JPH0339698A - Treatment of waste liquid containing nano3 - Google Patents
Treatment of waste liquid containing nano3Info
- Publication number
- JPH0339698A JPH0339698A JP17417089A JP17417089A JPH0339698A JP H0339698 A JPH0339698 A JP H0339698A JP 17417089 A JP17417089 A JP 17417089A JP 17417089 A JP17417089 A JP 17417089A JP H0339698 A JPH0339698 A JP H0339698A
- Authority
- JP
- Japan
- Prior art keywords
- reaction
- recovered
- waste liquid
- hno3
- naoh
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
- 239000007788 liquid Substances 0.000 title claims abstract description 32
- 239000002699 waste material Substances 0.000 title claims abstract description 27
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims abstract description 39
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims abstract description 20
- 239000007795 chemical reaction product Substances 0.000 claims abstract description 5
- 238000000034 method Methods 0.000 claims description 24
- 238000006243 chemical reaction Methods 0.000 abstract description 16
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Chemical compound [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 abstract description 12
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 abstract description 8
- 238000011038 discontinuous diafiltration by volume reduction Methods 0.000 abstract description 8
- 229910017604 nitric acid Inorganic materials 0.000 abstract description 8
- 238000011084 recovery Methods 0.000 abstract description 8
- 235000010344 sodium nitrate Nutrition 0.000 abstract description 6
- 239000007832 Na2SO4 Substances 0.000 abstract description 5
- PMZURENOXWZQFD-UHFFFAOYSA-L Sodium Sulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 abstract description 5
- 229910052938 sodium sulfate Inorganic materials 0.000 abstract description 5
- 235000011152 sodium sulphate Nutrition 0.000 abstract description 5
- 238000007711 solidification Methods 0.000 abstract description 4
- 230000008023 solidification Effects 0.000 abstract description 4
- 235000011149 sulphuric acid Nutrition 0.000 abstract description 4
- 150000001450 anions Chemical class 0.000 abstract description 2
- 238000005868 electrolysis reaction Methods 0.000 abstract description 2
- 150000001768 cations Chemical class 0.000 abstract 1
- 238000012958 reprocessing Methods 0.000 description 9
- 239000011734 sodium Substances 0.000 description 6
- 241000549556 Nanos Species 0.000 description 5
- 239000000047 product Substances 0.000 description 4
- 239000010426 asphalt Substances 0.000 description 3
- 239000004568 cement Substances 0.000 description 3
- 239000002915 spent fuel radioactive waste Substances 0.000 description 3
- 238000003860 storage Methods 0.000 description 3
- 239000003795 chemical substances by application Substances 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 239000003758 nuclear fuel Substances 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- WBHQBSYUUJJSRZ-UHFFFAOYSA-M sodium bisulfate Chemical compound [Na+].OS([O-])(=O)=O WBHQBSYUUJJSRZ-UHFFFAOYSA-M 0.000 description 2
- 229910000342 sodium bisulfate Inorganic materials 0.000 description 2
- 239000004317 sodium nitrate Substances 0.000 description 2
- LPXPTNMVRIOKMN-UHFFFAOYSA-M sodium nitrite Chemical compound [Na+].[O-]N=O LPXPTNMVRIOKMN-UHFFFAOYSA-M 0.000 description 2
- 229910002651 NO3 Inorganic materials 0.000 description 1
- IOVCWXUNBOPUCH-UHFFFAOYSA-N Nitrous acid Chemical compound ON=O IOVCWXUNBOPUCH-UHFFFAOYSA-N 0.000 description 1
- 125000000129 anionic group Chemical group 0.000 description 1
- 125000002091 cationic group Chemical group 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 230000005484 gravity Effects 0.000 description 1
- 239000002925 low-level radioactive waste Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 235000010288 sodium nitrite Nutrition 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Landscapes
- Removal Of Specific Substances (AREA)
Abstract
Description
【発明の詳細な説明】
〔産業上の利用分野〕
本発明は、硝酸ナトリウム（Ｎ ａＮ Ｏ２）を多量に
含む廃液を処理する方法に関するものである。さらに詳
しくは本発明は、使用済み原子核燃料の再処理工程で発
生する中・低レベル放射能の廃液を処理するのに適した
、廃液の処理法に関するもの／
である。DETAILED DESCRIPTION OF THE INVENTION [Industrial Application Field] The present invention relates to a method for treating waste liquid containing a large amount of sodium nitrate (NaN O2). More specifically, the present invention relates to a waste liquid treatment method suitable for treating waste liquid with medium to low level radioactivity generated in the process of reprocessing spent nuclear fuel.
従来、使用済みあるいは核燃料再処理施設で発生する中
・低レベル放射能の廃液は蒸発濃縮され、アスファルト
、セメント等で固化或は水分を除去して乾燥処理され、
保管貯蔵されている。しかしながら、この濃縮廃液は硝
酸ナトリウム（Ｎ ａＮ Ｏ、）を３０〜５０％含むた
め、固化処理による減容性が悪い。また、Ｎ ａ Ｎ
Ｏｓは酸化性物質であるので、固化剤を酸化劣化させる
おそれもあり、多量のＮ ａ Ｎ Ｏ２を長期間保管す
ることは好ましくない。Conventionally, waste liquid with medium to low level radioactivity generated at spent or nuclear fuel reprocessing facilities is evaporated and concentrated, solidified with asphalt, cement, etc., or dried by removing moisture.
It is stored and stored. However, since this concentrated waste liquid contains 30 to 50% sodium nitrate (NaN O), its volume reduction through solidification treatment is poor. Also, N a N
Since Os is an oxidizing substance, there is a risk of oxidative deterioration of the solidifying agent, so it is not preferable to store a large amount of NaNO2 for a long period of time.
そこで、Ｎ ａ Ｎ Ｏ３を無害化し、かつ固化による
減容率も大きくする、廃液の処理法が求められてきた。Therefore, there has been a demand for a waste liquid treatment method that renders NaNO3 harmless and also increases the rate of volume reduction due to solidification.
すなわち本発明は、Ｎ ａ Ｎ Ｏｓを含む廃液の処理
法において、硫酸を使用してＨＮＯ，を回収し、さらに
その反応生成物であるＮＩＬ２ＳＯ，を電解処理し、Ｎ
ａ ＯＨ、Ｈ２Ｓ Ｏ４をそれぞれ回収することを特
徴とする、廃液の処理法を提供するものである。That is, the present invention is a method for treating waste liquid containing NaNOs, in which HNO is recovered using sulfuric acid, and the reaction product NILSO is electrolytically treated to
The present invention provides a method for treating waste liquid, which is characterized by recovering a OH and H2S O4, respectively.
すなわち本発明は、Ｎ ａ Ｎ Ｏ）を含む廃液から、
ＨＮ ＯｓとＮａＯＨを回収するものであり、下記のプ
ロセスから構成される装
■ 廃液を濃縮処理し、Ｎ ａ Ｎ Ｏｘを高濃縮液と
して取出す。That is, the present invention enables the extraction of waste liquid containing N a N O),
HNOs and NaOH are recovered, and the process consists of the following steps: (1) The waste liquid is concentrated and NaNOx is extracted as a highly concentrated liquid.
■ このＮａＮＯ３溶液にＨ２ＳＯ，を加え、Ｎ ａ
Ｎ Ｏ３からＨＮ Ｏｓを回収する。■ Add H2SO, to this NaNO3 solution, and
Recover HN Os from N O3.
■ 反応生成物の１つであるＮａ２５Ｏ＜を電解して、
ＮａＯＨとＨ２ＳＯ４をそれぞれ回収する。■ By electrolyzing Na25O, one of the reaction products,
NaOH and H2SO4 are each recovered.
■およびＯの各プロセスで回収したＨ Ｎ ＯｓとＮａ
ＯＨは、再処理工程で再使用することができる。また■
の反応で回収したＨ、Ｓｏ、は、■のプロセスで再使用
することができるので、系外に放出される最終要処理物
が極めて少なく、減容率を高めることができる。また最
終固化物であるＮ ａ ２ Ｓ Ｏ４は、酸化性ではな
く安定な化合物であるので、アスファルト、セメント等
の固化剤を劣化させるおそれもない。■HNOs and Na recovered in each process of
OH can be reused in a reprocessing step. Also ■
Since the H, So, recovered in the reaction (2) can be reused in the process (2), the amount of final treatment products released outside the system is extremely small, and the volume reduction rate can be increased. Furthermore, since the final solidified product, Na 2 S O4, is a non-oxidizing and stable compound, there is no risk of degrading solidifying agents such as asphalt and cement.
以下に、本発明に関係する■と■のプロセスについて、
さらに説明する。Below, regarding the processes of ■ and ■ related to the present invention,
I will explain further.
ｉ ） Ｎ ａ Ｎ Ｏ３からのＨＮＯ，の回収Ｎ ａ
Ｎ Ｏ３にＨ，ＳＯ，を作用させ、複分解によりＨＮ
Ｏ＊を発生させ、回収する。この方法は、グリースハ
イム法と呼ばれる硝酸製造法の一つである０分解反応に
よるＨＮＯ，は、下記２段の反応式で進行する。i) Recovery of HNO from NaN O3
By acting H, SO, on N O3, HN is produced by double decomposition.
Generate and collect O*. This method is one of the nitric acid production methods called the Griesheim method, and HNO is produced by a zero decomposition reaction, which proceeds according to the following two-stage reaction formula.
ＮａＮＯｓ ＋Ｈ２ＳＯ４→ＮａＨＳＯ４＋ ’ＡＮＯ
ｓ −■ＮａＮ０ｉ＋ＮａＨＳＯ４→Ｎａ２ＳＯ４＋
ＨＮＯ３”・■廃液中のＮａＮＱｓの濃度を５０％とし
た場合、廃液中のＨ，ＳＯ，濃度が３０〜４０％となる
ようＨ２ＳＯ，を加える。温度は第１段が約５０℃、第
２段が約２００℃である。NaNOs +H2SO4→NaHSO4+ 'ANO
s −■NaN0i+NaHSO4→Na2SO4+
When the concentration of NaNQs in the waste liquid is 50%, H2SO is added so that the concentration of H, SO in the waste liquid becomes 30 to 40%.The temperature is approximately 50°C in the first stage, and The stage is approximately 200°C.
■および■式で回収したＨ Ｎ Ｏ３は再処理工程に戻
し、再使用する。The H 2 N O 3 recovered in formulas ① and ② is returned to the reprocessing step and reused.
一方、反応によって生成したＮ ａ ２ Ｓ Ｏ４は次
のｉｉで述べるプロセスにて処理する。On the other hand, Na 2 S O4 produced by the reaction is treated in the process described in the following ii.
ｉｉ ） Ｎ ａ２ Ｓ Ｏ４からのＮａＯＨおよびＨ
，ＳＯ，の回収
ｉ）で生成したＮ ａ ２ Ｓ Ｏ４は電気分解により
陽イオン成分としてＮａＯＨを、陰イオン成分としてＨ
２Ｓ Ｏ４をそれぞれ回収する。ii) NaOH and H from Na2SO4
, SO, produced in step i) is electrolyzed to form NaOH as a cationic component and H as an anionic component.
2SO4 is collected respectively.
回収したＮａＯＨは再処理工程で再使用し、またＨ２Ｓ
Ｏ４は■のＨＮＯ，回収工程で再使用することができる
。The recovered NaOH is reused in the reprocessing process, and H2S
O4 can be reused in the HNO recovery process described in (1).
Ｎａ２５Ｏ，の電解条件の１例を下記に示す。An example of electrolytic conditions for Na25O is shown below.
Ｎａ２ＳＯ４＋ ＨｚＯ→Ｈ２ＳＯ＜ ＋ ２８ａＯＨ
Ｎａ２ＳＯ，： １ｍｏｌ’／ １以上型流密度 ：４
＾／ｄ−２
電流効率 ＝４０％
生成液濃度：陰極ＮａＯＨ３，６ｍｏｌ／ １陽極Ｈ２
ＳＯ４１，１ｍｏｆ／ １
上記ｉおよびｉｉのプロセスの流れを第１図に示す。Na2SO4+ HzO→H2SO< + 28aOH
Na2SO,: 1 mol'/1 or more Mold flow density: 4
^/d-2 Current efficiency = 40% Product solution concentration: Cathode NaOH3.6 mol/1 Anode H2
SO41,1mof/1 The flow of the above processes i and ii is shown in FIG.
第１図において、■はＮ ａ Ｎ Ｏ３含有廃液貯蔵タ
ンクであり、■は硫酸貯蔵タンクである。まず■の反応
槽に、■からのＮ ａ Ｎ Ｏｓ含有廃液および■から
の硫酸を装入し、■の反応槽を■のヒーターで加熱し、
前述の反応を進行させる６反応により生成したＨＮＯ，
は■の硝酸回収タンクに回収される０反応終了後、反応
生成物であるＮａ、ＳＯ。In FIG. 1, ■ is a waste liquid storage tank containing NaN O3, and ■ is a sulfuric acid storage tank. First, the NaNOs-containing waste liquid from ■ and the sulfuric acid from ■ are charged into the reaction tank (■), and the reaction tank (■) is heated with the heater (■).
HNO produced by the 6 reactions that proceed with the aforementioned reactions,
After the reaction is completed, the reaction products Na and SO are recovered in the nitric acid recovery tank (①).
は■の３室型の電解槽に移送される。is transferred to the three-chamber electrolytic cell shown in (■).
この■の３室型セルは、陽極側はアニオン膜によって処
理液と隔離され、同様に陰極側はカチ木ン膜によって処
理液と隔離されている。電解によりＮａＯＨは陰極側に
回収され、■のＮａＯＨタンクに移送される。一方、Ｈ
２ＳＯ，は陽極側に回収され、■の硫酸タンクに移送さ
れる。これらはそれぞれ、次の再処理工程や、Ｎ ａ
Ｎ Ｏ３回収工程に使用されることは、前述したとおり
である。In this three-chamber type cell (2), the anode side is isolated from the processing solution by an anion membrane, and the cathode side is similarly isolated from the processing solution by a cathode membrane. NaOH is recovered to the cathode side by electrolysis and transferred to the NaOH tank (2). On the other hand, H
2SO, is recovered on the anode side and transferred to the sulfuric acid tank (2). These are required for the next reprocessing process and Na
As mentioned above, it is used in the NO3 recovery process.
ここで、廃液処理・固化の減容性について簡単に試算す
る。Here, we will briefly calculate the volume reduction properties of waste liquid treatment and solidification.
Ｎ ａＮ Ｏ３５０ａａ／ ｏ（重量％）溶液ＬＭ’を
処理した場合、これをアスファルトで固化した場合は固
化体の体積は約ＩＭ’となり、減容率は１でしかない、
これを本発明の方法で処理すると、次のように減容率が
非常に高くなる。When a NaN O350aa/o (wt%) solution LM' is treated and solidified with asphalt, the volume of the solidified material is approximately IM', and the volume reduction rate is only 1.
When this is treated by the method of the present invention, the volume reduction rate becomes extremely high as shown below.
すなわち、プロセスｉ〉の反応を完全に進めると、生成
物はＨＮＯ２およびＮ ａ ２ Ｓ Ｏ４となるが、Ｎ
ａ ２ Ｓ Ｏ４が固体となり回収が困難になるので
、回収率を９０％に留とめておく、ここで５００ｋ。In other words, if the reaction of process i> is completed, the products will be HNO2 and Na 2 SO4, but N
Since a 2 SO4 becomes solid and difficult to recover, the recovery rate is kept at 90%, which is 500k.
のＮ ａ Ｎ Ｏ３から約３３３ｋｇのＨＮ Ｏ３が回
収でき、Ｎａ２５Ｏ，が約４００ｋｇ生成する。Approximately 333 kg of HN O3 can be recovered from Na N O3, and approximately 400 kg of Na25O is produced.
プロセスｉｉ）の電解反応は、Ｎａ２ＳＯ２濃度が１ｍ
ｏ１／１以上で進行する。したがって、反応終点時のＮ
ＩＬ２ＳＯ，濃度を１ｍｏｉ’／１とし、使用液量を１
００１とすると、固化対象となる廃液中のＮ ａｔ Ｓ
Ｏ４は１４．２ｋｙとなる。この場合、Ｎ １１２
Ｓ Ｏ４がＬｏｗｌｏ（重１％）のセメント固化体とす
ることができるので、固化体の比重を２とすると、体積
は約７０１となる。したがって、被処理体の重量は処理
前のＮａＮＯｓ ５００ｋｇの１７３５であり、１０倍
以上（約１４倍）の減容率が得られる。In the electrolytic reaction of process ii), the Na2SO2 concentration is 1 m
Proceed at o1/1 or higher. Therefore, N at the end of the reaction
IL2SO, the concentration is 1moi'/1, the amount of liquid used is 1
001, N at S in the waste liquid to be solidified
O4 is 14.2ky. In this case, N 112
Since it is possible to form a cement solidified body with low SO4 (1% by weight), if the specific gravity of the solidified body is 2, the volume will be approximately 701. Therefore, the weight of the object to be treated is 1,735 times the weight of 500 kg of NaNOs before treatment, and a volume reduction rate of 10 times or more (approximately 14 times) can be obtained.
核燃料再処理施設から排出される、多量のＮ ａ Ｎ
Ｏｓを含み、中・低レベルの放射能を有する廃液を本発
明の方法で処理することにより、再処理施設中で再び使
用され得るＨＮＯ，、Ｈ２ＳＯ，、ＮａＯＨ等を回収す
ることができ、ＨＮＯ，、ＮａＯＨ溶液の閉サイクル化
が可能となり、廃棄物発生量の大巾な低減を図ることが
できる。この結果、従来に比べ中・低レベル廃液処理系
での固化体発生が大巾に減少する。Large amounts of NaN emitted from nuclear fuel reprocessing facilities
By treating waste liquid containing Os and having medium to low levels of radioactivity using the method of the present invention, it is possible to recover HNO, H2SO, NaOH, etc., which can be used again in a reprocessing facility. , It becomes possible to create a closed cycle for the NaOH solution, and it is possible to significantly reduce the amount of waste generated. As a result, the generation of solidified substances in medium- and low-level waste liquid treatment systems is greatly reduced compared to conventional systems.
なお、以上は使用済み核燃料の再処理工程がら排出され
る廃液の処理を中心にして説明したが、本発明はこれら
の用途に限定されるものではなく、Ｎ ａ Ｎ Ｏｓを
多量に含有する他の廃液の処理にも有用であることは勿
論である。Although the above description has focused on the treatment of waste liquid discharged from the reprocessing process of spent nuclear fuel, the present invention is not limited to these uses, and is applicable to waste liquids containing a large amount of NaNOs. Of course, it is also useful for treating waste liquid.
第１図は、本発明に係る廃液の処理法の流れの一例を示
す図である。
１・・・Ｎ ａＮ Ｏｚ含有廃液貯蔵タンク、２・・・
反応槽、３・・・ヒーター、４・・・電解槽、５・・・
硫酸タンク、６・・・硝酸回収タンク、７・・・水酸化
ナトリウム回収タンクFIG. 1 is a diagram showing an example of the flow of the waste liquid treatment method according to the present invention. 1...N aN Oz containing waste liquid storage tank, 2...
Reaction tank, 3... Heater, 4... Electrolytic tank, 5...
Sulfuric acid tank, 6... Nitric acid recovery tank, 7... Sodium hydroxide recovery tank
Claims (1)
してＨＮＯ＿３を回収し、その反応生成物であるＮａ＿
２ＳＯ＿４を電解処理し、ＮａＯＨ、Ｈ＿２ＳＯ＿４を
それぞれ回収することを特徴とする、廃液の処理法。In a method for treating waste liquid containing NaNO_3, sulfuric acid is used to recover HNO_3 and its reaction product Na_
A method for treating waste liquid, characterized by electrolytically treating 2SO_4 and recovering NaOH and H_2SO_4.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP17417089A JPH0339698A (en) | 1989-07-07 | 1989-07-07 | Treatment of waste liquid containing nano3 |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP17417089A JPH0339698A (en) | 1989-07-07 | 1989-07-07 | Treatment of waste liquid containing nano3 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH0339698A true JPH0339698A (en) | 1991-02-20 |
Family
ID=15973929
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP17417089A Pending JPH0339698A (en) | 1989-07-07 | 1989-07-07 | Treatment of waste liquid containing nano3 |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0339698A (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH04283700A (en) * | 1991-03-12 | 1992-10-08 | Toshiba Corp | Reducing method of volume of low-level concentrated liquid waste |
| EP0772205A3 (en) * | 1995-11-01 | 1997-12-17 | Douryokuro Kakunenryo Kaihatsu Jigyoudan | Process for treatment of radioactive waste |
| EP2192595A1 (en) * | 2007-12-05 | 2010-06-02 | JGC Corporation | Method for treating radioactive waste solution and treatment apparatus |
-
1989
- 1989-07-07 JP JP17417089A patent/JPH0339698A/en active Pending
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH04283700A (en) * | 1991-03-12 | 1992-10-08 | Toshiba Corp | Reducing method of volume of low-level concentrated liquid waste |
| EP0772205A3 (en) * | 1995-11-01 | 1997-12-17 | Douryokuro Kakunenryo Kaihatsu Jigyoudan | Process for treatment of radioactive waste |
| US5744020A (en) * | 1995-11-01 | 1998-04-28 | Douryokuro Kakunenryo Kaihatsu Jigyoudan | Process for treatment of radioactive waste |
| EP2192595A1 (en) * | 2007-12-05 | 2010-06-02 | JGC Corporation | Method for treating radioactive waste solution and treatment apparatus |
| EP2192595A4 (en) * | 2007-12-05 | 2012-10-03 | Jgc Corp | Method for treating radioactive waste solution and treatment apparatus |
| US8476481B2 (en) | 2007-12-05 | 2013-07-02 | Jgc Corporation | Method for treating radioactive liquid waste and apparatus for the same |
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