JP2006133198A - Tritium removal method at manufacturing of pharmaceutical products for positron emission tomography diagnosis - Google Patents

Tritium removal method at manufacturing of pharmaceutical products for positron emission tomography diagnosis Download PDF

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JP2006133198A
JP2006133198A JP2004325628A JP2004325628A JP2006133198A JP 2006133198 A JP2006133198 A JP 2006133198A JP 2004325628 A JP2004325628 A JP 2004325628A JP 2004325628 A JP2004325628 A JP 2004325628A JP 2006133198 A JP2006133198 A JP 2006133198A
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tritium
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target water
positron emission
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Yoichi Sakuma
洋一 佐久間
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Abstract

<P>PROBLEM TO BE SOLVED: To provide a method for safely discharging tritium as gas in the air, that has accumulated in target water as a byproduct, during manufacturing pharmaceutical products for positron emission tomography diagnosis. <P>SOLUTION: For discharging tritium T as HT gas in the air which is contained in target water, by having it irradiated with positrons by a cyclotron, the tritium-containing target water is lead to electrolysis cell 4 and decomposed by electrolysis into molecular oxygen<SP>18</SP>O<SB>2</SB>and HT gas. The HT gas is discharged through a stack 10, and for flow-out molecular oxygen<SP>18</SP>O<SB>2</SB>, a carrier gas N<SB>2</SB>and hydrogen gas H<SB>2</SB>are made to merge, and are cooled and collected as H<SB>2</SB><SP>18</SP>O by way of a coupling column 8. <P>COPYRIGHT: (C)2006,JPO&NCIPI

Description

本発明は、陽電子断層診断用医薬品の製造時に副産物として生じるトリチウムを、安全に処理するための方法に関する。   The present invention relates to a method for safely treating tritium generated as a by-product during the manufacture of a positron emission tomography diagnostic drug.

従来、陽電子断層診断（以下、Positron Emission Tomography の頭文字を組み合わせてＰＥＴと呼ぶ。）に用いられる医薬品としてのＦＤＧ（［18Ｆ］−２−ｆｌｕｏｒｏ−２−ｄｅｏｘｙ−Ｄ−ｇｌｕｃｏｓｅ）は、糖代謝診断に用いられているが、これに含まれる、フッ素の放射性同位体であるフッ素１８（18Ｆ）は、半減期１０９.８ｍｉｎの陽電子（ポジトロン）放出核種である。
ＦＤＧは一般に、サイクロトロンで陽子を酸素１８が濃縮された水（濃縮［18Ｏ］−Ｈ2Ｏ）に照射して、18Ｏ（ｐ，ｎ）18Ｆ反応によって18Ｆを生成し、それを原料にして合成されているが、その際、競合核反応である18Ｏ（ｐ，ｔ）16Ｏ反応によってトリチウム（3Ｈ）も生成される。
ある研究によれば、ターゲット水回収量は１回当たり約１ｍＬで、トリチウム生成量は18Ｆ生成量の２.４×１０-6であった。
トリチウム（3Ｈ）は水素の放射性同位体で半減期１２.３年のβ崩壊核種である。したがって、ＦＤＧ合成を行う作業者のトリチウムによる放射線被曝や使用済みターゲット水の処分などが問題になり、ターゲット水に蓄積されるトリチウムを取り除くことが望まれている。しかし、使用されるターゲット水が少量でかつ高価であることから、操作が困難であり、実際には行われていない。
伊藤茂樹他、第４回環境放射能研究会プロシーディングス、（２００３年）３４５−３５１頁 Conventionally, FDG ([ 18 F] -2-fluoro-2-deoxy-D-glucose) as a pharmaceutical used for positron emission tomography diagnosis (hereinafter referred to as PET in combination with the acronym of Positron Emission Tomography) is sugar Fluorine 18 ( 18 F), which is a radioisotope of fluorine, used for metabolic diagnosis, is a positron emission nuclide having a half-life of 109.8 min.
FDG generally by irradiating protons in water oxygen 18 enriched (enriched [18 O] -H 2 O) in a cyclotron, 18 O (p, n) 18 by F reaction generates 18 F, it In this case, tritium ( 3 H) is also produced by the 18 O (p, t) 16 O reaction which is a competitive nuclear reaction.
According to one study, the amount of target water recovered was about 1 mL per time, and the amount of tritium produced was 2.4 × 10 −6 of 18 F produced.
Tritium ( 3 H) is a radioisotope of hydrogen and a beta decay nuclide with a half-life of 12.3 years. Therefore, radiation exposure by tritium of an operator who performs FDG synthesis, disposal of used target water, and the like become problems, and it is desired to remove tritium accumulated in the target water. However, since the amount of target water used is small and expensive, it is difficult to operate and is not actually performed.
Shigeki Ito et al., 4th Environmental Radioactivity Research Group Proceedings, (2003) 345-351

本発明は、前述のＰＥＴ製造時に副産物としてターゲット水に蓄積されるトリチウムを、気体として大気中へ安全に放出できるようにした方法を提供することを課題とする。   An object of the present invention is to provide a method in which tritium accumulated in target water as a by-product during the above-described PET production can be safely released into the atmosphere as a gas.

前述の課題を解決するため、本発明のトリチウム除去方法は、陽電子断層診断用医薬品としてのフルオロ・デオキシ・グルコースを合成するため、酸素１８が濃縮されたターゲット水にサイクロトロンで陽子を照射して18Ｏ（ｐ，ｎ）18Ｆ反応により18Ｆを生成する際に、競合核反応である18Ｏ（ｐ，ｔ）16Ｏ反応によって生成されるトリチウム含有ターゲット水について、トリチウムを除去すべく、同トリチウム含有ターゲット水を電解セルへ導いて電気分解により分子状酸素18Ｏ2とＨＴガスとに分解し、流出する上記分子状酸素についてはキャリヤーガスＮ2および水素ガスＨ2を合流させて結合カラムを介しＨ2 18Ｏとして冷却捕集するとともに、上記ＨＴガスは大気中へ放出することを特徴としている。 To solve the problems mentioned above, tritium removal method of the present invention, for synthesizing fluoro-deoxy-glucose as a medicament for positron tomography, oxygen 18 is irradiated with protons in a cyclotron onto a target water enriched 18 In order to remove tritium from the tritium-containing target water produced by the 18 O (p, t) 16 O reaction, which is a competitive nuclear reaction, when 18 F is produced by the O (p, n) 18 F reaction, The tritium-containing target water is led to an electrolytic cell and decomposed into molecular oxygen 18 O 2 and HT gas by electrolysis, and for the molecular oxygen flowing out, carrier gas N 2 and hydrogen gas H 2 are combined to form a coupling column. The HT gas is cooled and collected as H 2 18 O through the gas, and the HT gas is released into the atmosphere.

上述の本発明のトリチウム除去方法では、陽電子断層診断用医薬品の製造時に生成されたトリチウム含有ターゲット水ＨＴ18Ｏが、電解セルへ導かれて、同電解セル内の陽極および陰極の作用で電気分解されることにより分子状酸素18Ｏ2とＨＴガスとに分解される。 In the above-described tritium removal method of the present invention, the tritium-containing target water HT 18 O produced during the production of the positron emission tomography diagnostic drug is led to the electrolysis cell and electrolyzed by the action of the anode and cathode in the electrolysis cell. As a result, it is decomposed into molecular oxygen 18 O 2 and HT gas.

このようにして生成されたＨＴガスは、所要の濃度限度以下であることを確かめながら大気中へ放出される。ＨＴガスはＨＴＯよりも遥かに人体影響が小さく、大気中におけるＨＴからＨＴＯへの変換速度は非常に遅い。さらに、半減期１２.３年でトリチウムは次第に無害なＨｅに壊変していくことから、安全性は十分に確保されることになる。   The HT gas produced in this way is released into the atmosphere while ensuring that it is below the required concentration limit. HT gas has much less human influence than HTO, and the conversion rate from HT to HTO in the atmosphere is very slow. Furthermore, since tritium gradually decays into harmless He with a half-life of 12.3 years, safety is sufficiently ensured.

また、分子状酸素18Ｏ2については、キャリヤーガスＮ2および水素ガスＨ2を合流させて、結合カラムを介し容易に無害のＨ2 18Ｏとして冷却捕集することができる。 Further, the molecular oxygen 18 O 2 can be easily cooled and collected as harmless H 2 18 O through the combined column by combining the carrier gas N 2 and the hydrogen gas H 2 .

糖代謝診断などに用いられるＰＥＴ用医薬品としてのＦＤＧの製造時に、サイクロトロンで陽子を照射されるターゲット水には、水素の放射性同位元素としての危険なトリチウムＴが含まれる。そこで、本実施例では、電解セルにおける電気分解によって、上記ターゲット水に含まれるトリチウムＴを、分子状水素（ＨＴ）に移動させてから、これを大気中へ放出する手段が採用される。   The target water irradiated with protons by a cyclotron at the time of production of FDG as a PET pharmaceutical used for sugar metabolism diagnosis and the like contains dangerous tritium T as a radioisotope of hydrogen. Therefore, in this embodiment, a means is adopted in which tritium T contained in the target water is moved to molecular hydrogen (HT) by electrolysis in an electrolytic cell and then released into the atmosphere.

すなわち、人体に対する影響の違いから、放射線管理区域から排出する場合、分子状水素（水素ガス）のトリチウムの法規制値は、水蒸気状に比べて［表１］に示すように、約１０,０００倍緩くなっているので放出には問題はない。

Figure 2006133198
That is, due to the difference in the effects on the human body, when discharged from a radiation control area, the legally regulated value of molecular hydrogen (hydrogen gas) tritium is about 10,000 as shown in [Table 1] as compared to that of water vapor. There is no problem with the release because it is twice as loose.
Figure 2006133198

上記の電気分解による反応は、［数１］式のように行われる。
［数１］
２1Ｈ3Ｈ18Ｏ（liquid）→ ２1Ｈ3Ｈ（gas）＋18Ｏ2（gas）
The reaction by the above electrolysis is performed as shown in [Formula 1].
[Equation 1]
2 1 H 3 H 18 O (liquid) → 2 1 H 3 H (gas) + 18 O 2 (gas)

また、再結合反応は、［数２］式のように行われる。
［数２］
２1Ｈ（gas）＋18Ｏ2（gas）→ ２1Ｈ2 18Ｏ（liquid）
In addition, the recombination reaction is performed as shown in [Formula 2].
[Equation 2]
2 1 H (gas) + 18 O 2 (gas) → 2 1 H 2 18 O (liquid)

本実施例では、図１に示すように、直流電源１に接続された陽極２および陰極３を有する電解セル４の内部に、トリチウム含有ターゲット水ＨＴ18Ｏが導かれて、同電解セル４の内部で電気分解により分子状酸素18Ｏ2とＨＴガスとに分解される作用が行われる。
なお、陽極２と陰極３との間にはＳＰＥ膜５が設けられている。
そして、発生したトリチウムを含むＨＴガスは、煙突10を通じ大気中へ放出される。 In this embodiment, as shown in FIG. 1, tritium-containing target water HT 18 O is led into an electrolytic cell 4 having an anode 2 and a cathode 3 connected to a DC power source 1, and The inside is decomposed into molecular oxygen 18 O 2 and HT gas by electrolysis.
An SPE film 5 is provided between the anode 2 and the cathode 3.
The generated HT gas containing tritium is released into the atmosphere through the chimney 10.

また、上記の分子状酸素18Ｏ2については、第１ボンベ６から導かれたキャリヤーガスＮ2と第２ボンベ７から導かれた水素ガスＨ2とを合流させることにより、結合カラム８を介し容易に無害のＨ2 18Ｏとしてタンク９内に冷却捕集することができる。
そして、余剰ガス（Ｈ2＋Ｎ2）は別の図示しないタンクへ移される。 The molecular oxygen 18 O 2 is combined with the carrier gas N 2 guided from the first cylinder 6 and the hydrogen gas H 2 guided from the second cylinder 7 through the coupling column 8. It can be easily cooled and collected in the tank 9 as harmless H 2 18 O.
The surplus gas (H 2 + N 2 ) is transferred to another tank (not shown).

このようにして、煙突10から大気中へ放出されたＨＴガスは、空気よりも軽いので大気圏上層へ向かって上昇し、安全性が確保されるようになるが、生活圏に存在しても、液体（ターゲット水）に含まれるトリチウムの場合に比べれば、ほとんど無害になるといえる。   In this way, the HT gas released from the chimney 10 into the atmosphere is lighter than air, so it rises toward the upper atmosphere, ensuring safety, but even if it exists in the living sphere, Compared to the case of tritium contained in the liquid (target water), it can be said that it is almost harmless.

ＰＥＴが急速に普及し始めているので、トリチウムの蓄積されたターゲット水の無害化処理が急がれることになるが、トリチウムの蓄積の割合が基準値を超えたターゲット水を処理センターに集めて、本発明の方法により総合的にトリチウム除去処理を施すことが望まれる。   Since PET has begun to spread rapidly, detoxification processing of target water with accumulated tritium will be urgent, but target water whose tritium accumulation rate has exceeded the standard value is collected at the treatment center. It is desirable to perform a tritium removal treatment comprehensively by the method of the present invention.

本発明の一実施例としての方法に用いられる装置を模式的に示す説明図である。It is explanatory drawing which shows typically the apparatus used for the method as one Example of this invention.

符号の説明Explanation of symbols

１ 直流電源
２ 陽極
３ 陰極
４ 電解セル
５ ＳＰＥ膜
６ 第１ボンベ
７ 第２ボンベ
８ 結合カラム
９ タンク
10 煙突 DESCRIPTION OF SYMBOLS 1 DC power supply 2 Anode 3 Cathode 4 Electrolysis cell 5 SPE film 6 1st cylinder 7 2nd cylinder 8 Coupling column 9 Tank
10 Chimney

Claims (1)

陽電子断層診断用医薬品としてのフルオロ・デオキシ・グルコースを合成するため、酸素１８が濃縮されたターゲット水にサイクロトロンで陽子を照射して18Ｏ（ｐ，ｎ）18Ｆ反応により18Ｆを生成する際に、競合核反応である18Ｏ（ｐ，ｔ）16Ｏ反応によって生成されるトリチウム含有ターゲット水について、トリチウムを除去すべく、同トリチウム含有ターゲット水を電解セルへ導いて電気分解により分子状酸素18Ｏ2とＨＴガスとに分解し、流出する上記分子状酸素についてはキャリヤーガスＮ2および水素ガスＨ2を合流させて結合カラムを介しＨ2 18Ｏとして冷却捕集するとともに、上記ＨＴガスは大気中へ放出することを特徴とする、陽電子断層診断用医薬品製造時のトリチウム除去方法。 To synthesize fluoro-deoxy-glucose as a medicament for positron tomography, irradiated with protons in a cyclotron onto a target water oxygen 18 is concentrated 18 O (p, n) 18 when generating F reaction with 18 F In addition, with respect to the tritium-containing target water produced by the 18 O (p, t) 16 O reaction which is a competitive nuclear reaction, in order to remove tritium, the tritium-containing target water is led to an electrolytic cell and electrolyzed to form molecular oxygen. The molecular oxygen that decomposes and flows out into 18 O 2 and HT gas is combined with carrier gas N 2 and hydrogen gas H 2 to be cooled and collected as H 2 18 O through a coupling column, and the HT gas Is a method for removing tritium during the manufacture of a positron emission tomography diagnostic drug, characterized by being released into the atmosphere.
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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR102177105B1 (en) * 2020-07-08 2020-11-10 김정묵 Device and method for safe water regeneration containing oxygen isotope 18

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS60228996A (en) * 1984-04-26 1985-11-14 昭和電工株式会社 Method of processing water containing tritium
JPS61191978A (en) * 1984-10-02 1986-08-26 Fuji Electric Co Ltd Measurement for concentration of tritium in gaseous phase
JPS6338197A (en) * 1986-08-04 1988-02-18 三菱重工業株式会社 Hydrogen isotope gas removing device
JP2004294300A (en) * 2003-03-27 2004-10-21 Sumitomo Heavy Ind Ltd Target device

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS60228996A (en) * 1984-04-26 1985-11-14 昭和電工株式会社 Method of processing water containing tritium
JPS61191978A (en) * 1984-10-02 1986-08-26 Fuji Electric Co Ltd Measurement for concentration of tritium in gaseous phase
JPS6338197A (en) * 1986-08-04 1988-02-18 三菱重工業株式会社 Hydrogen isotope gas removing device
JP2004294300A (en) * 2003-03-27 2004-10-21 Sumitomo Heavy Ind Ltd Target device

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR102177105B1 (en) * 2020-07-08 2020-11-10 김정묵 Device and method for safe water regeneration containing oxygen isotope 18

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