JP3042010B2 - Waste liquid treatment method and waste liquid treatment device - Google Patents
Waste liquid treatment method and waste liquid treatment deviceInfo
- Publication number
- JP3042010B2 JP3042010B2 JP3113474A JP11347491A JP3042010B2 JP 3042010 B2 JP3042010 B2 JP 3042010B2 JP 3113474 A JP3113474 A JP 3113474A JP 11347491 A JP11347491 A JP 11347491A JP 3042010 B2 JP3042010 B2 JP 3042010B2
- Authority
- JP
- Japan
- Prior art keywords
- waste liquid
- solvent
- carrier
- tank
- adsorbent
- 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.)
- Expired - Lifetime
Links
- 239000007788 liquid Substances 0.000 title claims description 86
- 239000002699 waste material Substances 0.000 title claims description 67
- 238000000034 method Methods 0.000 title claims description 14
- 239000002904 solvent Substances 0.000 claims description 53
- 238000001179 sorption measurement Methods 0.000 claims description 50
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 40
- 239000003463 adsorbent Substances 0.000 claims description 37
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 32
- 229910017604 nitric acid Inorganic materials 0.000 claims description 32
- 239000011347 resin Substances 0.000 claims description 19
- 229920005989 resin Polymers 0.000 claims description 19
- 238000010828 elution Methods 0.000 claims description 9
- 238000005406 washing Methods 0.000 claims description 7
- 238000001035 drying Methods 0.000 claims description 3
- 239000000463 material Substances 0.000 claims description 2
- 239000000243 solution Substances 0.000 description 35
- 238000012545 processing Methods 0.000 description 11
- 239000011148 porous material Substances 0.000 description 10
- 230000008929 regeneration Effects 0.000 description 9
- 238000011069 regeneration method Methods 0.000 description 9
- 239000002901 radioactive waste Substances 0.000 description 8
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 7
- -1 carbamyl methylene phosphate Chemical compound 0.000 description 6
- 230000004913 activation Effects 0.000 description 5
- 238000004132 cross linking Methods 0.000 description 5
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 4
- 238000000605 extraction Methods 0.000 description 4
- 229910052768 actinide Inorganic materials 0.000 description 3
- 150000001255 actinides Chemical class 0.000 description 3
- 230000007423 decrease Effects 0.000 description 3
- 230000004992 fission Effects 0.000 description 3
- 239000011521 glass Substances 0.000 description 3
- 229910052747 lanthanoid Inorganic materials 0.000 description 3
- 150000002602 lanthanoids Chemical class 0.000 description 3
- 229910052695 Americium Inorganic materials 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 2
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 238000005470 impregnation Methods 0.000 description 2
- 239000010808 liquid waste Substances 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 150000002894 organic compounds Chemical class 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 239000010452 phosphate Substances 0.000 description 2
- 238000000197 pyrolysis Methods 0.000 description 2
- 230000002285 radioactive effect Effects 0.000 description 2
- 238000012958 reprocessing Methods 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 239000004925 Acrylic resin Substances 0.000 description 1
- 229910052685 Curium Inorganic materials 0.000 description 1
- 229910052781 Neptunium Inorganic materials 0.000 description 1
- SDQIHNPBCMQMQH-UHFFFAOYSA-N P1(=O)(OC(N(C(C)(CCCCCC)CCCCCC)CC)=O)OCO1 Chemical compound P1(=O)(OC(N(C(C)(CCCCCC)CCCCCC)CC)=O)OCO1 SDQIHNPBCMQMQH-UHFFFAOYSA-N 0.000 description 1
- 229910052778 Plutonium Inorganic materials 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- 229910052770 Uranium Inorganic materials 0.000 description 1
- LXQXZNRPTYVCNG-UHFFFAOYSA-N americium atom Chemical compound [Am] LXQXZNRPTYVCNG-UHFFFAOYSA-N 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 229910052792 caesium Inorganic materials 0.000 description 1
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- MYRTYDVEIRVNKP-UHFFFAOYSA-N divinylbenzene Substances C=CC1=CC=CC=C1C=C MYRTYDVEIRVNKP-UHFFFAOYSA-N 0.000 description 1
- 239000003480 eluent Substances 0.000 description 1
- 239000000945 filler Substances 0.000 description 1
- 230000002209 hydrophobic effect Effects 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000000622 liquid--liquid extraction Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000003595 mist Substances 0.000 description 1
- LFNLGNPSGWYGGD-UHFFFAOYSA-N neptunium atom Chemical compound [Np] LFNLGNPSGWYGGD-UHFFFAOYSA-N 0.000 description 1
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 description 1
- 239000002952 polymeric resin Substances 0.000 description 1
- 238000003672 processing method Methods 0.000 description 1
- 239000012857 radioactive material Substances 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 238000000638 solvent extraction Methods 0.000 description 1
- 239000002915 spent fuel radioactive waste Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 description 1
- 229920003002 synthetic resin Polymers 0.000 description 1
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
Landscapes
- Water Treatment By Sorption (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
- Treatment Of Liquids With Adsorbents In General (AREA)
Description
【０００１】[0001]
【産業上の利用分野】本発明は、主として再処理工場等
で発生する放射性廃液中からＴＲＵ（長半減期核種）を
除去する廃液処理方法および廃液処理装置に関するもの
で、特に廃液処理に使用する吸着材の活性化および再生
システムを有する廃液処理方法および廃液処理装置であ
る。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a waste liquid treatment method and a waste liquid treatment apparatus for removing TRU (long half-life nuclide) from radioactive waste liquid mainly generated in a reprocessing plant or the like, and particularly to a waste liquid treatment. A waste liquid treatment method and a waste liquid treatment apparatus having an adsorbent activation and regeneration system.
【０００２】[0002]
【従来の技術】使用済み核燃料に対しては、再処理によ
りウラン（Ｕ）・プルトニウム（Ｐu）を回収し、残り
の放射性廃液をガラス固化する方法が我が国において採
択されている。この放射性廃液中にはセシウム（Ｃs）,
ストロンチウム（Ｓr）,ルテニウム（Ｒu）などの核分
裂生成物の他に、微量のネプツニウム（Ｎp）,アメリシ
ウム（Ａm）,キュリウム（Ｃm）等のＴＲＵ（長半減期
核種）が含まれている。2. Description of the Related Art A method of recovering uranium (U) and plutonium (Pu) from spent nuclear fuel by reprocessing and vitrifying the remaining radioactive liquid waste has been adopted in Japan. Cesium (Cs),
In addition to fission products such as strontium (Sr) and ruthenium (Ru), trace amounts of TRUs (long half-life nuclides) such as neptunium (Np), americium (Am) and curium (Cm) are contained.
【０００３】これらＴＲＵの中にはたとえば243Ａmや
245Ｃmのように半減期が５０００年以上にも及ぶα放射
体があり、廃棄物の処理処分という観点から、放射性廃
液中に含まれるＴＲＵを分離し、これを効果的に貯蔵管
理または適切に処分することが最も妥当な考え方であ
る。[0003] Among these TRUs, for example, 243 Am and
There is an α-emitter with a half-life of 5,000 years or more, such as 245 Cm. From the viewpoint of waste treatment and disposal, TRU contained in radioactive waste liquid is separated and this is effectively stored and managed or properly treated. Disposal is the most reasonable idea.
【０００４】放射性廃液からＴＲＵ（長半減期核種）を
分離する方法としては、液-液抽出法や液-（担体＋溶
媒）抽出法等が開発されている。上記抽出方法において
は、その性能を高める為に接触面積を大きくし、その抽
出系の充填器、分散装置（攪拌、分散板、トレー等）に
工夫を凝らした設計が開発されている。As a method for separating TRU (long half-life nuclide) from radioactive liquid waste, a liquid-liquid extraction method, a liquid- (carrier + solvent) extraction method and the like have been developed. In the above extraction method, a design has been developed in which the contact area is increased in order to enhance the performance, and the filler and disperser (stirring, dispersion plate, tray, etc.) of the extraction system are devised.
【０００５】[0005]
【発明が解決しようとする課題】しかしながら、接触面
積を大きくする為の種々の分散装置があるが、満足な性
能を得ることができず、また経済的にも不十分なもので
あった。特に、吸着材を再利用すること、その際、吸着
材の再生時間を短縮すること、また二次放射性廃棄物を
少なくすること、設備コストを最小にすること等が切望
されている。However, although there are various dispersing devices for increasing the contact area, satisfactory performance has not been obtained, and it has been economically insufficient. In particular, there is an urgent need to reuse the adsorbent, shorten the regeneration time of the adsorbent, reduce secondary radioactive waste, minimize equipment costs, and the like.
【０００６】本発明は前記課題を解決するためになされ
たもので、接触面積を大きくする手段として、多孔質の
樹脂を使い、その孔に溶媒を含浸させることにより、解
決するものである。その為に、本処理方法と本処理装置
は樹脂への溶媒含浸、洗浄システムを構築して対処する
ものである。さらに、初期活性化及び再生システムを導
入し、効率のよい運用ができるようにするものである。The present invention has been made to solve the above-mentioned problem, and is to solve the problem by using a porous resin as a means for increasing the contact area and impregnating the pores with a solvent. For this purpose, the present processing method and the present processing apparatus are to cope with the problem by constructing a system for impregnating a resin with a solvent and a cleaning system. Furthermore, an initial activation and reproduction system is introduced to enable efficient operation.
【０００７】[0007]
【課題を解決するための手段】請求項１記載の廃液処理
方法は、 多孔質樹脂からなる担体に溶媒を含浸した後に、 該担体の表面を水洗いし、 担体を乾燥して吸着材を活性化する。 活性化された吸着材に廃液を流通させて廃液中のＴＲ
Ｕを選択的に吸着分離する。 ＴＲＵが除去された処理液を排除した後に、ＴＲＵを
吸着した吸着材を硝酸溶液で洗浄して担体からＴＲＵを
溶離し、 ＴＲＵを含む硝酸溶液を溶離溶液タンクに送る。 残った硝酸溶液も抜水した後に、担体に再び溶媒を含
浸し、 担体の表面を水洗いし、 担体を乾燥して吸着材を再生する。According to a first aspect of the present invention, there is provided a waste liquid treatment method comprising: impregnating a carrier made of a porous resin with a solvent; washing the surface of the carrier with water; and drying the carrier to activate the adsorbent. I do. The waste liquid is passed through the activated adsorbent and the TR in the waste liquid
U is selectively adsorbed and separated. After removing the treatment liquid from which TRU has been removed, the TRU-adsorbed adsorbent is washed with a nitric acid solution to elute TRU from the carrier, and the nitric acid solution containing TRU is sent to an elution solution tank. After draining the remaining nitric acid solution, the carrier is impregnated with the solvent again, the surface of the carrier is washed with water, and the carrier is dried to regenerate the adsorbent.
【０００８】請求項２記載の廃液処理装置は、吸着材の
内設されている吸着塔に、廃液タンクと廃液ポンプを有
する第１供給循環機と、水タンクと水ポンプを有する第
２供給循環機と、溶媒中間タンクと溶媒ポンプを有する
第３供給循環機と、硝酸溶液中間タンクと硝酸溶液ポン
プを有する第４供給循環機と、乾燥機と、溶離溶液タン
クと、処理液タンクとが各々接続していることを特徴と
するものである。According to a second aspect of the present invention, in the waste liquid treatment apparatus, a first supply circulating machine having a waste liquid tank and a waste liquid pump, and a second supply circulation machine having a water tank and a water pump are provided in an adsorption tower provided with an adsorbent. A third supply circulator having a solvent intermediate tank and a solvent pump; a fourth supply circulator having a nitric acid solution intermediate tank and a nitric acid solution pump; a dryer; an elution solution tank; It is characterized by being connected.
【０００９】[0009]
【作用】本発明の廃液処理方法の抽出原理は、次の通り
である。 多孔質の樹脂（担体）に溶媒（抽出剤、例えば、二酸
化有機リン酸化合物（DHDECMP））を含浸させた後に、
樹脂表面に付着している溶媒を除去（水洗い）し、さら
に乾燥させてなる活性化状態の吸着材を使用する。 その活性化された吸着材にＴＲＵ（長半減期核種Ｐ
ｕ，Ａｍ，等）を含む廃液（放射性廃液）を通過させ
る。 選択的にＴＲＵを吸着する。 ＴＲＵの除去された処理液は一般の放射性廃液として
処理、処分する。 ＴＲＵを吸着した吸着材（担体＋溶媒）は、硝酸溶液
（０.１〜０.５Ｎ）で洗浄し、ＴＲＵを樹脂から溶離す
る。 溶離したＴＲＵを含む硝酸溶液は別途濃縮し、安定な
固化体（例えば、ガラス）として処分する。The principle of extraction of the waste liquid treatment method of the present invention is as follows. After impregnating the porous resin (carrier) with a solvent (extractant, for example, organic phosphoric acid dioxide compound (DHDECMP)),
An activated adsorbent obtained by removing (washing) the solvent adhering to the resin surface and drying the solvent is used. The activated adsorbent contains TRU (long half-life nuclide P
u, Am, etc.) (radioactive waste liquid). TRU is selectively adsorbed. The treatment liquid from which TRU has been removed is treated and disposed of as a general radioactive waste liquid. The adsorbent (carrier + solvent) on which TRU has been adsorbed is washed with a nitric acid solution (0.1 to 0.5N) to elute TRU from the resin. The nitric acid solution containing the eluted TRU is separately concentrated and disposed of as a stable solid (eg, glass).
【００１０】[0010]
【実施例】本発明の廃液処理装置の一例を図１を参照し
て説明する。吸着塔６０に、第１供給循環機１０と、第
２供給循環機２０と、第３供給循環機３０と、第４供給
循環機４０が第１配管１２を介して各々接続されてい
る。また、第３配管３２を介して乾燥機５０が、第２配
管２２を介して処理液タンク６６が、さらに溶離溶液タ
ンク６４が第４配管４２を介して各々吸着塔６０に接続
されている。吸着塔６０には、溶媒（抽出剤）の含浸さ
れた多孔質な樹脂からなる吸着材１４が内設されてい
る。尚、各機および各配管の接続部にはバルブが設けら
れ、廃液処理装置の作動時には各バルブを制御して運用
する。DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS An example of a waste liquid treatment apparatus according to the present invention will be described with reference to FIG. The first supply circulator 10, the second supply circulator 20, the third supply circulator 30, and the fourth supply circulator 40 are connected to the adsorption tower 60 via the first pipe 12, respectively. The dryer 50 is connected to the adsorption tower 60 via the third pipe 32, the processing liquid tank 66 via the second pipe 22, and the elution solution tank 64 via the fourth pipe 42. An adsorbent 14 made of a porous resin impregnated with a solvent (extractant) is provided in the adsorption tower 60. A valve is provided at a connection between each machine and each pipe, and each valve is controlled and operated when the waste liquid treatment apparatus is operated.
【００１１】第１供給循環機１０には廃液タンク１８と
廃液ポンプ１６が配設されている。廃液ポンプ１６は廃
液タンク１８中のＴＲＵを含んでいる廃液を第１配管１
２を介して吸着塔６０に供給し、また循環させる。The first supply circulator 10 is provided with a waste liquid tank 18 and a waste liquid pump 16. The waste liquid pump 16 discharges the waste liquid containing TRU in the waste liquid tank 18 to the first pipe 1.
The mixture is supplied to the adsorption tower 60 through the pipe 2 and circulated.
【００１２】第２供給循環機２０には水タンク２８と水
ポンプ２６が配設されている。水ポンプ２６は水タンク
２８中の水を第１配管１２を介して吸着塔６０に供給
し、また循環させる。A water tank 28 and a water pump 26 are provided in the second supply circulator 20. The water pump 26 supplies and circulates the water in the water tank 28 to the adsorption tower 60 via the first pipe 12.
【００１３】第３供給循環機３０には溶媒中間タンク３
８と溶媒ポンプ３６が配設されている。溶媒ポンプ３６
は溶媒中間タンク３８中の溶媒（抽出剤）を第１配管１
２を介して吸着塔６０に供給し、また循環させる。The third supply circulator 30 includes a solvent intermediate tank 3
8 and a solvent pump 36 are provided. Solvent pump 36
Represents the solvent (extractant) in the solvent intermediate tank 38 in the first pipe 1
The mixture is supplied to the adsorption tower 60 through the pipe 2 and circulated.
【００１４】第４供給循環機４０には硝酸溶液中間タン
ク４８と硝酸溶液ポンプ４６が配設されている。硝酸溶
液ポンプ４６は硝酸溶液中間タンク４８中の硝酸溶液を
第１配管１２を介して吸着塔６０に供給し、また循環さ
せる。The fourth supply circulator 40 is provided with a nitric acid solution intermediate tank 48 and a nitric acid solution pump 46. The nitric acid solution pump 46 supplies and circulates the nitric acid solution in the nitric acid solution intermediate tank 48 to the adsorption tower 60 via the first pipe 12.
【００１５】乾燥機５０には、クーラー（熱交換器）５
４とサイクロン５８とヒーター（熱交換器）５６とブロ
ワー５２が配設されている。この乾燥機５０は第３配管
３２を介して吸着塔６０内を脱水処理する。乾燥機５０
では、ブロワー５２で空気を循環させ、ヒーター（熱交
換器）５６で空気を加熱（１００℃以下）し、吸着塔６
０へ送り込み、さらに吸着塔６０から送り出された空気
をクーラー（熱交換器）５４で冷却し、空気中の水分を
凝縮分離する。サイクロン５８は凝縮水のミスト分離
器、ドレンポット５９は凝縮水の一時貯槽である。ドレ
ンポット５９の凝縮水は、水タンク２８へ送られる。The dryer 50 includes a cooler (heat exchanger) 5.
4, a cyclone 58, a heater (heat exchanger) 56, and a blower 52 are provided. The dryer 50 dehydrates the inside of the adsorption tower 60 through the third pipe 32. Dryer 50
Then, the air is circulated by the blower 52, the air is heated (100 ° C. or less) by the heater (heat exchanger) 56,
0, and the air sent out from the adsorption tower 60 is further cooled by a cooler (heat exchanger) 54 to condense and separate water in the air. The cyclone 58 is a mist separator for condensed water, and the drain pot 59 is a temporary storage tank for condensed water. The condensed water in the drain pot 59 is sent to the water tank 28.
【００１６】処理液タンク６６は吸着塔６０でＴＲＵの
除去された処理液を溜めるもので、所定量蓄えられた後
に処理処分する。The processing liquid tank 66 stores the processing liquid from which the TRU has been removed in the adsorption tower 60. After storing a predetermined amount, the processing liquid is disposed.
【００１７】溶離溶液タンク６４は吸着材１４を硝酸溶
液で洗浄した後に、ＴＲＵを含有する硝酸溶液を溜める
もので、所定量蓄えられた後にＴＲＵを別途濃縮し、安
定な固化体（例えば、ガラス）として処分する。The elution solution tank 64 is for storing the nitric acid solution containing TRU after the adsorbent 14 is washed with the nitric acid solution. After storing the predetermined amount, the TRU is separately concentrated, and the stable solidified material (eg, glass) ).
【００１８】吸着塔６２は吸着塔６０と同じ機能を果す
もので、吸着塔６２にも、第１供給循環機１０と、第２
供給循環機２０と、第３供給循環機３０と、第４供給循
環機４０が各々接続されている（図示省略）。さらに、
乾燥機５０と処理液タンク６６と溶離溶液タンク６４も
各々吸着塔６２に接続している。The adsorption tower 62 has the same function as the adsorption tower 60.
The supply circulator 20, the third supply circulator 30, and the fourth supply circulator 40 are connected to each other (not shown). further,
The dryer 50, the processing liquid tank 66, and the elution solution tank 64 are also connected to the adsorption tower 62, respectively.
【００１９】次にこの廃液処理装置を運用して廃液を処
理する場合について説明する。 まず、吸着塔６０内の吸着材１４を活性化する。溶媒
中間タンク３８から溶媒ポンプ３６を介して溶媒（カル
バミルメチレンリン酸エステル(ＣＭＰ)）を吸着塔６０
に供給し、吸着塔６０内の多孔質樹脂である担体に溶媒
を含浸する。含浸が完了したら、吸着塔６０内の溶媒を
溶媒中間タンク３８へ抜出す。Next, a case where waste liquid is treated by operating the waste liquid treatment apparatus will be described. First, the adsorbent 14 in the adsorption tower 60 is activated. The solvent (carbamyl methylene phosphate (CMP)) is supplied from the solvent intermediate tank 38 via the solvent pump 36 to the adsorption tower 60.
And the carrier, which is a porous resin in the adsorption tower 60, is impregnated with a solvent. When the impregnation is completed, the solvent in the adsorption tower 60 is discharged to the solvent intermediate tank 38.
【００２０】水タンク２８から水ポンプ２６を介し
て、吸着塔６０内に水を流入し、吸着塔６０内の担体表
面に付着した溶媒を水洗し、除去する。水洗いが完了し
たら、水タンク２８へ抜水する。汚れた水は別途溶媒と
水の分離機へ送る。Water flows into the adsorption tower 60 from the water tank 28 via the water pump 26, and the solvent attached to the surface of the carrier in the adsorption tower 60 is washed and removed. When the washing is completed, the water is drained to the water tank 28. Dirty water is sent separately to the solvent and water separator.
【００２１】水洗後、担体を乾燥させる為に、乾燥機
５０を使用して脱水処理する。ブロワー５２で循環され
る空気をヒーター（熱交換器）５６で空気を加熱（１０
０℃以下）し、吸着塔６０へ送り込み、さらに吸着塔６
０から送り出された空気をクーラー（熱交換器）５４で
冷却し、空気中の水分を凝縮分離する。尚、放射性物質
の拡散防止の為、クローズドシステムで運転する。こう
して、吸着塔６０内の吸着材１４の活性化が終了する。After washing with water, the carrier is dehydrated using a drier 50 in order to dry the carrier. The air circulated by the blower 52 is heated by a heater (heat exchanger) 56 (10).
0 ° C. or lower), and sent to the adsorption tower 60,
The air sent from 0 is cooled by a cooler (heat exchanger) 54, and the moisture in the air is condensed and separated. The system is operated in a closed system to prevent radioactive materials from diffusing. Thus, the activation of the adsorbent 14 in the adsorption tower 60 ends.
【００２２】次に、この廃液処理装置を運転して廃液
を処理する。廃液タンク１８から廃液ポンプ１６を介し
て吸着塔６０にＴＲＵを含む廃液を供給し、スタートア
ップする。廃液タンク１８、廃液ポンプ１６、吸着塔６
０と循環させて廃液中のＴＲＵが吸着材１４に吸着され
るまで循環する。吸着塔６０の頂部で、廃液中のＴＲＵ
濃度が所定の値にまで低下したら、廃液を処理液として
処理液タンク６６へ送る。処理液タンク６６に溜められ
た処理液は放射性廃液として処分する。Next, the waste liquid processing apparatus is operated to treat the waste liquid. The waste liquid containing TRU is supplied from the waste liquid tank 18 to the adsorption tower 60 via the waste liquid pump 16 to start up. Waste liquid tank 18, waste liquid pump 16, adsorption tower 6
It circulates to 0 and circulates until the TRU in the waste liquid is adsorbed on the adsorbent 14. At the top of the adsorption tower 60, TRU in waste liquid
When the concentration decreases to a predetermined value, the waste liquid is sent to the processing liquid tank 66 as a processing liquid. The processing liquid stored in the processing liquid tank 66 is disposed as radioactive waste liquid.
【００２３】吸着塔６０内の廃液を抜いた後に、吸着
材１４を再生する。硝酸溶液中間タンク４８と硝酸溶液
ポンプ４６を運転し、硝酸溶液（０.１〜０.５規定）を
吸着塔６０に充液し、吸着塔６０内の吸着材１４に吸着
されたＴＲＵを硝酸溶液で溶離させ、これを溶離溶液タ
ンク６４に洗い出す。ＴＲＵの濃度が所定値以下になっ
たら、溶離操作を停止する。吸着塔６０内に残った硝酸
溶液は硝酸溶液中間タンク４８に抜液する。溶離溶液タ
ンク６４に溜められた硝酸溶液中のＴＲＵは別途濃縮
し、安定な固化体（例えば、ガラス）として処分する。After draining the waste liquid in the adsorption tower 60, the adsorbent 14 is regenerated. The nitric acid solution intermediate tank 48 and the nitric acid solution pump 46 are operated to fill the adsorption tower 60 with the nitric acid solution (0.1 to 0.5N), and the TRU adsorbed by the adsorbent 14 in the adsorption tower 60 is converted into nitric acid. The solution is eluted and washed out into the elution solution tank 64. When the TRU concentration falls below the predetermined value, the elution operation is stopped. The nitric acid solution remaining in the adsorption tower 60 is drained to a nitric acid solution intermediate tank 48. The TRU in the nitric acid solution stored in the elution solution tank 64 is separately concentrated and disposed of as a stable solid (eg, glass).
【００２４】吸着塔６０内を硝酸溶液で洗浄し、抜液
が完了したら、溶媒中間タンク３８、溶媒ポンプ３６を
運転して、溶媒（ＣＭＰ）を吸着塔６０に供給する。樹
脂（担体）はイオン交換性がある為に、硝酸溶液よりも
溶媒を選択的に吸着する。吸着が完了したら、吸着塔６
０内の溶媒を溶媒中間タンク３８へ抜出す。After the inside of the adsorption tower 60 is washed with a nitric acid solution and draining is completed, the solvent intermediate tank 38 and the solvent pump 36 are operated to supply the solvent (CMP) to the adsorption tower 60. Since the resin (carrier) has ion exchangeability, it adsorbs the solvent more selectively than the nitric acid solution. When the adsorption is completed, the adsorption tower 6
The solvent in 0 is drawn out to the solvent intermediate tank 38.
【００２５】水タンク２８から水ポンプ２６を介し
て、吸着塔６０内に水を流入し、吸着塔６０内の担体
（樹脂）表面に付着した溶媒を水洗し、除去する。水洗
いが完了したら、水ポンプ２８へ抜水する。汚れた水は
別途溶媒と水の分離機へ送る。Water flows from the water tank 28 into the adsorption tower 60 via the water pump 26, and the solvent attached to the surface of the carrier (resin) in the adsorption tower 60 is washed with water and removed. When the washing is completed, the water is drained to the water pump 28. Dirty water is sent separately to the solvent and water separator.
【００２６】水洗後、担体を乾燥させる為に、乾燥機
５０を使用して脱水処理する。ブロワー５２で循環され
る空気をヒーター（熱交換器）５６で空気を加熱（１０
０℃以下）し、吸着塔６０へ送り込み、さらに吸着塔６
０から送り出される空気をクーラー（熱交換器）５４で
冷却し、空気中の水を凝縮分離させる。After washing with water, the carrier is dehydrated using a dryer 50 in order to dry the carrier. The air circulated by the blower 52 is heated by a heater (heat exchanger) 56 (10).
0 ° C. or lower), and sent to the adsorption tower 60,
The air sent from 0 is cooled by a cooler (heat exchanger) 54, and water in the air is condensed and separated.
【００２７】こうして、吸着塔６０中の吸着材１４が再
生される。そして再び、廃液タンク１８から廃液ポンプ
１６を介してＴＲＵを含む廃液を供給し、スタートアッ
プする。以後、上記〜の廃液処理と吸着材の再生を
繰返して運転する。Thus, the adsorbent 14 in the adsorption tower 60 is regenerated. Then, the waste liquid containing TRU is supplied again from the waste liquid tank 18 via the waste liquid pump 16 to start up. Thereafter, the operation of the above-mentioned waste liquid treatment and regeneration of the adsorbent are repeated.
【００２８】尚、吸着塔６０と吸着塔６２はシーケンシ
ャルコントロール方式を採用して交互運用する。即ち、
吸着塔６０の再生中は、吸着塔６２を廃液処理用に運転
し、吸着塔６０で廃液処理中には、吸着塔６２を再生
し、交互切換運転をする。The adsorption tower 60 and the adsorption tower 62 are operated alternately by adopting a sequential control system. That is,
During regeneration of the adsorption tower 60, the adsorption tower 62 is operated for waste liquid treatment. During waste liquid treatment in the adsorption tower 60, the adsorption tower 62 is regenerated and alternately switched.
【００２９】多孔質樹脂である担体は、疎水性、親水性
いずれの性質を有する高分子樹脂であっても構わない
が、細孔径や粒子径の調整が容易な低架橋度のスチレン
-ジビニルベンゼン共重合体(ＳＤＢ)やアクリル酸エス
テル樹脂等が好適である。担体の形状は特に限定される
ものではないが、粒状が好ましい。特に粒子径が小さい
程、短い反応時間でＴＲＵを除去することができるので
好適である。The carrier, which is a porous resin, may be a polymer resin having either hydrophobic or hydrophilic properties. However, styrene having a low degree of cross-linking, whose pore size and particle size can be easily adjusted, may be used.
-Divinylbenzene copolymer (SDB), acrylate resin and the like are preferred. The shape of the carrier is not particularly limited, but is preferably granular. In particular, the smaller the particle size, the better the TRU can be removed in a short reaction time, which is preferable.
【００３０】多孔質樹脂の性状としては、溶媒（抽出
剤）を多量かつ均一に含浸可能なように、低架橋度であ
り一定の細孔径と細孔容積とを有するものが好ましい。
ＳＤＢを使用した場合には、架橋度を３％以上２０％未
満、平均細孔径を７００オングストローム以上３０００
オングストローム未満にし、反応速度を大きくするため
に平均細孔容積を０.７ml／g以上２.２ml／g未満とする
ことが好ましい。As the properties of the porous resin, those having a low degree of cross-linking and having a fixed pore diameter and a constant pore volume are preferable so that a large amount of solvent (extractant) can be uniformly impregnated.
When SDB is used, the degree of crosslinking is 3% or more and less than 20%, and the average pore diameter is 700 Å or more and 3000 or more.
It is preferable that the average pore volume be 0.7 ml / g or more and less than 2.2 ml / g in order to make the average pore volume less than angstrom and increase the reaction rate.
【００３１】ここで架橋度が３％未満であると、担体の
強度が著しく低下する。また架橋度が２０％より大きい
と、樹脂の膨潤性が低下するために溶媒（有機リン酸抽
出剤）を均一に含浸できなくなる。平均細孔径が３００
０オングストローム以上になると、ＳＤＢ中の細孔容積
が大きくなり過ぎるために、担体の強度が低下する。７
００オングストローム未満であると溶媒（有機リン酸抽
出剤）の含浸量が著しく低下してしまう。平均細孔容積
が２.２ml／g以上であると、担体の強度が低下する。ま
た０．７ml／g未満であると、溶媒（抽出剤）が含浸さ
れて担体が膨潤した際に、放射性廃液の流通路となる空
隙が小さくなるので、反応速度が著しく低下してしま
う。Here, when the degree of crosslinking is less than 3%, the strength of the carrier is significantly reduced. On the other hand, if the degree of crosslinking is more than 20%, the swellability of the resin is reduced, and the solvent (organic phosphoric acid extractant) cannot be uniformly impregnated. Average pore size of 300
At 0 Å or more, the pore volume in the SDB becomes too large, and the strength of the carrier decreases. 7
If it is less than 00 angstroms, the impregnation amount of the solvent (organic phosphoric acid extractant) is significantly reduced. When the average pore volume is 2.2 ml / g or more, the strength of the carrier decreases. On the other hand, if it is less than 0.7 ml / g, when the solvent (extractant) is impregnated and the carrier swells, the space that becomes the flow path of the radioactive waste liquid becomes small, so that the reaction rate is significantly reduced.
【００３２】溶媒（抽出剤）としては、放射性廃液中の
ＴＲＵが配位可能なものであれば特に限定されるもので
はないが、有機リン酸化合物が好ましい。硝酸水溶液中
のランタノイド元素およびアクチノイド元素を効率的に
捕集可能な二座配位有機リン酸抽出剤を用いることがで
きる。これらを例示すれば、カルバミルメチレンリン酸
エステル(ＣＭＰ)やカルバミルメチレンリン酸(ＣＭＰ
Ｏ)及びこれらの誘導体等であり、特にジヘキシルジエ
チルカルバミルメチレンリン酸エステル(DHDECMP)やジ
ヘキシル−Ｎ,Ｎ−ジエチルカルバミルメチレンリン酸
(DHDECMPO)が好適である。The solvent (extractant) is not particularly limited as long as TRU in the radioactive waste liquid can be coordinated, but an organic phosphate compound is preferred. A bidentate organophosphate extractant that can efficiently collect lanthanoid elements and actinoid elements in a nitric acid aqueous solution can be used. For example, carbamyl methylene phosphate (CMP) or carbamyl methylene phosphate (CMP)
O) and their derivatives, especially dihexyl diethylcarbamyl methylene phosphate (DHDECMP) and dihexyl-N, N-diethylcarbamyl methylene phosphate
(DHDECMPO) is preferred.
【００３３】多孔質樹脂からなる担体の製造方法は特に
限定されるものではないが、担体が粒状のものである場
合には、例えば特開昭６１−２５２２０２号公報等に記
載された二重ノズル振動法を利用することができる。The method for producing the carrier made of a porous resin is not particularly limited. When the carrier is granular, for example, a double nozzle described in JP-A-61-252202 or the like can be used. A vibration method can be used.
【００３４】本実施例の廃液処理方法においては、廃液
との接触面積が大きい多孔質樹脂に溶媒を含浸した吸着
材を使用するものなので、性能が高く、しかも選択的に
ＴＲＵを吸着分離し、処理できるものである。In the waste liquid treatment method of the present embodiment, since the adsorbent obtained by impregnating the solvent with the porous resin having a large contact area with the waste liquid is used, the performance is high, and the TRU is selectively adsorbed and separated. It can be processed.
【００３５】さらに、吸着材は再生して使用するものな
ので、経済的にも有用である。特に、吸着塔６０を廃液
処理に使用する際には吸着塔６２を再生し、また吸着塔
６０を再生中には吸着塔６２を廃液処理に使用すること
で、廃液処理装置を継続的に循環運用することのできる
シーケンシャルコントロールシステムとすることがで
き、吸着材の再生時間にとらわれる不要な時間がなく、
効率が高い。Furthermore, since the adsorbent is regenerated and used, it is economically useful. In particular, when the adsorption tower 60 is used for waste liquid treatment, the adsorption tower 62 is regenerated, and during the regeneration of the adsorption tower 60, the adsorption tower 62 is used for waste liquid treatment, thereby continuously circulating the waste liquid treatment apparatus. It can be a sequential control system that can be operated, there is no unnecessary time tied to the regeneration time of the adsorbent,
High efficiency.
【００３６】また、吸着材の活性化、廃液処理、吸着材
の再生がクローズドシステムで運用できるので、安全で
ある。さらに、廃液、硝酸溶液、水等の各機への流入や
抜水にタイマーを利用することで、設備を簡単にするこ
とができ、設備コストの削減が容易である。また、使用
する設備にポンプやブロワーなど汎用性なものを利用す
ることができるので、経済的で安全である。Further, the activation of the adsorbent, the treatment of waste liquid, and the regeneration of the adsorbent can be operated in a closed system, which is safe. Furthermore, by using a timer for inflow and drainage of waste liquid, nitric acid solution, water and the like into each machine, the equipment can be simplified and the equipment cost can be easily reduced. In addition, since versatile equipment such as a pump and a blower can be used for the equipment to be used, it is economical and safe.
【００３７】尚、この実施例の廃液処理装置は、多孔質
樹脂である担体中に溶媒である有機リン酸化合物を含浸
したものを使用するものであるから、ＴＲＵのみならず
含浸した溶媒と配位可能な元素、たとえばランタノイド
元素およびアクチノイド元素の分離に利用することもで
きる。Since the waste liquid treatment apparatus of this embodiment uses a porous resin carrier impregnated with an organic phosphoric acid compound as a solvent, not only the TRU but also the impregnated solvent is used. It can also be used for the separation of potential elements, such as lanthanoid and actinoid elements.
【００３８】またＴＲＵを廃液中の核分裂生成物から選
択的に除去できるので、二次廃液が大量に発生すること
がない。さらに本実施例での吸着材は、担体と溶媒（抽
出剤）のいずれもが有機化合物であるために、乾留等の
操作により容易に減容することができ、廃棄物の処理、
処分の観点からも有効である。Further, since TRU can be selectively removed from the fission products in the waste liquid, a large amount of secondary waste liquid is not generated. Furthermore, since both the carrier and the solvent (extractant) are organic compounds, the volume of the adsorbent in this embodiment can be easily reduced by an operation such as dry distillation.
It is also effective from the viewpoint of disposal.
【００３９】[0039]
【発明の効果】本発明の廃液処理方法においては、廃液
との接触面積が大きい多孔質樹脂に溶媒を含浸した吸着
材を使用するものなので、性能が高く、しかも選択的に
ＴＲＵを吸着分離し、処理できるものである。特に、本
発明の廃液処理方法は吸着材を再生して使用するものな
ので、経済的にも有用である。さらに、本発明の廃液処
理装置では継続的に循環運用することのできるシーケン
シャルコントロールシステムが可能であり、吸着材の再
生時間にとらわれる不要な時間がなく、効率が高い。ま
た、吸着材の活性化、廃液処理、吸着材の再生がクロー
ズドシステムで運用でき、安全である。さらに、廃液、
硝酸溶液、水等の各機への流入や抜水にタイマーを利用
することで、設備を簡単にすることができ、設備コスト
の削減が容易である。また、使用する設備にポンプやブ
ロワーなど汎用性なものを利用することができるので、
経済的で安全である。According to the waste liquid treatment method of the present invention, since the adsorbent obtained by impregnating the solvent with the porous resin having a large contact area with the waste liquid is used, the performance is high, and the TRU is selectively adsorbed and separated. Can be processed. In particular, the waste liquid treatment method of the present invention is economically useful because the adsorbent is regenerated and used. Furthermore, the waste liquid treatment apparatus of the present invention enables a sequential control system that can be continuously circulated and operated, and there is no unnecessary time limited by the regeneration time of the adsorbent, and the efficiency is high. In addition, activation of the adsorbent, treatment of waste liquid, and regeneration of the adsorbent can be operated in a closed system, which is safe. In addition, wastewater,
By using a timer for inflow and drainage of nitric acid solution, water, etc. to each machine, the equipment can be simplified and the equipment cost can be easily reduced. Also, versatile equipment such as pumps and blowers can be used for the equipment used,
Economical and safe.
【００４０】尚、この発明の廃液処理方法は、多孔質樹
脂である担体中に溶媒（抽出剤）を含浸したものを使用
するものであるから、ＴＲＵのみならず溶媒と配位可能
な元素、例えば、ランタノイド元素およびアクチノイド
元素の分離にも利用することができる。また、ＴＲＵを
廃液中の核分裂生成物から選択的に除去できるので、二
次廃液が大量に発生することがない。さらに、この発明
で使用する吸着材は、担体と溶媒（抽出剤）のいずれも
が有機化合物であるために、乾留等の操作により容易に
減容することができ、廃棄物の処理、処分の観点からも
有効である。Since the waste liquid treatment method of the present invention uses a porous resin carrier impregnated with a solvent (extractant), not only TRU but also an element capable of coordinating with the solvent, For example, it can be used for separating lanthanoid elements and actinoid elements. Further, since TRU can be selectively removed from fission products in the waste liquid, a large amount of secondary waste liquid is not generated. Furthermore, since both the carrier and the solvent (extractant) are organic compounds, the volume of the adsorbent used in the present invention can be easily reduced by an operation such as dry distillation. It is also effective from a viewpoint.
【図１】本実施例の廃液処理装置の概略図である。FIG. 1 is a schematic diagram of a waste liquid treatment apparatus of the present embodiment.
１０ 第１供給循環機 １２ 第１配管 １４ 吸着材 １６ 廃液ポンプ １８ 廃液タンク ２０ 第２供給循環機 ２２ 第２配管 ２６ 水ポンプ ２８ 水タンク ３０ 第３供給循環機 ３２ 第３配管 ３６ 溶媒ポンプ ３８ 溶媒中間タンク ４０ 第４供給循環機 ４６ 硝酸溶液ポンプ ４８ 硝酸溶液中間タンク ５０ 乾燥機 ５２ ブロワー ５４ クーラー（熱交換器） ５６ ヒーター（熱交換器） ６０ 吸着塔 ６２ 吸着塔 ６４ 溶離溶液タンク ６６ 処理液タンク DESCRIPTION OF SYMBOLS 10 1st supply circulation machine 12 1st piping 14 Adsorbent 16 Waste liquid pump 18 Waste liquid tank 20 2nd supply circulation machine 22 2nd piping 26 Water pump 28 Water tank 30 3rd supply circulation machine 32 3rd piping 36 Solvent pump 38 Solvent Intermediate tank 40 Fourth supply circulator 46 Nitric acid solution pump 48 Nitric acid solution intermediate tank 50 Dryer 52 Blower 54 Cooler (Heat exchanger) 56 Heater (Heat exchanger) 60 Adsorption tower 62 Adsorption tower 64 Eluent solution tank 66 Treatment liquid tank
───────────────────────────────────────────────────── フロントページの続き (58)調査した分野(Int.Cl.7，ＤＢ名) G21F 9/06 G21F 9/12 ──────────────────────────────────────────────────続 き Continued on the front page (58) Field surveyed (Int.Cl. 7 , DB name) G21F 9/06 G21F 9/12
Claims (2)
た後に、該担体の表面を水洗いし、担体を乾燥して吸着
材を活性化し、活性化された吸着材に廃液を流通させて
廃液中のＴＲＵを選択的に吸着分離し、ＴＲＵの吸着さ
れた吸着材を硝酸溶液で洗浄して担体からＴＲＵを溶離
し、硝酸溶液を抜水した後に、担体に再び溶媒を含浸
し、担体の表面を水洗いし、担体を乾燥して吸着材を再
生することを特徴とする廃液処理方法。1. After impregnating a carrier made of a porous resin with a solvent, the surface of the carrier is washed with water, the carrier is dried to activate an adsorbent, and a waste liquid is passed through the activated adsorbent. The TRU contained therein is selectively adsorbed and separated, the TRU adsorbed material is washed with a nitric acid solution to elute the TRU from the carrier, the nitric acid solution is drained, the carrier is impregnated with a solvent again, and the carrier is impregnated with the solvent. A method for treating waste liquid, comprising washing the surface with water and drying the carrier to regenerate the adsorbent.
タンクと廃液ポンプを有する第１供給循環機と、水タン
クと水ポンプを有する第２供給循環機と、溶媒中間タン
クと溶媒ポンプを有する第３供給循環機と、硝酸溶液中
間タンクと硝酸溶液ポンプを有する第４供給循環機と、
乾燥機と、溶離溶液タンクと、処理液タンクとが各々接
続していることを特徴とする廃液処理装置。2. A first supply circulator having a waste liquid tank and a waste liquid pump, a second supply circulator having a water tank and a water pump, a solvent intermediate tank, and a solvent in an adsorption tower provided inside the adsorbent. A third supply circulator having a pump, a fourth supply circulator having a nitric acid solution intermediate tank and a nitric acid solution pump,
A waste liquid treatment apparatus, wherein a dryer, an elution solution tank, and a treatment liquid tank are connected to each other.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP3113474A JP3042010B2 (en) | 1991-05-17 | 1991-05-17 | Waste liquid treatment method and waste liquid treatment device |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP3113474A JP3042010B2 (en) | 1991-05-17 | 1991-05-17 | Waste liquid treatment method and waste liquid treatment device |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH0580196A JPH0580196A (en) | 1993-04-02 |
| JP3042010B2 true JP3042010B2 (en) | 2000-05-15 |
Family
ID=14613182
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP3113474A Expired - Lifetime JP3042010B2 (en) | 1991-05-17 | 1991-05-17 | Waste liquid treatment method and waste liquid treatment device |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3042010B2 (en) |
-
1991
- 1991-05-17 JP JP3113474A patent/JP3042010B2/en not_active Expired - Lifetime
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0580196A (en) | 1993-04-02 |
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