JPH0259433A - Method for adsorbing and separating technetium - Google Patents
Method for adsorbing and separating technetiumInfo
- Publication number
- JPH0259433A JPH0259433A JP20943688A JP20943688A JPH0259433A JP H0259433 A JPH0259433 A JP H0259433A JP 20943688 A JP20943688 A JP 20943688A JP 20943688 A JP20943688 A JP 20943688A JP H0259433 A JPH0259433 A JP H0259433A
- Authority
- JP
- Japan
- Prior art keywords
- technetium
- active carbon
- contg
- thiocyanate
- ion
- 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.)
- Pending
Links
- 229910052713 technetium Inorganic materials 0.000 title claims abstract description 40
- GKLVYJBZJHMRIY-UHFFFAOYSA-N technetium atom Chemical compound [Tc] GKLVYJBZJHMRIY-UHFFFAOYSA-N 0.000 title claims abstract description 40
- 238000000034 method Methods 0.000 title claims abstract description 12
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 37
- ZMZDMBWJUHKJPS-UHFFFAOYSA-N thiocyanic acid Chemical compound SC#N ZMZDMBWJUHKJPS-UHFFFAOYSA-N 0.000 claims abstract description 16
- ZMZDMBWJUHKJPS-UHFFFAOYSA-M Thiocyanate anion Chemical compound [S-]C#N ZMZDMBWJUHKJPS-UHFFFAOYSA-M 0.000 claims abstract description 5
- 239000003463 adsorbent Substances 0.000 claims abstract description 5
- 238000000926 separation method Methods 0.000 claims description 9
- 238000001179 sorption measurement Methods 0.000 claims description 8
- -1 thiocyanate ions Chemical class 0.000 claims description 5
- 239000003929 acidic solution Substances 0.000 claims description 4
- 238000011084 recovery Methods 0.000 abstract description 8
- 239000003758 nuclear fuel Substances 0.000 abstract description 5
- ZNNZYHKDIALBAK-UHFFFAOYSA-M potassium thiocyanate Chemical compound [K+].[S-]C#N ZNNZYHKDIALBAK-UHFFFAOYSA-M 0.000 abstract description 5
- 229940116357 potassium thiocyanate Drugs 0.000 abstract description 5
- 150000002500 ions Chemical class 0.000 abstract description 4
- 229910052799 carbon Inorganic materials 0.000 abstract 5
- 230000002378 acidificating effect Effects 0.000 abstract 3
- 239000000243 solution Substances 0.000 description 10
- 239000007788 liquid Substances 0.000 description 6
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 5
- 229910017604 nitric acid Inorganic materials 0.000 description 5
- 239000002699 waste material Substances 0.000 description 4
- 241000196324 Embryophyta Species 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 229910052770 Uranium Inorganic materials 0.000 description 2
- JHIVVAPYMSGYDF-UHFFFAOYSA-N cyclohexanone Chemical compound O=C1CCCCC1 JHIVVAPYMSGYDF-UHFFFAOYSA-N 0.000 description 2
- 238000012958 reprocessing Methods 0.000 description 2
- 239000002915 spent fuel radioactive waste Substances 0.000 description 2
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 description 2
- NWUYHJFMYQTDRP-UHFFFAOYSA-N 1,2-bis(ethenyl)benzene;1-ethenyl-2-ethylbenzene;styrene Chemical compound C=CC1=CC=CC=C1.CCC1=CC=CC=C1C=C.C=CC1=CC=CC=C1C=C NWUYHJFMYQTDRP-UHFFFAOYSA-N 0.000 description 1
- 229910052778 Plutonium Inorganic materials 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- GKLVYJBZJHMRIY-OUBTZVSYSA-N Technetium-99 Chemical compound [99Tc] GKLVYJBZJHMRIY-OUBTZVSYSA-N 0.000 description 1
- 235000006732 Torreya nucifera Nutrition 0.000 description 1
- 244000111306 Torreya nucifera Species 0.000 description 1
- 239000012670 alkaline solution Substances 0.000 description 1
- 238000005349 anion exchange Methods 0.000 description 1
- 238000010923 batch production Methods 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 230000005251 gamma ray Effects 0.000 description 1
- 239000002927 high level radioactive waste Substances 0.000 description 1
- 239000003456 ion exchange resin Substances 0.000 description 1
- 229920003303 ion-exchange polymer Polymers 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- XTAZYLNFDRKIHJ-UHFFFAOYSA-N n,n-dioctyloctan-1-amine Chemical compound CCCCCCCCN(CCCCCCCC)CCCCCCCC XTAZYLNFDRKIHJ-UHFFFAOYSA-N 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 239000000700 radioactive tracer Substances 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000000638 solvent extraction Methods 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 239000006228 supernatant Substances 0.000 description 1
- WAGFXJQAIZNSEQ-UHFFFAOYSA-M tetraphenylphosphonium chloride Chemical compound [Cl-].C1=CC=CC=C1[P+](C=1C=CC=CC=1)(C=1C=CC=CC=1)C1=CC=CC=C1 WAGFXJQAIZNSEQ-UHFFFAOYSA-M 0.000 description 1
- STCOOQWBFONSKY-UHFFFAOYSA-N tributyl phosphate Chemical compound CCCCOP(=O)(OCCCC)OCCCC STCOOQWBFONSKY-UHFFFAOYSA-N 0.000 description 1
- 230000002747 voluntary effect Effects 0.000 description 1
Landscapes
- Inorganic Compounds Of Heavy Metals (AREA)
Abstract
Description
【発明の詳細な説明】 （産業上の利用分野） 本発明はテクネチウムの吸着分離方法に関する。[Detailed description of the invention] (Industrial application field) The present invention relates to a method for adsorption and separation of technetium.
詳しくは、本発明は、使用済核燃料の再処理によって発
生する高レベル放射性廃液、使用済核燃料溶解液等のテ
クネチウムを含む酸性溶液からテクネチウムを活性炭に
より吸着分離する方法に関する。Specifically, the present invention relates to a method for adsorbing and separating technetium from acidic solutions containing technetium, such as high-level radioactive waste liquids generated by reprocessing spent nuclear fuels and spent nuclear fuel dissolved liquids, using activated carbon.
（従来の技術）
使用済核燃料の再処理工場、回収したウランの濃縮工場
、ウランやプルトニウムの燃料加工工場、原子力発電所
等の核燃料サイクル施設において発生する廃液中には、
半減期約２０万年のテクネチウム−９９が含まれている
。これらの廃液からのテクネチウムの分離回収又は除去
は、廃液の処理処分における長期にわたる環境影響をで
きるだけ少なくするという観点から、また、回収したテ
クネチウムを鋼材の腐食防止や触媒として有効に利用で
きるという観点から、最近特に注目されている。(Conventional technology) Waste liquid generated at spent nuclear fuel reprocessing plants, recovered uranium enrichment plants, uranium and plutonium fuel processing plants, nuclear fuel cycle facilities such as nuclear power plants, etc.
It contains technetium-99, which has a half-life of about 200,000 years. The separation, recovery, or removal of technetium from these waste liquids is important from the perspective of minimizing the long-term environmental impact of waste liquid treatment and disposal, and from the perspective that the recovered technetium can be effectively used to prevent corrosion of steel materials and as a catalyst. has received particular attention recently.
このため、核燃料サイクル施設から発生する廃液からの
テクネチウムの分離回収又は除去は特に有効である。For this reason, separation, recovery, or removal of technetium from waste liquid generated from nuclear fuel cycle facilities is particularly effective.
従来から用いられてきたテクネチウムの分離回収法又は
除去法には、リン酸トリブチル、トリーｎ−オクチルア
ミン、シクロヘキサノン等による溶媒抽出法、塩化テト
ラフェニルフォスフオニウムや硫化物による沈澱法、陰
イオン交換樹脂吸着法などがある。Conventionally used methods for separating, recovering, or removing technetium include solvent extraction using tributyl phosphate, tri-n-octylamine, cyclohexanone, etc., precipitation using tetraphenylphosphonium chloride or sulfide, and anion exchange. Examples include resin adsorption methods.
しかしながら、これらの方法においては、比較的高い酸
性度の溶液からのテクネチウムの分離回収又は除去にお
いてその分離効率が低（、高い回収率又は除去率を得る
ためには、多量の抽出剤や沈澱剤、イオン交換樹脂を必
要とするなどのおおくの問題点があった。However, these methods have low separation efficiency in the separation, recovery or removal of technetium from solutions with relatively high acidity (in order to obtain high recovery or removal rates, large amounts of extractants or precipitants are required). However, there were many problems such as the need for ion exchange resin.
（発明が解決しようとする課題）
本発明の目的は、このような問題点のないテクネチウム
の活性炭による吸着分離方法を提供することである。(Problems to be Solved by the Invention) An object of the present invention is to provide a method for adsorption and separation of technetium using activated carbon, which is free from such problems.
（課題を解決するための手段）
本願発明者は、先に、テクネチウムを含む溶液に活性炭
を添加することによって、或いはテクネチウムを含む溶
液を活性炭を充填したカラムに通すことによって、テク
ネチウムを活性炭により吸着分離できることを発見し、
特許出願したが（特願昭６３−３７６２５号）、さらに
鋭意研究の結果、テクネチウムを含むｐＨ２以下の硝酸
溶液にチオシアン酸又はチオシアン酸イオンを共存させ
ることによって、テクネチウムを高い回収率又は除去率
で、活性炭により吸着分離できることを発見し、本願発
明の目的を達成するに到った。(Means for Solving the Problems) The inventors of the present invention have discovered that technetium can be adsorbed by activated carbon by first adding activated carbon to a solution containing technetium, or by passing a solution containing technetium through a column filled with activated carbon. discovered that it is possible to separate
Although a patent application was filed (Japanese Patent Application No. 63-37625), as a result of further intensive research, it was possible to obtain technetium with a high recovery or removal rate by coexisting thiocyanate or thiocyanate ions in a nitric acid solution containing technetium with a pH of 2 or less. It was discovered that activated carbon can be used to adsorb and separate the particles, and the object of the present invention has been achieved.
従って、本願発明の方法は、核燃料サイクル施設等から
発生するテクネチウムを含む酸性溶液から、テクネチウ
ムを分離回収又は除去するため、活性炭を吸着剤として
使用するテクネチウムの吸着分離法において、チオシア
ン酸又はチオシアン酸イオンを共存させることを特徴と
する。Therefore, the method of the present invention is a technetium adsorption separation method using activated carbon as an adsorbent in order to separate and recover or remove technetium from an acidic solution containing technetium generated from a nuclear fuel cycle facility or the like. It is characterized by the coexistence of ions.
（実施例）
本発明を実施例についてさらに具体的に説明する。しか
し、本発明は実施例によって限定されるものではない。(Example) The present invention will be described in more detail with reference to Examples. However, the present invention is not limited to the examples.
活性炭０．２５ｇを入れた２０ｍＩのバイアルビンに、
過テクネチウム酸イオンを含む硝酸溶液及びチオシアン
酸カリウム溶液を加えて、全液量を１０ｍ１とした。こ
の試料を２５℃に設定したエアバスに入れ、回転ローラ
ー上で１時間攪拌した。In a 20 mI vial containing 0.25 g of activated carbon,
A nitric acid solution containing pertechnetate ions and a potassium thiocyanate solution were added to bring the total volume to 10 ml. This sample was placed in an air bath set at 25°C and stirred on a rotating roller for 1 hour.
試料を取り出して遠心分離機にかけた後、上澄液の１ｍ
ｌをサンプリングし、トレーサーとして加えた９Ｓ＋″
Ｔｃのγ線放射能強度をＧｏ半導体検出器で測定するこ
とにより、テクネチウムの活性炭への吸着率（％）及び
分配係数（ｍｌ／ｇ）を求めた。After removing the sample and centrifuging, 1 m of supernatant
9S+'' which was sampled and added as a tracer
By measuring the γ-ray radioactivity intensity of Tc with a Go semiconductor detector, the adsorption rate (%) of technetium to activated carbon and the distribution coefficient (ml/g) were determined.
ここに分配係数は次式で表される。Here, the distribution coefficient is expressed by the following formula.
活性炭中の””ＴＣＲ１度（ｐｃｉ／ｇ）硝酸濃度を０
．−Ｉ Ｍとして、チオシアン酸カリウムの濃度を１０
−’Ｍから１０−’Ｍまで変化させた時のテクネチウム
の活性炭への吸着率及び分配係数を第１表に示した。ま
た、硝酸濃度を０．５Ｍとした場合の値を第２表に示し
た。""TCR1 degree (pci/g) nitric acid concentration in activated carbon is 0
．． -IM, the concentration of potassium thiocyanate is 10
Table 1 shows the adsorption rate and distribution coefficient of technetium on activated carbon when changing from -'M to 10-'M. Further, Table 2 shows the values when the nitric acid concentration was 0.5M.
Ｏ−４
９９，９１
９９，６５
９７，４５
９７，４１
９７，３９
４，５７
１，１７
１，５３
１，５１
１，４９
茅１表
１０−’ ９９．９７ １．５５
ｘ １．０’１０−” ９９．９４
７．０４ ｘ １０’１０−’
９Ｂ、８０ ３．２９ ｘ １０’１０
−’ ９１．７２ ４．４３ ｘ
１．０２１０−’ ９０．８８
３．９９ ｘ １０”第１表及び第２表から明ら
かなように、テクネチウムの吸着に及ぼすチオシアン酸
カリウムの添加効果は、０．１ Ｍ硝酸溶液の場合より
も０．５Ｍ硝酸溶液の場合の方がより大きく、０．５Ｍ
硝酸溶液の場合にはチオシアン酸カリウムの濃度が０−
０１Ｍ以上であれば、９９．９％以上のテクネチウムを
吸着できることがわかる。テクネチウムのより戦い回収
率又は除去率を得るためには、活性炭を充填したカラム
にチオシアン酸又はチオシアン酸イオンを添加したテク
ネチウムを含む溶液を通過させることが効果的であるが
、本発明の方法を使用すれば、バッチ法においても、溶
液１０ｍ１に対して活性炭０．２５ｇを使用することに
よりテクネチウムについて９９．９％以上の回収率又は
除去率を得ることができる。O-4 99,91 99,65 97,45 97,41 97,39 4,57 1,17 1,53 1,51 1,49 Kaya 1 Table 10-' 99.97 1.55
x 1.0'10-" 99.94
7.04 x 10'10-'
9B, 80 3.29 x 10'10
-' 91.72 4.43 x
1.0210-' 90.88
3.99 is larger, 0.5M
In the case of nitric acid solution, the concentration of potassium thiocyanate is 0-
It can be seen that 99.9% or more of technetium can be adsorbed if it is 01M or more. In order to obtain a higher recovery rate or removal rate of technetium, it is effective to pass a solution containing technetium to which thiocyanate or thiocyanate ions have been added through a column packed with activated carbon. If used, even in a batch process, a recovery or removal rate of 99.9% or more for technetium can be obtained by using 0.25 g of activated carbon per 10 ml of solution.
このため、テクネチウムを含む酸性溶液からテクネチウ
ムを分離回収又は除去するため、活性炭を吸着剤として
使用するテクネチウムの吸着分離法において、チオシア
ン酸又はチオシアン酸イオンを共存させることが特に有
効である。Therefore, in order to separate, recover, or remove technetium from an acidic solution containing technetium, it is particularly effective to coexist thiocyanic acid or thiocyanate ions in a technetium adsorption separation method that uses activated carbon as an adsorbent.
なお、本発明の方法において活性炭に吸着させたテクネ
チウムを溶出するためには、チオシアン酸イオンを含む
アルカリ性溶液を使用することが効果的であり（昭和６
３年８月１８日付は特許出願中）、２Ｍチオシアン酸カ
リウムを含む０．１Ｍ水酸化ナトリウム溶液を使用する
場合には、１回のバッチ操作で９０％以上のテクネチウ
ムを溶出することができる。In addition, in order to elute technetium adsorbed on activated carbon in the method of the present invention, it is effective to use an alkaline solution containing thiocyanate ions (Showa 6).
When a 0.1M sodium hydroxide solution containing 2M potassium thiocyanate is used, more than 90% of technetium can be eluted in one batch operation.
手続（甫正書（自発） 昭和６３年１１月２５日Procedures (Hoshosho (voluntary) November 25, 1986
Claims (1)
収又は除去するために吸着剤として活性炭を使用するテ
クネチウムの吸着分離法において、チオシアン酸又はチ
オシアン酸イオンを共存させることを特徴とするテクネ
チウムの吸着分離方法。A technetium adsorption separation method that uses activated carbon as an adsorbent to separate, recover, or remove technetium from an acidic solution containing technetium, the method comprising the coexistence of thiocyanate or thiocyanate ions.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP20943688A JPH0259433A (en) | 1988-08-25 | 1988-08-25 | Method for adsorbing and separating technetium |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP20943688A JPH0259433A (en) | 1988-08-25 | 1988-08-25 | Method for adsorbing and separating technetium |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH0259433A true JPH0259433A (en) | 1990-02-28 |
Family
ID=16572830
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP20943688A Pending JPH0259433A (en) | 1988-08-25 | 1988-08-25 | Method for adsorbing and separating technetium |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0259433A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0726329A1 (en) * | 1995-02-09 | 1996-08-14 | Hitachi, Ltd. | A method for separating technetium and apparatus therefor |
-
1988
- 1988-08-25 JP JP20943688A patent/JPH0259433A/en active Pending
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0726329A1 (en) * | 1995-02-09 | 1996-08-14 | Hitachi, Ltd. | A method for separating technetium and apparatus therefor |
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