JPS614530A - Radioactive nuclide and heavy metal collecting material - Google Patents
Radioactive nuclide and heavy metal collecting materialInfo
- Publication number
- JPS614530A JPS614530A JP12297984A JP12297984A JPS614530A JP S614530 A JPS614530 A JP S614530A JP 12297984 A JP12297984 A JP 12297984A JP 12297984 A JP12297984 A JP 12297984A JP S614530 A JPS614530 A JP S614530A
- Authority
- JP
- Japan
- Prior art keywords
- collection
- immersed
- acrylic fibers
- mno2
- collecting material
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
Description
【発明の詳細な説明】 （イ）発明の目的 本発明は放射性核種および重金属等の捕集材である。[Detailed description of the invention] (b) Purpose of the invention The present invention is a collection material for radionuclides, heavy metals, etc.
本発明は原子力発電所、放射性同位元素取扱等事業所を
始めとする原子力施設から発生する放射性廃液中に含ま
れる放射性核種の分離除去および“海洋河川“あるいは
産業廃水等に含まれている放射性核種および重金属等の
分離除去に利用される。The present invention is directed to the separation and removal of radionuclides contained in radioactive waste fluid generated from nuclear facilities such as nuclear power plants and radioisotope handling facilities, and the separation and removal of radionuclides contained in "marine rivers" or industrial wastewater. It is also used for separating and removing heavy metals, etc.
従来の技術
原子力発電所（水型）、放射性同位元素取扱事業所等各
種原子力施設から発生する放射性廃液には各種放射性核
種が含まれている。これらの放射性廃液の処理において
は、被曝低減の観点などから廃液中に含まれる放射性核
種を分離除去して放射線レベルを低減させることが必要
である。又、海洋河川中には微量ではあるが６０ＣＯ１
５４Ｍｎ、９０Ｓｒ、６５ｚｎ、１３７Ｃ８など種々の
人工性核種の存在が確認されており、これらの放射性核
種の濃度および分布に関するデータを長期間にわたり蓄
積することは海洋学、海洋生態学また中低レベル放射性
廃棄物の海洋投棄などの観点から重要なことである。BACKGROUND OF THE INVENTION Radioactive waste fluid generated from various nuclear power facilities, such as nuclear power plants (water type) and facilities that handle radioactive isotopes, contains various radionuclides. In the treatment of these radioactive waste liquids, it is necessary to separate and remove radionuclides contained in the waste liquids to reduce the radiation level from the perspective of reducing exposure. Also, although it is a small amount, 60CO1 is present in oceanic rivers.
The existence of various artificial nuclides such as 54Mn, 90Sr, 65zn, and 137C8 has been confirmed, and it is important to accumulate data on the concentration and distribution of these radionuclides over a long period of time in order to study oceanography, marine ecology, and medium- and low-level radioactivity. This is important from the perspective of preventing waste from being dumped into the ocean.
従来、放射性廃液中の放射性核種の分離・除去あるいは
海洋河川からの放射性核種および重金属の回収には主と
して凝集沈殿法およ、びイオン交換法が利用されている
。Conventionally, coagulation-sedimentation methods and ion exchange methods have been mainly used to separate and remove radionuclides from radioactive waste liquids or to recover radionuclides and heavy metals from marine rivers.
凝集沈殿法は、廃液に凝集剤を混合して放射性物質の電
荷を中和し、これを凝集させて大きな分子の集団、すな
わちフロックを生成させ、このフロックを沈降、分離さ
せる処理方法で、一般にＡｃ１（ＳＯ４）３ ＋ Ｃａ
（ＯＨ）２ 、粘土（＋高分子凝集剤）、ＦｅＣｌ３
＋Ｎａ２Ｓ 、 Ｎａ３ＰＯ４＋Ｃａ（ＯＨ）２等が凝
集剤として使用されている。この方法は、小量ないし複
雑な廃液の処理には、手数がかかる割に除染係数は大き
くなるが安価簡便であり、単純な液質の大量廃液を肌理
するのに適するので広く用いられている。イオン交換法
は各種合成陽イオン交換体、合成陰イオン交換体、混床
イオン交換樹脂、あるいは石炭、褐炭、泥炭等をベース
とする天然有機交換体、グリンサイド、カオリナイト、
ゼオライ処理を行う方法である。かかる凝集沈殿法およ
びイオン交換法によって廃液を処理するとき放射能は各
々スラッジ（汚泥）および再生廃液に濃縮される。非放
射性廃液の場合には浄化された水を得さえすればこれら
濃縮液は一般に放置廃棄されるのであるが、放射性廃液
の場合には濃縮放射能を再拡散させず保持固定するため
二次処理が必要である。現在、かかるスラッジ、再生廃
液は沈降、砂床口過、加圧口過、真空口過、遠心分離、
オートクレーブ処理等の二次処理方法で脱水減容をはか
った後固型化が施されているが、これらの二次処理によ
る減容比は各々く１．４．５〜１０．１０〜１５．２５
〜３５および２〜４というのが実情である。The coagulation-sedimentation method is a treatment method in which a flocculant is mixed with the waste liquid to neutralize the electric charge of the radioactive material, and this is coagulated to produce a group of large molecules, that is, a floc, and this floc is settled and separated. Ac1(SO4)3 + Ca
(OH)2, clay (+polymer flocculant), FeCl3
+Na2S, Na3PO4+Ca(OH)2, etc. are used as flocculants. This method is widely used for treating small volumes or complex waste liquids, although it requires a lot of work and a large decontamination coefficient, but it is cheap and simple, and is suitable for cleaning large quantities of simple liquid waste liquids. There is. The ion exchange method uses various synthetic cation exchangers, synthetic anion exchangers, mixed bed ion exchange resins, natural organic exchangers based on coal, lignite, peat, etc., greenside, kaolinite,
This method involves zeolite treatment. When wastewater is treated by such coagulation-sedimentation and ion exchange methods, radioactivity is concentrated into sludge and recycled wastewater, respectively. In the case of non-radioactive waste liquids, these concentrated liquids are generally disposed of as long as purified water is obtained, but in the case of radioactive waste liquids, secondary treatment is required to retain and fix the concentrated radioactivity without re-diffusion. is necessary. Currently, such sludge and recycled waste liquid are processed through sedimentation, sand bed filtration, pressure filtration, vacuum filtration, centrifugation,
Solidification is performed after dehydration and volume reduction using secondary treatment methods such as autoclave treatment, but the volume reduction ratios due to these secondary treatments are 1.4.5 to 10.10 to 15. 25
-35 and 2-4 are the actual circumstances.
上述した理由により、各種原子力事業所から発生する放
射性廃液に含まれ６放射性核種・海洋河 イ用
あるいは産業廃水等に含まれる放射性核種あるいは重金
属を効率よく分離・除去し且つ減容比が高い捕集材が斯
界で望まれていた。For the reasons mentioned above, it is possible to efficiently separate and remove 6 radionuclides contained in radioactive waste fluids generated from various nuclear power plants, radionuclides or heavy metals contained in marine or industrial wastewater, etc., and to achieve a high volume reduction ratio. Collection of materials was desired in this industry.
本発明者等はアクリル繊維に一般式に２Ｍ■［’ Ｆｅ
Ｃ（ＣＮ）６〕ＣＭＨはコバルト、亜鉛、＝ノケル等
２価の金属〕で表わされるフェロシアン酸塩化合物を担
持・固定して成る放射性核種および重金属捕集材（以下
ゝゝ捕捕集−ＫＣＦＣ“と略記する場合がある）を開発
してすでに特許出願した〔特願昭５９−°り特開昭
〉〕。捕集あることがわかった。そこで本発
明者等は鋭意研の開発に成功した。The present inventors have applied the general formula 2M [' Fe to acrylic fibers.
C(CN)6 [CMH is a divalent metal such as cobalt, zinc, or nokel] A radioactive nuclide and heavy metal trapping material (hereinafter referred to as a trapping material) is made by supporting and fixing a ferrocyanate compound represented by cobalt, zinc, or a divalent metal such as Nokel. KCFC (sometimes abbreviated as "KCFC") has been developed and a patent application has been filed.
〉〕. It turned out that there was a catch. Therefore, the present inventors succeeded in developing the Eiriken.
発明が解決しようとする問題点
本発明によって捕集効率および減容比の高い放射性核種
および重金属捕集材が提供される、本発明によってｐＨ
７〜９の範囲で放射性廃液、海洋河川あるいは産業廃水
中に含まれる放射性核種特に５４Ｍ＋１．５９Ｆ、 ６
０ｏｏ、 ６５Ｚｎ］０３＋１０６．ｕ。Problems to be Solved by the Invention The present invention provides a radionuclide and heavy metal trapping material with high collection efficiency and volume reduction ratio.
Radioactive nuclides contained in radioactive waste liquids, marine rivers or industrial wastewater in the range of 7 to 9, especially 54M + 1.59F, 6
0oo, 65Zn]03+106. u.
１３４＋］３７ｃ３．１４４ｃｅ を多量のＮａ十
存在下にぢいてもほぼ１００％の高い効率で捕集し且つ
高い比率で減容される捕集材が提供される。134+]37c3.144ce with a large amount of Na+
Provided is a collection material that can collect with a high efficiency of almost 100% even in the presence of water and whose volume is reduced at a high rate.
本発明によって深属海水中の微量放射性核種を採水現場
で捕集することが可能な捕集材が提供される。The present invention provides a collection material capable of collecting trace amounts of radionuclides in deep seawater at a water sampling site.
本発明によって解決される問題点は以下逐次間らかにさ
れる。The problems solved by the present invention will be successively identified below.
口）発明の構成
問題点を解決するための手段
上述した問題点は捕集材−ＫＣＦＣとアクリル繊堆にＭ
ｎＯ２を担持・固定した捕集材（以下ゝゝゝ集１オーＭ
ｎＯ２“と略記する場合がある）を捕集装置内に混合し
て使用するか、両袖集材を連結して使用することによっ
て解決される。更に、別法としては上述した問題点は、
アクリル繊維に一般式に２Ｍ■ＣＦｅ （ＣＮ）６ ］
で表わされるフェロシアン酸塩化合物（、ｈ、ｈ−ｃ−
ＭｕはＣｏ、 Ｚｎ、 Ｎｉ、 Ｚｒ等２価金属から選
ばれる一種）およびＭｎＯ２を同時に担持・固定１−た
捕集材（以下“捕集材−ＫＣＦＣ＋ＭｎＯ２“ と略記
する場合がある）を使用することによって解決される。(1) Means for solving the structural problems of the invention The above-mentioned problems are solved by using M
A collection material that supports and fixes nO2 (hereinafter referred to as a collection of 1 Ohm
This can be solved by mixing ``nO2'' (sometimes abbreviated as ``nO2'') in the collection device or by connecting both sleeves of collected material.Furthermore, as an alternative method, the above-mentioned problems can be solved by:
2M■CFe (CN)6 in general formula for acrylic fiber]
A ferrocyanate compound represented by (, h, h-c-
Mu is a type selected from divalent metals such as Co, Zn, Ni, and Zr) and MnO2 are supported and fixed at the same time (hereinafter sometimes abbreviated as "collection material-KCFC+MnO2"). This is solved by
以下、本発明の捕集材の製造方法の一態様について述べ
る。Hereinafter, one embodiment of the method for manufacturing the collection material of the present invention will be described.
アクリル繊維１００Ｆを１０％フェロンアン化カリウム
水溶液に浸漬し３時間加温し、取り出した後、１０％Ｍ
■（ＮＯ３）２ （ＭｎはＣｏ１Ｚｎ 、 Ｎｉ 。Acrylic fiber 100F was immersed in a 10% potassium ferronanide aqueous solution, heated for 3 hours, taken out, and 10% M
■(NO3)2 (Mn is Co1Zn, Ni.
Ｚｒ等２価の金属）水溶液に浸漬し３時間加温した後水
洗後６０〜７０ ’Ｃで１０時間乾燥し、この操作を３
回繰返すことによってアクリル繊維に一般式に２Ｍ”
［Ｆｅ （ＣＮ） ６ ：］ （ＭＩＩはＣｏ、 Ｎｉ
、 ＺｎＳＺｒ等２価の金属）を担持・固定させた赤褐
色の捕集材が製造される。Divalent metal such as Zr) was immersed in an aqueous solution, heated for 3 hours, washed with water, and dried at 60-70'C for 10 hours.
The general formula for acrylic fiber is 2M” by repeating it several times.
[Fe (CN) 6:] (MII is Co, Ni
, ZnSZr, and other divalent metals) are supported and fixed thereon. A reddish-brown collection material is produced.
捕集材−Ｍｎ０２
アクリル繊維］００Ｊを０．５Ｍ過マンガンカリａ
ｔ″水溶液に４日間浸漬し繊維が黒色を示
はら引き上げ過剰の過マンガン酸カリウムを純水で洗浄
したのち、６０〜７０ ℃で乾燥することによってアク
リル繊維にＭｎＯ２を担持・固定させた黒色の捕集材が
製造される。Collection material - Mn02 acrylic fiber] 00J with 0.5M permanganese potassium a
The fibers were immersed in a t'' aqueous solution for 4 days, turned black, pulled up, washed with pure water to remove excess potassium permanganate, and dried at 60 to 70°C to produce a black colored acrylic fiber with MnO2 supported and fixed. A collection material is manufactured.
捕集材−ＫＣ，Ｆ Ｃ＋Ｍｎ Ｏ２
アクリル繊維１０Ｏｒを１０％フェロンアン化カリウム
水溶液に浸漬し３時間加温し、取り出した後、１０％Ｍ
■（ＮＯ３） ２ （ＭｌｌはＣ０１Ｚｎ、Ｎｉ、Ｚｒ
等２価の金属水溶液に浸漬し３時間加温した後水洗後６
０〜７０℃で１０時間乾燥する。この操作を３回繰返し
再び０．５Ｍ過マンガン酸カリウム水溶液に４日間浸漬
し、繊維が黒色を示したら引き上げ過剰の過マンガン酸
カリウムを純水で洗浄したのち６０〜７０℃で乾燥する
ことによってアクリル繊維に一般式Ｋ２ＭＩＩ（Ｆｅ（
ＣＮ）６）で表わされるフェロシアン酸塩化合物および
ＭｎＯ２を同時に担持・固定した捕集材が製造される。Collection material - KC, FC + Mn O2 Acrylic fiber 10Or was immersed in 10% potassium ferronanide aqueous solution, heated for 3 hours, taken out, and 10% Mn O2
■(NO3) 2 (Mll is C01Zn, Ni, Zr
After immersing in a divalent metal aqueous solution and heating for 3 hours, washing with water 6
Dry at 0-70°C for 10 hours. This operation was repeated three times, and the fibers were immersed in a 0.5M potassium permanganate aqueous solution for 4 days. When the fibers turned black, they were pulled up, washed with pure water to remove excess potassium permanganate, and then dried at 60 to 70°C. General formula K2MII (Fe(
A collection material is produced in which a ferrocyanate compound represented by CN)6) and MnO2 are simultaneously supported and fixed.
又、別の方法としては、アクリル繊維１００７を１ｏ％
Ｍｌｌ（Ｎｏ３）２（Ｍｌｌは前述した通り）水溶液７
浸清１３時間加Ｌ・取９出ｌ後”°％７
ンエロシアン化カリウム水溶液に浸漬し３時間加温し
た後水洗後６０〜７０℃で１０時間乾燥する。In addition, as another method, acrylic fiber 1007 is 10%
Mll (No. 3) 2 (Mll is as described above) aqueous solution 7
After soaking for 13 hours and removing 9 liters ”°% 7
The sample was immersed in an aqueous potassium erocyanide solution, heated for 3 hours, washed with water, and dried at 60 to 70°C for 10 hours.
この操作を３回繰返し再び上述した０、５Ｍ過マンガン
酸カリウム水溶液による処理以下の処理を施すことによ
っても捕集材−ＫＣＦＣ＋ＭｎＯ２が製造される。A collection material -KCFC+MnO2 is also produced by repeating this operation three times and performing the following treatment with the 0.5 M potassium permanganate aqueous solution described above.
本発明者等が本発明以前に開発した捕集材−Ｋ ＣＦ
ＣはＪ３４＋ｌ３７Ｃ８，５９Ｆｅ、−６５Ｚｎ、およ
び１４４Ｃｅ等をほぼ１００％捕集することが出来るが
５４Ｍｎを高捕集率で捕集することが出来ない。Collection material developed by the present inventors prior to the present invention - K CF
C can collect almost 100% of J34+l37C8, 59Fe, -65Zn, 144Ce, etc., but cannot collect 54Mn at a high collection rate.
一方、本発明の捕集材の一部を構成する捕集材−八’１
ｎ０２は５４Ｍｎの他６５ｚｎおよび１４４Ｃｅ 等
を１００％捕集することが出来る。而って、捕集材−Ｋ
ＣＦＣおよび捕集材−Ｍｎ０２を捕集装置内に混合して
入れるか、両袖集材を連結して使用することによって５
４１ＶＩｎ、 ５９Ｆ、 ６０Ｃｏ、 ６５Ｚｎ
、 １３４＋］３７Ｃ３および１４４Ｃｅ等を１００％
捕集することが出来る。更に、捕集材−Ｋ ＣＦ Ｃと
捕集材−Ｍｎ０２を併用する代りにアクリルＭ維にに２
Ｍ” （Ｆｅ （ＣＮ） ６ ）（ＭＩＩは前述した通
り）で表わされるフエロシアント庄塩化合物およびＭｎ
Ｏ２を同時に担持・固定させた抽隅材−Ｋ ＣＦ Ｃ４
ＭｎＯ２を使用しても同じ捕集効果を得ることが出来る
。On the other hand, the collection material-8'1 constituting a part of the collection material of the present invention
n02 can collect 100% of 65zn, 144Ce, etc. in addition to 54Mn. So, the collection material-K
By mixing CFC and collection material-Mn02 into the collection device, or by using both sleeves of collection material connected,
41VIn, 59F, 60Co, 65Zn
, 134+] 100% of 37C3 and 144Ce, etc.
It can be collected. Furthermore, instead of using the collection material-KCF C and the collection material-Mn02 together, 2
A ferrocyant salt compound represented by M” (Fe (CN) 6 ) (MII is as described above) and Mn
Bolt corner material that simultaneously supports and fixes O2 - K CF C4
The same trapping effect can be obtained using MnO2.
本発明の捕集材を製造するのに使用されるアクリル繊維
は繊径１８μｍ、８ｗｔ％のアクリル酸メチルを共重合
したものでアニオン基として０．０５ｍｅｑ／ｇ繊維の
ＳＯ３−を含有している。３０％以下の塩酸、硝酸、硫
酸等の耐酸性は非常に強く、逆に耐アルカリ性は弱く１
％水酸化ナトリウム溶液でも変性する。The acrylic fiber used to produce the collection material of the present invention has a fiber diameter of 18 μm, is copolymerized with 8 wt% methyl acrylate, and contains 0.05 meq/g fiber SO3- as an anion group. . Acid resistance of 30% or less, such as hydrochloric acid, nitric acid, and sulfuric acid, is very strong, while alkali resistance is weak.
% sodium hydroxide solution.
本発明の捕集材はｐＨ７〜９の範囲Ｑ ５４Ｍｎ、６５
Ｚｎ、５９Ｆ、 ６０Ｃｏ１１０３＋１０６Ｒｕ、
１３７Ｃ８および１４４ｃｅを略々１００％捕集する。The collection material of the present invention has a pH range of 7 to 9 Q 54Mn, 65
Zn, 59F, 60Co1103+106Ru,
Almost 100% of 137C8 and 144ce are collected.
更に重要なことは多量のＮａ＋の存在下においても上記
核種を捕集することが出来るという特徴をもっている。More importantly, it has the characteristic of being able to collect the above-mentioned nuclides even in the presence of a large amount of Na+.
本発明の捕集材は放射性廃液の態様によって使い分ける
ことが好ましい、例えば軽水Ｐ−次冷却水系中の放射性
核種を分離・除去するにはフェロシアン化コバルト舎カ
リウムに替えてフェロシアン化ニンケル・カリウムおよ
び二酸化マンガンを担持・固定させた捕集材を用いる方
が好ましい。It is preferable to use the collection material of the present invention depending on the type of radioactive waste liquid. For example, in order to separate and remove radionuclides in a light water P-cooling water system, ferrocyanide nickel potassium ferrocyanide should be used instead of ferrocyanide cobalt potassium. It is preferable to use a collection material supporting and fixing manganese dioxide.
以下実施例および参考例によって本発明をより具体的に
説明する。The present invention will be explained in more detail below using Examples and Reference Examples.
実施例−捕集材の製造
材料および試薬
（ａ） アクリル繊維：繊径１８μｍ、８ｗｔ％のア
クリル酸メチルを共重合したもので、アニオン基として
０．０５ ｍｅｑ／ｇ繊維の５ｏ３−を含有している。Examples - Materials and reagents for manufacturing the collection material (a) Acrylic fiber: Copolymerized with 8 wt% methyl acrylate with a fiber diameter of 18 μm, containing 0.05 meq/g fiber of 5O3- as an anion group. ing.
（ｂ） フェロシアン化カリウム：試薬特級（ｃ）
硝酸コバルト：試薬特級
（ｄ） 過マンガン酸カリウム：試薬特級実施例−１
捕集材−Ｍｎ０２
アクリル繊維１００Ｊを０．５Ｍ過マンガン酸カリウム
溶液に４日間浸漬し繊維が黒色を呈したら引き上げ過剰
の過マンガン酸カリウムを純水で洗浄したのち６０〜７
０℃で乾燥することによって黒色の綿状捕集材−Ｍｎ０
２を製造した。(b) Potassium ferrocyanide: special reagent grade (c)
Cobalt nitrate: Reagent special grade (d) Potassium permanganate: Reagent special grade Example-1 Collection material - Mn02 100 J of acrylic fibers are immersed in a 0.5M potassium permanganate solution for 4 days, and when the fibers turn black, the excessive After washing potassium permanganate with pure water, 60-7
Black flocculent absorbent - Mn0 by drying at 0 °C
2 was manufactured.
実施例−２
捕集材−ＫＣＦＣ
アクリル繊維１０ｏｚを１０％フェロシアン化カリウム
溶液に浸漬し３時間加温した。取り出した後、１０％硝
酸コバルト溶液に浸漬し３時間加温した。水洗後６０°
〜７ｏ℃で１０時間乾燥した。Example-2 Collection material - KCFC 10 oz of acrylic fiber was immersed in a 10% potassium ferrocyanide solution and heated for 3 hours. After taking it out, it was immersed in a 10% cobalt nitrate solution and heated for 3 hours. 60° after washing
It was dried at ~7oC for 10 hours.
この操作を３回繰り返してアクリル繊維にフェロシアン
化コバルト、カリウム（Ｋ２Ｃｏ［Ｆｅ （ＣＮ） ６
１ ）を担持・固定した赤褐色の綿状捕集材−ＫＣＦＣ
を製造した。This operation was repeated three times to coat the acrylic fiber with cobalt ferrocyanide and potassium (K2Co[Fe (CN) 6
1) Reddish brown cotton-like collection material supporting and fixing - KCFC
was manufactured.
実施例−３
捕集材−ＫＣＦＣ＋ＭｎＯ２
アクリル繊維１００１を１０％フェロシアン化カリウム
水溶液に浸漬し３時間加温した。取り出した後、１０％
硝酸コバルト水溶液に浸漬し３時間加温した。水洗後６
０°Ｃ〜７０℃で１０時間乾燥した。この操作を３回繰
り返し、再び０．５Ｍ過マンガンカリウム水溶液に４日
間浸漬し、繊維が黒色を示したら引き上げ、過剰の過マ
ンガン酸カリウムを純水で洗浄したのち、６０〜７０’
Ｃで乾燥して黒色の綿状捕集材−Ｋ ＣＦ Ｃ＋ Ｍｎ
Ｏ２を製造 ・イした。Example-3 Collection material-KCFC+MnO2 Acrylic fiber 1001 was immersed in a 10% potassium ferrocyanide aqueous solution and heated for 3 hours. 10% after taking out
It was immersed in a cobalt nitrate aqueous solution and heated for 3 hours. After washing with water 6
It was dried at 0°C to 70°C for 10 hours. This operation was repeated three times, and the fibers were immersed in a 0.5M potassium permanganate aqueous solution for 4 days. When the fibers turned black, they were pulled out, and the excess potassium permanganate was washed with pure water.
Dried with C to form black cotton-like collection material-K CF C+ Mn
Manufacture O2.
次に実施例で製造した３種の捕集材を使用して海水から
の各種放射性核種の捕集テストを行って得た結果を参考
例として記載する。Next, the results obtained by performing a collection test of various radionuclides from seawater using the three types of collection materials manufactured in the examples will be described as a reference example.
参考例 １、実験材料 Ａ、カラム ガラス製、内径１５胴χ′、長さ２０偏を使用した。Reference example 1. Experimental materials A, column It was made of glass, had an inner diameter of 15 mm, and had a length of 20 mm.
Ｂ、海 水
海水（千葉県勝浦市で採水）は富士フィルム社製・ミク
ロフィルター（０４５μｍ）で口過したものを使用し、
トレーサーとしての各種の放射性核種添加後、塩酸なら
びに水酸化ナトリウム溶液でｐｌｉを８．０−１−０．
５に調整した。また使用した海水の塩分は３３７％であ
った。B. Seawater Seawater (collected in Katsuura City, Chiba Prefecture) was passed through a microfilter (045 μm) manufactured by Fuji Film.
After adding various radionuclides as tracers, the pli was adjusted to 8.0-1-0 with hydrochloric acid and sodium hydroxide solution.
Adjusted to 5. Moreover, the salinity of the seawater used was 337%.
Ｃ１使用核種
５４Ｍｎ（Ｍｎｃｚ２．＋ ｏ、５６ｃｅ） 無担体
５９Ｆｅ （ＦｅＣ１３，０，５ＮＨＣｅ） １］
ｍＣｉ／ｍｇＦｅ６０Ｃｏ （ＣｏＣ１２＝ ０．１Ｎ
ＨＣ１） １３６ｍＣ１／ｍｇＣ。C1 used nuclide 54Mn (Mncz2.+ o, 56ce) carrier-free 59Fe (FeC13,0,5NHCe) 1]
mCi/mgFe60Co (CoC12= 0.1N
HC1) 136mC1/mgC.
６５Ｚｎ （ＺｎＣＪ２，０．５ＮＨＣｅ） ２．
８ｍＣ１／ｍｇＺｎ８５Ｓｒ （ＳｒＣ１！２，０．５
ＮＨＣ／） ７．４ｍＣ１／ｉｎｇｓｒ１０６Ｒｕ
（塩化物、４ＮＨＣ１） ７．７ｍＣ１／ｒｎ
ｇＲｕ１３７Ｃｓ（ＣｓＣ／！ 、０．５ＮＨＣ／’）
９．０ｍＣ１／ｉｎｇｃｓ１４４Ｃｅ（ＣｅＣ
１！３． １ＮＨｃｌ）、 ２５０ｍＣ４／ｉｎｇ
ｃｅこれらの核種を放射能濃度として約１００ｎＣｉ／
ｉｎｅに希釈したのち海水に添加した。65Zn (ZnCJ2, 0.5NHCe) 2.
8mC1/mgZn85Sr (SrC1!2,0.5
NHC/) 7.4mC1/ingsr106Ru
(chloride, 4NHC1) 7.7mC1/rn
gRu137Cs (CsC/!, 0.5NHC/')
9.0mC1/ingcs144Ce (CeC
1!3. 1N Hcl), 250mC4/ing
ce These nuclides have a radioactivity concentration of approximately 100 nCi/
It was added to seawater after being diluted with 1.
Ｄ、 ＮａＩ（ＴＩりシンチレーシ邑ンスベクトロメ
ーター７４４０Ｘ５１ｍｍ井戸型ＮａＩ（ＴＩ）検出器
ヲＡｅ ｏ ｋ ａ 社ＩＪＪ ユニバーサルスケーラ
（モデルＴＤＣ−５０１）に接続して測定した。D. NaI (TI) scintillation was measured using a 7440 x 51 mm well-type NaI (TI) detector connected to an IJJ universal scaler (model TDC-501) manufactured by Aeoka.
２実験際作
２．１ バッチ法による攪拌時間と捕集率３つのバッ
チの海水２００ｍ１毎に各種のトレーサーを添加した。2 Experimental Work 2.1 Stirring time and collection rate by batch method Various tracers were added to every 200 ml of seawater in three batches.
これに実施例１〜３で製造した捕集材を加え、攪拌時間
を２．５．１０．２０分と変化させた。各攪拌時間が終
了した後、海水の一定量を測定用ポリエチレン管に移し
入れ、ＮａＩ（Ｔｊり検出器で測定し捕集率を求めた。The collection materials produced in Examples 1 to 3 were added to this, and the stirring time was changed to 2, 5, 10, and 20 minutes. After each stirring period ended, a certain amount of seawater was transferred into a polyethylene tube for measurement, and the collection rate was determined by measuring with a NaI (Tj) detector.
捕集率Ａは次式のように定義した。パンチ法による実験
条件を表−１に示す。The collection rate A was defined as follows. Table 1 shows the experimental conditions for the punch method.
Ａ（％）＝（（Ｒ１−Ｒ２）／Ｒ１）Ｘ１００Ａ ：繊
維（ＫＣＦＣ）の捕集率
Ｒ１ニドレーサー添加海水の計数率
Ｒ２：攪拌後の海水の計数率
表−１バッチ法の実験条件
’ ２．２． カラム法による流
速と捕集率内径１５ｍｆｌのガラス製捕集カラムに実施
例１〜３で製造した捕集材を詰め、トレーサーを添加し
た海水２００ｍ１を流速を変化させて通した。通過液の
一定量を測定用ポリエチレン管に移し入れ、ＮａＩ（Ｔ
／）検出器で測定し捕集率を求めた。捕集率Ａは次式の
ように定義した。カラム法による実験条件を表−２に示
す。A (%) = ((R1-R2)/R1) .2. Flow rate and collection rate by column method A glass collection column with an inner diameter of 15 mfl was filled with the collection materials produced in Examples 1 to 3, and 200 ml of seawater added with a tracer was passed through it at varying flow rates. Transfer a certain amount of the flow through to a polyethylene tube for measurement, and add NaI(T
/) The collection rate was determined by measuring with a detector. The collection rate A was defined as follows. Table 2 shows the experimental conditions for the column method.
Ａ（％） ＝ （（Ｒ１−Ｒ３）／Ｒ１）Ｘ１００Ａ
： 繊維（ＫＣＦＣ）の捕集率
Ｒ１： トレーサー添加海水の計数率
Ｒ３： 繊維（ＫＣＦＣ）カラム通過液の計数率銅
３結果と考察
３１ 攪拌時間と捕集率
バッチ法での実験結果を第１〜３図に示した。A (%) = ((R1-R3)/R1)X100A
: Collection rate of fiber (KCFC) R1: Count rate of tracer-added seawater R3: Count rate of fiber (KCFC) column passing liquid Copper 3 Results and discussion 31 Stirring time and collection rate - Shown in Figure 3.
図から明らかなように捕集材−Ｍｎ０２には２０分間の
攪拌時間で５４Ｍｎ、６０Ｃｏ、Ｉ ４４Ｃｅがほぼ１
００％捕集されている。一方、捕集材−ＫＣＦＣには２
０分間の攪拌時間で６５Ｚｎ、１０６Ｒｕ、１４４Ｃｅ
が９０％以上とよく捕集される他、５４Ｍｎ、６０Ｃｏ
、５９Ｆｅ が一部捕集されている。しかしながら８５
Ｓｒは全く捕集されていないことが明らかとなった。As is clear from the figure, 54Mn, 60Co, and I44Ce were added to the scavenger Mn02 at a rate of about 1 after stirring for 20 minutes.
00% collected. On the other hand, the collection material - KCFC has 2
65Zn, 106Ru, 144Ce with stirring time of 0 minutes
In addition to 90% or more of 54Mn, 60Co
, 59Fe were partially collected. However, 85
It became clear that Sr was not collected at all.
捕集材−Ｍｎ０２で捕集率の低かった］０６Ｒｕαζ抽
集材−ＫＣＦＣで９１％と高い捕集率を示したのは非常
に興味深い結果である。又、捕集材−Ｍｎ０２と捕輿材
−ＫＣＦＣの両方の機能を有する捕集材−Ｋ ＣＦ Ｃ
＋ＭｎＯ２は５４Ｍｎ、 ５９Ｆｅ１’
６０Ｃｏ、６５．。、１３７Ｃ８オヨｆｆ
１４４ｒ２８ヲはぼ１００％捕集することがわかる。The collection rate was low with the collection material Mn02] It is a very interesting result that the collection rate was as high as 91% with the 06Ruαζ extraction material-KCFC. In addition, a collection material that has the functions of both a collection material - Mn02 and a collection material - KCFC - K CF C
+MnO2 is 54Mn, 59Fe1'
60Co, 65. . , 137C8 oyoff
It can be seen that almost 100% of 144r28 is collected.
３２ 流速と捕集率
結果を第４〜６図に示した。第４図かられがるように、
捕集材−Ｍｎ０２の場合流速２０ｍ１／ｍｉｎで１４４
Ｃ８，５４Ｍｎ、 ６０Ｃｏ、 ６５Ｚｎの捕集率は９
０％以上であり、流速を２００ ｍｌＪ ／ｍｉｎ以上
に増加しても１４４Ｃｅおよび５４Ｍｎの捕集率は９０
％以上を保持している。一方、第５図かられかるように
捕集材−ＫＣＦＣの場合、流速２０ｍ１／ｍｉｎで５９
Ｆ、、６０Ｃｏ、 ６５Ｚｎ、１３７Ｃ，。32 The flow rate and collection rate results are shown in Figures 4-6. As shown in Figure 4,
Collection material - In the case of Mn02, 144 at a flow rate of 20 m1/min
The collection rate of C8,54Mn, 60Co, and 65Zn is 9
0% or more, and even if the flow rate was increased to 200 mlJ/min or more, the collection rate of 144Ce and 54Mn remained at 90%.
% or more. On the other hand, as shown in Figure 5, in the case of the collection material - KCFC, the flow rate is 59 m1/min at a flow rate of 20 m1/min.
F,, 60Co, 65Zn, 137C,.
１４４Ｃｅの捕集率は９０％以上であり、１８０ｍ１／
ｍｉｎと流速を増加しても、これらの核種は８０％と高
い捕集率を示した。６５Ｚｎ、１３７Ｃ８，１４４Ｃｅ
では捕集率の減少がみられなかったが、５９Ｆｅで５％
、６０Ｃｏで１０％の減少が認められた。１０６Ｒｕは
２０ ｍｌ／ｍｉｎと１８０のａｌｌ／ｍｉｎでは５５
％と大幅な減少を示した。第６図は捕集材−Ｍｎ０２と
捕集材−ＫＣＦＣの両方の機能を有する捕集材−ＫＣＦ
Ｃ＋ＭｎＯ２の結−果を イ示すグラフ
であるが、流速を１８０〜２００ｍ１１分の間で５４Ｍ
ｎ、 １３７Ｃ，，１４４Ｃｅ、６０ｃｏ、６５ｚｎ、
５９Ｆｅをほぼ９０％以上の捕集率で捕集することがわ
かる。The collection rate of 144Ce is over 90%, and 180m1/
Even when the min and flow rate were increased, these nuclides showed a high collection rate of 80%. 65Zn, 137C8, 144Ce
No decrease in collection rate was observed with 59Fe, but 5% with 59Fe.
, 60Co, a 10% decrease was observed. 106Ru is 55 at 20 ml/min and 180 all/min
%, which showed a significant decrease. Figure 6 shows a collection material - KCF that has the functions of both a collection material - Mn02 and a collection material - KCFC.
This is a graph showing the results of C+MnO2.
n, 137C,, 144Ce, 60co, 65zn,
It can be seen that 59Fe is collected with a collection rate of approximately 90% or more.
以上の実験より、アクリル繊維にＭｎＯ２を担持・固定
させて成る捕集材とアクリル繊維に一般式Ｋ２ＭＩＩ（
Ｆｅ （ＣＮ） ６）で表わされるフェロシアン酸塩化
合物を担持・固定させて族６捕集材を併用するか又はア
クリル繊維にＭｎＯ２および一般式に２Ｍｎ（Ｆｅ（Ｃ
Ｎ）６） で表わされるフェロシアン酸塩化合物を同
時に担持・固定させて成る捕集材を使用することによっ
て主として５４Ｍｎ、 ５９Ｆｅ、６０Ｃｏ。From the above experiments, we found that the general formula K2MII (
A ferrocyanate compound represented by Fe (CN) 6) can be supported and fixed and a group 6 trapping material can be used in combination, or MnO2 and 2Mn (Fe(C
N) 6) Mainly 54Mn, 59Fe, and 60Co by using a collection material that supports and immobilizes the ferrocyanate compounds represented by 6) at the same time.
捕集することがわかる。You can see that it can be collected.
発明の効果
以上を通覧することによって本発明の捕集材は；（１）
ｐ８７〜９の範囲で５４Ｍｎ、 ５９Ｆｅ、 ６０
Ｃｏ、 ６５Ｚｎ。By reviewing the effects of the invention, the collection material of the present invention has; (1)
54Mn, 59Fe, 60 in the p87-9 range
Co, 65Zn.
１０３＋１０６Ｒｕ、 １３４＋１３７Ｃ８，１４４Ｃ
ｅ を捕集すること、
（２）多量のＮａ＋の存在下に於いても上記核種を捕集
すること、
（３）綿状であるためフィルターへの加工が容易であり
またカートリッジ式にも加工出来ること、（４）綿状で
あるため燃焼させると廃棄物としての処理が極めて容易
である。等の効果があること等が理解される。103+106Ru, 134+137C8, 144C
(2) To collect the above-mentioned nuclides even in the presence of a large amount of Na+; (3) Because it is cotton-like, it can be easily processed into filters, and it can also be processed into cartridge type. (4) Since it is flocculent, it is extremely easy to dispose of it as waste when burned. It is understood that it has the following effects.
第１図は捕集材−Ｍｎ０２を用いた攪拌時間と捕集率と
の関係を示すグラフ、
第２図は捕集材−ＫＣＦＣを用いた攪拌時間と捕集率と
を示すグラフ、
第３図は捕集材−ＫＣＦＣ＋ＭｎＯ２を用いた撹拌時間
との関係を示すグラフ、
第４図は捕集材−Ｍｎ０２を用いた流速と捕集率との関
係を示すグラフ、
第５図は捕集材−ＫＣＦＣを用いた流速と捕集率との関
係を示すグラフ、
第６図は捕集材−ＫＣＦＣ＋ＭｎＯ２を用いた流速と捕
集率との関係を示すグラフである。
特許出願人 財団法人 日本分析センター０（Ｄ＠Ｇ
０６８８
＠ｓｉ＠−Ｘ
０Φ・ＧＯｅ５ のｅ
悪＠＠＋メ
鳶−催λFig. 1 is a graph showing the relationship between stirring time and collection rate using the collection material Mn02, Fig. 2 is a graph showing the relationship between stirring time and collection rate using the collection material KCFC, and Fig. 3 The figure is a graph showing the relationship between stirring time using the scavenger - KCFC + MnO2. Figure 4 is a graph showing the relationship between flow rate and collection rate using the scavenger - Mn02. Figure 5 is the graph showing the relationship between the collection rate and the scavenger - KCFC + MnO2. - A graph showing the relationship between the flow rate and the collection rate using KCFC. Fig. 6 is a graph showing the relationship between the flow rate and the collection rate using the collection material -KCFC+MnO2. Patent applicant Japan Analysis Center 0 (D@G)
0688 @si@-X 0Φ・GOe5 noe evil@@+Metobi-event λ
Claims (4)
る放射性核種および重金属捕集材。(1) Radioactive nuclide and heavy metal trapping material made by supporting and fixing MnO_2 on acrylic fibers.
）＿６）（Ｍ＾IIは２価の金属）で表わされるフェロシ
アン酸塩化合物を担持・固定させて成る捕集材およびア
クリル繊維にＭｎＯ＿２を担持・固定させて成る捕集材
の組合せから成る放射性核種および重金属捕集材。(2) General formula K_2M^II (Fe(CN)
)_6) (M^II is a divalent metal) consisting of a combination of a collection material made by supporting and fixing a ferrocyanate compound and a collecting material made by supporting and fixing MnO_2 on acrylic fibers. Radionuclide and heavy metal trapping material.
）＿６）（Ｍ＾IIは２価の金属）およびＭｎＯ＿２を担
持・固定させて成る放射性核種および重金属捕集材。(3) General formula K_2M^II (Fe(CN)
)_6) (M^II is a divalent metal) and MnO_2 are supported and fixed on the radioactive nuclide and heavy metal collecting material.
から選択される特許請求の範囲第２又は３項記載の放射
性核種および重金属捕集材。(4) The radionuclide and heavy metal collecting material according to claim 2 or 3, wherein M^II is selected from the group consisting of Co, Zn, Zr and Ni.
Priority Applications (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP12297984A JPS614530A (en) | 1984-06-15 | 1984-06-15 | Radioactive nuclide and heavy metal collecting material |
| US06/719,433 US4720422A (en) | 1984-06-06 | 1985-04-03 | Material for collecting radionuclides and heavy metals |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP12297984A JPS614530A (en) | 1984-06-15 | 1984-06-15 | Radioactive nuclide and heavy metal collecting material |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS614530A true JPS614530A (en) | 1986-01-10 |
| JPS6324415B2 JPS6324415B2 (en) | 1988-05-20 |
Family
ID=14849304
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP12297984A Granted JPS614530A (en) | 1984-06-06 | 1984-06-15 | Radioactive nuclide and heavy metal collecting material |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS614530A (en) |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| JPS6439600A (en) * | 1987-08-06 | 1989-02-09 | Ebara Corp | Treatment of radioactive waste liquid containing salts at high concentration |
| EP0666577A1 (en) * | 1994-02-07 | 1995-08-09 | BRADTEC Limited | Magnetic particles, a method for the preparation thereof and their use in the purification of solutions |
| JP2012046399A (en) * | 2010-08-30 | 2012-03-08 | National Institute Of Advanced Industrial Science & Technology | Electrode material for lithium ion secondary battery using non-defective prussian blue analogue |
| JP2012250904A (en) * | 2011-05-06 | 2012-12-20 | National Institute Of Advanced Industrial Science & Technology | Composite containing metal complex, and radiocesium adsorbent using the same |
| WO2013065829A1 (en) * | 2011-11-02 | 2013-05-10 | ダイワボウホールディングス株式会社 | Radioactive-substance adsorbent, method for manufacturing same, and textile good including radioactive-substance adsorbent |
| JP2013142573A (en) * | 2012-01-10 | 2013-07-22 | Japan Atomic Energy Agency | Method for separating/removing radioactive element from liquid |
| JP2014102240A (en) * | 2012-11-20 | 2014-06-05 | Kankyo Joka Kenkyusho:Kk | Method for decontaminating accumulated radioactive liquid and device for the same |
| JPWO2013027652A1 (en) * | 2011-08-19 | 2015-03-19 | 一般財団法人生産技術研究奨励会 | Radioactive cesium adsorbent, method for producing the same, and method for removing radioactive cesium in the environment using the adsorbent |
| WO2015083688A1 (en) * | 2013-12-02 | 2015-06-11 | 国立大学法人東京工業大学 | Cesium adsorption agent, production method therefor, and cesium removal method using cesium adsorption agent |
| JP2017121616A (en) * | 2016-01-08 | 2017-07-13 | 日本化学工業株式会社 | Absorbent |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| JP2013061220A (en) * | 2011-09-13 | 2013-04-04 | Futaba Shoji Kk | Radioactive cesium adsorptive cloth |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS4932466A (en) * | 1972-07-24 | 1974-03-25 | ||
| JPS5035753A (en) * | 1973-06-14 | 1975-04-04 |
-
1984
- 1984-06-15 JP JP12297984A patent/JPS614530A/en active Granted
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS4932466A (en) * | 1972-07-24 | 1974-03-25 | ||
| JPS5035753A (en) * | 1973-06-14 | 1975-04-04 |
Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS6439600A (en) * | 1987-08-06 | 1989-02-09 | Ebara Corp | Treatment of radioactive waste liquid containing salts at high concentration |
| EP0666577A1 (en) * | 1994-02-07 | 1995-08-09 | BRADTEC Limited | Magnetic particles, a method for the preparation thereof and their use in the purification of solutions |
| JP2012046399A (en) * | 2010-08-30 | 2012-03-08 | National Institute Of Advanced Industrial Science & Technology | Electrode material for lithium ion secondary battery using non-defective prussian blue analogue |
| JP2012250904A (en) * | 2011-05-06 | 2012-12-20 | National Institute Of Advanced Industrial Science & Technology | Composite containing metal complex, and radiocesium adsorbent using the same |
| JPWO2013027652A1 (en) * | 2011-08-19 | 2015-03-19 | 一般財団法人生産技術研究奨励会 | Radioactive cesium adsorbent, method for producing the same, and method for removing radioactive cesium in the environment using the adsorbent |
| WO2013065829A1 (en) * | 2011-11-02 | 2013-05-10 | ダイワボウホールディングス株式会社 | Radioactive-substance adsorbent, method for manufacturing same, and textile good including radioactive-substance adsorbent |
| JP2013142573A (en) * | 2012-01-10 | 2013-07-22 | Japan Atomic Energy Agency | Method for separating/removing radioactive element from liquid |
| JP2014102240A (en) * | 2012-11-20 | 2014-06-05 | Kankyo Joka Kenkyusho:Kk | Method for decontaminating accumulated radioactive liquid and device for the same |
| WO2015083688A1 (en) * | 2013-12-02 | 2015-06-11 | 国立大学法人東京工業大学 | Cesium adsorption agent, production method therefor, and cesium removal method using cesium adsorption agent |
| JP2015128760A (en) * | 2013-12-02 | 2015-07-16 | 国立大学法人東京工業大学 | Cesium adsorbent, manufacturing method thereof, and method for removing cesium using cesium adsorbent |
| JP2017121616A (en) * | 2016-01-08 | 2017-07-13 | 日本化学工業株式会社 | Absorbent |
Also Published As
| Publication number | Publication date |
|---|---|
| JPS6324415B2 (en) | 1988-05-20 |
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