JPH04188099A - Processing of chemical decontamination liquid waste - Google Patents
Processing of chemical decontamination liquid wasteInfo
- Publication number
- JPH04188099A JPH04188099A JP31573790A JP31573790A JPH04188099A JP H04188099 A JPH04188099 A JP H04188099A JP 31573790 A JP31573790 A JP 31573790A JP 31573790 A JP31573790 A JP 31573790A JP H04188099 A JPH04188099 A JP H04188099A
- Authority
- JP
- Japan
- Prior art keywords
- waste liquid
- decontamination
- chelate
- decontamination waste
- generated
- 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.)
- Granted
Links
- 238000009390 chemical decontamination Methods 0.000 title claims description 21
- 239000010808 liquid waste Substances 0.000 title abstract 4
- 239000002699 waste material Substances 0.000 claims abstract description 116
- 238000005202 decontamination Methods 0.000 claims abstract description 72
- 230000003588 decontaminative effect Effects 0.000 claims abstract description 71
- 239000013522 chelant Substances 0.000 claims abstract description 35
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 15
- 229910052751 metal Inorganic materials 0.000 claims abstract description 14
- 239000002184 metal Substances 0.000 claims abstract description 14
- 239000007788 liquid Substances 0.000 claims description 84
- 238000000034 method Methods 0.000 claims description 27
- 238000000354 decomposition reaction Methods 0.000 claims description 18
- 239000002738 chelating agent Substances 0.000 claims description 14
- 239000011259 mixed solution Substances 0.000 claims description 12
- 239000003929 acidic solution Substances 0.000 claims description 9
- 229910021645 metal ion Inorganic materials 0.000 claims description 9
- 230000001590 oxidative effect Effects 0.000 claims description 9
- 150000007524 organic acids Chemical class 0.000 claims description 4
- 238000001035 drying Methods 0.000 claims description 3
- 239000012530 fluid Substances 0.000 claims description 3
- 230000003472 neutralizing effect Effects 0.000 claims description 3
- KCXVZYZYPLLWCC-UHFFFAOYSA-N EDTA Chemical compound OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O KCXVZYZYPLLWCC-UHFFFAOYSA-N 0.000 abstract description 21
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 abstract description 18
- 229910017604 nitric acid Inorganic materials 0.000 abstract description 12
- 238000006243 chemical reaction Methods 0.000 abstract description 11
- 238000005868 electrolysis reaction Methods 0.000 abstract description 11
- 229910052697 platinum Inorganic materials 0.000 abstract description 9
- 239000007789 gas Substances 0.000 abstract description 7
- 230000000694 effects Effects 0.000 abstract description 5
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 abstract description 4
- 239000002253 acid Substances 0.000 abstract description 4
- 230000003647 oxidation Effects 0.000 abstract 1
- 238000007254 oxidation reaction Methods 0.000 abstract 1
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 description 48
- 239000000243 solution Substances 0.000 description 19
- 235000006408 oxalic acid Nutrition 0.000 description 16
- QAOWNCQODCNURD-UHFFFAOYSA-N sulfuric acid Substances OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 16
- 239000003456 ion exchange resin Substances 0.000 description 12
- 229920003303 ion-exchange polymer Polymers 0.000 description 12
- 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 11
- 238000006722 reduction reaction Methods 0.000 description 5
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 4
- 230000002378 acidificating effect Effects 0.000 description 4
- 239000010936 titanium Substances 0.000 description 4
- 229910052719 titanium Inorganic materials 0.000 description 4
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 3
- 150000001875 compounds Chemical class 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 238000006386 neutralization reaction Methods 0.000 description 3
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 2
- 239000007800 oxidant agent Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 238000007711 solidification Methods 0.000 description 2
- 230000008023 solidification Effects 0.000 description 2
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000011033 desalting Methods 0.000 description 1
- 230000005684 electric field Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 235000019253 formic acid Nutrition 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 150000004679 hydroxides Chemical class 0.000 description 1
- 238000007689 inspection Methods 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000003758 nuclear fuel Substances 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000003672 processing method Methods 0.000 description 1
- 230000002285 radioactive effect Effects 0.000 description 1
- 238000011946 reduction process Methods 0.000 description 1
- 230000001172 regenerating effect Effects 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 239000010802 sludge Substances 0.000 description 1
- 239000002689 soil Substances 0.000 description 1
Landscapes
- Water Treatment By Electricity Or Magnetism (AREA)
Abstract
Description
【発明の詳細な説明】
［発明の目的］
（産業上の利用分野）
本発明は原子力発電設備及び核燃料サイクル関連施設等
で使用される有機酸またはキレート剤及びこれら混合溶
液からなる除染液で除染した後に発生する使用済み化学
除染廃液（以下、キレート除染廃液と記す）の廃液処理
方法に関する。[Detailed Description of the Invention] [Object of the Invention] (Industrial Application Field) The present invention is a decontamination liquid consisting of an organic acid or chelating agent and a mixed solution thereof used in nuclear power generation equipment and nuclear fuel cycle related facilities. The present invention relates to a waste liquid treatment method for used chemical decontamination waste liquid (hereinafter referred to as chelate decontamination waste liquid) generated after decontamination.
（従来の技術）
一般に原子力施設においては、運転利用中のプラント機
器の保守・点検や補修作業時の放射線被曝量の低減と、
作業し易い作業環境を確保するために、系統構成機器、
配管ライン等の除染にキレート除染剤が使用される。こ
の除染方法は除染能力が比較的高く、しかも除染後機器
は十分な健全性を維持することができる。(Conventional technology) In general, in nuclear facilities, it is necessary to reduce radiation exposure during maintenance, inspection, and repair work of plant equipment during operation and use.
In order to ensure a comfortable working environment, system components,
Chelate decontamination agents are used to decontaminate piping lines, etc. This decontamination method has a relatively high decontamination capacity, and the equipment can maintain sufficient integrity after decontamination.
従来、この除染廃液の処理は、キレート剤に吸着された
放射能及び金属イオンをイオン交換樹脂により脱塩し、
キレート剤及びイオン交換樹脂は固化して保管していた
。Conventionally, this decontamination waste liquid is treated by desalting radioactivity and metal ions adsorbed by chelating agents using ion exchange resin.
The chelating agent and ion exchange resin were stored solidified.
（発明が解決しようとする課題）
しか［、なから、上述した除染廃液の処理方法は次のよ
うな課題を有していた。(Problems to be Solved by the Invention) However, the above-described method for treating decontamination waste liquid had the following problems.
（１）キレート除染廃液は、イオン交換樹脂により脱塩
処理していたため、使用済みイオン交換樹脂か二次廃棄
物として発生する。(1) Since the chelate decontamination waste liquid was desalted using ion exchange resin, it is generated as used ion exchange resin or secondary waste.
（２）脱塩処理したキレ−１・除染廃液は、乾燥−固化
していたためキレート剤か廃棄物として発生する。(2) Since the desalinated KIRE-1/decontamination waste liquid had been dried and solidified, it was generated as a chelating agent or waste.
（３，、キレート剤及びイオン交換樹脂に吸着された放
射能は、廃棄物とし７て貯蔵または処分された際、放射
能か土壌中に放出される可能性かある。(3) Radioactivity adsorbed on chelating agents and ion exchange resins may be released into the soil when stored or disposed of as waste.
本発明は上記課題を解決するためになされたちので、キ
レート除染廃液を酸化剤により分解し、二次廃棄物の発
生量を低減することかできる化学除染廃液の処理方法を
提供することにある。The present invention has been made to solve the above-mentioned problems, and therefore, an object of the present invention is to provide a method for treating chemical decontamination waste liquid that can reduce the amount of secondary waste generated by decomposing chelate decontamination waste liquid with an oxidizing agent. be.
［発明の構成］
（課題を解決するための手段）
本発明は原子力施設から発生する放射能で汚染された廃
棄物を、自機酸またはキし・−ト斉ｊ及びこれら混合溶
液からなる除染液で除染した後に発生ギる使用済み化学
除染廃液コ）処理方法において、前記キレート除染廃液
をＣｅ４−Ｃｅ’ −酸性溶液中に注入し、不活性金
属からなる陽極と不活性金属からなる陰極とを浸漬して
前記両電極間に直流電圧を印加して前記陽極てＣｅ’を
酸化してＣｅ４−を生成し、放射能及び金属イオンを吸
着したキレート剤をＣｅ４−の酸化力により分解するこ
とを特徴とする。また、前記キじ−ｒ除除染液液分解終
了後に残留するＣｅ４−をＣｅ３＋に還元し、中和剤に
より中和し、濃縮乾燥して固化することを特徴とする。[Structure of the Invention] (Means for Solving the Problems) The present invention treats radioactively contaminated waste generated from nuclear facilities by treating it with organic acid, chloride acid, and a mixed solution thereof. In the treatment method, the chelate decontamination waste liquid is injected into a Ce4-Ce'-acidic solution, and an anode made of an inert metal and an inert metal A DC voltage is applied between the two electrodes, and the anode oxidizes Ce' to produce Ce4-, and the chelating agent adsorbing radioactivity and metal ions is immersed in the chelating agent with the oxidizing power of Ce4-. It is characterized by being decomposed by Further, after completion of liquid decomposition of the KIJI-R decontamination liquid, residual Ce4- is reduced to Ce3+, neutralized with a neutralizing agent, concentrated and dried to solidify.
（作 用）
キレート除染膣液はキレート剤（Ｙ）と放射能及び金属
イオン（Ｎ１）とキレート化合物（Ｍ ’１’ ）を形
成している。Ｃｅ″’−Ｃｅ”−酸性溶液中にキレート
除染廃液を注入すると、Ｃｅ４の酸化力によりキレート
剤０°）はＣｅ、、Ｎ［（、、Ｈ。(Function) Chelate decontamination vaginal fluid forms a chelate compound (M'1') with the chelating agent (Y), radioactivity, and metal ion (N1). When the chelate decontamination waste liquid is injected into the Ce''-Ce''-acidic solution, the chelating agent 0°) becomes Ce,,N[(,,H) due to the oxidizing power of Ce4.
Ｏ等に分解するため、無機の化学除染廃液±して取り扱
うことかできる。還元されたＣｅ１は不活性金属からな
る陽極と不活性金属からなる陰極との間に直流電圧を印
加して陽極てＣｅ３＋に再生することかできるため、Ｃ
ｅ４−は分解剤として繰り返し使用することかできる。Since it decomposes into O, etc., it can be treated as inorganic chemical decontamination waste liquid. The reduced Ce1 can be regenerated into Ce3+ by applying a DC voltage between the anode made of an inert metal and the cathode made of an inert metal.
e4- can be used repeatedly as a decomposer.
キレート除染廃液の分解処理後は酸化剤であるＣｅ”か
残留するため、電解還元により安定なＣｅ’−に還元す
る。還元処理した後の無機の化学除染廃液は、酸性であ
るため中和剤を添加して中和し５、濃縮、乾燥／固化し
て安定な状態で保管することかできる。。After the decomposition treatment of the chelate decontamination waste liquid, the oxidizing agent Ce'' remains, so it is reduced to stable Ce'- by electrolytic reduction.The inorganic chemical decontamination waste liquid after the reduction treatment is acidic and therefore It can be neutralized by adding an admixture, concentrated, dried/solidified, and stored in a stable state.
（実施例）
本発明に係る化学除染廃液の処理方法の実施例を第１図
を参照しながら説明する。(Example) An example of the method for treating chemical decontamination waste liquid according to the present invention will be described with reference to FIG.
第１図は本発明方法を説明するだめのキレート廃液の分
解装置の一例を示した断面図であり、図中符号１はキレ
ート除染廃液貯留槽、２は電解槽である。この電解槽２
には分解剤であるＣｅ３−酸性溶液３か貯留されている
。電解槽２内のＣｅ３゛−酸性溶液３は循環ポシプ４に
より電解槽内を循環する。また、電解槽２には不活性金
属からなる陽極５と陰極６．ヒーター７か浸漬されてい
る。FIG. 1 is a sectional view showing an example of a chelate waste liquid decomposition apparatus for explaining the method of the present invention. In the figure, reference numeral 1 indicates a chelate decontamination waste liquid storage tank, and 2 indicates an electrolytic cell. This electrolytic cell 2
Ce3-acidic solution 3, which is a decomposition agent, is stored in the tank. The Ce3'-acidic solution 3 in the electrolytic cell 2 is circulated within the electrolytic cell by a circulation pump 4. The electrolytic cell 2 also includes an anode 5 and a cathode 6 made of inert metal. Heater 7 is immersed.
電解槽２の上部にはＣｅ”−酸性溶液３から発生する蒸
気、カスを処理下るだめの排カス処理系８か接続されて
いるっ
前記不活性金属からなる陽極５は白金と同等か若しくは
白金より酸素過電圧の高い金属または金属酸化物陽極で
、前記（ｅ Ｊ −Ｃｅ−１−酸性溶液中に、容は出
さないことか必要である。Connected to the upper part of the electrolytic cell 2 is a waste disposal system 8 for treating vapor and waste generated from the Ce"-acidic solution 3. The anode 5 made of an inert metal is made of platinum or similar material A metal or metal oxide anode with a higher oxygen overvoltage is required to be used in the (e J -Ce-1-acidic solution) without leaving any volume.
前記不活性金属からなる陰極６は白金と同等か若しくは
白金より水素過電圧の低い金属または金属酸化物陰極で
、前記Ｃｅ”−Ｃｅ’−酸性溶液中に溶は出さないこと
か必要である。The cathode 6 made of an inert metal is a metal or metal oxide cathode having a hydrogen overvoltage equal to or lower than that of platinum, and must not dissolve into the Ce''-Ce'-acidic solution.
次に第１図に示したキレート廃液の分解装置を使用して
本発明に係る化学除染廃液の処理方法の第１の実施例に
ついて説明する。Next, a first embodiment of the method for treating chemical decontamination waste liquid according to the present invention will be described using the chelate waste liquid decomposition apparatus shown in FIG.
第１の実施例は分解剤としてＣｅ”−硝酸溶液を選択し
、キレート除染廃液としてＥＤＴＡ （エチレンジアミ
ン四酢酸）除染廃液を処理する。ＥＤ Ｔ Ａ除染廃液
はＥＤＴＡ（Ｙ）に放射能及び金属イオン（Ｎ１）か吸
着しキレート化合物（ＭＹ）を形成している。In the first embodiment, a Ce"-nitric acid solution is selected as a decomposition agent, and EDTA (ethylenediaminetetraacetic acid) decontamination waste is treated as a chelate decontamination waste. EDTA (Y) decontamination waste is radioactive and metal ions (N1) are adsorbed to form a chelate compound (MY).
電解槽にＣｅ”−硝酸溶液を貯留し、加熱用ヒ−ターて
Ｃｅ ”−硝酸溶液を８０℃に昇温する。次に、ＥＤＴ
Ａ除染廃液を電解槽２に注入すると共に前記不活性陽極
５と不活性陰極６の間に所定の電流密度の直流電圧を印
加すると、前記陽極５て以下に示す反応か起こる。A Ce''-nitric acid solution is stored in an electrolytic cell, and the temperature of the Ce''-nitric acid solution is raised to 80°C using a heater. Next, E.D.T.
When the A decontamination waste liquid is injected into the electrolytic cell 2 and a DC voltage of a predetermined current density is applied between the inert anode 5 and the inert cathode 6, the following reaction occurs at the anode 5.
Ｃｅ ３−Ｉ−Ｃｅ ’−＋ ｅ
−（１）上記（１）式により生成したＣｅ４−は極めて
酸化力が強いため、電解槽２に注入したＥＤＴＡ除染廃
液（ＭＹ）とＣｅ４−とは以下に示す反応が起こる。Ce 3-I-Ce '-+ e
-(1) Since the Ce4- produced by the above formula (1) has extremely strong oxidizing power, the following reaction occurs between the EDTA decontamination waste liquid (MY) injected into the electrolytic cell 2 and Ce4-.
Ｃｅ’”＋ＭＹ→
Ｃｅ”＋Ｍ’−＋ＣＯ２＋ＮＨ３＋Ｈ２ＣＬ・１２）Ｅ
ＤＴＡの分解により発生するＣＯ２及びＮＨ３ガス、ま
たは蒸気は排ガス処理系８て処理される。一方、上記
（２）式の反応により還元されたＣ ｅ ”は前記不活
性陽極５と不活性陰極６の間に所定の電流密度の直流電
圧を印加しているため、（１）式の反応が生起し陽極５
でＣｅ３＋に再生される。Ce'"+MY→ Ce"+M'-+CO2+NH3+H2CL・12)E
CO2 and NH3 gases or steam generated by the decomposition of DTA are treated in an exhaust gas treatment system 8. On the other hand, the above
Since C e '' reduced by the reaction of formula (2) is applied between the inert anode 5 and the inert cathode 6 with a DC voltage of a predetermined current density, the reaction of formula (1) occurs. Anode 5
It is played back on Ce3+.
上記（１）式と （２）式の反応を確認するために、Ｅ
ＤＴＡ除染廃液の濃度０．０４ｍｏ１．＃ 、 Ｃｅ
３−濃度０、１ｍｏｌ／ｌ、硝酸濃度１．０ｍｏｆ／Ａ
’の混合溶液を電流密度０，３＾／ａ［！で電解した結
果を第２図によって説明する。第２図中の縦軸は電解に
よって陽極で生成されるＣｅ’″濃度、横軸は電解時間
を示す。In order to confirm the reactions of equations (1) and (2) above, E
The concentration of DTA decontamination waste liquid is 0.04mol. #, Ce
3-Concentration 0, 1 mol/l, nitric acid concentration 1.0 mof/A
' mixed solution at a current density of 0.3^/a [! The results of electrolysis will be explained with reference to FIG. In FIG. 2, the vertical axis shows the Ce''' concentration generated at the anode by electrolysis, and the horizontal axis shows the electrolysis time.
また、曲線ａはＣｅ ”−硝酸単独溶液を電解した場合
、曲線すはＥＤＴＡ除染廃液とＣｅ”−硝酸混合溶液を
電解した場合を示す。Ｃｅ”−硝酸単独溶液を電解した
場合は、はぼ電解時間に比例してＣｅ”濃度は増加する
が、ＥＤＴＡ除染廃液とＣｅ”−硝酸溶液との混合溶液
を電解した場合は、（２）式の分解反応が起こり、Ｃｅ
４−はＣｅ３＋に還元される。混合溶液中のＥＤＴＡが
全量分解した時点でＣｅ４°濃度は増加する。Further, curve a shows the case where a Ce''-nitric acid solution alone was electrolyzed, and curve a shows the case where an EDTA decontamination waste liquid and a Ce''-nitric acid mixed solution were electrolyzed. When a Ce"-nitric acid solution alone is electrolyzed, the Ce" concentration increases in proportion to the electrolysis time, but when a mixed solution of EDTA decontamination waste and Ce"-nitric acid solution is electrolyzed, the Ce" concentration increases (2 ) decomposition reaction occurs, and Ce
4- is reduced to Ce3+. The Ce4° concentration increases when the entire amount of EDTA in the mixed solution is decomposed.
このようにＥＤＴＡ除染廃液を分解剤であるＣｅ、 ４
＝によりＣＯ２、ＮＨ３、Ｈ２０に分解てき、また分
解剤であるＣｅ４−は、電界により再生して再使用する
ことができるため二次廃棄物量を低減することができる
。In this way, EDTA decontamination waste liquid is treated with Ce, which is a decomposer, 4
= is decomposed into CO2, NH3, and H20, and Ce4-, which is a decomposing agent, can be regenerated and reused by an electric field, so the amount of secondary waste can be reduced.
次に本発明の効果を確認するために行った従来例と、本
発明に係る化学除染廃液の処理方法の第１の実施例につ
いて説明する。第１の実施例として前記濃度のＥＤＴＡ
除染廃液１０ｍ３をＣｅ ” −硝酸溶液で処理した場
合の廃棄物発生量を求める。Next, a conventional example conducted to confirm the effects of the present invention and a first example of the method for treating chemical decontamination waste liquid according to the present invention will be described. As a first example, the concentration of EDTA
The amount of waste generated when 10 m3 of decontamination waste liquid is treated with Ce''-nitric acid solution is determined.
ＥＤＴＡ除染廃液はＥＤＴＡにＦｅが吸着しているもの
とする。本発明に係る処理方法ではＥＤＴＡを分解して
ガス化できるためＦｅのみが廃棄物として発生する。It is assumed that the EDTA decontamination waste liquid has Fe adsorbed to EDTA. In the treatment method according to the present invention, since EDTA can be decomposed and gasified, only Fe is generated as waste.
Ｆ ｅ ＝Ｏ，ＯＩｍｏｌ＃！ ｘ ｉｏ’ Ｉ Ｘ
５６ｇ／ｍｏｌ／１０００＝５．６ｋｇ
次に従来例のＥＤＴＡ除染廃液を廃棄する場合の廃棄物
発生量を求める。従来例ではＥＤＴＡとＦｅが廃棄物と
して発生する。F e =O, OImol#! x io' I
56g/mol/1000=5.6kg Next, the amount of waste generated when the conventional EDTA decontamination waste liquid is disposed of is determined. In the conventional example, EDTA and Fe are generated as waste.
ＥＤＴＡ
＝０．Ｏ１ｍｏｌ／Ａ’ ｘ１０４１ Ｘ ２９０ｇ／
ａ＋ｏｌ／１０００＝２９．０ｋｇ
Ｆ ｅ ＝Ｏ，ＤＩｍｏＩ／Ｉ ｘ １０４１ Ｘ ５
６ ｇ／ｍｏＶＩｏＯ［１＝５．６ｋｇ
合計＝３４．６ｋｇ
第１表に本発明に係る実施例と従来例のＥＤＴＡ除染廃
液を廃棄する場合の処理方法に伴う廃棄物発生量を検討
した結果を比較して示す。EDTA=0. O1mol/A' x 1041 x 290g/
a+ol/1000=29.0kg F e =O, DImol/I x 1041 x 5
6 g/moVIoO [1 = 5.6 kg Total = 34.6 kg Table 1 shows the results of examining the amount of waste generated in accordance with the processing methods when disposing of EDTA decontamination waste liquid in the embodiment according to the present invention and the conventional example. Compare and show.
第１表
第１表から明らかなように、除染廃液を１０ｍ３を廃棄
処理した場合の廃棄物発生量は、本発明の実施例の場合
は５．６ｋｇ、従来例の場合は３４．６ｋｇとなること
が認められた。また従来例の場合は、キレート除染廃液
をイオン交換樹脂で脱塩処理するため、さらに使用済み
イオン交換樹脂か廃棄物として発生する。Table 1 As is clear from Table 1, the amount of waste generated when 10 m3 of decontamination waste liquid is disposed of is 5.6 kg in the case of the embodiment of the present invention and 34.6 kg in the case of the conventional example. It was accepted that this would happen. Furthermore, in the case of the conventional example, since the chelate decontamination waste liquid is desalinated with an ion exchange resin, used ion exchange resin is also generated as waste.
次に本発明に係る化学除染廃液の処理方法の第２の実施
例について説明する。Next, a second embodiment of the method for treating chemical decontamination waste liquid according to the present invention will be described.
第２の実施例は分解剤としてＣｅ”−硫酸溶液を選択し
、キレート除染廃液としてシュウ酸（Ｈ２Ｃ２０，１）
除染廃液を処理する。シュウ酸除染廃液はシュウ酸（Ｙ
）に放射能及び金属イオン（Ｍ）が吸着しキレート化合
物（ＭＹ）を形成している。In the second example, Ce''-sulfuric acid solution was selected as the decomposing agent, and oxalic acid (H2C20,1) was used as the chelate decontamination waste liquid.
Treat decontamination waste liquid. Oxalic acid decontamination waste liquid is oxalic acid (Y
), radioactivity and metal ions (M) are adsorbed to form a chelate compound (MY).
電解槽にＣｅ’ −硫酸溶液を貯留し、加熱用ヒータ
ーてＣｅ”−硫酸溶液を８０°Ｃに昇温する。次にシュ
ウ酸除染廃液を電解槽に注入すると共に前記不活性陽極
と不活性陰極の間に所定の電流密度の直流電圧を印加す
ると前記陽極で前記 ・：１．式に示す反応が起こる。A Ce'-sulfuric acid solution is stored in an electrolytic cell, and the temperature of the Ce'-sulfuric acid solution is raised to 80°C using a heating heater.Next, the oxalic acid decontamination waste solution is injected into the electrolytic cell, and the inert anode and inert When a DC voltage of a predetermined current density is applied between the active cathodes, the reaction shown in the above formula .:1 occurs at the anode.
前記 （１）式により生成したＣｅ４−は極めて酸化力
か強いため、電解槽に注入したシュウ酸除染廃液（ＭＹ
）とＣｅ４−とは以下に示す反応か起こる。Since the Ce4- produced by the above formula (1) has extremely strong oxidizing power, the oxalic acid decontamination waste liquid (MY
) and Ce4-, the following reaction occurs.
Ｃｅ ” ＋ Ｍ Ｙ→
Ｃｅ”十〜り’−＋ＣＯ２＋Ｈ２０” ｆ３＋シュウ酸
の分解により発生するＣＯ２ガスまたは蒸気は排ガス処
理系で処理される。一方、上記（３）式の反応により還
元されたＣｅ’−は前記不活性陽極と不活性陰極の間に
所定の電流密度の直流電圧を印加しているため、前記
（１）式の反応か生起し陽極てＣｅ”’に再生される。Ce" + MY→ Ce"10~ri'-+CO2+H20" f3+ CO2 gas or steam generated by the decomposition of oxalic acid is treated in the exhaust gas treatment system. On the other hand, the Ce reduced by the reaction of equation (3) above '- is applying a DC voltage of a predetermined current density between the inert anode and the inert cathode, so the
The reaction of formula (1) occurs and Ce'' is regenerated at the anode.
上記ｆＤ式と １３）式の反応を確認するためにシュウ
酸除染廃液濃度０．４ｍｃ！、／Ａ 、Ｃｅ ’−，ｌ
ｌｉ度０１ｍｏ１．＃ 、硫酸濃度０５ｍｏｌ＃の混合
溶液を電流密度０． 、’Ａ、−’ ｄで電解した結果
を第２×によって説明する。第２図中の縦軸は電解によ
って陽極で生成されるＣｅ４−濃度、横軸は電解時間を
示す。また曲線ａはＣｅ”−硫酸単独溶液を電解した場
合、曲線すはンユウ酸除染廃液とＣｅ″−硫酸溶液との
混合溶液を電解した場合を示す。Ｃｅ３−硫酸単独溶液
を電解した場合は、はぼ電解時間に比例してＣｅ４−濃
度は増加するか、シュウ酸除染廃液とＣｅ ”−硫酸溶
液この混合溶液を電解した場合は、 （３″式の分解反
応か起こり、Ｃｅ”はＣｅ’に還元される。混合溶液中
のシュウ酸か全量分解した時点てＣｅ４濃度は増加する
。To confirm the reaction of the above fD equation and equation 13), the concentration of oxalic acid decontamination waste liquid is 0.4mc! , /A ,Ce'-,l
Li degree 01mo1. A mixed solution with a sulfuric acid concentration of 0.5 mol # and a current density of 0. , 'A, -' The results of electrolysis in d will be explained by the second x. In FIG. 2, the vertical axis shows the Ce4 concentration generated at the anode by electrolysis, and the horizontal axis shows the electrolysis time. Curve a shows the case where a Ce''-sulfuric acid solution alone was electrolyzed, and curve a shows the case where a mixed solution of the oxalic acid decontamination waste liquid and the Ce''-sulfuric acid solution was electrolyzed. When a Ce3-sulfuric acid solution alone is electrolyzed, the Ce4- concentration increases in proportion to the electrolysis time, or when a mixed solution of an oxalic acid decontamination waste solution and a Ce"-sulfuric acid solution is electrolyzed, (3" The decomposition reaction of the formula occurs, and Ce'' is reduced to Ce'. When the entire amount of oxalic acid in the mixed solution is decomposed, the Ce4 concentration increases.
このようにシュウ酸除染交液を分解剤であるＣｅ４″に
よりＣｏ２．Ｈ，Ｏに分解でき、また分解剤であるＣｅ
”は、電解により再生して再使用することかできるため
二次廃棄物の発生量を低減することかできる。In this way, the oxalic acid decontamination solution can be decomposed into Co2.H, O by the decomposing agent Ce4'', and the decomposing agent Ce4''
” can be regenerated and reused by electrolysis, reducing the amount of secondary waste generated.
次に本発明の効果を確認するために行った従来例と、本
発明に係る化学除染廃液の処理方法の第２の実施例につ
いて説明する。第２の実施例として前記濃度のンユウ酸
除染廃液１０ｍ３をＣｅ ’−硫酸溶液で処理した場合
の廃棄物発生量を求める。Next, a conventional example conducted to confirm the effects of the present invention and a second example of the method for treating chemical decontamination waste liquid according to the present invention will be described. As a second example, the amount of waste generated when 10 m3 of sulfuric acid decontamination waste liquid having the above concentration is treated with Ce'-sulfuric acid solution is determined.
シュウ酸除染廃液はシュウ酸にＦｅか吸着しているもの
とする４１本発明に係る処理方法ではンユウ酸を分解し
てカス化できるためＦｅのみか廃棄物として発生する。It is assumed that the oxalic acid decontamination waste liquid has some Fe adsorbed to the oxalic acid.41 In the treatment method according to the present invention, the oxalic acid can be decomposed and turned into scum, so only Fe is generated as waste.
Ｆ ｅ ＝０． Ｏ１ｍｏｌ／Ａ’ Ｘ １０４１ Ｘ
５６ ｇ ／ｒｏｍ／ＩＱＱ○＝５．６ｋｇ
次に従来例のシュウ酸除染廃液を廃棄する場合の廃棄物
発生量を求める。従来例てはンユウ酸とＦｅか廃棄物と
して発生する。F e =0. O1mol/A'X 1041X
56 g / rom / IQQ○ = 5.6 kg Next, calculate the amount of waste generated when the conventional oxalic acid decontamination waste liquid is disposed of. In the conventional example, sulfuric acid and Fe are generated as waste.
ＥＤＴＡ＝０．０１ｍｏｌ、、’１ｘｌＱ４１ Ｘ４８
ｇ／ｍｏｉ／１０００＝４．８府
Ｆ ｅ−０，０ｉｉｏ１／／ ｘｌＯ４１Ｘ５６ｇ／ｎ
ｏ：／１ｏ００＝５．６ｋｇ
合計−１０４ｋｇ
第２表に本発明に係る実施例と従来例のシュウ酸除染廃
液を廃棄する場合の処理方法に伴う廃棄物発生量を検討
した結果を比較して示す。EDTA=0.01mol,,'1xlQ41X48
g/moi/1000=4.8fuF e-0,0iio1//xlO41X56g/n
o:/1o00=5.6kg Total -104kg Table 2 compares the results of examining the amount of waste generated in the treatment methods for disposing of the oxalic acid decontamination waste liquid of the embodiment according to the present invention and the conventional example. Shown.
第２表
１本発明に係る実施例□ 従 米 例 □第２表か
ら明らかなように、除染廃液を１０ｍ“を廃棄処理した
場合の廃棄物発生量は、本発明の実施例の場合は５．５
ｋｇ、従来例の場合は１０４ｋｇとなることか認められ
た。また従来例の場合は、キレート除染憂液をイオン交
換樹脂て脱塩処理するため、さら使用済みイオン交換樹
脂か廃棄物として発生する。Table 2 1 Example according to the present invention □ Example □ As is clear from Table 2, the amount of waste generated when 10 m of decontamination waste liquid is disposed of is 5.5
kg, and in the case of the conventional example it was 104 kg. Furthermore, in the case of the conventional example, since the chelate decontamination solution is desalinated using an ion exchange resin, used ion exchange resin is also generated as waste.
以上説明したように第１の実施例及び第２の実施例では
キレート除染廃液をＣｅ”の酸化力によりキレート剤か
分解するため、放射能及び金属イオンのみか溶解した無
機の化学除染廃液とすることかできる。従って、従来の
廃液処理方法と比較し、二次廃棄物の発生量を低減する
ことかできる。As explained above, in the first and second embodiments, in order to decompose the chelate decontamination waste liquid into a chelating agent by the oxidizing power of Ce, an inorganic chemical decontamination waste liquid in which only radioactivity and metal ions are dissolved is used. Therefore, compared to conventional waste liquid treatment methods, the amount of secondary waste generated can be reduced.
なお、第１の実施例及び第２の実施例において、前記除
染廃液はＥＤＴＡ及びンユウ酸の代わりに、ＮＴＡ に
トロ三酢酸）、クエン酸、ギ酸等の一般に化学除染剤と
使用されているキレート剤または有機酸及びこれら混合
溶液でも処理可能である。In addition, in the first and second embodiments, the decontamination waste liquid is generally used with a chemical decontamination agent such as NTA (Thorotriacetic acid), citric acid, or formic acid instead of EDTA and phosphoric acid. The treatment can also be carried out using a chelating agent or an organic acid, or a mixed solution thereof.
また、これら除染廃液の濃度は０．０ｉｚｏｉ＃から飽
和溶解度まで処理可能である。分解剤であるＣｅ３−濃
度は０． ：ｍｏ：／ｌの代わりに０． Ｄｉ −２，
Ｌｎｏ１７’Ａの範囲で使用可能である。また、硝酸及
び硫酸の酸濃度は１． Ｏｍｏｉ＃の代わりに９０！ｍ
ｏｌ／Ａ’ 〜１０． ＯｍｏＬ’ｌの範囲で使用可能
である。キレート除染廃液の分解処理温度は８０℃に限
らす、１５〜９０℃の範囲で処理可能である。前記陽極
としてチタンに白金コーティングを施したものの代わり
に白金、チタン以外の金属に白金コーティングを施した
ものを用いることも可能である。前記陰極としてチタン
に白金コーティングを施したものの代わりに白金、チタ
ン以外の金属に白金コーティングを施したものを用いる
ことも可能である。前記陽極及び陰極の間に印加する直
流電圧の電流密度は、０３．へ／ｃｄの代わりに００５
〜２．０Ａ／ｃｄでも使用可能である。Further, the concentration of these decontamination waste liquids can be treated from 0.0 izoi# to saturated solubility. The concentration of Ce3, which is a decomposing agent, is 0. :mo:/l instead of 0. Di-2,
It can be used within the range of Lno17'A. Also, the acid concentration of nitric acid and sulfuric acid is 1. 90 instead of Omoi #! m
ol/A' ~10. It can be used within the range of OmoL'l. The decomposition treatment temperature of chelate decontamination waste liquid is limited to 80°C, but it can be treated in the range of 15 to 90°C. Instead of titanium coated with platinum, platinum or a metal other than titanium coated with platinum may be used as the anode. Instead of titanium coated with platinum, platinum or a metal other than titanium coated with platinum may be used as the cathode. The current density of the DC voltage applied between the anode and the cathode is 0.3. 005 instead of /cd
It can also be used at ~2.0 A/cd.
次に本発明に係る化学除染廃液の処理方法の第３の実施
例を第３図のブロックフロー図で説明する。廃液処理手
順としては、キレート除染廃液９を分解工程１０てＣｅ
４− 酸性溶液を電解再生しながら分解する。キレー
ト除染廃液の処理後は除染廃液中にＣｅ”−Ｃｅ”、放
射能及び金属イオン（Ｍ″゛）か残留する。Ｃｅ’−は
酸化力か強いため、そのままの状態で既設の廃液処理系
で処理すると他の機器に腐食を及ぼす危険がある。そこ
で電解還元工程１］て分解工程１０の電解再生電極の極
性を逆転して直流電圧を印加する。陰極では以下に示す
還元反応か起こり、Ｃｅ”はＣｅ’−に還元される。Next, a third embodiment of the method for treating chemical decontamination waste liquid according to the present invention will be described with reference to the block flow diagram of FIG. As a waste liquid treatment procedure, the chelate decontamination waste liquid 9 is decomposed in the decomposition process 10 and Ce
4- Decompose the acidic solution while electrolytically regenerating it. After the chelate decontamination waste liquid is treated, Ce"-Ce", radioactivity and metal ions (M") remain in the decontamination waste liquid.Ce'- has a strong oxidizing power, so it can be used as is in the existing waste liquid. If treated in the treatment system, there is a risk of corrosion to other equipment.Therefore, in the electrolytic reduction step 1], the polarity of the electrolytic regeneration electrode in the decomposition step 10 is reversed and a DC voltage is applied.At the cathode, the following reduction reaction occurs. occurs, and Ce'' is reduced to Ce'-.
Ｃｅ’−＋ｅ→Ｃｅ”
Ｍ″−４−６−４Ｍ”−１１
Ｍ ”” ＋ Ｃｅ ”→Ｍ”−十Ｃｅ ３゜Ｃｅ’
−の還元終了後は、無機の酸性化学除染廃液として取り
扱うことができるため、中和工程１２て中和剤を添加し
てＣｅ及び放射能及び金属イオンを水酸化物としてスラ
ッジ化する。中和処理後は濃縮・乾燥工程１３て除染廃
液を粉体化し、固化工程１４てプラスチック固化または
セメント固化して保管する。Ce'-+e→Ce"M"-4-6-4M"-11 M "" + Ce "→M"-tenCe 3°Ce'
After the reduction of - can be handled as an inorganic acidic chemical decontamination waste liquid, a neutralizing agent is added in a neutralization step 12 to turn Ce, radioactivity, and metal ions into hydroxides into sludge. After the neutralization treatment, the decontamination waste liquid is pulverized in a concentration/drying step 13, solidified into plastic or cement in a solidification step 14, and stored.
以上説明したように本実施例によれば、キレート除染廃
液をＣｅ４−を用いて分解し、無機の酸性化学除染廃液
として既設の廃液処理系で処理するものである。従って
、従来の廃液処理方法であるキレート除染廃液をイオン
交換樹脂により脱塩処理し、イオン交換樹脂及び脱塩処
理したキレート除染廃液を固化する場合と比べ、二次廃
棄物の発生量を極端に低減することかできると共に、固
化体の安定性も良い。As explained above, according to this embodiment, the chelate decontamination waste liquid is decomposed using Ce4- and is treated as an inorganic acidic chemical decontamination waste liquid in the existing waste liquid treatment system. Therefore, compared to the conventional waste liquid treatment method, in which chelate decontamination waste liquid is desalted using ion exchange resin, and the ion exchange resin and the desalted chelate decontamination waste liquid are solidified, the amount of secondary waste generated can be reduced. It can be extremely reduced and the stability of the solidified product is also good.
［発明の効果］ 本発明によれば以下の効果かある。[Effect of the invention] According to the present invention, there are the following effects.
（１）キレート除染廃液中のキレート剤をＣｅ”の酸化
力により分解でき、またＣｅ４−は電解再生して繰り返
し使用できるため、二次廃棄物の発生量を低減すること
かできる。(1) Since the chelating agent in the chelate decontamination waste liquid can be decomposed by the oxidizing power of Ce'', and Ce4- can be electrolytically regenerated and used repeatedly, the amount of secondary waste generated can be reduced.
（２）キレート除染廃液を分解処理した後の廃液は無機
の酸性化学除染廃液であるため、既設の廃液処理系で処
理可能である。(2) Since the waste liquid after decomposing the chelate decontamination waste liquid is an inorganic acidic chemical decontamination waste liquid, it can be treated in an existing waste liquid treatment system.
（３）従来の廃液処理方法であるキレート除染廃液をイ
オン交換樹脂により脱塩処理して固化する場合と比へ、
固化体の安定性は高い。(3) Compared to the conventional waste liquid treatment method, in which chelate decontamination waste liquid is desalted and solidified using an ion exchange resin,
The stability of the solidified product is high.
第１図は本発明に係る化学除染廃液の処理方法における
キレート除染廃液の分解装置の一例を線図的に示す断面
図、第２図はキレート除染廃液の分解例を示したグラフ
図、第３図は本発明に係る化学除染廃液の処理方法を示
すブロックフロー図である。
１・・キレート除染廃液貯留槽
２・・電解槽 ３・・・分解剤４・・・循環ポ
ンプ ５・・・陽極６・・・陰極 ７・
・・ヒーター８・・排ガス処理系 ９・・・除染廃液
１０・・・分解工程 １１・・還元工程１２・・
・中和工程 １３・・・濃縮・乾燥工程１４・・
・固化工程
（８７３３）代理人 弁理士 猪 股 祥 晃（ほか
１名）Fig. 1 is a cross-sectional view diagrammatically showing an example of a decomposition device for chelate decontamination waste liquid in the method for treating chemical decontamination waste liquid according to the present invention, and Fig. 2 is a graph diagram showing an example of decomposition of chelate decontamination waste liquid. , FIG. 3 is a block flow diagram showing a method for treating chemical decontamination waste liquid according to the present invention. 1... Chelate decontamination waste liquid storage tank 2... Electrolytic tank 3... Decomposition agent 4... Circulation pump 5... Anode 6... Cathode 7.
...Heater 8...Exhaust gas treatment system 9...Decontamination waste liquid 10...Decomposition process 11...Reduction process 12...
・Neutralization process 13...Concentration/drying process 14...
・Solidification process (8733) Agent: Yoshiaki Inomata, patent attorney (and others)
1 person)
Claims (2)
物を、有機酸またはキレート剤及びこれら混合溶液から
なる除染液で除染した後に発生する使用済み化学除染廃
液の処理方法において、前記キレート除染廃液をＣｅ＾
４＾＋‐Ｃｅ＾３＾＋‐酸性溶液中に注入し、不活性金
属からなる陽極と不活性金属からなる陰極とを浸漬して
前記両電極間に直流電圧を印加して前記陽極でＣｅ＾３
＾＋を酸化してＣｅ＾４＾＋を生成し、放射能及び金属
イオンを吸着したキレート剤をＣｅ＾４＾＋の酸化力に
より分解することを特徴とする化学除染廃液の処理方法
。(1) In a method for treating used chemical decontamination waste fluid generated after radioactively contaminated waste generated from nuclear facilities is decontaminated with a decontamination fluid consisting of an organic acid or chelating agent and a mixed solution thereof, Ce^ the chelate decontamination waste liquid
4^+-Ce^3^+- is injected into an acidic solution, an anode made of an inert metal and a cathode made of an inert metal are immersed, and a DC voltage is applied between the two electrodes to remove Ce at the anode. ^3
A method for treating chemical decontamination waste liquid, which comprises oxidizing ^+ to generate Ce^4^+, and decomposing a chelating agent adsorbing radioactivity and metal ions by the oxidizing power of Ce^4^+.
ｅ＾４＾＋をＣｅ＾３＾＋に還元し、中和剤により中和
し、濃縮乾燥して固化することを特徴とする請求項１記
載の化学除染廃液の処理方法。(2) C remaining after decomposition treatment of the chelate decontamination waste liquid
The method for treating chemical decontamination waste liquid according to claim 1, characterized in that e^4^+ is reduced to Ce^3^+, neutralized with a neutralizing agent, and solidified by concentration and drying.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP31573790A JP2854706B2 (en) | 1990-11-22 | 1990-11-22 | Chemical decontamination waste liquid treatment method |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP31573790A JP2854706B2 (en) | 1990-11-22 | 1990-11-22 | Chemical decontamination waste liquid treatment method |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH04188099A true JPH04188099A (en) | 1992-07-06 |
| JP2854706B2 JP2854706B2 (en) | 1999-02-03 |
Family
ID=18068933
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP31573790A Expired - Lifetime JP2854706B2 (en) | 1990-11-22 | 1990-11-22 | Chemical decontamination waste liquid treatment method |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2854706B2 (en) |
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1990
- 1990-11-22 JP JP31573790A patent/JP2854706B2/en not_active Expired - Lifetime
Also Published As
| Publication number | Publication date |
|---|---|
| JP2854706B2 (en) | 1999-02-03 |
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