JPH09243796A - Method for processing reactor fuel reprocessed waste liquid - Google Patents

Method for processing reactor fuel reprocessed waste liquid

Info

Publication number
JPH09243796A
JPH09243796A JP5590696A JP5590696A JPH09243796A JP H09243796 A JPH09243796 A JP H09243796A JP 5590696 A JP5590696 A JP 5590696A JP 5590696 A JP5590696 A JP 5590696A JP H09243796 A JPH09243796 A JP H09243796A
Authority
JP
Japan
Prior art keywords
americium
extractant
waste liquid
solution
curium
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.)
Withdrawn
Application number
JP5590696A
Other languages
Japanese (ja)
Inventor
Hiroichi Tachikawa
博一 立川
Takaaki Imoji
敬明 出雲路
Yoichi Enokida
洋一 榎田
Tsuneaki Fujioka
綱昭 藤岡
Mamoru Hatano
守 波多野
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Mitsubishi Heavy Industries Ltd
Original Assignee
Mitsubishi Heavy Industries Ltd
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Mitsubishi Heavy Industries Ltd filed Critical Mitsubishi Heavy Industries Ltd
Priority to JP5590696A priority Critical patent/JPH09243796A/en
Publication of JPH09243796A publication Critical patent/JPH09243796A/en
Withdrawn legal-status Critical Current

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Abstract

PROBLEM TO BE SOLVED: To shorten the separating time and reduce the generation of waste solution in the separation of americium and curium from a reactor fuel reprocessed waste solution. SOLUTION: In this waste solution processing method, pH of the simulated raffinate of a reactor fuel reprocessed waste liquid containing lanthanides and americium is regulated to 2-3, and the regulated reffinate is then brought into contact with a mixed solvent, as extracting agent, formed of 0.3M of di-2- ethylhexyl phosphate, 0.2M of tributyl phosphate, and n-dodecane as diluent under temperature condition to extract lanthanides and americium to the extracting agent. Thereafter, a solution of 1M of glycolic acid and 0.01M of pentasodium diethylenetriaminepentacetate whose pH is regulated to >=3 by caustic side is used as a reverse extracting agent, and this solution and the extracting agent containing americium make contact the each other at a liquid temperature of 40-60 deg.C for one minute, and americium is reversely extracted and separated from lanthanides.

Description

【発明の詳細な説明】Detailed Description of the Invention

【0001】[0001]

【発明の属する技術分野】本発明は、原子炉燃料の再処
理によって生ずる廃液の処理方法に関し、特にランタニ
ド及び超ウラン元素を含む高レベル放射性廃液からアメ
リシウム及びキュリウムを分離する方法に関する。
BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for treating waste liquid generated by reprocessing of nuclear fuel, and more particularly to a method for separating americium and curium from a high level radioactive waste liquid containing lanthanides and transuranium elements.

【0002】[0002]

【従来の技術】原子炉燃料として広く使用されているウ
ラン燃料は、核反応により核分裂性物質であるプルトニ
ウムを生じ、その再処理によりプルトニウム及びウラン
が回収されている。しかしながら前述の核反応によりア
メリシウムやキュリウム等も生じており、これらは前記
再処理に際しランタニドと一緒に高レベル放射性廃棄物
となっている。この高レベル放射性廃棄物はかなりの長
期間厳重に保管しなければならないため、できるだけ容
量が少ない方がよい。又アメリシウムやキュリウムは高
速増殖炉で燃焼可能な有用物質であるので、その分離が
推奨されている。
2. Description of the Related Art Uranium fuel, which is widely used as a nuclear reactor fuel, produces plutonium which is a fissile material by a nuclear reaction, and plutonium and uranium are recovered by reprocessing the same. However, the above-mentioned nuclear reaction also produces americium, curium, and the like, which are high-level radioactive wastes together with lanthanides during the reprocessing. This high-level radioactive waste must be stored strictly for a long period of time, so it is better to have the smallest possible volume. Further, since americium and curium are useful substances that can be burned in a fast breeder reactor, their separation is recommended.

【0003】このようなアメリシウムとキュリウムの分
離方法としては、次のようなプロセスが知られている。
即ち燃料再処理廃液のpHを苛性ソウダ(NaOH)で
1.5に調整し、これを0.4Mのジ−2−エチルヘキ
シル リン酸(D2EHPA)と0.4Mのリン酸トリ
ブチル及び希釈剤としてのn−炭化水素からなる抽出剤
に25℃で10分間接触させ、アメリシウム及びキュリ
ウムを抽出する。しかる後、逆抽出剤として苛性ソウダ
でpHを3.3に調整した0.5Mのヒドロキシ酢酸と
0.089Mのジエチレントリアミン五酢酸との混合溶
媒を用いてこのアメリシウム及びキュリウムを逆抽出す
る。逆抽出条件は、有機相である抽出剤と水相である逆
抽出剤との比を4、温度を25℃、接触時間は10分で
ある。なお、同様な分離方法が米国特許第346361
9号明細書に記載されている。
The following process is known as a method for separating such americium and curium.
That is, the pH of the fuel reprocessing waste liquid was adjusted to 1.5 with caustic soda (NaOH), and this was adjusted to 0.4M di-2-ethylhexylphosphoric acid (D2EHPA) and 0.4M tributyl phosphate and as a diluent. Americium and curium are extracted by contacting with an extractant composed of n-hydrocarbon at 25 ° C. for 10 minutes. Then, the americium and curium are back-extracted using a mixed solvent of 0.5M hydroxyacetic acid whose pH is adjusted to 3.3 with caustic soda and 0.089M diethylenetriaminepentaacetic acid as a back extractor. The back extraction conditions are as follows: the ratio of the organic phase extractant to the aqueous phase back extractant is 4, the temperature is 25 ° C., and the contact time is 10 minutes. A similar separation method is disclosed in US Pat. No. 346361.
No. 9 is described.

【0004】[0004]

【発明が解決しようとする課題】しかるに、前述したア
メリシウム及びキュリウムの分離方法では、抽出操作及
び逆抽出操作の接触時間が10分と長く、又ジ−2−エ
チルヘキシル リン酸、リン酸トリブチル及びジエチレ
ントリアミン五酢酸の濃度が高く、廃液量が多くなると
いう問題がある。従って、本発明は接触時間等の処理時
間が短く、且つ有機廃棄物の発生量の少ない原子炉燃料
再処理廃液からのアメリシウム及びキュリウムの分離方
法を提供することを課題とするものである。
However, in the above-described method for separating americium and curium, the contact time for the extraction operation and the back extraction operation is as long as 10 minutes, and di-2-ethylhexylphosphoric acid, tributyl phosphate and diethylenetriamine are used. There is a problem that the concentration of pentaacetic acid is high and the amount of waste liquid increases. Therefore, it is an object of the present invention to provide a method for separating americium and curium from a nuclear reactor fuel reprocessing waste liquid which has a short treatment time such as contact time and produces a small amount of organic waste.

【0005】[0005]

【課題を解決するための手段】如上の課題を解決するた
め、本発明によれば、ランタニド、アメリシウム及びキ
ュリウムを含む原子炉燃料再処理廃液のpHを先ず2〜
3に調整し、次に0.3Mのジ−2−エチルヘキシル
リン酸(Di-2-ethylhexyl phosphoric acid,D2EH
PA)及び0.2Mのリン酸トリブチル(tributhyl ph
oshate)並びに希釈剤としてのn−ドデカンからなる混
合溶媒を抽出剤としてこれに前述の調整済み廃液を室温
条件下で5分間接触させ、ランタニド、アメリシウム及
びキュリウムを抽出剤に抽出する。しかる後、1Mのグ
リコール酸と苛性ソウダでpHを〜3に調整した0.0
1Mのジエチレントリアミン五酢酸五ナトリウム(pent
asodium diethylenetriaminepentaacetate,Na5DT
PA)の溶液を逆抽出剤としてこれと前述の抽出剤(ア
メリシウム等を含む)とを液温40〜60℃で1分間接
触させ、アメリシウムとキュリウムとを逆抽出し、ラン
タニドから分離する。
In order to solve the above-mentioned problems, according to the present invention, the pH of the nuclear fuel reprocessing waste liquid containing lanthanide, americium and curium is first adjusted to 2 to 2.
Adjusted to 3, then 0.3M di-2-ethylhexyl
Phosphoric acid (Di-2-ethylhexyl phosphoric acid, D2EH
PA) and 0.2M tributyl phosphate (tributhyl ph)
ashate) and n-dodecane as a diluent are used as an extractant, and the prepared waste liquid is brought into contact with the extractant for 5 minutes at room temperature to extract lanthanide, americium and curium into the extractant. Thereafter, the pH was adjusted to ˜3 with 1 M glycolic acid and caustic soda, and then adjusted to 0.0.
1M diethylenetriaminepentaacetic acid pentasodium (pent
asodium diethylenetriaminepentaacetate, Na5DT
The solution of PA) is used as a back extractant and this extractant (including americium, etc.) is brought into contact with the solution at a liquid temperature of 40 to 60 ° C. for 1 minute to back extract americium and curium and separate them from the lanthanide.

【0006】[0006]

【発明の実施の形態】以下本発明の実施形態を説明す
る。原子炉燃料の再処理方法としては、比較的広く採用
されているピューレックス法を想定し、軽水炉燃料のウ
ラン燃料をピューレックス法により処理してウラン、プ
ルトニュウム及びランタニドを除く核分裂生成物を抽出
した後の水相であるラフィネート(抽出残液)を本発明
方法により処理してアメリシウム及びキュリウムを分離
する場合を説明する。先ず前述のラフィネートを模擬し
た模擬ラフィネートを、ランタニドとしてのセリウム
(Ce),ネオジム(Nd),サマリウム(Sm)、ユ
ーロピウム(Eu),ガドリニウム(Gd)の硝酸塩と
トレーサとして添加されたアメリシウム(Am)の水溶
液を硝酸を用いてpH1.3〜3.0に調整して作成した。ラ
ンタニド濃度は次のとおりである。 セリウム 975ppm ネオジム 1570ppm サマリウム 457ppm ユーロピウム 56ppm ガドリニウム 45ppm
Embodiments of the present invention will be described below. As a method for reprocessing nuclear fuel, the Purex method, which is relatively widely adopted, is assumed, and fission products other than uranium, plutonium and lanthanide are extracted by processing the uranium fuel of the light water reactor fuel by the Purex method. The case where the raffinate (extraction residual liquid) which is the subsequent aqueous phase is treated by the method of the present invention to separate americium and curium will be described. First, a simulated raffinate simulating the above-described raffinate was prepared by adding nitrates of cerium (Ce), neodymium (Nd), samarium (Sm), europium (Eu), and gadolinium (Gd) as lanthanides and americium (Am) added as a tracer. Was prepared by adjusting the pH to 1.3 to 3.0 using nitric acid. The lanthanide concentrations are as follows. Cerium 975ppm Neodymium 1570ppm Samarium 457ppm Europium 56ppm Gadolinium 45ppm

【0007】抽出剤として、n−ドデカンを希釈剤とし
た0.3Mのジ−2−エチルヘキシル リン酸と0.2
Mのリン酸トリブチルの混合溶媒を用いる。逆抽出剤と
しては、1Mのグリコール酸と苛性ソウダでpHを〜3
に調整した0.01Mのジエチレントリアミン五酢酸五
ナトリウムの溶液を用い、前述の模擬ラフィネートを図
1に示すフローチャートに従って処理した。即ち、模擬
ラフィネートと抽出剤とを混合し、液温20℃で5分間
接触させて抽出操作を行った。そして、水相のランタニ
ドは発行分光分析計で定量し、水相、有機相のアメリシ
ウムはゲルマニウム半導体検出器で定量する。ところで
以上のランタニドとアメリシウムの分配係数と分配平衡
時のpHとの関係は図2のように示される。pHが1.
1付近の2点は、初期pHが1.3〜1.5に調整され
た系であり、残りの4点は初期pHが2.4〜3.0に
調整されたものである。初期pHを2.0以上に調整す
ると、ランタニドの分配係数が10以上になる。即ち、
以上のランタニドとアメリシウムは、十分に抽出剤に抽
出される。
As an extractant, 0.3 M di-2-ethylhexyl phosphoric acid with n-dodecane as a diluent and 0.2
A mixed solvent of M tributyl phosphate is used. As a back extractor, the pH is adjusted to ~ 3 with 1 M glycolic acid and caustic soda.
The above simulated raffinate was treated according to the flow chart shown in FIG. 1 using a solution of 0.01 M diethylenetriaminepentaacetic acid pentasodium adjusted to 1. That is, the simulated raffinate and the extractant were mixed and brought into contact with each other at a liquid temperature of 20 ° C. for 5 minutes to carry out an extraction operation. Then, the lanthanide in the water phase is quantified by an emission spectrophotometer, and the americium in the water phase and the organic phase is quantified by a germanium semiconductor detector. By the way, the relationship between the distribution coefficient of lanthanide and americium and the pH at the distribution equilibrium is shown in FIG. pH is 1.
Two points near 1 are the systems whose initial pH was adjusted to 1.3 to 1.5, and the remaining four points were those whose initial pH was adjusted to 2.4 to 3.0. When the initial pH is adjusted to 2.0 or higher, the distribution coefficient of lanthanide becomes 10 or higher. That is,
The above lanthanides and americium are sufficiently extracted by the extractant.

【0008】次にランタニドとアメリシウムを抽出した
抽出剤と前述の逆抽出剤とを40〜60℃に加温し、混
合後、所定の接触時間で逆抽出操作を実施した。ここで
抽出剤と逆抽出剤との間のランタニドの分配係数と接触
時間は図3に示されている。図においで白抜きの記号
は、室温での接触時間を示し、塗りつぶしの記号は、5
5℃に加温した状態での接触時間を示している。本発明
では、逆抽出操作において40〜60℃に加熱されてい
るので、従来の同様の分配係数は1分程度の接触時間で
得られる。なお、このときのランタニドとアメリシウム
の分離係数は次のとおりとなる。 セリウム 91 ネオジム 19 サマリウム 23 ユーロピウム 33 ガドリニウム 23
Next, the extractant from which lanthanide and americium were extracted and the above-mentioned back extractor were heated to 40 to 60 ° C., and after mixing, a back extraction operation was carried out at a predetermined contact time. Here, the partition coefficient and contact time of the lanthanide between the extractant and the back extractant are shown in FIG. In the figure, the open symbols indicate the contact time at room temperature, and the filled symbols indicate 5
The contact time in the state heated at 5 ° C is shown. In the present invention, since it is heated to 40 to 60 ° C. in the back-extraction operation, a conventional similar distribution coefficient can be obtained in a contact time of about 1 minute. The separation factors of lanthanide and americium at this time are as follows. Cerium 91 Neodymium 19 Samarium 23 Europium 33 Gadolinium 23

【0009】[0009]

【発明の効果】以上説明したように、本発明によれば、
以上のように特別の組成の抽出剤及び逆抽出剤を使用
し、逆抽出操作において加温するので接触時間が短くて
すみ、アメリシウム及びキュリウムの分離を短時間で行
うことができる。又、抽出剤のリン酸系試薬及び逆抽出
剤の試薬の濃度が小さくてすむので、抽出剤の廃液量を
減量することができる。
As described above, according to the present invention,
As described above, the extractant and the back extractant having the special composition are used, and the heating is performed in the back extraction operation, so that the contact time is short, and the americium and the curium can be separated in a short time. Further, since the concentrations of the phosphoric acid type reagent of the extracting agent and the reagent of the back extracting agent can be small, the amount of the extracting agent waste liquid can be reduced.

【図面の簡単な説明】[Brief description of drawings]

【図1】本発明方法の1実施形態のフローチャートであ
る。
1 is a flow chart of one embodiment of the method of the present invention.

【図2】本発明方法の抽出操作における分配係数とpH
の関係を示すグラフである。
FIG. 2 Partition coefficient and pH in the extraction operation of the method of the present invention
6 is a graph showing the relationship of.

【図3】本発明方法の逆抽出操作における分配係数と接
触時間の関係を示すグラフである。
FIG. 3 is a graph showing the relationship between the distribution coefficient and the contact time in the back extraction operation of the method of the present invention.

───────────────────────────────────────────────────── フロントページの続き (72)発明者 藤岡 綱昭 東京都千代田区丸の内二丁目5番1号 三 菱重工業株式会社内 (72)発明者 波多野 守 東京都千代田区丸の内二丁目5番1号 三 菱重工業株式会社内 ─────────────────────────────────────────────────── ─── Continuation of front page (72) Inventor Tsunaaki Fujioka 2-5-1, Marunouchi, Chiyoda-ku, Tokyo Sanryo Heavy Industries Co., Ltd. (72) Mamoru Hatano 2-5-1, Marunouchi, Chiyoda-ku, Tokyo Sanryo Heavy Industries Co., Ltd.

Claims (1)

【特許請求の範囲】[Claims] 【請求項1】 ランタニド、アメリシウム及びキュリウ
ムを含む原子炉燃料再処理廃液のpHを先ず2〜3に調
整し、次に0.3Mのジ−2−エチルヘキシル リン酸
及び0.2Mのリン酸トリブチル並びに希釈剤としての
n−ドデカンからなる混合溶媒を抽出剤としてこれに前
述の調整済み廃液を室温条件下で、5分間接触させ、ラ
ンタニド、アメリシウム及びキュリウムを抽出剤に抽出
し、しかる後、1Mのグリコール酸と苛性ソウダでpH
を〜3に調整した0.01Mのジエチレントリアミン五
酢酸五ナトリウムとの溶液を逆抽出剤としてこれとアメ
リシウム等を含む前記抽出剤とを液温40〜60℃で1
分間接触させ、アメリシウムとキュリウムとを逆抽出
し、ランタニドから分離することを特徴とする原子炉燃
料再処理廃液の処理方法。
1. The pH of a reactor fuel reprocessing waste liquid containing lanthanide, americium, and curium is first adjusted to 2-3, and then 0.3M di-2-ethylhexylphosphoric acid and 0.2M tributyl phosphate. Also, a mixed solvent consisting of n-dodecane as a diluent is used as an extractant, and the adjusted waste liquid is brought into contact with this for 5 minutes under room temperature conditions to extract lanthanide, americium and curium into the extractant, and then 1M. PH with glycolic acid and caustic soda
As a back extractant with a solution of 0.01 M diethylenetriaminepentaacetic acid pentasodium adjusted to 3 to 3 and the extractant containing americium and the like at a liquid temperature of 40 to 60 ° C.
A method for treating waste liquid for reprocessing of nuclear reactor fuel, which comprises contacting for a minute, back-extracting americium and curium, and separating from lanthanide.
JP5590696A 1996-03-13 1996-03-13 Method for processing reactor fuel reprocessed waste liquid Withdrawn JPH09243796A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP5590696A JPH09243796A (en) 1996-03-13 1996-03-13 Method for processing reactor fuel reprocessed waste liquid

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP5590696A JPH09243796A (en) 1996-03-13 1996-03-13 Method for processing reactor fuel reprocessed waste liquid

Publications (1)

Publication Number Publication Date
JPH09243796A true JPH09243796A (en) 1997-09-19

Family

ID=13012167

Family Applications (1)

Application Number Title Priority Date Filing Date
JP5590696A Withdrawn JPH09243796A (en) 1996-03-13 1996-03-13 Method for processing reactor fuel reprocessed waste liquid

Country Status (1)

Country Link
JP (1) JPH09243796A (en)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114113284A (en) * 2021-11-26 2022-03-01 中国辐射防护研究院 Analysis method of yttrium-90 as americium and curium chemical separation tracer

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN114113284A (en) * 2021-11-26 2022-03-01 中国辐射防护研究院 Analysis method of yttrium-90 as americium and curium chemical separation tracer
CN114113284B (en) * 2021-11-26 2023-10-20 中国辐射防护研究院 Analysis method of yttrium-90 as americium and curium chemical separation tracer

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