration in the working environment is reduced.
  • Radioactive exposure to workers by a radioisotope is reduced.
  • the apparatus used in the present invention are small-sized and convenient to handle, they can be manipulated in a small-sized glove box easy to seal (without the use of a large-sized hood).
  • the apparatus used in the present invention are disposable and also economical because such expensive apparatus as a particular vacuum line (particularly, fitting glass joints and cocks) are not at all used.
  • itemizing the gaseous radioisotope can be conveniently carried out by connecting a plurality of recovery vials for the gaseous radioisotope of which capacities are the same or different to a capillary tube in such a way that the openings of said vials are communicated with the capillary tube respectively and connecting the gaseous radioisotope ampoule to an end of the capillary.
  • at least one of said recovery vials is filled with the adsorbent.
  • At least one of said recovery vials is filled with a reacting agent instead of the adsorbent.
  • a reacting agent instead of the adsorbent.
  • water tritiated can be produced by breaking in vacuum the vial filled with the reacting agent, allowing the reacting agent to stand at room temperature or an elevated temperature and reacting the reacting agent with tritium remaining in the confined zone. Water tritiated thus obtained can be used as materials.
  • the reacting agent which reacts with tritium at room temperature or an elevated temperature to convert it to tritiated water includes metal oxides such as copper oxide, platinum oxide and palladium oxide.
  • gaseous radioisotope ampoule 31 is connected to an end of glass tube 32 while a vacuum pump is connected to the other end of glass tube 32 and recovery vials 33 to 41 are communicated with the glass tube respectively.
  • Ampoule 31 is broken in vacuum by piece of iron 4 and thus diffused gas is adsorbed on the adsorbent of vial 41 under cooling. After melt-sealing of connecting portion B the adsorbed gas is released to the confined zone by allowing the adsorbent to stand at room temperature or an elevated tem- Furthermore, it is clear that if tubes to be melt-sealed are of capillary it is easy for even those unskilled in glass work to melt-seal them.
  • a hood for the gaseous radioisotope manipulating apparatus is characterized in that the gaseous radioisotope manipulating apparatus is always operated in an opeation box maintained under negative pressure without ventilating and that the escaping gas is recycled through a treatment apparatus provided with recycle and recovery means therein to remove the radioisotope.
  • a concentration of the gaseous radioisotope in the operation box is extremely reduced due to recycle of the gas stream, as compared with the conventional methods.
  • the treatment apparatus to be used is provided with a treating agent and treating means in accordance with the treating method as mentioned below.
  • connecting portion C, D, E, F, G, H, I and J are melt-sealed respectively.
  • the gaseous radioisotope remaining in the capillary is adsorbed on the adsorbent by again cooling vial 41 and thereafter connecting portion K is meltsealed.
  • via] 41 connected with trap 42 is filled with a reacting agent instead of the adsorbent and connected to the glass tube 32 in such a way that the opening of vial 41 is communicated with the glass tube.
  • tritium gas ampoule 31 is broken in vacuum, tritium gas is immediately subdivided to each of vials and then connecting tube B, C, D, E, F, G, H, l and J are melt-sealed respectively.
  • trap 42 is cooled while vial 41 is heated, thereby tritium remaining in the confined zone being collected in trap 42 as tritiated water. Atter completion of recovery connecting tube L and then K are melt-sealed.
  • the itemizing process of the present invention has the advantages that tritiuim gas can be subdivided as tritiated water which is available as materials and that the subdivided amounts to each vial can be accurately determined by measurement of the amount of tritiated water and its radioactivity, in addition to the advantages 1) to 11) mentioned hereinbefore in respect of the process for the preparation of labelled compounds.
  • the above mentioned treating methods may be used in combination in the treatment apparatus.
  • operation box 51 provided with a radioisotope manipulating apparatus 54 therein is connected to ventilation box 56 provided with a treatment apparatus 57 for recycle and recovery therein. Furthermore, ventilation box 56 is connected with a ventilation equipment.
  • Treatment apparatus 57 is provided with means for recycling a fluid containing a gaseous radioisotope and means for recovering the radioisotope.
  • the gas diffused in operation box 51 is recycled through recovery apparatus 60, trap 61 and pipe 62 by recycle pume 59.
  • Symbol 58 is a valve and symbol 63 a flow meter.
  • the operation box, before operating, is sealed under negative pressure by opening door 64, driving the ventilation equipment, adjusting the pressure gauge 55 and then closing door 64.
  • Treatment apparatus 57 for recycle and recovery.
  • door 64 of operation box 51 is opened to pass a fluid stream containing an extremely dilute gas below a tolerance limit through the upper part of ventilation box 56.
  • the exhaust gas is then passed through filter 65 and discharged through exhaust ducts 67 to the outdoors by pump 66.
  • Symbol 52 is a peep-window, symbol 53 operation-gloves, symbol 55 a pressure gauge and symbol 68 a table.
  • the operation box, treatment apparatus for recycle and recovery and ventilation equipment may be arranged by the available apparatus.
  • the operation gloves used in the operation box may be substituted with mechanical hand.
  • box 56 is provided with gloves so that valve 58, pump 59, recovery apparatus 60, trap 61, pipe 62 and flow meter 63 can be operated by hand if desired. It is preferred to make trap 61 shape suitable for recovery of scrap after treatment.
  • positions of the inlet and outlet at box 51 and ventilation box 56 are decided taking the work efficiency into consideration. Water conduits, gas conduits, drainpipes, wirings and pipings, and their fitting equipment may be provided, if desired, like the con- 'ventional drafts, hoods and gloveboxes.
  • Materials of box 51 are not limited in kind so far as they are airproof.
  • the hood, according to the present invention has the following advantages:
  • Tritiated water with a high specific activity is obtained. Tritiated water can be reused as materials.
  • EXAMPLE 1 As shown in FIG. 2, 1g of salicylic acid was charged into vial 2 and 2g of a granulated active carbon dehydrated'and degased by heating at 400C under vacuum for an hour were charged into vial l or 8cc capacity. Magnet 4 was fixed within the opening of vial 2 and then a lOCi tritium gas ampoule 3 itemized according to Example 13 set forth hereinafter was connected therewith through a polyvinyl chloride tube. The dotted line indicates the connected part. After a vacuum pump was connected to an opening of vial 1 and operated to make a pressure of the system ,l l0' mmI-Ig, portion A was melt-sealed by a gas burner.
  • a specific activity of radiochemically pure salicylic acid-l-I-3 obtained thus was 0.2mCi/g.
  • the specific activity was measured by liquid scintillation spectrometer (made by Packard Co.). This is so with the following examples.
  • Tritium gas amouple l recovered in the above procedure can be reused as tritium gas ampoule 3 as shown in FIG. 2 for preparing a labelled compound.
  • vial 2 is filled with 200mg of salicylic acid and 200mg of platinum black as the catalyst while vial 1 was filled with lg of a granulated porous titanium degased by heating at 700 to 800C.
  • Magnet 4 was fixed in an opening of vial 2 and ampoule 3 containing lCi tritium gas was connected to the opening with a polyvinyl chloride tube. The connected portion is indicated by a dotted line.
  • a vacuum pump was connected to the other opening of via] 2 and then operated to make a degree of vacuum of the system l0 -l0 mmHg while heating vial l to a temperature of 600C by the external electric furnace.
  • portion D was melt-sealed by a gas burner.
  • a breakable seal of ampoule 3 is then broken by magnet 4.
  • the temperature of the titanium was gradually reduced to allow the titanium to adsorb the tritium gas diffused in the system.
  • a degree of vacuum of the system because l0 l O mmHg.
  • portion E is melt-sealed by a gas burner. Again, vial l was heated to temperatures of 700 to 800C to release the adsorbed tritium gas into the system and the system was allowed to stand for two hours.
  • vial 1 is gradually cooled again to allow the titanium to adsorb the remaining tritium gas and hydrogen. At that time a degree of vacuum of the system became l0' 10 mmI-Ig. After completion of adsorption portion F was melt-sealed to separate the sample vial from the tritium gas vial and a tritium-labelled compound was removed.
  • EXAMPLE 3 As shown in FIG. 4, 0.5g of digitoxin and 3g of a granulated active carbon dehydrated and degased by heating at 400C under vacuum for an hour were fed to vial 5. Opening a of vial 5 in which magnet 4 is set up was connected to ampoule 3 containing 30 Ci tritium gas through a polyvinylchloride tube. The connected portion is indicated by a dotted line. After a vacuum pump was connected to opening b and then operated to make the system a degree of vacuum of l0 l0" mml-Ig, portion G was melt-sealed by a gas burner.
  • Vial 1 was cooled by liquid nitrogen to allow the acitive carbon to adsorb the tritium gas diffused in the confined system. At that time a degree of vacuum of the system became l0 mmHg. After completion of adsorption portion J was melt-sealed by a gas burner to recover the remaining tritium gas and to obtain digitoxin-H-3.
  • EXAMPLE 4 As shown in FIG. 5, tritium recovery vial 8 and hydrogen recovery vial 7 each filled with 2g of an active carbon dehydrated and degased by heating at 400C for an hour, mercury manometer l1, ampoule 10 containing 30ml hydrogen gas, ampoule 9 containing 10Ci tritium gas, and catalytic reduction vial 6 provided with magnetic stirrer 13, containing 01g of linolic acid, 50mg ofa platinum black catalyst and 10 ml of dioxane were connected to capilllary tube 12 respectively through polyvinylchloride tubes. The connected portions were indicated by the dotted lines.
  • a vacuum pump was connected to opening e of the capillary and then operated to make a degree of vacuum of the system l0 -lO' mmHg while cooling catalytic reduction vial 6 by liquid nitrogen, and thereafter portion K was melt-sealed by a gas burner.
  • Tritium recovery vial 8 was cooled by liquid nitrogen to allow the active carbon to adsorb the tritium gas diffused in the confined system. At that time a degree of vacuum of the system became l0 -l0 mmHg. After completion of adsorption portion L was melt-sealed by a gas burner. Then, when vial 8 was brought to room temperature by ceasing the cooling, the adsorbed tritium gas was released completely in the system. After reaction vial 6 was brought to room temperature by ceasing the cooling, the reduction reaction of the compound to be labelled with tritium was carried out while agitating with magnetic stirrer 13.
  • a reaction amount of tritium was read on by mercury manometer 11. After completion of reduction with tritium, tritium recovery vial 8 was cooled by liquid nitrogen to allow the active carbon to adsorb the unreacted tritium gas while cooling again the catalytic reduction vial by liquid nitrogen and then portion M was melt-sealed by a gas burner.
  • Acetic acid-C-l4 was obtained by the sam procedure as Example 1 except that Grignards reagent, CH MgCl was reacted with carbon dioxide-C-14.
  • Example 3 5.0 X 10' uCi/cc B.G. 4
  • Example 4 3.0 X 10 #Ci/cc B.G.
  • FIG. 6 In this example apparatus set forth in FIG. 6, FIG. 7 and FIG. 8 are used in combination with one another.
  • Connecting portions of vials are preferably a capillary tube with the outside diameter of 8mm and inside diameter of 2mm.
  • an ampoule contain ing 20Ci tritium gas provided with an opening in which a magnet is fixed was connected with opening c, through a polyvinylchloride tube and a vacuum pump was connected to opening
  • the active carbon was dehydrated and degased by heating at 450C for 30 minutes while operating the vacuum pump, and after a degree of vacuum of the system became l0 10*mmHg, portion C was melt-sealed.
  • the tritium gas ampoule was broken by the magnet and the vial 14 with the active carbon was cooled by liquid nitrogen to allow the active carbon to adsorb the tritium gas diffused in the confined system. At that time a degree of vacuum of the system became l0 10*mmHg. After completion of adsorption portion C, was melt-sealed. When ceasing the cooling of the active carbon to make the system the room temperature, the adsorbed tritium gas was completely released in the system and brought into contact with salicylic acid at room temperature for 10 days.
  • vial 12 shown in FIG. 7 through opening 12 were charged 3g of a granulated active carbon and portion B was melt-sealed so that the inner volume of vial 12 except the bulk of the active carbon becomes 10ml.
  • the active carbon of vial 12 was dehydrated and degased by heating at 450C for 30 minutes while operating a vacuum pump connected with opening b., and after a degree of vacuum of the system became l0' -1Omml-lg, portion B was melt-sealed.
  • Opening b of vial 12 in which a magnet is fixed was connected with opening 0 of apparatus 14 through a polyvinylchloride tube, and after a vacuum pump connected to opening b, was operated to make the system vacuum, portion B, was melt-sealed. Then, vials l2 and 14 was communicated with each other by breaking breakable seals and vial 12 of the active carbon was cooled by liquid nitrogen to cause the active carbon to adsorb the tritium gas diffused in the confined system.
  • portion C was melt-sealed to separate vial 13 containing a product therein from vial 14.
  • vial 11 FIG. 6 with opening a in which a magnet is fixed were fed 20ml of methanol and opening a was connected with opening 0;, of via] 13 through a polyvinylchloride tube.
  • a vacuum pump connected to opening a was operated to make vial 11 and the connected portion vacuum, and thereafter portion A, was melt-sealed.
  • Vial 11 was communicated with vial 13 by breaking its breakable seal and then brought into an elevated temperature while cooling vial 13, so that methanol was transferred into via] 13 to clean the product contained therein. Thereafter, methanol was recovered in vial 11 by warming vial 13 while cooling vial 11 and then portion C,, was melt-sealed.
  • the appartus shown in FIG. 8 is intended to charge a compound to be labelled and an adsorbent into separate vials, respectively, but a vial for charging a mixture of a compound to be labelled and adsorbent, provided with connecting openings can be used to the same purpose. In the latter case, it is preferred to use such an adsorbent that the adsorbed gase ous radioisotope can be released at the norma temperature.
  • EXAMPLE 7 In this example apparatus set forth in FIGS. 6, 7 and 9 are used in combination with one another.
  • portion D was melt-sealed.
  • the tritium gas ampoule was broken and vial 16 was cooled by liquid nitrogen to cause the active carbon to adsorb the tritium gas diffused in the confined system.
  • a degree of vacuum of the system became l0 1O mmHg.
  • the adsorbed tritium gas was completely released into the confined system in which the gas was then brought into contact with vitamin B at room temperature for 5 days.
  • vial 12 (FIG. 7) of 35ml capacity filled with 5g of an active carbon, prepared in advance was connected to opening d, (FIG. 9), and thus the tritium gas was recovered by vial l2 and then portion D, was melt-sealed.
  • the cleaning solvent via] 11 was connected to opening d to remove the unstable tritium as mentioned in Example 6.
  • vitamin B -H-3 When the product, namely vitamin B -H-3 was withdrawn from vial 15 in the glove-box, no diffusion of tritium gas into the glove-box could be practically perceived.
  • a radiochemically pure vitamin B -H-3 was obtained by purifying in the conventional procedure, its specific activity being mCi/g.
  • EXAMPLE 8 In this example apparatus set forth in FIG. 6, FIG. 7 and FIG. 8 are used in combination with one another as mentioned in Example 6 except that vial 12 is filled with a reacting agent instead of the active carbon and also another empty vial 11 is used for recovery of tritrum.
  • vial 12 was communicated with vial 14 by breaking the breakable seals while heating the copper oxide at a temperature of 450C, and then vial 12 was broken to communicate with vial 11 which was connected to the bottom of vial 12.
  • vial 11 was cooled by dry ice to freeze and recover tritiated water obtained thus, a degree of vacuum of the system being l0"- l0 mmI-Ig.
  • portions A B and C were melt-sealed to separate vial l1, vial l2, vial l3 and vial 14 from one another.
  • Salicylic acid-H-3 having a specific activity of I lmCi/g was obtained by purifying in the conventional procedure.
  • Acetic acid-C44 was obtained by the same procedure as Example 6 except that Grignards reagent, CH MgCl is reacted with carbon dioxide-C-l4.
  • EXAMPLE 11 Apparatus set forth in FIG. 6, FIG. 7 and FIG. 9 are used in combination with one another.
  • Example 6 In the same procedure as Example 6 except that 0.5g of digitoxin are used instead of 0.5g of salicylic acid, the digitoxin was brought into contact with tritium at room temperature for 5 days. Thereafter, 5g of a porous metallic titanium were charged into vial 12 of 10ml inner volume through opening and portion 8;, was melt-sealed. Then, the porous titanium was dehydrated and degased by heating at 700C for 30 minutes while operating a vacuum pump connected to opening 17 and when a degree of vacuum of the system became l0 -1OmmHg, portion 8,, was melt-sealed. Next, opening b in which a magnet is fixed was connected to opening (FIG.
  • vial 12 was communicated with vial 14 by breaking the breakable seals, and the tritium gas diffused in the confined system was recovered as a tritiated titanium by heating the porous titanium to a temperature of 700C and then lowering the temperature at a rate of 5C per a minute. At that time a degree of vacuum of the system became I0 I lO mmHg and portion B was melt-sealed, thus vial 12 filled with tritiated titanium being removed.
  • each of the vials was removed in the same procedure as Example 6.
  • digitoxin-H-3 was withdrawn from the vial in the glove-box, no diffusion of tritium into the glove-box could practically be perceived.
  • a radiochemically pure digitoxin-H-3 was obtained by purifying in the conventional procedure, its specific activity being mCi/g.
  • portion E was melt-sealed. Then, the 50Ci tritium gas ampoule was broken and the active carbon was cooled by liquid nitrogen to adsorb the tritium gas diffused in the confined system. At that time a degree of vacuum of the system became 110 l mmHg. After completion of adsorption portion E was melt-sealed, and when ceasing the cooling of the active carbon to make the system room temperature, the adsorbed tritium gas was released into the system.
  • reaction vial 17 was brought to room temperature by ceasing the cooling and the reduction reaction with tritium was carried out while agitating by magnetic stirrer 23. A reaction amount of tritium was read on by mercury manometer. When the tritium gas amount corresponding to 25Ci was consumed, the reduction reaction was ceased. Again the reaction vial 17 was cooled by liquid nitrogen while tritium recovery vial 20 was cooled to allow the active carbon to adsorb an unreacted tritium gas remaining in the system, and thereafter portion F was melt-sealed.
  • a 30 ml dioxane containing vial ofa 80 ml inner volume, provided with a glass filter (25mm in diameter, 3mm in thickness) for removal of the catalyst as shown in FIG. 14 is prepared in advance for recovery of a labelled compound.
  • Opening g, (FIG. 14) was connected to opening e,, (a magnet fixed therein) of the above mentioned vial 17 through a silicone rubber tube. While cooling vial 22 by liquid nitrogen, a vacuum pump connected to opening 3 was operated to make the system vacuum and then portion G was meltsealed.
  • dioxane first was transferred into vial 17 by breaking opening e with the magnet and cooling vial 17 while warming via] 22, and then the reaction product was recovered in vial 22 by including vial 22 while cooling to remove the catalyst with the glass filter 21. Then, portions G G, and J, respectively were melt-sealed.
  • a radiochemically pure stearic acid-H-3 was withdrawn from the product recovery vial 22, its specific activity being 23OCi/g.
  • tritium concentration in air within the room and about the exhaust was 1 X l0' uCi/ml to 1 X 1O uCi/ml because of the escaping gas from the apparatus while working.
  • EXAMPLE 13 As shown in FIG. 15, vials 33 and 34 of a 4m] capacity each, vials 35 and 36 of a 16 ml capacity each, vials 37, 38, 39 and 40 of a 6 ml capacity each, and vial 41 ofa 6 ml capacity filled with 4 g (2 ml) of an active carbon, respectively were connected to capillary tube 32 with polyvinylchloride tubes in such a way that openings of each vials are communicated with the capillary tube.
  • Openings B in which magnet 4 is fixed was connected to a lOOCi tritium gas ampoule 31 through a polyvinylchloride tube and a vacuum pump connected to opening A was operated to make a degree of vacuum of the confined system l0 -lO mmHg, and then portion A was melt-sealed by a gas burner.
  • vial 41 was cooled by liquid nitrogen to allow the active carbon to adsorb the tritium gas remaining in the system.
  • connected portion K was meltsealed by a gas burner.
  • capillary tube 32 was melt-sealed in pieces and scrapped.
  • Example 13 of the present invention To compare Example 13 of the present invention with the conventional method, a tritium concentration in air of the working environment was measured during the operation by the tritium monitor. The measured results in average are shown in Table 3.
  • vials 33 and 34 of a 10 ml capacity each, vials 35 and 36 of a 40 ml capacity each, vials 37, 38, 39, and 40 of a 20 ml capacity each, and via] 41 of a 10 ml capacity filled with 30g of copper oxide (CuO: an elementary analysis grade, degased by heating at a temperature of 450C), respectively were connected to capillary tube 32, for example with polyvinylchloride tubes in such a way that opening of each vials are communicated with the capillary tube. Further, trap 42 is communicated with the bottom of vial 41.
  • CuO copper oxide
  • Opening B in which magnet 4 is fixed was connected to a IOOCi tritium gas ampoule 31, for example through a polyvinylchloride tube. After a vacuum pump connected to another opening A was operated to make a degree of vacuum of the confined system lO l mmHg, connected portion A was meltsealed. When a breakable seal of ampoule 31 was broken by magnet 4 to diffuse the tritium gas into the confined system, the tritium gas was immediately itemized in accordance with the volume ratio of each vials. Consequently, connected portions C, D, E, F, G, H, l, and J were melt-sealed, respectively.
  • vial 41 After a breakable seal of vial 41 filled with copper oxide was broken by magnet 4, vial 41 was heated to about 450C by an electric heater while cooling trap 42 by dry ice, whereby the remaining tritium gas in the system was collected in trap 42 as tritiated water. At that time a degree of vacuum of the system became 1O -lO mmHg. Thereafter, connected portions L, K, and then B were melt-sealed.
  • another vial or trap 42 was communicated with the bottom of the vial filled with a reacting agent (vial 41) to capture the reaction product.
  • a reacting agent vial 41
  • any one or more of tritium recovery vials 33 to 40 are applied as a vial for capture of the reaction product so that tritiated water can be captured by cooling it in the same manner.
  • EXAMPLE 16 An operation of enclosing lOOCi of tritium gas in an ampoule filled with a compound to be labelled was made with use of the normal Wilzbachs labelling apparatus in operation box 51 (FIG. 17) ofa 500 l inner volume closed under a negative pressure of6OmmH O to the external pressure. After completion of the operation the tritium concentration in air of the operation box became l.6p.Ci/cm This means that 800mCi of tritium gas was diffused in the box.
  • the laboratory used herein is provided with a ventilation equipment having a ventilative capacity of 200m per minute so that when discharging the exhaust gas at it is the average concentration during 8 hours about the exhaust is as follows:
  • treatment apparatus is provided with a quartz pipe of 20mm in inner diameter therein which was filled with 200g of CuO, wire for elementary analysis.
  • a recycle stream with 25 l/min was fed through pump 59 while heating treatment apparatus 60 to a temperature 450C, and the recycle and treatment were carried on for three hours while tritiated water formed thus was captured by trap 61 of glass filled with a freezing mixture of dryice-methanol.
  • the tritium concentration in air within the closed operation box 51 was measured by the ion chamber, its result being O.0O6;1.Ci/cm or 3mCi.
  • an average concentration during 8 hours about the exhaust was 3 X 10";rCi/cm so that the tritium gas with a concentration far less than the legal tolerance limits could be discharged to dilute.
  • the tritiated water captured with trap 61 was measured by the liquid scintillation spectrometer and counted, its result being 725mCi. 8.4ml of the tritiated water have a concentration sufficient for use as materials in the preparation of a labelled compound.
  • EXAMPLE 17 As apparatus of glass are in general used in the manipulation of tritium gas, in some cases the leakage of tritium gas due to their breakage is apprehended. This example was carried out under the assumption of such an accident.
  • Example 16 An ampoule filled with 2Ci of tritium gas was broken in the operation box 51 used in Example 16 which was closed under a negative pressure of -60mmH O and the tritium gas was diffused in the box, and as the result the tritium concentration in the box became 4p.Ci/cm based on calculation.
  • treatment apparatus 60 is provided with a glass pipe ob 20mm in diameter therein which was filled with asbestos sprinkled with 10g of PtO The recycle and treatment were carried on for 5 hours and thus formed tritiated water was captured in the same manner as Example 16.
  • EXAMPLE l8 Catalytic reduction vial 6 (FIG. containing stearic acid-H-3 obtained in Example 4 was transferred to operation box 51 (FIG. 17) of a 50 L capacity, and the filtration for removal of the catalyst was carried out in a state closed under a negative pressure of 6OmmH O to the external pressure, and as the result an unstable tritium adsorbed on the catalyst diffused and therefor a tritium gas concentration in the box became 8 BCi/cm. This means that 0.4Ci of tritium gas leaked.
  • a quartz pipe of 20mm in diameter wherein electrodes are set up and a relay is operated as to discharge at intervals of a second with the use of tesla coil.
  • a recycle stream with 5 l/mi. was passed through the above treatment apparatus and the recycle and treatment were carried on for three hours while tritiated water formed thus was captured by trap 61 filled with a freezing mixture of dry ice-methanol.
  • a tritium concentration in the operation box became 1.6 X l() ,u.Ci/cm or 0.8mCi, door 14 was opened to pass the gas stream through the ventilation equipment.
  • a tritium concentration in average during eight hours about the exhaust was 8.3 X uCi/cm which was far less than the legal limit 2 X 10- uCi/cm Moreover, 2.4m] of a 396mCi tritiated water were recovered which are of course applicable as a material for the preparation of a labelled compound.
  • a surface contamination of the inside of the operation box according to the smear method after completion of the operation was measured by a liquid scintillation spectrometer, its results having practically indicated background.
  • EXAMPLE Examples 6 to 15 were repeated within the operation box 51 closed under a negative pressure as shown in FIG. 17 and as a result there were no troubles in manipulating the glass vials and apparatus under vacuum.
  • the tritium gas was under a double-sealed state by the vacuum-sealed vial or apparatus and also the closed operating box so that the workers could manipulate the tritium with safety. Further, a tritium concentration in air about the hood and within the laboratory was continuously monitored by the tritium monitor and as the result there was no leakage of tritium at all.
  • a process for the preparation of a labelled compound comprising carrying out a reaction by contacting a compound to be labelled with a gaseous radioisotope in a closed vacuum system, the system including an adsorbent, a reacting agent or a combination thereof by means of which any unreacted gaseous radioisotope may be recovered, the labelled compound being re moved under vacuum from the system by melt sealing and the adsorbent, the reacting agent, its reaction product or combinations thereof being removed under vacuum from the system by melt sealing.
  • a process of claim 1 which comprises communicating a vial containing a compound to be labelled with an adsorbent containing vial through a glass tube, said two vials each being provided with openings for connection, or providing a vial containing a mixture of the compound to be labelled and adsorbent with openings for connection, breaking in vacuum an ampoule of gaseous radioisotope connected to any one of the openings of said vials to diffuse the gaseous radioisotope into the closed system, adsorbing the diffused gas by the adsorbent under cooling, removing said ampoule by meltsealing, thereafter releasing the adsorbed gas by allowing the adsorbent to stand at room temperature or at an elevated temperature to bring said gas into contact with the compound to be labelled, and recovering then an unreacted gas remaining in the closed system by again cooling the adsorbent.
  • adsorbent is an active carbon, silicagel or alumina, or a metal such as platinum, palladium, titanium, uranium, zirconium, rubidium, erbium, cesium, nickel, calcium, strontium, sodium and lithium.
  • radioisotope is tritium, argon-37, krypton-85, gaseous labelled compounds-G14 or gaseous labelled compounds-S-35.
  • a process of claim 2 wherein comprises communicating in vacuum another vial containing an adsorbent or reacting agent for recovery of the gaseous radioisotope with the adsorbent containing vial after the reaction of the compound to be labelled with said gaseous radioisotope, recovering the gas remaining in the closed system by cooling or heating said adsorbent or reacting agent for recovery and then removing the recovery vial by melt-sealing, and furthermore communicating in vacuum a cleaning solvent vial with the vial contained the labelled compound therein, establishing a temperature difference between said two vials to transfer the solvent thereby separating the labelled compound from unstable gaseous radioisotopes.
  • a process of claim 5 wherein said reacting agent is copper oxide, platinum oxide or palladium oxide.
  • said cleaning solvent is a solvent with a low boiling point and dissociative hydrogen, such as water and alcohols.
  • a process of claim 1 which comprises communicating in vacuum a reaction vial containing a compound to be labelled and optionally a catalyst and solvent, a vial containing an adsorbent for recovery of hydrogen, a vial containing an adsorbent for recovery of tritium, a hydrogen gas ampoule and a tritium gas ampoule respectively with a glass tube, breaking in vacuum said tritium gas ampoule to diffuse tritium gas into the closed system, adsorbing the diffused gas by the adsorbent for tritium under cooling, removing said ampoule by melt-sealing, thereafter releasing the adsorbed gas by allowing the adsorbent for tritium to stand at recovery of the unreacted tritium and hydrogen according to the process of claim 9, communicating in vacuum a solvent containing vial provided with a filter for recovery of the labelled compounds with the reaction vial, cooling the reaction vial to clean its inner part with the solvent, and then recovering the labelled compound by cooling the recovery vial while removing the catalyst

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US5312592A (en) * 1990-06-13 1994-05-17 Scanditronix Ab Disposable kit for preparation
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US3700602A (en) * 1969-09-04 1972-10-24 Atomic Energy Commission Method for mass tagging sand with a radioactive isotope
US3725295A (en) * 1971-07-20 1973-04-03 Atomic Energy Commission Technetium labeling

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US3700602A (en) * 1969-09-04 1972-10-24 Atomic Energy Commission Method for mass tagging sand with a radioactive isotope
US3725295A (en) * 1971-07-20 1973-04-03 Atomic Energy Commission Technetium labeling

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CN111649230A (zh) * 2020-05-29 2020-09-11 原子高科股份有限公司 一种Kr-85密封放射源真空充气系统及充气方法
CN111649230B (zh) * 2020-05-29 2022-07-01 原子高科股份有限公司 一种Kr-85密封放射源真空充气系统

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