JPH0335997B2 - - Google Patents
Info
- Publication number
- JPH0335997B2 JPH0335997B2 JP8367487A JP8367487A JPH0335997B2 JP H0335997 B2 JPH0335997 B2 JP H0335997B2 JP 8367487 A JP8367487 A JP 8367487A JP 8367487 A JP8367487 A JP 8367487A JP H0335997 B2 JPH0335997 B2 JP H0335997B2
- Authority
- JP
- Japan
- Prior art keywords
- radioactive wastewater
- adsorbent
- wastewater
- actinide elements
- actinide
- 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
Links
- 229910052768 actinide Inorganic materials 0.000 claims description 28
- 150000001255 actinides Chemical class 0.000 claims description 28
- 238000000034 method Methods 0.000 claims description 24
- 239000003463 adsorbent Substances 0.000 claims description 20
- 239000002354 radioactive wastewater Substances 0.000 claims description 17
- 229920001864 tannin Polymers 0.000 claims description 15
- 239000001648 tannin Substances 0.000 claims description 15
- 235000018553 tannin Nutrition 0.000 claims description 15
- 229910052770 Uranium Inorganic materials 0.000 claims description 13
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical group [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 claims description 13
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 8
- ZSLUVFAKFWKJRC-IGMARMGPSA-N 232Th Chemical compound [232Th] ZSLUVFAKFWKJRC-IGMARMGPSA-N 0.000 claims description 5
- 229910052776 Thorium Inorganic materials 0.000 claims description 5
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 4
- 229910017604 nitric acid Inorganic materials 0.000 claims description 4
- 229910052778 Plutonium Inorganic materials 0.000 claims description 2
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 claims description 2
- 238000003672 processing method Methods 0.000 claims 1
- 239000002351 wastewater Substances 0.000 description 18
- 238000001179 sorption measurement Methods 0.000 description 9
- 238000007796 conventional method Methods 0.000 description 8
- 239000002253 acid Substances 0.000 description 7
- 230000000694 effects Effects 0.000 description 5
- 229910052500 inorganic mineral Inorganic materials 0.000 description 5
- 239000011707 mineral Substances 0.000 description 5
- 150000007513 acids Chemical class 0.000 description 4
- 239000011347 resin Substances 0.000 description 4
- 229920005989 resin Polymers 0.000 description 4
- 238000003795 desorption Methods 0.000 description 3
- 238000005406 washing Methods 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- 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 2
- 235000011511 Diospyros Nutrition 0.000 description 2
- 244000236655 Diospyros kaki Species 0.000 description 2
- 239000013522 chelant Substances 0.000 description 2
- 239000003456 ion exchange resin Substances 0.000 description 2
- 229920003303 ion-exchange polymer Polymers 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 238000002336 sorption--desorption measurement Methods 0.000 description 2
- 239000002699 waste material Substances 0.000 description 2
- 230000002301 combined effect Effects 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- -1 nitric acid Chemical class 0.000 description 1
- 239000003758 nuclear fuel Substances 0.000 description 1
- 230000002285 radioactive effect Effects 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 239000002910 solid waste Substances 0.000 description 1
- 238000004065 wastewater treatment Methods 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
- B01J20/24—Naturally occurring macromolecular compounds, e.g. humic acids or their derivatives
Landscapes
- Chemical & Material Sciences (AREA)
- Analytical Chemistry (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Water Treatment By Sorption (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Description
【発明の詳細な説明】
（産業分野）
本発明はアクチニド元素含有の放射性廃水にお
いて該アクチニド元素濃度の低減化を目的とする
放射性廃水の処理方法に関するものである。DETAILED DESCRIPTION OF THE INVENTION (Industrial Field) The present invention relates to a method for treating radioactive wastewater containing actinide elements, the purpose of which is to reduce the concentration of actinide elements in the radioactive wastewater.
（従来技術とその問題点）
原子力施設から排出される廃水のうち、ウラン
等のアクチニド元素を含む廃水については可能な
限り、これらアクチニド元素濃度の低減化が望ま
れている。(Prior art and its problems) Of the wastewater discharged from nuclear facilities, it is desirable to reduce the concentration of these actinide elements as much as possible with respect to wastewater containing actinide elements such as uranium.
アクチニド元素を含む放射性廃水の処理方法と
しては従来イオン交換樹脂吸着法及びキレート樹
脂吸着法等があり、これらの方法によつてそれぞ
れ該廃水中のアクチニド元素濃度の低減化がはか
られてきた。 Conventional methods for treating radioactive wastewater containing actinide elements include ion exchange resin adsorption methods and chelate resin adsorption methods, and each of these methods has been used to reduce the actinide element concentration in the wastewater.
しかしながら、これらの従来方法では該廃水中
に比較的多量の塩類が共存し、また廃水のPHが８
以上のアルカリ側であるのが一般的であるので、
該廃水からのこれらアクチニド元素の除去は困難
であつた。また、従来方法で一般生活環境に放出
できるレベルまで、アクチニド元素濃度を低減し
ようとする場合には、該廃水の処理速度を遅く
し、たとえば、固定層吸着カラムにおけるSV値
を30h-1未満にする必要があるなど、処理能力の
点においても問題があつた。 However, in these conventional methods, a relatively large amount of salts coexists in the wastewater, and the pH of the wastewater is 8.
Since it is generally on the alkaline side,
Removal of these actinide elements from the wastewater was difficult. In addition, when attempting to reduce the actinide element concentration to a level that can be released into the general living environment using conventional methods, the treatment rate of the wastewater should be slowed down, for example, to reduce the SV value in a fixed bed adsorption column to less than 30 h -1 . There were also problems in terms of processing power, such as the need to
さらに、従来方法では、一度樹脂に吸着された
アクチニド元素を硝酸等の鉱酸で脱着させる場合
には、１規定以上の比較的高い濃度の酸を必要と
し、吸脱着サイクルでの繰返し使用において、樹
脂の劣化の問題や酸の使用量が多くなるなどの問
題が発生した。 Furthermore, in the conventional method, when desorbing actinide elements once adsorbed onto the resin with mineral acids such as nitric acid, a relatively high concentration of acid of 1N or more is required, and when repeatedly used in adsorption/desorption cycles, Problems arose, such as resin deterioration and the amount of acid used.
（発明の目的）
本発明者らは上記の従来方法の問題点を解決
し、アクチニド元素含有の放射性廃水の処理能力
を効率よくかつ経済的に向上せしめ得る処理方法
を提供すべく、種々研究を重ねた結果、吸着体と
して固定化タンニン系吸着体を使用することによ
つて、上記の目的を達成し得ることを見出し、本
発明に到達した。(Objective of the Invention) The present inventors have carried out various studies in order to solve the problems of the above-mentioned conventional methods and provide a treatment method that can efficiently and economically improve the treatment capacity of radioactive wastewater containing actinide elements. As a result of repeated efforts, it was discovered that the above object could be achieved by using a fixed tannin-based adsorbent as an adsorbent, and the present invention was achieved.
（発明の構成）
すなわち、本発明によれば、アクチニド元素含
有の放射性廃水の処理方法において、固定化タン
ニン系吸着体を固定層カラムに充填し、該吸着体
の単位量に対する１時間当りの該放射性廃水通水
量をSV＝30〜300h-1とすることを特徴とする放
射性廃水の処理方法、が得られる。(Structure of the Invention) That is, according to the present invention, in a method for treating radioactive wastewater containing actinide elements, a fixed bed column is packed with an immobilized tannin-based adsorbent, and the adsorption rate per hour for a unit amount of the adsorbent is A method for treating radioactive wastewater is obtained, which is characterized in that the flow rate of radioactive wastewater is set to SV = 30 to 300 h -1 .
本発明で吸着体として使用される固定化タンニ
ン系吸着体には安価な固定化柿渋タンニン、固定
化五倍子タンニンなどがあり、これら吸着体にア
クチニド元素が吸着される機構の要因としては吸
着体の分子構造、アクチニド元素のイオン半径な
どが重要と考えられる。これらの要因の綜合効果
として、アクチニド元素、殊にウラン、トリウ
ム、プルトニウムは類似した吸着挙動を示すもの
と判断される。 Immobilized tannin-based adsorbents used as adsorbents in the present invention include inexpensive immobilized persimmon tannin and immobilized five-fold tannin, and the mechanism by which actinide elements are adsorbed to these adsorbents is The molecular structure and the ionic radius of the actinide element are considered to be important. As a combined effect of these factors, actinide elements, especially uranium, thorium, and plutonium, are considered to exhibit similar adsorption behavior.
本発明方法では、従来のイオン交換樹脂吸着法
やキレート樹脂吸着法の場合の約10倍程度のSV
値においても、廃水中のアクチニド元素を充分に
吸着除去することが可能である。本発明方法にお
いて、SV値が300h-1を越えると、第１図に示す
ように、アクチニド元素の除去率が低下しはじ
め、またSV値が30h-1未満では充分に除去はでき
るものの、廃水処理効率が低下するので、不適当
である。すなわち、本発明方法では工業的には
SV値は30〜300h-1の範囲が必要であり、好まし
くは50〜200h-1の範囲である。また、本発明方法
では、固定化タンニン系吸着体の再生は、0.01〜
0.5規定の薄い鉱酸（希硝酸、希硫酸）で容易に
吸着アクチニド元素を脱着することができる。第
２図に示すように、該吸着体の10回の繰返し使用
においても、吸着能力の低下は殆んど見られな
い。この場合、0.01規定未満の鉱酸ではアクチニ
ド元素の脱着は充分でなく、また0.5規定を越え
る鉱酸ではいたずらに量を消費するだけであり、
得策でない。従つて、本発明方法において脱着に
使用される鉱酸の濃度は0.01〜0.5規定の範囲で
あり、好ましくは0.01〜0.07規定の範囲である。
このように、本発明方法では使用する固定化タン
ニン系吸着体自体が安価であり、吸着効率は極め
て高くかつ脱着も容易であるので、その経済的効
果は大である。また、従来方法では、アクチニド
元素の吸着除去が困難とされているPHが８以上の
廃水及び比較的多量の塩類を含んでいる廃水にお
いても、本発明方法によれば、充分にアクチニド
元素の吸着除去が可能となる。例えば原子燃料加
工施設のプロセス廃液は一般にPH８以上のアルカ
リ側であるが、本発明方法では、第３図に示すよ
うに、PH6.2〜10.5の範囲で充分にアクチニド元
素を吸着除去できる。 The method of the present invention has an SV of about 10 times that of conventional ion exchange resin adsorption methods and chelate resin adsorption methods.
Even at this value, actinide elements in wastewater can be sufficiently adsorbed and removed. In the method of the present invention, when the SV value exceeds 300 h -1 , the removal rate of actinide elements begins to decrease as shown in Figure 1, and when the SV value is less than 30 h -1 , although sufficient removal is possible, the wastewater This is inappropriate because the processing efficiency will be reduced. That is, in the method of the present invention, industrially
The SV value needs to be in the range of 30 to 300 h -1 , preferably in the range of 50 to 200 h -1 . In addition, in the method of the present invention, the regeneration of the immobilized tannin adsorbent is from 0.01 to
Adsorbed actinide elements can be easily desorbed with 0.5N dilute mineral acids (dilute nitric acid, dilute sulfuric acid). As shown in FIG. 2, even after repeated use of the adsorbent 10 times, there is hardly any decrease in adsorption capacity. In this case, mineral acids of less than 0.01N will not desorb actinide elements sufficiently, and mineral acids of more than 0.5N will simply waste the amount.
It's not a good idea. Therefore, the concentration of the mineral acid used for desorption in the method of the invention is in the range of 0.01 to 0.5N, preferably in the range of 0.01 to 0.07N.
As described above, in the method of the present invention, the immobilized tannin-based adsorbent itself used is inexpensive, the adsorption efficiency is extremely high, and desorption is easy, so the economic effect is large. In addition, the method of the present invention can sufficiently adsorb actinide elements even in wastewater with a pH of 8 or higher and wastewater containing a relatively large amount of salts, where it is difficult to adsorb and remove actinide elements using conventional methods. Removal becomes possible. For example, process waste liquid from nuclear fuel processing facilities is generally alkaline with a pH of 8 or higher, but in the method of the present invention, as shown in FIG. 3, actinide elements can be sufficiently adsorbed and removed within the pH range of 6.2 to 10.5.
次に、本発明を実施例によつて、さらに具体的
に説明するが、以下の実施例は本発明の範囲を限
定するものではない。 Next, the present invention will be explained in more detail with reference to Examples, but the following Examples do not limit the scope of the present invention.
実施例 １
内径1.0cm、高さ10.5cmのカラムに固定化柿渋
タンニンを乾量で0.5ｇ充填し、PH＝9.8で85ppm
のウランを含む廃水をSV＝185h-1で5.6流して
吸着させた。処理後の該廃水におけるウラン濃度
を測定した結果、4.3ppmであり、ウラン除去率
は95％であつた。Example 1 A column with an inner diameter of 1.0 cm and a height of 10.5 cm was filled with 0.5 g of immobilized persimmon tannin in dry weight, and the pH was 85 ppm at 9.8.
Wastewater containing uranium was adsorbed by flowing it at SV = 185h -1 for 5.6 hours. As a result of measuring the uranium concentration in the wastewater after treatment, it was found to be 4.3 ppm, and the uranium removal rate was 95%.
次いで、純水で充分吸着体を洗浄した後、0.07
規定の希硝酸を上記カラムに通液し、ウランを脱
着したところ、吸着したウランの99.8％が回収さ
れた。 Next, after thoroughly washing the adsorbent with pure water,
When a specified amount of dilute nitric acid was passed through the column to desorb uranium, 99.8% of the adsorbed uranium was recovered.
実施例 ２
内径1.0cm、高さ10.5cmのカラムに固定化五倍
子タンニンを乾量で0.6ｇ充填し、PH＝8.2で
65ppmのトリウムを含む廃水をSV＝55h-1で７
流し、吸着させた。処理後の廃水におけるトリウ
ム濃度を測定した結果、1.3ppmであり、その除
去率は98％であつた。Example 2 A column with an inner diameter of 1.0 cm and a height of 10.5 cm was filled with 0.6 g of immobilized fivefold tannin in dry weight, and the column was heated at a pH of 8.2.
Wastewater containing 65ppm thorium at SV = 55h -1 7
Rinse it and let it absorb. As a result of measuring the thorium concentration in the wastewater after treatment, it was found to be 1.3 ppm, and the removal rate was 98%.
次いで、純水で吸着体を洗浄した後0.05規定の
希硫酸をカラムに通液したところ、吸着したトリ
ウムの99.9％が脱着により回収された。 Next, after washing the adsorbent with pure water, 0.05 N dilute sulfuric acid was passed through the column, and 99.9% of the adsorbed thorium was recovered by desorption.
実施例 ３
内径1.0cm、高さ10.5cmのカラムに固定化五倍
子タンニンを乾量で0.6ｇ充填し、PH＝7.5で
100ppbのウランを含む廃水をSV＝70h-1で、24.6
通液し、処理後の廃水におけるウラン濃度を測
定した結果、3ppbであり、ウラン除去率は97％
であつた。Example 3 A column with an inner diameter of 1.0 cm and a height of 10.5 cm was filled with 0.6 g of immobilized fivefold tannin in dry weight, and the column was heated at pH = 7.5.
Wastewater containing 100ppb uranium at SV = 70h -1 , 24.6
The uranium concentration in the wastewater after treatment was measured and found to be 3 ppb, with a uranium removal rate of 97%.
It was hot.
更に、純水で吸着体を洗浄した後0.02規定の希
硫酸をカラムに通液してウランを脱着させたとこ
ろ、吸着したウランの99.9％が回収された。 Furthermore, after washing the adsorbent with pure water, 0.02 N dilute sulfuric acid was passed through the column to desorb uranium, and 99.9% of the adsorbed uranium was recovered.
（発明の効果）
本発明は上記のように、吸着体として固定化タ
ンニン系吸着体を使用することによつて次の効果
を示すものである。(Effects of the Invention) As described above, the present invention exhibits the following effects by using a fixed tannin adsorbent as an adsorbent.
(1) 従来方法に比して放射性廃水処理能力を大幅
に増進する。(1) Significantly improve radioactive wastewater treatment capacity compared to conventional methods.
(2) 従来方法で困難とされていたアルカリ性廃水
においても、アクチニド元素を充分に除去する
ことができる。(2) Actinide elements can be sufficiently removed even from alkaline wastewater, which was considered difficult to use with conventional methods.
(3) 固定化タンニンは安価であり、かつ繰返し使
用が可能である。従つて、(1)、(2)の効果と相俟
つて経済的効果は大きい。(3) Fixed tannins are inexpensive and can be used repeatedly. Therefore, combined with the effects (1) and (2), the economic effect is large.
(4) 使用済吸着体については、容易に焼却ができ
るので放射性固体廃棄物の発生量は極めて少な
い。(4) Since used adsorbents can be easily incinerated, the amount of radioactive solid waste generated is extremely small.
第１図は放射性廃水のカラム通液のSV値とア
クチニド元素除去率との関係を示すグラフ図、第
２図は吸脱着サイクルの繰返し回数とアクチニド
元素除去率との関係を示すグラフ図、第３図は放
射性廃水のPHとアクチニド元素除去率との関係を
示すグラフ図である。
Figure 1 is a graph showing the relationship between the SV value of radioactive wastewater flowing through the column and the actinide element removal rate. Figure 2 is a graph showing the relationship between the number of adsorption/desorption cycle repetitions and the actinide element removal rate. Figure 3 is a graph showing the relationship between the PH of radioactive wastewater and the actinide element removal rate.
Claims (1)
において、固定化タンニン系吸着体を固定層カラ
ムに充填し、該吸着体の単位量に対する１時間当
りの該放射性廃水通水量（SV値）を30〜300h-1
とすることを特徴とする放射性廃水の処理方法。 ２ 特許請求の範囲第１項に記載の放射性廃水の
処理方法であつて、前記固定化タンニン系吸着体
に吸着されたアクチニド元素を0.01〜0.5規定の
硝酸または硫酸で脱着し、該固定化タンニン系吸
着体を繰返し使用することを特徴とする処理方
法。 ３ 特許請求の範囲第１項に記載の放射性廃水の
処理方法であつて、前記放射性廃水のPHは6.2〜
10.5の範囲であることを特徴とする処理方法。 ４ 特許請求の範囲第１項に記載の放射性廃水の
処理方法であつて、前記アクチニド元素はウラ
ン、トリウムまたはプルトニウムであることを特
徴とする処理方法。[Claims] 1. In a method for treating radioactive wastewater containing actinide elements, a fixed bed column is packed with an immobilized tannin-based adsorbent, and the flow rate of the radioactive wastewater per hour per unit amount of the adsorbent (SV value) from 30 to 300h -1
A method for treating radioactive wastewater, characterized by: 2. A method for treating radioactive wastewater according to claim 1, wherein actinide elements adsorbed on the immobilized tannin adsorbent are desorbed with 0.01 to 0.5 N nitric acid or sulfuric acid, and the immobilized tannin A treatment method characterized by repeatedly using a system adsorbent. 3. The method for treating radioactive wastewater according to claim 1, wherein the radioactive wastewater has a pH of 6.2 to 6.2.
A processing method characterized by a range of 10.5. 4. The method for treating radioactive wastewater according to claim 1, wherein the actinide element is uranium, thorium, or plutonium.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP8367487A JPS63248491A (en) | 1987-04-04 | 1987-04-04 | Treatment of waste water containing actinide element |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP8367487A JPS63248491A (en) | 1987-04-04 | 1987-04-04 | Treatment of waste water containing actinide element |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS63248491A JPS63248491A (en) | 1988-10-14 |
| JPH0335997B2 true JPH0335997B2 (en) | 1991-05-30 |
Family
ID=13809030
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP8367487A Granted JPS63248491A (en) | 1987-04-04 | 1987-04-04 | Treatment of waste water containing actinide element |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS63248491A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP1813838A2 (en) | 2006-01-30 | 2007-08-01 | Aichi Machine Industry Co. Ltd. | Transmission |
Families Citing this family (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5158711A (en) * | 1990-01-09 | 1992-10-27 | Mitsubishi Nuclear Fuel Co. | Insoluble tannin preparation process, waste treatment process employing insoluble tannin and adsorption process using tannin |
| JP3183354B2 (en) * | 1991-08-23 | 2001-07-09 | 三菱原子燃料株式会社 | Method for adsorbing and separating heavy metals using tannin-based adsorbent and method for regenerating the adsorbent |
| JP3037178B2 (en) * | 1997-02-04 | 2000-04-24 | 核燃料サイクル開発機構 | Equipment for treating plutonium-containing waste liquid using tannin |
-
1987
- 1987-04-04 JP JP8367487A patent/JPS63248491A/en active Granted
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP1813838A2 (en) | 2006-01-30 | 2007-08-01 | Aichi Machine Industry Co. Ltd. | Transmission |
Also Published As
| Publication number | Publication date |
|---|---|
| JPS63248491A (en) | 1988-10-14 |
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