JP6218357B2 - Method and apparatus for separating and removing radioactive cesium contained in waste water - Google Patents
Method and apparatus for separating and removing radioactive cesium contained in waste water Download PDFInfo
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- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 title claims description 60
- 230000002285 radioactive effect Effects 0.000 title claims description 60
- 238000000034 method Methods 0.000 title claims description 24
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 60
- 238000001179 sorption measurement Methods 0.000 claims description 58
- 229910021536 Zeolite Inorganic materials 0.000 claims description 31
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 31
- 239000010457 zeolite Substances 0.000 claims description 31
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- 229910052680 mordenite Inorganic materials 0.000 claims description 3
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- 229910052732 germanium Inorganic materials 0.000 description 1
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Description
本発明は、排水、とくに放射性物質の除染により発生した排水や、汚染された可燃物を焼却処理する一般廃棄物処分場からの浸出水に含まれる放射性セシウムを、簡易に分離除去する方法と、その方法の実施に使用する装置に関する。 The present invention is a method for easily separating and removing radioactive cesium contained in wastewater, particularly wastewater generated by decontamination of radioactive materials, and leachate from a general waste disposal site that incinerates contaminated combustible materials. And an apparatus used for carrying out the method.
原子力発電所から放出された放射性物質のうち、放射性セシウム(以下「134Cs、137Cs」と記すことがある)は、広い範囲に拡散してさまざまな物の表面に付着し、または内部に含有されており、半減期が長く長期にわたってその影響が続くことから、その安全かつ簡易な除去が当面の重要な課題となっている。 Among the radioactive material released from the nuclear power plants, (sometimes hereinafter referred to as "134 Cs, 137 Cs") radioactive cesium diffuses over a wide range adhered to the surface of various objects, or contained within Therefore, since the half-life is long and the influence continues for a long time, the safe and easy removal is an important issue for the time being.
放出された放射性セシウムは、風にのって遠距離まで運ばれたものが降雨とともに地上に落ち、屋根に積もったり、雨樋や側溝に流れたりしたほか、農作物や樹木に付着している。建造物の除染作業に伴い発生する排水には、ほとんどが水溶性の化合物となっている放射性セシウムが含有されている。一方、樹木からの落ち葉のような可燃物は、都市ゴミ最終処分場において焼却炉で焼却されると、含まれていた放射性セシウムの大部分は、主として飛灰に濃縮される。出願人は、焼却灰および飛灰中の放射性セシウムを濃縮して分離する技術を確立し、すでに開示した(特許文献1)。
飛灰はセメント固化され、不燃残渣、余剰炉砂や、し尿処理施設余剰汚泥焼却灰などとともに埋め立て処分されており、その放射能が埋立て基準とされている8,000Bq/kg以下であれば、そのまま埋立て可能である。しかし、多量の降雨などによって埋立地が湛水し、飛灰セメント固化物から放射性セシウムが溶出すれば、浸出水の放射能濃度は許容限度を容易に超えてしまう。そうなれば、浸出水は、その中の放射性セシウムを除去した上でなければ排出することができない。 Fly ash is solidified in cement and disposed of in landfill with incombustible residue, surplus furnace sand, surplus sludge incineration ash, etc. If the radioactivity is 8,000 Bq / kg or less, which is the landfill standard It can be landfilled as it is. However, if the landfill is flooded due to heavy rainfall and radioactive cesium is eluted from the fly ash cement solidified material, the radioactive concentration of the leachate easily exceeds the allowable limit. In that case, the leachate can only be discharged after removing the radioactive cesium in it.
発明者らは、他の共同研究者らと、一般廃棄物処理場からの浸出水に含まれる放射性セシウムを分離除去して浸出水を放流可能にする手段を求めて研究し、無機系の吸着剤、とりわけモルデナイト系のゼオライトを浸出水に接触させ、放射性セシウムを吸着除去するのが適切であることを確認した。この確認実験については、後述する。さらに、これも後述のように、いったん吸着された放射性セシウムはゼオライトから溶出しないこと、したがって、放射性セシウムを吸着したゼオライトは埋立て処分しても安全であることが確認できた。 The inventors studied with other collaborators for a means to separate and remove radioactive cesium contained in the leachate from the general waste treatment plant so that the leachate can be discharged. It was confirmed that it was appropriate to bring the agent, especially mordenite zeolite, into contact with the leachate and adsorb and remove radioactive cesium. This confirmation experiment will be described later. Further, as described later, it was confirmed that once adsorbed radioactive cesium does not elute from the zeolite, and therefore, the zeolite adsorbed with radioactive cesium can be safely disposed of in landfill.
こうした事実に基づけば、浸出水に含まれる放射性セシウムを除去するには、浸出水を放流するための処理工程のどこかでゼオライトの粉末を投入し、浸出水中に分散させて十分な接触をさせることにより、放射性セシウムを吸着することが効果的である。既存の浸出水処理設備は、通常、つぎのようなフローに従っており、それぞれの工程に使用する装置が設けてある。
[調整槽]→[反応槽]→[第一混和槽]→[第一凝集槽]→[第一沈殿槽]→[生物処理工程]→[第二凝集処理工程]→[濾過・活性炭処理工程]
このような設備において浸出水にゼオライトを接触させる操作を行なおうとすれば、処理工程の初めに設けてある調整槽を利用することが得策である。調整槽は一般に撹拌機能を持っているので、ゼオライト粉末の分散にそのまま利用できる。しかし、ゼオライト粉末が調整槽の隅に堆積してしまい、調整槽から長期間放射線が出ることになるので、浚渫が必要になる。
Based on these facts, in order to remove the radioactive cesium contained in the leachate, the zeolite powder is introduced somewhere in the treatment process for discharging the leachate and dispersed in the leachate to ensure sufficient contact. Therefore, it is effective to adsorb radioactive cesium. Existing leachate treatment facilities usually follow the following flow, and are equipped with devices used for each process.
[Adjustment tank] → [Reaction tank] → [First mixing tank] → [First coagulation tank] → [First precipitation tank] → [Biological treatment process] → [Second coagulation process] → [Filtering / activated carbon treatment] Process]
If an operation to bring the zeolite into contact with the leachate in such an installation is performed, it is advantageous to use the adjustment tank provided at the beginning of the treatment process. Since the adjusting tank generally has a stirring function, it can be used as it is for dispersing the zeolite powder. However, since zeolite powder accumulates in the corner of the adjustment tank and radiation is emitted from the adjustment tank for a long time, soot is required.
そうした不利益を避けてゼオライト粉末による処理を実施するとなれば、上記の凝集処理工程において粉末を一定量添加して放射性セシウムの吸着除去を行ない、凝集剤で沈殿させ、脱水処理してケークとし、それを埋立て処分する、という操作が考えられる。しかし、この方式は、粉末状ゼオライトを使用する際に粉塵が発生するので防塵が必要になるという問題に加えて、放射性セシウムを含んだゼオライトのスラリーやケークを取扱う過程における、作業員の被爆の危険が大きいという問題がある。 If processing with zeolite powder is carried out avoiding such disadvantages, a certain amount of powder is added in the above aggregation processing step to perform adsorption removal of radioactive cesium, precipitation with a flocculant, dehydration treatment to make a cake, An operation of landfilling it can be considered. However, this method, in addition to the problem that dust is generated when using powdered zeolite, requires dust prevention, and in the process of handling zeolite slurries and cakes containing radioactive cesium, There is a problem that the danger is great.
この問題の解決を意図して、発明者らは、粉粒状のものを運搬するために常用されているフレキシブルコンテナー(「フレコン」と通称されているので、以下この語を用いる。)を利用すること、ゼオライトを粉末でなく粒子状としてフレコンに充填して使用し、使用済みのものはそのまま埋立て処分に回す、という実用的な技術を確立することに成功した。さらに、粒子状ゼオライトをフレコンに充填した吸着手段は、一般廃棄物処分場からの浸出水だけでなく、さまざまな除染作業にともなって発生する排水中の放射性セシウムの吸着除去にも効果的に使用できることを確認した。 In order to solve this problem, the inventors use a flexible container (commonly referred to as “flexible container”, which is commonly used to carry powdered particles). In addition, we have succeeded in establishing a practical technique in which zeolite is used in the form of particles instead of powder in a flexible container and used ones are sent to landfill as they are. In addition, the adsorption means filled with particulate zeolite in FIBC is effective not only for the leachate from general waste disposal sites but also for the adsorption and removal of radioactive cesium in wastewater generated by various decontamination operations. Confirmed that it can be used.
したがって本発明の目的は、発明者らの得た知見を利用し、上記した排水、とくに一般廃棄物処理場からの浸出水や、除染作業に伴って発生する排水(以下、単に「排水」という。)に含まれる放射性セシウムの分離除去をゼオライトにより行なうための、短時間で設置できコストがかからない簡易な設備を用い、防塵対策の必要なく、かつ、作業員の放射線への被曝を実質上防止して、特段のノウハウを要することなく実施できる技術を提供することにある。 Therefore, the object of the present invention is to utilize the knowledge obtained by the inventors, and the above-described wastewater, particularly leachate from a general waste treatment plant, and wastewater generated during decontamination work (hereinafter simply referred to as “drainage”). The use of simple equipment that can be installed in a short time and does not cost much to separate and remove the radioactive cesium contained in the product), eliminates the need for dust-proof measures, and effectively exposes workers to radiation. It is to provide a technology that can be implemented without requiring special know-how.
この目的を達成する本発明の方法は、処理すべき排水(以下「被処理水」という。)に含まれる放射性セシウムを分離除去する方法であって、図3にみるように、
フレコンの外径(DF)より大きな内径(DT)をもつ有底筒状体であり、その底部近くに水平なストレーナ(2)をそなえ、最上部に被処理水(WR)の供給管(8)が開口するとともに、上部に処理済み水(WT)の排出口(3)を備えた吸着タンク(1)の内部に、側面にラミネート(6)を施して透水性を失わせ、または不透水性の生地を用い、その一方で底面にはメッシュ生地(7)を用いて透水性を高めたフレコンバッグ(5)の内部に吸着剤(Ab)を充填したものを配置し、上記供給管から被処理水を供給してフレコンの吸着剤に接触させ、降下する被処理水に含まれる放射性セシウムを吸着させて水から分離し、放射性セシウムを含有しなくなった処理済み水をフレコン底部のメッシュを通して吸着タンクの側方を上昇させ、上記排出口を通して排出し、放射性セシウムを吸着した吸着剤を収容するフレコンは吸着タンクから取出すことからなる方法である。
The method of the present invention that achieves this object is a method for separating and removing radioactive cesium contained in wastewater to be treated (hereinafter referred to as “treated water”), as shown in FIG.
A bottomed cylindrical body having a larger inner diameter (D T) outer diameter (D F) of the flexible container, the bottom portion includes a horizontal strainer (2) near the supply of the water to be treated (W R) at the top A pipe (8) is opened and a laminate (6) is applied on the side to the inside of the adsorption tank (1) equipped with a treated water (W T ) outlet (3) at the top to lose water permeability. Or, using a water-impermeable fabric, on the bottom, a mesh container (7) is used to place a flexible container bag (5) filled with an adsorbent (Ab) inside a flexible container bag (5), The treated water is supplied from the supply pipe and brought into contact with the adsorbent of the flexible container, and the radioactive cesium contained in the falling treated water is adsorbed and separated from the water, and the treated water that does not contain the radioactive cesium is removed from the flexible container. The side of the adsorption tank through the mesh at the bottom Raising, and discharged through the discharge port, FIBC which houses an adsorbent that has adsorbed the radioactive cesium is a method which consists in taking the adsorption tank.
上記の方法に使用する本発明の装置は、排水に含まれる放射性セシウムを分離除去する装置であって、図1および図2に示すような、下記の構成部分からなる装置である。
イ)図1に示すフレコンの外径(DF)より大きな内径(DT)をもつ、図2に示す有底筒状体であって、最上部に被処理水(WR)の供給管(8)が開口し、底部近くに水平なストレーナ(2)を、上部に処理済み水(WT)の排出口(3)を、また底部にドレン管(4)を備えた吸着タンク(1)、
ロ)図1に示す、フレコンバッグ(5)の側面にラミネート(6)を施して透水性を失わせ、または不透水性の生地を用い、その一方で、底面にはメッシュ生地(7)を用いて透水性を高めたフレコンの内部に、吸着剤(Ab)を充填したもの、
ハ)被処理水および処理済み水を移送するためのポンプ(図示してない)、および
ニ)放射性セシウム未吸着の吸着剤を収容したフレコンを吊り下げて吸着タンク内に配置し、また、放射性セシウム吸着済みの吸着剤を収容しているフレコンを吊り上げて吸着タンクから取り出すためのクレーン(図示してない)。
The apparatus of the present invention used in the above method is an apparatus for separating and removing radioactive cesium contained in waste water, and is an apparatus comprising the following components as shown in FIGS.
B) the outer diameter of the flexible container shown in FIG. 1 (D F) larger inner diameter with (D T), a bottomed tubular body shown in FIG. 2, the supply pipe of the water to be treated (W R) at the top (8) is open, an adsorption tank (1) equipped with a horizontal strainer (2) near the bottom, an outlet (3) for treated water (W T ) at the top, and a drain pipe (4) at the bottom. ),
B) Laminate (6) is applied to the side of the flexible container bag (5) shown in FIG. 1 to lose water permeability or use a water-impermeable fabric, while a mesh fabric (7) is used on the bottom surface. What is filled with adsorbent (Ab) inside the flexible container that has increased water permeability using
C) A pump (not shown) for transporting treated water and treated water, and d) a flexible container containing a non-adsorbing adsorbent for radioactive cesium, suspended in an adsorption tank, and radioactive. A crane (not shown) for lifting a flexible container containing an adsorbent that has adsorbed cesium and removing it from the adsorption tank.
本発明の技術によって排水に含まれる放射性セシウムを分離除去すれば、粒子状の吸着剤を一定量フレコンに充填してあるものを使用するため、まず、粉末の使用に伴って必要になる防塵対策が不要である。凝集沈殿の対象にゼオライト粉末が加わらないため、凝集剤を余分に使用する必要もなく、かつスラリーの濾過や発生したケークの取扱いに代えて、フレコンを上記吸着タンクから運び出すだけで足りる。このように、操作はきわめて簡単であって、特段のノウハウないしスキルを必要としないから、任意の清掃工場、廃棄物処分場、さらには除染の現場において、容易に実施することができる。 If the radioactive cesium contained in the wastewater is separated and removed by the technology of the present invention, since a fixed amount of particulate adsorbent is filled in a flexible container, first, dust prevention measures that are necessary with the use of powder Is unnecessary. Since zeolite powder is not added to the target of coagulation sedimentation, it is not necessary to use extra coagulant, and instead of filtering the slurry and handling the generated cake, it is only necessary to carry out the FIBC from the adsorption tank. In this way, the operation is very simple and does not require special know-how or skills, so that it can be easily carried out at any cleaning factory, waste disposal site, and decontamination site.
設備面でも、粉末の定量投入のための設備が不要であり、濾過装置も不要であって、フレコンを装入して浸出水と接触させる吸着タンクを設けるだけで足りる。好ましい態様に従って、吸着剤として粒子状のものを使用すれば、被処理水がフレコン内部の吸着剤に対して行き渡り、上方から下方に向かう平行な流れとなって下るから、均等で十分な接触が行なわれる。粉末を使用すれば吸着平衡に近いレベルまで被処理水に含まれていた放射性セシウムが吸着除去されるところ、粒子状であれば吸着量はそれに及ばないものの、後記する好ましい態様で実施すれば吸着剤の効率的な使用が可能であり、懸念するほどの差は出ない。 In terms of equipment, there is no need for equipment for quantitative powder injection, and no filtration device is required, and it is sufficient to install an adsorber tank in which a flexible container is inserted and brought into contact with leachate. According to a preferred embodiment, if a particulate material is used as the adsorbent, the water to be treated spreads over the adsorbent inside the flexible container and falls in a parallel flow from the upper side to the lower side. Done. If the powder is used, the radioactive cesium contained in the water to be treated is adsorbed and removed to a level close to the adsorption equilibrium. Efficient use of the agent is possible and there is no appreciable difference.
供給管開口を出た被処理水に含有されていた放射性セシウムは、吸着剤に吸着されて吸着タンクの中で蓄積されて行くが、フレコンは周囲を処理済み水と吸着タンクの壁で囲まれているので、外部に出る放射線は減衰し、周辺で作業にあたる作業員が被爆する危険は低い。放射性セシウムを含んだ吸着剤の取扱いが、フレコンの取出しと運搬だけで足りるから、埋立て処分の完了に至るまで被爆の心配が少ない。 The radioactive cesium contained in the treated water exiting the supply pipe opening is adsorbed by the adsorbent and accumulated in the adsorption tank, but the flexible container is surrounded by the treated water and the adsorption tank wall. As a result, the radiation emitted to the outside is attenuated, and the risk of exposure to workers working in the vicinity is low. Since handling of the adsorbent containing radioactive cesium is sufficient only to take out and transport the flexible container, there is little concern about exposure until the landfill disposal is completed.
本発明の除去方法を実施すべき段階としては、前記の浸出水を対象とする処理フローに適用する場合であれば、まず排水を調整槽に集水した段階が考えられる。通常、調整槽は大容量の地下タンクとして設置されるので、地上に吸着タンクを設置して、そこに吸着剤入りのフレコンを配置し、ポンプアップした被処理水を吸着剤に接触させた後、反応槽に送ることになる。浸出水の放射性セシウム含有量が高い場合には、まずその低減が緊急の課題であるから、この実施態様が必要であるか、または少なくとも好ましい。 As a stage at which the removal method of the present invention should be carried out, a stage in which wastewater is first collected in a regulating tank can be considered if it is applied to the treatment flow for leachate. Normally, the adjustment tank is installed as a large-capacity underground tank. After installing an adsorption tank on the ground, placing a flexible container with an adsorbent there, and bringing the treated water pumped up into contact with the adsorbent , Will be sent to the reaction vessel. This embodiment is necessary or at least preferred if the leachate has a high radioactive cesium content, since its reduction is an urgent task first.
一方、浸出水が含有する放射性セシウムがそれほど高濃度ではない場合、吸着剤との接触は、処理フローの任意の段解で行なうことができる。その中でも、最終の濾過・活性炭処理工程が終了し、放流に先立つ段階が適切である。その理由は、吸着処理に先だって活性炭処理を行なえば、活性炭によりその他の不純物が吸着除去されるため、吸着剤に吸着される放射性セシウム以外の成分が減少しており、吸着剤の使用効率が高まるということにある。 On the other hand, when the radioactive cesium contained in the leachate is not so high, the contact with the adsorbent can be performed at any stage of the treatment flow. Among these, the final filtration and activated carbon treatment process is completed, and the stage prior to discharge is appropriate. The reason is that if the activated carbon treatment is performed prior to the adsorption treatment, other impurities are adsorbed and removed by the activated carbon, so the components other than radioactive cesium adsorbed on the adsorbent are reduced, and the use efficiency of the adsorbent is increased. That is to say.
しかしながら、何らかの原因で浸出水に含有される放射性セシウムの量が急激に増大する可能性がある環境であれば、上記の調整槽段階の吸着除去の設備も備えておき、ふだんは後段の、処理フロー終了後の吸着除去だけを行ない、緊急事態が発生したときは前段の、調整槽段階の吸着除去を先立てて前段・後段の吸着除去を併用する、という態様が安全であろう。 However, if there is a possibility that the amount of radioactive cesium contained in the leachate will increase sharply for some reason, it will also be equipped with the above-mentioned adsorption tank equipment for adsorption removal, usually at the later stage. It may be safe to perform only the adsorption removal after the end of the flow, and in the event of an emergency, the first stage and the rear stage adsorption removal are used in combination with the first stage, prior to the adjustment tank stage.
吸着剤の吸着能力の低下は、フレコンから流出する処理済み水の線量を、たとえば吸着タンクの側面において上昇する水を対象に測定することによって、継続的に知ることができる。線量の値が一定のレベルを超えたとき、余力が失われたと判定するわけである。吸着剤が吸着余力を失ったならば、フレコンを吊り上げて吸着タンクから取り出し、それに代えて新しい吸着剤を充填したフレコンを配置し、被処理水を供給して吸着を継続すればよい。放射性セシウムを吸着した吸着剤を収容しているフレコンは、水切り処理をしたのち埋立て場所に運び、そのまま埋立て処分すればよい。 The decrease in the adsorption capacity of the adsorbent can be continuously detected by measuring the dose of treated water flowing out of the flexible container, for example, on the water rising on the side of the adsorption tank. When the dose value exceeds a certain level, it is determined that the remaining power is lost. If the adsorbent loses the adsorption capacity, the flexible container is lifted and taken out from the adsorption tank, and a flexible container filled with a new adsorbent is placed in place of it, and the water to be treated is supplied to continue the adsorption. The flexible container containing the adsorbent adsorbing the radioactive cesium can be drained and then transported to a landfill, where it can be disposed of as landfill.
吸着タンクの構造に関し、図示した例では、説明の便宜のため、吸着タンクの側壁内部は単なる円筒形とし、底部は平面的なストレーナとして示した。しかし、被処理水の接触の間、側壁に沿って流れる水の量または速度を各所で均等に保つことが、フレコン内部の被処理水の平行な流れの実現にとって好ましい。このためには、吸着タンク内部でフレコンの形状を一定に保つことが必要であり、その目的で、吊り下げて配置したフレコンの中心線が吸着タンクの中心線と一致して維持されるよう、フレコンの側面においてその長さの一部または全部をカバーするように、ストレーナをパレット状に形成することが好ましい。 Regarding the structure of the adsorption tank, in the illustrated example, for the convenience of explanation, the inside of the side wall of the adsorption tank is shown as a simple cylinder and the bottom is shown as a planar strainer. However, during the contact of the water to be treated, it is preferable to realize the parallel flow of the water to be treated inside the flexible container to keep the amount or speed of the water flowing along the side wall even in each place. For this purpose, it is necessary to keep the shape of the flexible container inside the adsorption tank constant, and for that purpose, the center line of the flexible container arranged in a suspended manner is maintained in line with the central line of the adsorption tank. It is preferable that the strainer is formed in a pallet shape so as to cover a part or all of the length on the side surface of the flexible container.
以下の参考例は、発明者らが他の共同研究者らと協力して行なった試験のデータである。
一般廃棄物処分場浸出水中の放射性セシウム
伊勢崎市の清掃リサイクルセンター21の一般廃棄物処分場の第三期埋立地において、平成23年9月12日の台風12号がもたらした大量の降雨のため生じた浸出水の原水、および、それを常用の、すなわち前記した処理フローによって処理した最終処理水が含有する放射性セシウムの量は、つぎの表1のとおりであった。
The following reference examples are data of tests conducted by the inventors in cooperation with other collaborators.
Radiocesium in leachate from general waste disposal site Mass produced by Typhoon No. 12 on September 12, 2011 at the third landfill site of the general waste disposal site of the cleaning and recycling center 21 in Isesaki City Table 1 below shows the amount of radioactive cesium contained in the raw water of the leachate generated due to the rain and the final treated water that was used, that is, treated by the treatment flow described above.
表1
ここで「濃度限度比」は、処理水が示した放射線量の放流可能な限度に対する比であって、下記の式によって定義される値である。
濃度限度比=(Cs-134濃度)[Bq/L]/60[Bq/L]+(Cs-137濃度)[Bq/L]/90[Bq/L]
Table 1
Here, the “concentration limit ratio” is the ratio of the radiation dose indicated by the treated water to the limit at which discharge is possible, and is a value defined by the following equation.
Concentration limit ratio = (Cs-134 concentration) [Bq / L] / 60 [Bq / L] + (Cs-137 concentration) [Bq / L] / 90 [Bq / L]
放射性セシウムの分析は、ゲルマニウム半導体検出器(Ganberra MODEL)によるガンマ線スペクトロメトリー(1992年 文部科学省「放射能測定シリーズ7」に準拠)により行なった。検出限界は、134Cs、137Csともに、10Bq/kgまたは10Bq/Lである。 Radioactive cesium was analyzed by gamma-ray spectrometry using a germanium semiconductor detector (Ganberra MODEL) (according to 1992, Ministry of Education, Culture, Sports, Science and Technology "Radioactivity Measurement Series 7"). The detection limit is 10 Bq / kg or 10 Bq / L for both 134 Cs and 137 Cs.
ゼオライトを用いた平衡吸着試験
上記の原水および最終処理水それぞれ300mLに対して、モルデナイト系天然ゼオライトを粉末状にしたものを、2.5g、5g、25gまたは50g添加し、往復振とう機により24時間振とうした。その後、孔径0.45μmのメンブレンフィルターで濾過し、濾液について放射能を測定した。結果は下記の表2および表3に示すとおりである。
Equilibrium adsorption test using zeolite 2.5 g, 5 g, 25 g, or 50 g of mordenite-based natural zeolite in powder form are added to 300 mL of the above raw water and final treated water, respectively. Shake for 24 hours with a machine. Then, it filtered with the membrane filter with the hole diameter of 0.45 micrometer, and radioactivity was measured about the filtrate. The results are as shown in Table 2 and Table 3 below.
表2 原水
*134Csおよび137Csが検出限界濃度で存在するとして算出
Table 2 Raw water
* Calculated assuming that 134 Cs and 137 Cs exist at the detection limit concentration.
表3 最終処理水
*同上
Table 3 Final treated water
* Same as above
ゼオライトからの溶出試験
上記の結果から、放射性セシウムの濃度が高い原水であってもゼオライトを10g/L使用すればほとんど吸着除去できることがわかったので、その条件で使用したゼオライトから放射性セシウムが、使用済みゼオライトの埋立地から、たとえば多量の降雨による湛水によって溶出するおそれがないか、つぎのようにして確認した。すなわち、13.5Bq/gの放射性セシウムを吸着したゼオライト10gを蒸留水1000mL中に分散させ、24時間振とうし、その後、前記と同じメンブレンフィルターで濾過して、濾液の放射能を測定した。その結果を、吸着試験のデータと併せて、表4に示す。表4にみるとおり、放射性セシウムの量は検出限度以下であって、いったんゼオライトに吸着された放射性セシウムは、溶出しないと考えてよいことが確認できた。
Elution test from zeolite From the above results, it was found that even if the raw water with a high concentration of radioactive cesium was used, it was found that the adsorption could be removed almost by using 10 g / L of zeolite. It was confirmed as follows whether cesium was likely to be eluted from the landfill site of spent zeolite, for example, by flooding due to heavy rainfall. That is, 10 g of zeolite adsorbed with 13.5 Bq / g of radioactive cesium was dispersed in 1000 mL of distilled water, shaken for 24 hours, and then filtered through the same membrane filter as above, and the radioactivity of the filtrate was measured. The results are shown in Table 4 together with the adsorption test data. As seen in Table 4, the amount of radioactive cesium was below the detection limit, and it was confirmed that the radioactive cesium once adsorbed on the zeolite may be considered not to elute.
表4 吸着−溶出試験
Table 4 Adsorption-elution test
フレコンバッグ
図1に示す形状を有する、下記の仕様のフレコンバッグを用意した。材質は、各部分ともPP(ポリプロピレン)繊維の織布である。
容量/質量:1000L/1000kg
本 体:1100mmφ×1100mmH
側面の外周全面にわたりPPフィルムをラミネート
投入口:1100mmφ×800mmH
排出口:なし
底 面:全面メッシュ生地、底支えロープ補強
吊ベルト:70mm幅×2本
Flexible container bag A flexible container bag having the shape shown in FIG. 1 and having the following specifications was prepared. The material of each part is a woven fabric of PP (polypropylene) fiber.
Capacity / mass: 1000L / 1000kg
Body: 1100mmφ x 1100mmH
PP film laminating slot over the entire outer periphery of the side: 1100mmφ × 800mmH
Discharge port: None Bottom surface: Full mesh fabric, bottom support rope reinforced hanging belt:
吸着タンク
一方、図2に示す構造の、ポリエチレン製で蓋と底とをもつ円筒形で、底部にストレーナ(2)を備え、側面上部に処理済み水排出口(3)、底部にドレン管(4)を備えた吸着タンク(1)を、下記の寸法で製作した。蓋は、フレコンの出入時は外す構造である。
高 さ:1560mm
内 径:1420mm
ストレーナ高さ:底面から100mm
排出口高さ:底面から1410mm
この吸着タンク内に、上記のフレコンバッグに粒状ゼオライト800kgを充填したものを吊り下げて装入する。吸着タンクの内壁とフレコンとの間には160mmの空隙があって、ストレーナを通過した水がそこを上昇する。
Adsorption tank On the other hand, it is made of polyethylene and has a cylindrical shape with a lid and a bottom. An adsorption tank (1) equipped with a drain pipe (4) was manufactured with the following dimensions. The lid is structured to be removed when the flexible container is in and out.
Height: 1560mm
Inner diameter: 1420mm
Strainer height: 100mm from the bottom
Discharge port height: 1410mm from the bottom
In this adsorption tank, the above flexible container bag filled with 800 kg of granular zeolite is suspended and charged. There is a 160 mm gap between the inner wall of the adsorption tank and the flexible container, and the water that has passed through the strainer rises there.
緊急処理
前記した、台風のもたらした降雨に起因して発生した、放射性セシウムを高い濃度で含有する浸出水(総計1820m3)を放流可能なものにするため、つぎの処理をした。すなわち、粉末状のゼオライトを常用の処理フローのために設置されている2基の調整槽に投入した。吸着タンクは2基製作し、浸出水処理の最後段階で行なうよう、処理フローの最終段階である濾過・活性炭処理工程のつぎに位置させて直列に接続し、それぞれの内部に粒状ゼオライト800kgを充填したフレコンを装入した。被処理水は、まず調整槽においてゼオライト粉末に接触して放射性セシウムの吸着除去を受けた後、フローにしたがった処理を受け、さらに上記のゼオライト吸着タンクを通過して(空間速度SV=5)吸着除去を受けてから再度調整槽に返送し、循環処理を行なった。
Emergency treatment In order to be able to discharge leachate containing a high concentration of radioactive cesium (total 1820 m 3 ) generated due to the typhoon-induced rainfall, the following treatment was performed. . That is, the powdery zeolite was put into two adjustment tanks installed for a regular processing flow. Two adsorption tanks are manufactured and connected in series after the filtration and activated carbon treatment process, which is the final stage of the treatment flow, so that it is performed at the final stage of the leachate treatment, and each inside is filled with 800 kg of granular zeolite. The flexible container which was done was inserted. First, the water to be treated comes into contact with the zeolite powder in the adjustment tank and is subjected to adsorption removal of radioactive cesium, and then undergoes treatment according to the flow, and further passes through the zeolite adsorption tank (space velocity SV = 5). After receiving the adsorption removal, it was returned to the adjustment tank again and circulated.
調整槽へのゼオライト粉末の投入を5〜6日おきに4回行ない、合計15.2トンを投入した。一方、2基の吸着タンクにはそれぞれ800kgの粒状ゼオライトを充填したフレコンが装入してあるから、使用したゼオライトは総計16.8トンになる。この緊急処理を受けた浸出水中の放射性セシウムの濃度変化を示せば、図4のとおりである。図において、「T−Cs」は、134Csと137Csの合計をあらわす。処理開始後23日を経過したとき、最終処理水中の放射性セシウム濃度が検出限界以下となり、放流可能となった。 The zeolite powder was charged into the adjustment tank four times every 5 to 6 days, and a total of 15.2 tons was charged. On the other hand, each of the two adsorption tanks is filled with flexible containers filled with 800 kg of granular zeolite, so the total amount of zeolite used is 16.8 tons. If the concentration change of the radioactive cesium in the leachate which received this emergency treatment is shown, it will be as FIG. In the figure, “T-Cs” represents the total of 134 Cs and 137 Cs. When 23 days passed from the start of the treatment, the concentration of radioactive cesium in the final treated water was below the detection limit, and discharge was possible.
定常処理
放射性セシウムを高濃度に含有する浸出水の緊急処理が済んで放流した後は、さらに2基の吸着タンクを設置し、粒子状ゼオライトそれぞれ800kgを充填したフレコンを装入して、調整槽の前段に位置させた。ただし、この設備は放射性セシウム濃度の急激な上昇に備えたもので、検出される線量が低ければパスさせ、常用のフローを通したのち、活性炭処理が済んだ後、前記したさきに設置した2基の直列に接続した吸着タンクで粒状ゼオライトによる吸着除去を行なって、処理済み水を放流している。
Steady-state treatment After the emergency treatment of leachate containing high concentration of radioactive cesium, after discharging it, two more adsorption tanks were installed and charged with flexible containers filled with 800 kg of particulate zeolite. And placed in the front stage of the adjustment tank. However, this equipment was prepared for a rapid increase in the concentration of radioactive cesium, and if the detected dose was low, it was passed, and after passing through a normal flow, the activated carbon treatment was completed, and it was installed 2 above. Adsorption removal with granular zeolite is performed in an adsorption tank connected in series, and treated water is discharged.
以上本発明を、一般廃棄物最終処分場の浸出水に関して生じた放射性セシウム分離除去の必要に対処して行なった試験に例をとって説明したが、容易に理解されるように、本発明の放射性セシウム分離除去の技術は、さまざまな除染作業の結果発生する排水中に含まれる放射性セシウム分離除去に当っても適用可能であって、全体の処理フローをどのように組み立てるべきか、また、本発明の方法をそのフローのどの局面で適用したらよいかは、当業者が状況に応じて適宜選択することができるであろう。 Although the present invention has been described above by taking an example of a test conducted in response to the need for separation and removal of radioactive cesium generated in relation to leachate from a general waste final disposal site, as will be easily understood, The radioactive cesium separation and removal technology can be applied to the separation and removal of radioactive cesium contained in wastewater generated as a result of various decontamination operations. Which aspect of the flow the method of the present invention should be applied to can be appropriately selected by those skilled in the art depending on the situation.
1 吸着タンク
2 ストレーナ
3 処理済み水の排出口
4 ドレン管
5 フレコンバッグ
6 ラミネート
7 メッシュ生地
8 被処理水の供給管
Ab 吸着剤
DF フレコンの外径
DT 吸着タンクの内径
WR 被処理水
WT 処理済み水
1 the inner diameter W R-treatment water of the outer diameter D T adsorption tank of the
Claims (5)
イ)フレコンバッグの外径(DF)より大きな内径(DT)をもつ有底筒状体であって、最上部に被処理水(WR)の供給管(8)が開口し、底部近くに水平なストレーナ(2)を、上部に処理済み水(WT)の排出口(3)を、また底部にドレン管(4)を備えた吸着タンク(1)、
ロ)側面にラミネート(6)を施して透水性を失わせ、または不透水性の生地を用い、その一方で、底面にはメッシュ生地(7)を用いて透水性を高め、内部に吸着剤(Ab)を充填するフレコンバッグ(5)であって、前記吸着タンク内において、前記供給管に対して下方、かつ、前記ストレーナ上に配置されるフレコンバッグ(5)、
ハ)被処理水および処理済み水を移送するためのポンプ、および
ニ)放射性セシウム未吸着の吸着剤を収容したフレコンバッグを吊り下げて吸着タンク内に配置し、また、放射性セシウム吸着済みの吸着剤を収容しているフレコンバッグを吊り上げて吸着タンクから取り出すためのクレーン、を備え、
前記吸着タンクの内壁と前記フレコンバッグとの間には、前記フレコンバッグの前記メッシュ生地および前記ストレーナを通過した水が、前記フレコンバッグの周囲を囲むように上昇する間隔を有し、
前記排出口は、前記吸着タンクの内壁と前記フレコンバッグとの間の間隔と連通している、装置。 An apparatus for separating and removing radioactive cesium contained in waste water,
B) A bottomed cylindrical body having an inner diameter (DT) larger than the outer diameter (DF) of the flexible container bag, and a supply pipe (8) for water to be treated (WR) is opened at the top and horizontally near the bottom A strainer (2), an adsorption tank (1) with a treated water (WT) outlet (3) at the top and a drain pipe (4) at the bottom,
B) Laminate (6) on the side surface to lose water permeability or use a water-impermeable fabric, while the bottom surface uses a mesh fabric (7) to increase water permeability and adsorbent inside A flexible container bag (5) filled with (Ab), wherein the flexible container bag (5) is disposed below the supply pipe and on the strainer in the adsorption tank;
C) A pump for transporting treated water and treated water, and d) a flexible container bag containing an adsorbent that has not been adsorbed with radioactive cesium, suspended in an adsorption tank, and adsorbed with radioactive cesium adsorbed A crane for lifting the flexible container bag containing the agent and taking it out from the adsorption tank,
Between the inner wall of the adsorption tank and the flexible container bag, there is an interval in which the water passing through the mesh fabric and the strainer of the flexible container bag rises so as to surround the flexible container bag,
The discharge port is in communication with an interval between an inner wall of the adsorption tank and the flexible container bag.
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US4087375A (en) * | 1975-05-07 | 1978-05-02 | Shin Tohoku Chemical Industry Co., Ltd. | Method for treating radioactive waste water |
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