JP2008116280A - Material for collecting radioactive iodine, and collection method therefor - Google Patents
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本発明は、医療施設や原子力施設などで発生した放射性ガスから放射性ヨウ素を捕集除去する捕集材およびその捕集方法に関するものである。 The present invention relates to a collection material for collecting and removing radioactive iodine from a radioactive gas generated in a medical facility or a nuclear facility, and a method for collecting the same.
近年、エネルギー消費量が増加し、それに伴って原子力発電所が多く建設されている。これらの原子力施設等から排出される排出ガス中の放射性ガスは、完全に除去する必要がある。また、原子力施設の増加により、不慮の原子力災害に効果的に対処するため環境における放射性ガスを捕集し、モニタリングすることが重要となっている。また、ラジオアイソトープが大学、各種の研究機関、医療施設等の多くの場所で使用されるようになり、その排気処理やモニタリングが重要となっている。これらの場所で放出される放射性ガス中の放射性成分は主にヨウ素であるが、その捕集材としては主に活性炭が使用されている（特許文献１参照）。 In recent years, energy consumption has increased, and many nuclear power plants have been built accordingly. It is necessary to completely remove the radioactive gas in the exhaust gas discharged from these nuclear facilities. In addition, with the increase in nuclear facilities, it is important to collect and monitor radioactive gases in the environment in order to effectively cope with accidental nuclear disasters. In addition, radioisotopes are used in many places such as universities, various research institutes, medical facilities, etc., and exhaust treatment and monitoring are important. Although the radioactive component in the radioactive gas discharged | emitted in these places is mainly iodine, activated carbon is mainly used as the collection material (refer patent document 1).
活性炭はヨウ素単体に対しては捕集性能を有するが、有機系ヨウ素化合物、特にヨウ化アルキルに変化した場合などは十分な捕集性能を有しない。これに対して有機系ヨウ素化合物の捕集のために、ヨウ化カリウム等の有機系ヨウ素化合物と同位体反応が期待される物質を添着した活性炭や特許文献１のように有機系ヨウ素化合物と直接反応する物質を添着した活性炭を使用することが提案されている。しかしながら、このような従来の活性炭は有機系ヨウ素化合物を吸着した後、多量に脱離を生じてしまうという問題を抱えていた。 Activated carbon has a collection performance for iodine alone, but does not have a sufficient collection performance when it is changed to an organic iodine compound, particularly alkyl iodide. On the other hand, in order to collect organic iodine compounds, activated carbon impregnated with an organic iodine compound such as potassium iodide and a substance expected to undergo an isotope reaction or directly with an organic iodine compound as in Patent Document 1 It has been proposed to use activated carbon impregnated with reacting substances. However, such conventional activated carbon has a problem that a large amount of desorption occurs after adsorption of an organic iodine compound.
この問題を克服するために、平均細孔直径３〜３０ｎｍの細孔容積が０．１５ｃｃ／ｇ以下であって平均細孔直径３ｎｍ以下の細孔容積が０．５０ｃｃ／ｇ以上である繊維状活性炭からなるシートにアミンを添着してなる材料で捕集することにより有機系ヨウ素化合物の脱離を低減せしめ、モニタリング材料としての信頼性を向上させることが提案されている（特許文献２参照）。 In order to overcome this problem, a fibrous shape having an average pore diameter of 3 to 30 nm having a pore volume of 0.15 cc / g or less and an average pore diameter of 3 nm or less having a pore volume of 0.50 cc / g or more. It has been proposed to reduce the elimination of organic iodine compounds by collecting with a material formed by attaching amine to a sheet made of activated carbon to improve the reliability as a monitoring material (see Patent Document 2). .
この方法によって従来に比べて有機系ヨウ素を効率よく捕集できるようになったが、捕集材の寿命は有機系ヨウ素用捕集材が無機系ヨウ素用捕集材に比べて未だ短いのが現状である。また、病院や研究機関などでは発生する放射性ヨウ素がどのような構成成分からなるのかが不明である。このため各施設は排出される放射性ヨウ素が全て有機系ヨウ素であることを前提として排気フィルターの交換目安を設定していることが多い。この場合、各施設において無機系ヨウ素と有機系ヨウ素の含有比率を測定し、無機系ヨウ素の比率が高ければ、排気フィルターやモニタリング材料の使用時間を長くすることが可能である。有機系ヨウ素と無機系ヨウ素を定量的に分離する方法としては、ラジオクラマトグラフを用いる方法（非特許文献１参照）や、無機系ヨウ素をアルカリ水溶液中で捕集し、有機系ヨウ素成分を活性炭フィルターで捕集する方法（非特許文献２参照）が提案されている。しかしながら、これらの方法では設備が複雑なものとなるため、一般の利用施設でモニタリングすることが困難である。 With this method, organic iodine can be collected more efficiently than before, but the life of the collector is still shorter than that of inorganic iodine. Currently. In addition, it is unclear what component the radioactive iodine generated in hospitals and research institutions is composed of. For this reason, each facility often sets replacement guidelines for exhaust filters on the assumption that all of the radioactive iodine emitted is organic iodine. In this case, the content ratio of inorganic iodine and organic iodine is measured at each facility, and if the ratio of inorganic iodine is high, the use time of the exhaust filter and the monitoring material can be extended. As a method for quantitatively separating organic iodine and inorganic iodine, a method using a radiochromatograph (see Non-Patent Document 1), or collecting inorganic iodine in an alkaline aqueous solution, and converting the organic iodine component into activated carbon A method of collecting with a filter (see Non-Patent Document 2) has been proposed. However, these methods make the equipment complicated, and it is difficult to monitor at a general facility.
本発明は、上記従来技術の問題を解消するために創案されたものであり、その目的は、放射性ガスを有機系ヨウ素と無機系ヨウ素に簡易に分別して捕集する材料および方法を提供することにある。 The present invention was devised to solve the above-described problems of the prior art, and its purpose is to provide a material and method for easily separating and collecting radioactive gas into organic iodine and inorganic iodine. It is in.
本発明はかかる問題点に鑑み、鋭意検討した結果得られたものである。
即ち、本発明は、活性炭素繊維シートを用いた放射性ヨウ素捕集材であって、前記活性炭素繊維が少なくとも有機系ヨウ素捕集薬剤を含む層と、前記薬剤を含まない層とから構成されることを特徴とする放射性ヨウ素捕集材である。
また、本発明は、放射性ヨウ素を含有するガスを上記放射性ヨウ素捕集材に一方向から一定風速で通気して放射性ヨウ素を捕集する方法であって、有機系ヨウ素捕集薬剤を含む層を下流側に、前記薬剤を含まない層を上流側に配設して通気することを特徴とする放射性ヨウ素の捕集方法である。
The present invention has been obtained as a result of intensive studies in view of such problems.
That is, the present invention is a radioactive iodine collecting material using an activated carbon fiber sheet, wherein the activated carbon fiber is composed of a layer containing at least an organic iodine collecting agent and a layer not containing the agent. This is a radioactive iodine scavenger.
Further, the present invention is a method for collecting radioactive iodine by aerating a gas containing radioactive iodine through the radioactive iodine collecting material from one direction at a constant wind speed, and comprising a layer containing an organic iodine collecting agent. A method for collecting radioactive iodine, wherein a layer not containing the drug is disposed on the downstream side and ventilated on the downstream side.
本発明によれば、吸着特性の異なる有機系ヨウ素と無機系ヨウ素を同時に捕集でき、かつ分離して捕集できるため、放射性ヨウ素の分離モニタリングが可能となる。これにより、今まで煩雑な方法によって分析されていた有機系ヨウ素と無機系ヨウ素の定量化を簡単に行うことができる。 According to the present invention, organic iodine and inorganic iodine having different adsorption characteristics can be collected at the same time, and separated and collected, so that separation monitoring of radioactive iodine becomes possible. This makes it possible to easily quantify organic iodine and inorganic iodine that have been analyzed by complicated methods.
以下、本発明の放射性ヨウ素捕集材およびその捕集方法を以下に詳細に説明する。
本発明の放射性ヨウ素捕集材は活性炭素繊維シートを用いた放射性ヨウ素捕集材であり、活性炭素繊維シートが少なくとも有機系ヨウ素捕集薬剤を含む層と、前記薬剤を含まない層とから構成されるものである。ガス状の放射性ヨウ素は無機系と有機系に分類される。無機系ヨウ素としてはＩ２、ＨＩＯ３、ＨＩＯ４などが知られ、代表的なものはＩ２である。有機系ヨウ素としてはＣＨ３Ｉ、Ｃ２Ｈ５Ｉが知られ、代表的なものはＣＨ３Ｉである。無機系ヨウ素は活性炭素繊維による吸着特性が非常に高く、吸着速度も高い。また、脱着による再飛散はほとんどないことが知られている。反面、有機系ヨウ素における活性炭素繊維単体での吸着特性は無機系ヨウ素に対する特性に比べてかなり悪く、脱着による再飛散が起こりやすい。そこで、有機系ヨウ素の捕集性能に優れた既知の薬剤を活性炭素繊維に添着することによって有機系ヨウ素の捕集性能が保持される。本発明はこうした活性炭素繊維の捕集特性の差を利用して混在状態にある放射性ヨウ素ガスを分離捕集するものである。具体的には、無機系ヨウ素吸着特性のみに優れる活性炭素繊維シートと、有機系ヨウ素の吸着特性に優れる薬剤が添着された活性炭素繊維を層状に構成することによって捕集材とし、該捕集材シートの一方から捕集ガスを一定時間流通させる。この場合、無機系ヨウ素のみを吸着する活性炭素繊維シート層を上流側に配設し、有機系ヨウ素の吸着特性に優れる薬剤が添着された活性炭素繊維シートを下流側に配設することによって、上流側から入った混合ガスのうち無機系ヨウ素成分が選択的に上流側の活性炭素繊維シートに吸着され、残った有機系ヨウ素が下流側の活性炭素繊維シートに捕集される。一定時間通気することによって有機系ヨウ素と無機系ヨウ素が完全に分離されて捕集される。
Hereinafter, the radioactive iodine collection material and the collection method of the present invention will be described in detail below.
The radioactive iodine collecting material of the present invention is a radioactive iodine collecting material using an activated carbon fiber sheet, and the activated carbon fiber sheet is composed of a layer containing at least an organic iodine collecting agent and a layer not containing the agent. It is what is done. Gaseous radioactive iodine is classified into inorganic and organic types. As inorganic iodine, I 2 , HIO 3 , HIO 4 and the like are known, and a typical one is I 2 . CH 3 I and C 2 H 5 I are known as organic iodine, and a typical one is CH 3 I. Inorganic iodine has very high adsorption characteristics with activated carbon fibers and has a high adsorption rate. It is also known that there is almost no re-scattering due to desorption. On the other hand, the adsorption characteristic of activated carbon fiber alone in organic iodine is considerably worse than that of inorganic iodine, and re-scattering due to desorption is likely to occur. Therefore, the organic iodine collection performance is maintained by attaching a known agent excellent in organic iodine collection performance to the activated carbon fiber. The present invention separates and collects radioactive iodine gas in a mixed state using the difference in the collection characteristics of activated carbon fibers. Specifically, the active carbon fiber sheet excellent only in the inorganic iodine adsorption property and the activated carbon fiber impregnated with the chemical excellent in the organic iodine adsorption property are used as a collection material, and the collection material The collected gas is circulated from one side of the material sheet for a certain period of time. In this case, an activated carbon fiber sheet layer that adsorbs only inorganic iodine is disposed on the upstream side, and an activated carbon fiber sheet to which an agent excellent in organic iodine adsorption properties is attached is disposed on the downstream side, Of the mixed gas entering from the upstream side, the inorganic iodine component is selectively adsorbed on the activated carbon fiber sheet on the upstream side, and the remaining organic iodine is collected on the activated carbon fiber sheet on the downstream side. By aeration for a certain time, organic iodine and inorganic iodine are completely separated and collected.
本発明の捕集材で用いられる活性炭素繊維は、有機系ヨウ素捕集薬剤が添着されない層の場合は公知のいずれのものも利用できる。即ち、活性炭素繊維の原料としては綿、麻などの天然セルロース繊維の他、レーヨン、ポリノジック、溶融紡糸法等による再生セルロース繊維、さらにはポリビニルアルコール繊維、アクリル系繊維、芳香族ポリアミド繊維、架橋ホルムアルデヒド繊維、リグニン繊維、フェノール系繊維、石油ピッチ繊維等の合成繊維が挙げられるが、得られる繊維状活性炭の物性（強度等）や吸着性能の高さの点で再生セルロース繊維、フェノール系繊維、アクリル系繊維を用いて製造することが好ましい。具体的には、これら原料繊維の短繊維あるいは長繊維を用いて製織、製編、不織布化した布帛に必要に応じて適当な耐炎化剤を含有させた後、４５０℃以下の温度で耐炎化処理を施し、次いで５００℃以上１０００℃以下の温度で炭化賦活する方法によって得られたものであって、ＪＩＳ Ｋ １４７７−１９９５にて示されるトルエン吸着量が２５〜６０％でかつ窒素吸着等温線より産出されるＢＥＴ法による比表面積が６００〜２０００ｍ２／ｇである活性炭素繊維を用いることが好ましい。活性炭素繊維の形態としては原料布帛の形態を残した状態、即ち織布、不織布、編地が好ましいが、特に限定されない。繊維状活性炭と他の繊維材料とを混抄した紙状のものも使用可能である。また、これらを複数層積層して接合したものでもよい。 As the activated carbon fiber used in the collecting material of the present invention, any known carbon fiber can be used in the case of a layer to which no organic iodine collecting agent is attached. That is, as raw materials for activated carbon fibers, in addition to natural cellulose fibers such as cotton and hemp, regenerated cellulose fibers by rayon, polynosic, melt spinning, etc., as well as polyvinyl alcohol fibers, acrylic fibers, aromatic polyamide fibers, crosslinked formaldehyde Synthetic fibers such as fiber, lignin fiber, phenolic fiber, petroleum pitch fiber, etc. are mentioned. Regenerated cellulose fiber, phenolic fiber, acrylic in terms of physical properties (strength etc.) and high adsorption performance of the obtained fibrous activated carbon It is preferable to manufacture using a system fiber. Specifically, after adding a suitable flameproofing agent to the fabric made by weaving, knitting or non-woven fabric using the short fibers or long fibers of the raw material fibers as necessary, flameproofing is performed at a temperature of 450 ° C. or lower. It is obtained by a method of performing carbonization activation at a temperature of 500 ° C. or higher and 1000 ° C. or lower, and having a toluene adsorption amount of 25 to 60% as shown in JIS K 1477-1995 and a nitrogen adsorption isotherm. It is preferable to use activated carbon fibers having a specific surface area of 600 to 2000 m 2 / g produced by the BET method. The activated carbon fiber is preferably in the form of the raw material fabric, that is, a woven fabric, a nonwoven fabric, or a knitted fabric, but is not particularly limited. A paper-like material obtained by mixing fibrous activated carbon with other fiber materials can also be used. Moreover, what laminated | stacked these layers and joined may be used.
一方、有機系ヨウ素捕集薬剤が添着される層の場合は公知の活性炭素繊維の中でも特に有機系ヨウ素の再飛散量を少なくできる細孔径の小さいものが好適に使用される。特に平均細孔直径が２ｎｍ以下のものは放射性ガスの吸着速度が増大し、また平均細孔直径３〜３０ｎｍの細孔容積が０．１５ｃｃ／ｇ以下であって平均細孔直径３ｎｍ以下の細孔容積が０．５０ｃｃ／ｇ以上であるものは脱離および加熱による脱着が生じにくくなるため好ましく使用される。ここでいう平均細孔直径及び細孔容積は、例えば高速比表面積・細孔分布測定装置（島津製作所製Ｊｅｍｉｎｉ２３７５）を用いて液体窒素温度における窒素吸着等温線を測定し、所定の式に従って計算することにより求められる。有機系ヨウ素捕集薬剤は公知のものを使用できる。具体的にはアミン系薬剤、特に１，４−ジアザ−２，２，２−ピシクロオクタン（トリエチレンジアミン）、Ｎ，Ｎ'−ビス−（３−アミノプロピル）−ピペラジン、Ｎ，Ｎ−ジメチル−アミノエチルメタクリレート、Ｎ，Ｎ−ジメチルアミノプロピルアミン、３−アミノプロピルトリメトキシシラン、１，５−ジアザビシクロウンデセン、ポリ−３級−ブチルアミノエチルメタクリレート、ポリエチレンイミン、１，５−ジアザピシクロ〔４，３，０〕ノン−５−エン、１，５−ジアザピシクロ〔５，４，０〕ウンデ７−５−エン、２−メチル−１，４−ジアザピシクロ〔２，２，２〕オクタン、フェニルヒドラジン、２−シアノピリジン、ジイソプロピルアミン、トリメチルアミノエチルピペラジン、ヘキサメチレンテトラミン、メチルポリエチレンイミン、ポリアルキルポリアミン等が挙げられる。これらのアミン系薬剤の他には無機系ヨウ化物、特にヨウ化カリウム、ヨウ化ナトリウム、ヨウ化錫が挙げられる。活性炭素繊維の有機系ヨウ素捕集層はこれらの有機系ヨウ素捕集薬剤を活性炭素繊維の単位重量あたり０．１〜２０重量％添着することによって得られる。添着方法としては有機系ヨウ素捕集薬剤を所定の濃度の水溶液にし、該活性炭素繊維シートを数時間含浸させ、脱水した後に乾燥させる方法が挙げられる。 On the other hand, in the case of a layer to which an organic iodine scavenging agent is attached, among the known activated carbon fibers, those having a small pore diameter that can reduce the amount of organic iodine re-scattering are preferably used. In particular, when the average pore diameter is 2 nm or less, the adsorption rate of the radioactive gas is increased, and the pore volume with an average pore diameter of 3 to 30 nm is 0.15 cc / g or less and the average pore diameter is 3 nm or less. Those having a pore volume of 0.50 cc / g or more are preferably used because desorption and desorption due to heating are less likely to occur. The average pore diameter and pore volume mentioned here are calculated according to a predetermined formula by measuring a nitrogen adsorption isotherm at a liquid nitrogen temperature using, for example, a high-speed specific surface area / pore distribution measuring device (Jemi 2375 manufactured by Shimadzu Corporation) Is required. A well-known thing can be used for an organic iodine collection chemical | medical agent. Specifically, amine drugs, particularly 1,4-diaza-2,2,2-picyclooctane (triethylenediamine), N, N′-bis- (3-aminopropyl) -piperazine, N, N-dimethyl -Aminoethyl methacrylate, N, N-dimethylaminopropylamine, 3-aminopropyltrimethoxysilane, 1,5-diazabicycloundecene, poly-tert-butylaminoethyl methacrylate, polyethyleneimine, 1,5-diazapicyclo [4,3,0] non-5-ene, 1,5-diazapicyclo [5,4,0] unde-7-5-ene, 2-methyl-1,4-diazapicyclo [2,2,2] octane, Phenylhydrazine, 2-cyanopyridine, diisopropylamine, trimethylaminoethylpiperazine, hexamethylenetetramine, methyl Examples include reethyleneimine and polyalkylpolyamine. In addition to these amine drugs, inorganic iodides, particularly potassium iodide, sodium iodide, and tin iodide can be mentioned. The organic iodine collection layer of activated carbon fiber is obtained by adding 0.1 to 20% by weight of these organic iodine collection agents per unit weight of activated carbon fiber. Examples of the attaching method include a method in which an organic iodine scavenger is made into an aqueous solution having a predetermined concentration, the activated carbon fiber sheet is impregnated for several hours, dehydrated and then dried.
かくして得られた２種類の活性炭素繊維シートを層状にする。この場合、２種類の活性炭素繊維をどの程度積層するかは使用されるサンプラーによって異なるが、少なくとも有機系ヨウ素捕集薬剤を含む層と該薬剤を含まない層とから構成される必要がある。有機系ヨウ素を捕集する薬剤を含む層のみでシートが構成された場合、有機系ヨウ素と無機系ヨウ素の分離能が好ましくなく、また該薬剤を含まない層のみで構成された場合もまた有機系ヨウ素と無機系ヨウ素が分離されずに捕集率が低下するため好ましくない。この２種類の活性炭素繊維シートは濃度評価時に別々に評価されるため、接合されずにパッケージングされることが望ましい。具体的には、所定の直径と高さを有する紙、金属またはプラスチック製の円筒ケースを用意し、２種類の活性炭素繊維シートを円筒ケース内に積層充填する方法によって得ることができる。円筒ケースにはシート固定用のつめを有し、セッティングした後の活性炭素繊維シートが動かないようにする。測定時においてはケースからシートを順番に取り外し、測定する。 The two types of activated carbon fiber sheets thus obtained are layered. In this case, the degree to which the two types of activated carbon fibers are laminated differs depending on the sampler used, but it is necessary to be composed of at least a layer containing an organic iodine scavenging agent and a layer not containing the agent. When the sheet is composed only of a layer containing a chemical that collects organic iodine, the separation ability of organic iodine and inorganic iodine is not preferable, and when the sheet is composed only of a layer not containing the chemical, it is also organic. Since iodine is not separated from inorganic iodine and the collection rate is lowered, it is not preferable. Since these two types of activated carbon fiber sheets are evaluated separately at the time of concentration evaluation, it is desirable that they are packaged without being joined. Specifically, it can be obtained by a method of preparing a cylindrical case made of paper, metal or plastic having a predetermined diameter and height and laminating and filling two types of activated carbon fiber sheets in the cylindrical case. The cylindrical case has a claw for fixing the sheet so that the activated carbon fiber sheet after setting does not move. At the time of measurement, remove the sheets in order from the case and measure.
また、捕集材の最上流側、および２種類の活性炭素繊維の層間には、除塵機能を有するフィルターが配置されていることが望ましい。これらのフィルターは粒子に付着したヨウ素成分の捕集を目的としており、最上流側のフィルターは大気中の粒子状ヨウ素を捕集し、層間に配設されたフィルターは評価のための通気の間に上流側の層の一部の活性炭素繊維が脱落して下流側の有機系ヨウ素捕集層に移動することを防止するためのもので、エアサンプラー用として用いられる石英繊維からなる濾紙（例えば東洋濾紙株式会社製ＱＲ−１００）やダストモニターとして用いられる濾紙（例えば東洋濾紙株式会社製ＨＥ−４０Ｔ）が好適に用いられる。また、それら以外ではＰＴＦＥ系のフィルターや高分子を用いたメルトブロー不織布などを用いてもよい。また、ポリプロピレンを主体としたメルトブロー不織布は粉塵の捕集率向上のためエレクトレット化して用いてもよい。エレクトレット化の方法は通常コロナ放電によるものが一般的であるが、この方法に限定されない。 Moreover, it is desirable that a filter having a dust removing function is disposed between the uppermost stream side of the collecting material and between the two types of activated carbon fibers. These filters are intended to collect iodine components adhering to the particles, the filter on the most upstream side collects particulate iodine in the atmosphere, and the filter placed between the layers is used for ventilation during evaluation. A filter paper made of quartz fibers used for an air sampler (for example, a filter paper (for example, Toyo Filter Paper QR-100) and filter paper used as a dust monitor (for example, Toyo Filter Paper HE-40T) are preferably used. Other than these, a PTFE filter, a melt blown nonwoven fabric using a polymer, or the like may be used. Further, a melt blown nonwoven fabric mainly composed of polypropylene may be used as an electret for improving the dust collection rate. The electretization method is generally based on corona discharge, but is not limited to this method.
本発明の捕集方法について説明する。本発明の放射性ヨウ素捕集材は面速度が２５〜５０ｃｍ／ｓの一方向からの通気条件において、有機系ヨウ素捕集薬剤を含む層を下流側に、該薬剤を含まない層を上流側に配設して使用することが重要である。使用される活性炭素繊維量は、上流側の有機系ヨウ素捕集薬剤を含まない層および下流側の薬剤を含む層の各々の捕集層の嵩密度が０．０５〜０．２５ｇ／ｃｍ３、好ましくは０．０６〜０．２４ｇ／ｃｍ３で調製され、かつ層厚１．０ｍｍから１５ｍｍ、好ましくは１．５ｍｍから１０ｍｍに充填されることが望ましい。該捕集材の嵩密度は捕集性能と通気圧損を考慮して決定されるが、嵩密度が上記下限未満の場合、必要な捕集性能を得ることができず、捕集率を保持するために必要以上に層厚を長く設定する必要が出てくるため好ましくなく、嵩密度が上記上限より大きい場合、圧力損失が高くなるため必然的に層厚を低く設定する必要が生じ、有機系ヨウ素と無機系ヨウ素を分離するために必要な層厚を保持できなくなるため好ましくない。層厚が１．０ｍｍ未満である場合、捕集された無機系ヨウ素が下流側に移動して誤差を生じる可能性があり、層厚が１５ｍｍ以上の場合、長時間にわたって通気しないと有機系ヨウ素が上流側に残存して誤差を生じる可能性があり、好ましくない。また、本発明における捕集材の通気時間は１０分から９０分、好ましくは１５分から６０分であることが望ましい。通気時間が上記下限未満の場合、有機系ヨウ素と無機系ヨウ素の充分な分離がなされず、通気時間が上記上限を越える場合、捕集された放射性ヨウ素が脱離して再飛散する場合があり、好ましくない。 The collection method of the present invention will be described. The radioactive iodine scavenger of the present invention has a surface velocity of 25 to 50 cm / s in one direction, and a layer containing an organic iodine scavenging agent is on the downstream side, and a layer not containing the agent is on the upstream side. It is important to arrange and use. The amount of activated carbon fiber used is such that the bulk density of each of the collection layers of the layer not containing the upstream organic iodine collection agent and the layer containing the downstream agent is 0.05 to 0.25 g / cm 3. , Preferably 0.06 to 0.24 g / cm 3 , and the layer thickness is 1.0 mm to 15 mm, preferably 1.5 mm to 10 mm. The bulk density of the trapping material is determined in consideration of trapping performance and aeration pressure loss. However, when the bulk density is less than the lower limit, necessary trapping performance cannot be obtained and the trapping rate is maintained. Therefore, it is not preferable because it is necessary to set the layer thickness longer than necessary, and when the bulk density is larger than the above upper limit, the pressure loss becomes high, so it is inevitably necessary to set the layer thickness low, and the organic type This is not preferable because the layer thickness necessary for separating iodine and inorganic iodine cannot be maintained. If the layer thickness is less than 1.0 mm, the collected inorganic iodine may move to the downstream side and cause an error. If the layer thickness is 15 mm or more, organic iodine must be vented for a long time. May remain on the upstream side and cause an error, which is not preferable. Further, the aeration time of the collecting material in the present invention is 10 minutes to 90 minutes, preferably 15 minutes to 60 minutes. If the aeration time is less than the above lower limit, organic iodine and inorganic iodine are not sufficiently separated, and if the aeration time exceeds the upper limit, the collected radioactive iodine may be detached and rescattered. It is not preferable.
以下実施例によって本発明を更に詳述するが、下記実施例は本発明を制限するものではなく、本発明の趣旨を逸脱しない範囲で変更実施することは全て本発明の技術範囲に包含される。なお、物性の測定方法は下記方法に従った。 The present invention will be described in further detail with reference to the following examples. However, the following examples are not intended to limit the present invention, and all modifications that do not depart from the spirit of the present invention are included in the technical scope of the present invention. . The physical properties were measured according to the following methods.
吸着等温線の測定：島津製作所製Ｊｅｍｉｎｉ２３７５を使用し、液体窒素温度（７７Ｋ）にて相対圧０．０２から０．９５までの吸着容量を求めた。
比表面積（Ａｓ）： ＢＥＴ法に基づいて算出した。（相対圧０．０２〜０．１５）
平均細孔直径：吸着等温線を外挿し、相対圧１．００の窒素吸着容量（ｃｍ３／ｇ）を求め、これと密度補正係数（０．００１５４６８）の積を全細孔容積（Ｖｐ）とした。平均細孔直径（Ｄｐ）は数式１によって求められる。
Measurement of adsorption isotherm: Jemi 2375 manufactured by Shimadzu Corporation was used, and the adsorption capacity from a relative pressure of 0.02 to 0.95 was determined at a liquid nitrogen temperature (77 K).
Specific surface area (As): Calculated based on the BET method. (Relative pressure 0.02-0.15)
Average pore diameter: extrapolation of adsorption isotherm, nitrogen adsorption capacity (cm 3 / g) at a relative pressure of 1.00 was determined, and the product of this and density correction coefficient (0.0015468) was the total pore volume (Vp) It was. The average pore diameter (Dp) is obtained by Equation 1.
細孔容積：吸着等温線より求めた。３〜３０ｎｍの細孔容積についてはＢＪＨ（Ｂａｒｒｅｔｔ−Ｊｏｙｎｅｒ−Ｈａｌｅｎｄａ）法により、３ｎｍ以下の細孔容積についてはＭＰ法により求められた細孔分布から算出した。
アミン添着量：アミン水溶液に添着する前の活性炭重量と、添着後１００℃で１時間乾燥した後の活性炭重量の差より計算して求めた。
Pore volume: determined from adsorption isotherm. The pore volume of 3 to 30 nm was calculated by the BJH (Barrett-Joyner-Halenda) method, and the pore volume of 3 nm or less was calculated from the pore distribution determined by the MP method.
Amine addition amount: It was calculated from the difference between the weight of the activated carbon before being attached to the aqueous amine solution and the weight of the activated carbon after being dried at 100 ° C. for 1 hour after the addition.
捕集率：上流側から試料、バックアップフィルターＣＨＣ−５０（アドバンテック東洋製）の順に捕集用ホルダーに装着した。化学反応により発生させたＣＨ３ １３１Ｉを含む調湿された空気を風量５０Ｌ／ｍｉｎで上流側より０〜６０分間流通させた。放射性物質１３１Ｉの放射能は、フィルターの全量またはＣＨＣ−５０の場合は粒状活性炭の一部をガンマカウンター（パーキンエルマージャパンパッカード５００３型）で測定した。試料の捕集率は、最上流側、及び上流側と下流側の間に設けられた濾紙を除いた試料とバックアップフィルターの捕集放射能に関して計算し、試料の各層の捕集放射能を試料の全層とバックアップフィルターの合計の捕集放射能で除して求めた。 Collection rate: A sample and a backup filter CHC-50 (manufactured by Advantech Toyo) were attached to the collection holder in this order from the upstream side. Humidified air containing CH 3 131 I generated by a chemical reaction was circulated for 0 to 60 minutes from the upstream side at an air volume of 50 L / min. The radioactivity of the radioactive substance 131 I was measured with a gamma counter (Perkin Elmer Japan Packard model 5003) for the total amount of the filter or, in the case of CHC-50, a part of the granular activated carbon. The collection rate of the sample is calculated with respect to the collected radioactivity of the sample and the backup filter except the filter paper provided between the upstream and downstream sides and the upstream filter, and the collected radioactivity of each layer of the sample is measured. Divided by the total collected radioactivity of all layers and backup filter.
（実施例１）
目付２１０ｇ／ｍ２、厚み２．８ｍｍ、比表面積１３５０ｍ２／ｇ、嵩密度０．０７５ｇ／ｃｍ３、平均繊維直径２０μｍの活性炭素繊維不織布シートを３層積層し、上流側無機系ヨウ素捕集層とした。さらに目付２００ｇ／ｍ２、厚み２．９ｍｍ、比表面積１４５０／ｇ、平均細孔直径が１．８ｎｍ、平均細孔直径３〜３０ｎｍの細孔容積が０．０３ｃｃ／ｇ、平均細孔直径３ｎｍ以下の細孔容積が０．６０ｃｃ／ｇ以上の活性炭素繊維不織布シートに１，４−ジアザ−２，２，２−ピシクロオクタン（トリエチレンジアミン）を１０重量％添着し、これを３層積層して下流側有機系ヨウ素捕集層とした。最上流側、及び上流側捕集層と下流側捕集層の間に、石英繊維からなる濾紙（東洋濾紙株式会社製ＱＲ−１００）を配設し、これを４８ｍｍφに打ち抜き、内径４８ｍｍφの円筒ケースに設置して捕集剤とした（図１、図２参照）。各シートの１３１Ｉ２、およびＣＨ３ １３１Ｉ捕集率（％）を表１に示す。
(Example 1)
Three layers of activated carbon fiber nonwoven fabric sheets with a basis weight of 210 g / m 2 , a thickness of 2.8 mm, a specific surface area of 1350 m 2 / g, a bulk density of 0.075 g / cm 3 and an average fiber diameter of 20 μm are laminated, and upstream inorganic iodine collection Layered. Furthermore, the basis weight is 200 g / m 2 , the thickness is 2.9 mm, the specific surface area is 1450 / g, the average pore diameter is 1.8 nm, the average pore diameter is 3 to 30 nm, the pore volume is 0.03 cc / g, and the average pore diameter is 3 nm. 10% by weight of 1,4-diaza-2,2,2-picyclooctane (triethylenediamine) is attached to an activated carbon fiber nonwoven fabric sheet having the following pore volume of 0.60 cc / g or more, and three layers are laminated. Thus, a downstream organic iodine collection layer was obtained. A filter paper made of quartz fiber (QR-100 manufactured by Toyo Roshi Kaisha, Ltd.) is disposed between the upstream-most collection layer and the upstream-side collection layer and the downstream-side collection layer, punched into 48 mmφ, and a cylinder with an inner diameter of 48 mmφ. It installed in the case and was set as the collection agent (refer FIG. 1, FIG. 2). The collection rate (%) of 131 I 2 and CH 3 131 I for each sheet is shown in Table 1.
（実施例２）
目付６０ｇ／ｍ２、厚み０．５０ｍｍ、比表面積１３５０ｍ２／ｇ、嵩密度０．１２ｇ／ｃｍ３、繊維径１２μｍの繊維状活性炭からなる編物状シート２枚を目付１５ｇ／ｍ２の熱溶融性接着シート（鞘ＰＶＡ／芯ＰＰ）により８２℃で積層接着してシート化した。このシートを３層積層して上流側無機系ヨウ素捕集層とした。さらに目付６０ｇ／ｍ２、厚み０．５０ｍｍ、比表面積１３５０ｍ２／ｇ、平均細孔直径３〜３０ｎｍの細孔容積が０．０２ｃｃ／ｇ、平均細孔直径３ｎｍ以下の細孔容積が０．５８ｃｃ／ｇ、さらに平均細孔直径が１．７２ｎｍ，繊維径１２μｍの繊維状活性炭からなる編物状シート２枚を目付１５ｇ／ｍ２の熱溶融性接着シート（鞘ＰＶＡ／芯ＰＰ）により８２℃で積層接着してシート化した。このシートに１，４−ジアザ−２，２，２−ピシクロオクタン（トリエチレンジアミン）を１４重量％添着し、これを３層積層して下流側有機系ヨウ素捕集層とした。最上流側、及び上流側捕集層と下流側捕集層の間に、石英繊維からなる濾紙（東洋濾紙株式会社製ＱＲ−１００）を配設し、これを４８ｍｍφに打ち抜き、内径４８ｍｍφの円筒ケースに設置して捕集剤とした（図１、図２参照）。各シートの１３１Ｉ２、およびＣＨ３ １３１Ｉ捕集率（％）を表２に示す。
(Example 2)
Thermal fusion of two knitted sheets made of fibrous activated carbon having a basis weight of 60 g / m 2 , a thickness of 0.50 mm, a specific surface area of 1350 m 2 / g, a bulk density of 0.12 g / cm 3 , and a fiber diameter of 12 μm. Laminated at 82 ° C. with a conductive adhesive sheet (sheath PVA / core PP) to form a sheet. Three layers of this sheet were laminated to form an upstream inorganic iodine collection layer. Furthermore, the basis weight is 60 g / m 2 , the thickness is 0.50 mm, the specific surface area is 1350 m 2 / g, the pore volume with an average pore diameter of 3 to 30 nm is 0.02 cc / g, and the pore volume with an average pore diameter of 3 nm or less is 0.00. Two knitted sheets made of fibrous activated carbon having an average pore diameter of 1.72 nm and a fiber diameter of 12 μm were obtained at a temperature of 82 ° C. by a heat-melt adhesive sheet (sheath PVA / core PP) having a basis weight of 15 g / m 2. And laminated to form a sheet. To this sheet, 14% by weight of 1,4-diaza-2,2,2-picyclooctane (triethylenediamine) was impregnated, and three layers thereof were laminated to form a downstream organic iodine collection layer. A filter paper made of quartz fiber (QR-100 manufactured by Toyo Roshi Kaisha, Ltd.) is disposed between the upstream-most collection layer and the upstream-side collection layer and the downstream-side collection layer, punched into 48 mmφ, and a cylinder with an inner diameter of 48 mmφ. It installed in the case and was set as the collection agent (refer FIG. 1, FIG. 2). The collection rate (%) of 131 I 2 and CH 3 131 I for each sheet is shown in Table 2.
（比較例１）
粒状活性炭シートＣＰ−２０（東洋濾紙株式会社）４７ｍｍφ３枚を積層して上流側無機系ヨウ素捕集層とした。またＣＰ−２０の１，４−ジアザ−２，２，２−ピシクロオクタン（トリエチレンジアミン）１０重量％添着品を３枚積層して下流側有機系ヨウ素捕集層とした。最上流側、及び上流側捕集層と下流側捕集層の間に、石英繊維からなる濾紙（東洋濾紙株式会社製ＱＲ−１００）４７ｍｍφを配設し、これを内径４７ｍｍφの円筒ケースに設置して捕集剤とした（図１、図２参照）。各シートの１３１Ｉ２、およびＣＨ３ １３１Ｉ捕集率（％）を表３に示す。
(Comparative Example 1)
Granular activated carbon sheet CP-20 (Toyo Roshi Kaisha, Ltd.) 47 mmφ3 was laminated to form an upstream inorganic iodine collection layer. In addition, three 10 wt% 1,4-diaza-2,2,2-picyclooctane (triethylenediamine) impregnation products of CP-20 were laminated to form a downstream organic iodine collection layer. 47mmφ of filter paper (QR-100 manufactured by Toyo Roshi Kaisha, Ltd.) made of quartz fiber is placed between the upstream and upstream collection layers and the downstream collection layer, and this is installed in a cylindrical case with an inner diameter of 47mmφ. Thus, a collecting agent was obtained (see FIGS. 1 and 2). Table 3 shows 131 I 2 and CH 3 131 I collection rates (%) of the respective sheets.
本発明によれば、有機系ヨウ素と無機系ヨウ素を同時に分離して捕集できるため、放射性ヨウ素の分離モニタリングが可能であり、有機系ヨウ素と無機系ヨウ素の定量化を簡単に行なうことができる。 According to the present invention, since organic iodine and inorganic iodine can be separated and collected simultaneously, separation monitoring of radioactive iodine is possible, and organic iodine and inorganic iodine can be easily quantified. .
１ ： 捕集材シート単体
２ ： 捕集材シート積層体（上流側：薬剤未添着）
３ ： 捕集材シート積層体（下流側：薬剤添着）
４ ： 粒子捕集用濾紙
５ ： 捕集材固定用円筒ケース
1: Collection material sheet simple substance 2: Collection material sheet laminated body (upstream side: chemical unattached)
3: Collection material sheet laminate (downstream side: chemical attachment)
4: Filter paper for collecting particles 5: Cylindrical case for fixing collection material
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| JP2006298774A JP2008116280A (en) | 2006-11-02 | 2006-11-02 | Material for collecting radioactive iodine, and collection method therefor |
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| JP2006298774A JP2008116280A (en) | 2006-11-02 | 2006-11-02 | Material for collecting radioactive iodine, and collection method therefor |
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