JP2013104723A - METHOD AND APPARATUS FOR TREATING Sr-CONTAINING WATER - Google Patents
METHOD AND APPARATUS FOR TREATING Sr-CONTAINING WATER Download PDFInfo
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Abstract
Description
本発明は、Ｓｒ含有水の処理方法及び処理装置に関する。詳しくは、ＳｒとＣａ２＋，Ｍｇ２＋等の陽イオンを含有する水を凝集、固液分離により処理する方法及び装置に関する。 The present invention relates to a method and apparatus for treating Sr-containing water. Specifically, the present invention relates to a method and apparatus for treating water containing cations such as Sr and Ca 2+ , Mg 2+ by agglomeration and solid-liquid separation.
放射性ストロンチウム９０Ｓｒは、放射性Ｃｓと同様に、半減期が長く、また、水への拡散性が高い核***生成物であり、放射性Ｃｓと同様、放射性Ｓｒにより汚染された水についても、その水処理システムの改良が望まれている。 Radioactive strontium 90 Sr is a fission product having a long half-life and high diffusibility to water, similar to radioactive Cs. Like radioactive Cs, water treated with radioactive Sr is also treated with water. Improvement of the system is desired.
従来、水中の放射性Ｓｒの処理には、オルトチタン酸で吸着除去する方法が適用されており（非特許文献１）、従来において、凝集処理は行われていない。 Conventionally, a method of adsorbing and removing with orthotitanic acid has been applied to the treatment of radioactive Sr in water (Non-Patent Document 1), and conventionally, no aggregation treatment has been performed.
オルトチタン酸等の吸着材を用いてＳｒを吸着除去する従来法では、次のような問題があった。
（１） 放射性Ｓｒで汚染された海水など、放射性Ｓｒ含有水は、通常、放射性Ｓｒ以外の陽イオンを多く含有するため、これら陽イオンが放射性Ｓｒの吸着を妨害し、放射性Ｓｒのみを選択的に吸着材で吸着除去することができない。このため、放射性Ｓｒ含有水の吸着処理に当っては、予め他の陽イオンを除去するための前処理が必要となる。
（２） 高濃度Ｓｒ含有水の処理では、吸着材の交換頻度が高く、ランニングコストが嵩む。
（３） 大量のＳｒ含有水の処理には、処理効率が悪く、不適当である。
The conventional method of adsorbing and removing Sr using an adsorbent such as orthotitanic acid has the following problems.
(1) Since radioactive Sr-containing water such as seawater contaminated with radioactive Sr usually contains many cations other than radioactive Sr, these cations interfere with the adsorption of radioactive Sr, and only radioactive Sr is selectively used. It cannot be removed by adsorption with an adsorbent. For this reason, in the adsorption treatment of radioactive Sr-containing water, pretreatment for removing other cations in advance is required.
(2) In the treatment of high-concentration Sr-containing water, the replacement frequency of the adsorbent is high and the running cost increases.
(3) The treatment efficiency is poor and inappropriate for the treatment of a large amount of Sr-containing water.
本発明は、高濃度Ｓｒ含有水や大量のＳｒ含有水であっても、低コストで効率的に水中のＳｒを分解除去することができるＳｒ含有水の処理方法及び処理装置を提供することを課題とする。 The present invention provides a treatment method and a treatment apparatus for Sr-containing water that can efficiently decompose and remove Sr in water at low cost even with high-concentration Sr-containing water or a large amount of Sr-containing water. Let it be an issue.
本発明者らは、上記課題を解決すべく鋭意検討を重ねた結果、水中のＳｒは、アルカリ条件下で炭酸塩と反応して炭酸ストロンチウムの沈殿を生成すること、従って、Ｓｒ含有水の処理に、凝集、固液分離を適用することができることを見出した。 As a result of intensive studies to solve the above problems, the present inventors have found that Sr in water reacts with a carbonate under alkaline conditions to form a precipitate of strontium carbonate, and thus treatment of Sr-containing water. In addition, it has been found that aggregation and solid-liquid separation can be applied.
本発明はこのような知見に基いて達成されたものであり、以下を要旨とする。 The present invention has been achieved on the basis of such findings, and the gist thereof is as follows.
［１］ Ｓｒ含有水にアルカリ条件下で炭酸塩を添加して凝集、固液分離することを特徴とするＳｒ含有水の処理方法。 [1] A method for treating Sr-containing water, characterized in that carbonate is added to Sr-containing water under alkaline conditions for aggregation and solid-liquid separation.
［２］ ［１］において、前記アルカリ条件がｐＨ９〜１３．５であることを特徴とするＳｒ含有水の処理方法。 [2] The method for treating Sr-containing water according to [1], wherein the alkaline condition is pH 9 to 13.5.
［３］ ［１］又は［２］において、前記炭酸塩がアルカリ金属の炭酸塩であることを特徴とするＳｒ含有水の処理方法。 [3] The method for treating Sr-containing water according to [1] or [2], wherein the carbonate is an alkali metal carbonate.
［４］ ［１］ないし［３］のいずれかにおいて、前記Ｓｒ含有水がＳｒとＳｒ以外の陽イオンを含むことを特徴とするＳｒ含有水の処理方法。 [4] The method for treating Sr-containing water according to any one of [1] to [3], wherein the Sr-containing water contains a cation other than Sr and Sr.
［５］ ［４］において、前記Ｓｒ含有水がＳｒを含む海水であることを特徴とするＳｒ含有水の処理方法。 [5] The method for treating Sr-containing water according to [4], wherein the Sr-containing water is seawater containing Sr.
［６］ Ｓｒ含有水に炭酸塩を添加する炭酸塩添加手段と、Ｓｒ含有水をｐＨアルカリ性に調整するｐＨ調整手段と、該炭酸塩添加手段とｐＨ調整手段を経たＳｒ含有水を凝集、固液分離する手段とを有することを特徴とするＳｒ含有水の処理装置。 [6] Carbonate addition means for adding carbonate to Sr-containing water, pH adjustment means for adjusting Sr-containing water to pH alkalinity, and Sr-containing water passed through the carbonate addition means and pH adjustment means are aggregated and solidified. An apparatus for treating Sr-containing water.
［７］ ［６］において、前記ｐＨ調整手段によりＳｒ含有水をｐＨ９〜１３．５に調整することを特徴とするＳｒ含有水の処理装置。 [7] The apparatus for treating Sr-containing water according to [6], wherein the pH adjusting means adjusts the Sr-containing water to a pH of 9 to 13.5.
［８］ ［６］又は［７］において、前記炭酸塩がアルカリ金属の炭酸塩であることを特徴とすることを特徴とするＳｒ含有水の処理装置。 [8] The apparatus for treating Sr-containing water according to [6] or [7], wherein the carbonate is an alkali metal carbonate.
［９］ ［６］ないし［８］のいずれかにおいて、前記Ｓｒ含有水がＳｒとＳｒ以外の陽イオンを含むことを特徴とするＳｒ含有水の処理装置。 [9] The apparatus for treating Sr-containing water according to any one of [6] to [8], wherein the Sr-containing water contains cations other than Sr and Sr.
［１０］ ［９］において、前記Ｓｒ含有水がＳｒを含む海水であることを特徴とするＳｒ含有水の処理装置。 [10] The apparatus for treating Sr-containing water according to [9], wherein the Sr-containing water is seawater containing Sr.
本発明によれば、Ｓｒ含有水にアルカリ条件下で炭酸塩を添加することにより、水中のＳｒを以下の反応で炭酸ストロンチウムとして効率的に析出、沈殿させ、これを凝集、固液分離することにより、効率的に除去することができる。
Ｓｒ２＋＋ＣＯ３ ２−→ＳｒＣＯ３↓ ・・・（１）
According to the present invention, by adding carbonate to Sr-containing water under alkaline conditions, Sr in water is efficiently precipitated and precipitated as strontium carbonate by the following reaction, and this is agglomerated and solid-liquid separated. Thus, it can be efficiently removed.
Sr 2+ + CO 3 2− → SrCO 3 ↓ (1)
また、Ｓｒ含有水がＣａ２＋，Ｍｇ２＋などのＳｒ以外の他の陽イオンを含む場合、以下のように、例えば、Ｃａ２＋は、炭酸カルシウムとして析出、沈殿させて除去することができ、また、Ｍｇ２＋もｐＨ１２以上で水酸化マグネシウムとして析出させて除去することができる。
Ｃａ２＋＋ＣＯ３ ２−→ＣａＣＯ３↓ ・・・（２）
Ｍｇ２＋２ＯＨ−→Ｍｇ（ＯＨ）２↓ ・・・（３）
特に、Ｓｒ含有水にＣａ２＋が含まれる場合、ＣａＣＯ３とＳｒＣＯ３とが共沈することで、沈殿物が高密度となり、汚泥の沈降性、固液分離性が良好となる。
Moreover, when Sr containing water contains other cations other than Sr, such as Ca < 2+ > , Mg <2+> , for example, Ca <2+> can be precipitated and precipitated as calcium carbonate, and can be removed. Mg 2+ can also be deposited and removed as magnesium hydroxide at pH 12 or higher.
Ca 2+ + CO 3 2− → CaCO 3 ↓ (2)
Mg 2+ 2OH − → Mg (OH) 2 ↓ (3)
In particular, when Ca 2+ is contained in the Sr-containing water, CaCO 3 and SrCO 3 co-precipitate, the precipitate becomes dense, and sludge sedimentation and solid-liquid separation properties are improved.
本発明によれば、Ｓｒ含有水に凝集処理を適用することが可能となり、大量のＳｒ含有水であっても容易かつ効率的に安価に処理することができる。しかも、海水のように高塩類濃度のＳｒ含有水であっても、凝集処理であれば、容易かつ効率的に安価に処理することができる。 According to the present invention, it is possible to apply a coagulation treatment to Sr-containing water, and even a large amount of Sr-containing water can be easily and efficiently treated at low cost. Moreover, even Sr-containing water with a high salt concentration such as seawater can be easily and efficiently treated at low cost if it is agglomeration treatment.
本発明において、炭酸塩添加時のアルカリ条件は、ｐＨ９〜１３．５の範囲、特にｐＨ１０〜１３の範囲が好ましく（請求項２，７）、炭酸塩としては、炭酸ナトリウム、炭酸カリウム等のアルカリ金属の炭酸塩が好ましい（請求項３，８）。 In the present invention, the alkali condition at the time of adding carbonate is preferably in the range of pH 9 to 13.5, particularly preferably in the range of pH 10 to 13 (Claims 2 and 7), and the carbonate is an alkali such as sodium carbonate or potassium carbonate. Metal carbonates are preferred (claims 3 and 8).
このような本発明によるＳｒ含有水の処理は、特にＳｒ以外のＣａ２＋，Ｍｇ２＋等の陽イオンを含むＳｒ含有水に有効であり、例えば、Ｓｒを含む海水、とりわけ放射性Ｓｒを含む海水の処理に好適である（請求項４，５，９，１０）。 Such treatment of Sr-containing water according to the present invention is particularly effective for Sr-containing water containing cations other than Sr, such as Ca 2+ and Mg 2+ , for example, seawater containing Sr, especially seawater containing radioactive Sr. Suitable for processing (claims 4, 5, 9, 10).
以下、図面を参照して本発明の実施の形態を詳細に説明するが、以下に説明する実施形態は、本発明の理解を容易にするためのものであって、何ら本発明を限定するものではなく、本発明はその要旨を超えない範囲において、以下の実施形態に開示される各要素を種々変更して実施することができる。 Hereinafter, embodiments of the present invention will be described in detail with reference to the drawings. However, the embodiments described below are for facilitating the understanding of the present invention and do not limit the present invention. Instead, the present invention can be implemented by variously changing each element disclosed in the following embodiments without departing from the scope of the invention.
図１は、本発明のＳｒ含有水の処理方法及び処理装置の実施の形態を示す系統図である。 FIG. 1 is a system diagram showing an embodiment of a method and apparatus for treating Sr-containing water according to the present invention.
図１に示す実施形態では、Ｓｒ含有水（原水）を反応槽１に導入して攪拌下に炭酸塩を添加すると共にｐＨ調整剤を添加してアルカリ条件下に反応させる。 In the embodiment shown in FIG. 1, Sr-containing water (raw water) is introduced into the reaction tank 1 and a carbonate is added with stirring and a pH adjuster is added to react under alkaline conditions.
原水に添加する炭酸塩としては、炭酸ナトリウム（Ｎａ２ＣＯ３）、炭酸カリウム（Ｋ２ＣＯ３）等のアルカリ金属の炭酸塩が好適に用いられる。これらは１種を単独で用いてもよく、２種以上を併用してもよい。また、これらの炭酸塩を含む排水を用いることもできる。 As the carbonate added to the raw water, alkali metal carbonates such as sodium carbonate (Na 2 CO 3 ) and potassium carbonate (K 2 CO 3 ) are preferably used. These may be used alone or in combination of two or more. Moreover, the waste water containing these carbonates can also be used.
炭酸塩の添加量は、少な過ぎると原水中のＳｒやその他の共存陽イオンを十分に除去することができず、多過ぎても添加量に見合う除去効果は得られなくなることから、原水中のＳｒやその他の陽イオンの濃度に応じて反応当量に見合うように適宜決定される。前記の（１）及び（２）式から、原水中のＳｒとＣａの濃度がわかれば必要な炭酸塩の添加量を算出できる。但し、反応に寄与しない炭酸塩もあるので、理論必要量の１〜４倍当量の炭酸塩を添加することが好ましい。 If the amount of carbonate added is too small, Sr and other coexisting cations in the raw water cannot be removed sufficiently, and if too much, the removal effect commensurate with the amount added cannot be obtained. Depending on the concentration of Sr and other cations, it is appropriately determined so as to meet the reaction equivalent. From the above formulas (1) and (2), if the concentrations of Sr and Ca in the raw water are known, the necessary amount of carbonate added can be calculated. However, since there are carbonates that do not contribute to the reaction, it is preferable to add 1 to 4 equivalents of the theoretically required amount of carbonate.
Ｓｒは、ｐＨ９〜１３．５のアルカリ条件下でＳｒＣＯ３として析出するため、ｐＨ調整剤として、水酸化ナトリウム（ＮａＯＨ）、水酸化カリウム（ＫＯＨ）等のアルカリを添加して、原水をｐＨ９〜１３．５に調整する。特に、原水がＭｇ２＋を含む場合には、前述の如く、Ｍｇ２＋はｐＨ１２以上でＭｇ（ＯＨ）２として析出するため、この場合にはｐＨ１０〜１３．５に調整することが好ましい。なお、ｐＨ調整に用いるアルカリとしては、アルカリ排水を用いてもよい。 Since Sr precipitates as SrCO 3 under alkaline conditions of pH 9 to 13.5, alkali such as sodium hydroxide (NaOH) and potassium hydroxide (KOH) is added as a pH adjuster, and the raw water is pH 9 to Adjust to 13.5. In particular, when the raw water contains Mg 2+ is, as described above, since Mg 2+ is precipitated as Mg (OH) 2 at pH12 or more, in this case preferably adjusted to PH10～13.5. In addition, as the alkali used for pH adjustment, alkaline drainage may be used.
反応槽１では、原水中のＳｒ、その他の陽イオンと炭酸塩とを十分に反応させて析出物を得るべく、１〜３０分程度の滞留時間（反応時間）が得られるように設計することが好ましい。 The reaction tank 1 should be designed so that a residence time (reaction time) of about 1 to 30 minutes can be obtained in order to sufficiently react Sr, other cations in the raw water with carbonates to obtain precipitates. Is preferred.
反応槽１の流出液は、次いで凝集槽２で高分子凝集剤（図１ではアニオン性高分子凝集剤（アニオンポリマー））が添加されて撹拌下に凝集処理される。 Next, a polymer flocculant (an anionic polymer flocculant (anionic polymer) in FIG. 1) is added to the effluent from the reaction tank 1 in the flocculant tank 2 and is agglomerated with stirring.
炭酸ストロンチウム及び炭酸カルシウムは、沈降性に優れた良好な凝集フロックを形成するが、水酸化マグネシウムは沈降性が悪くかさ高いフロックである。水酸化マグネシウムは表面電荷がやや正に帯電しているのでアニオンポリマーを添加することで粗大フロックとなり、沈降性を改善することができる。 Strontium carbonate and calcium carbonate form a good floc floc with excellent sedimentation, while magnesium hydroxide is a bulky floc with poor sedimentation. Magnesium hydroxide has a slightly positive surface charge, so adding an anionic polymer results in coarse flocs and can improve sedimentation.
アニオンポリマーとしては、特に限定されないが、例えばポリアクリルアミドの部分加水分解物、ポリアクリルアミドとアクリル酸ナトリウムとの共重合物、アクリルアミドとビニルスルホン酸ナトリウムとの共重合物、及びアクリルアミドとアクリル酸ナトリウムと２−アクリルアミド−２−メチルプロパンスルホン酸ナトリウムとの三元共重合物などが挙げられ、これらの１種又は２種以上を用いることができる。 Although it does not specifically limit as an anionic polymer, For example, the partial hydrolyzate of polyacrylamide, the copolymer of polyacrylamide and sodium acrylate, the copolymer of acrylamide and sodium vinylsulfonate, and acrylamide and sodium acrylate, Examples thereof include terpolymers with sodium 2-acrylamido-2-methylpropanesulfonate, and one or more of these can be used.
アニオンポリマーの添加量は、少な過ぎると十分な凝集効果を得ることができず、多過ぎると凝集不良を引き起こす恐れがあることから、０．５〜５ｍｇ／Ｌ程度とすることが好ましい。 When the amount of the anionic polymer added is too small, a sufficient aggregation effect cannot be obtained, and when it is too large, there is a possibility of causing poor aggregation, so it is preferable to be about 0.5 to 5 mg / L.
なお、凝集槽２において、凝集フロックを十分に粗大化させるために、凝集槽２は、滞留時間（反応時間）が１〜３０分となるように設計することが好ましい。 In the flocculation tank 2, the flocculation tank 2 is preferably designed so that the residence time (reaction time) is 1 to 30 minutes in order to sufficiently coarsen the flocculation floc.
凝集槽２の凝集処理液は、次いで沈殿槽３に導入されて固液分離される。沈殿槽３の分離液は更に濾過器４で濾過されることにより、Ｓｒが除去された処理水を得ることができる。 The flocculation treatment liquid in the flocculation tank 2 is then introduced into the precipitation tank 3 and subjected to solid-liquid separation. The separated liquid in the settling tank 3 is further filtered by the filter 4 to obtain treated water from which Sr has been removed.
なお、図１は、本発明の実施の形態の一例を示すものであって、本発明はその要旨を超えない限り、何ら図１の形態に限定されるものではない。 FIG. 1 shows an example of an embodiment of the present invention, and the present invention is not limited to the form of FIG. 1 as long as the gist thereof is not exceeded.
例えば、炭酸塩やｐＨ調整剤は、反応槽１に添加する他、反応槽１への原水の導入配管に添加してもよく、アニオンポリマーについても反応槽１の流出液を凝集槽２に導入する配管に添加してもよい。
また、炭酸塩を添加する第１反応槽と、第１反応槽からの流出液にｐＨ調整剤を添加する第２反応槽とに分けて各々の薬剤を添加してもよい。凝集槽２と沈殿槽３は省いてもよい。濾過器４は膜濾過装置でもよい。
For example, in addition to adding carbonate and a pH adjuster to the reaction tank 1, it may be added to a pipe for introducing raw water into the reaction tank 1, and an effluent of the reaction tank 1 is introduced into the coagulation tank 2 for the anionic polymer. It may be added to the piping.
Moreover, you may add each chemical | medical agent separately in the 1st reaction tank which adds carbonate, and the 2nd reaction tank which adds a pH adjuster to the effluent from a 1st reaction tank. The aggregation tank 2 and the precipitation tank 3 may be omitted. The filter 4 may be a membrane filtration device.
このような本発明のＳｒ含有水の処理方法は、Ｓｒの他にＣａ２＋，Ｍｇ２＋等の陽イオンを高濃度で含む水の処理に好適であり、適用される原水の水質としては、例えば、導電率１００〜５０００ｍＳ／ｍ、Ｃａ１〜５００ｍｇ／Ｌ、Ｍｇ１〜１５００ｍｇ／Ｌ、Ｓｒ１〜１０ｍｇ／Ｌ、ｐＨ５〜９の水が挙げられる。 Such a method for treating Sr-containing water of the present invention is suitable for treating water containing a high concentration of cations such as Ca 2+ and Mg 2+ in addition to Sr. , Conductivity 100 to 5000 mS / m, Ca 1 to 500 mg / L, Mg 1 to 1500 mg / L, Sr 1 to 10 mg / L, pH 5 to 9 water.
以下、実施例及び比較例を挙げて本発明をより具体的に説明する。 Hereinafter, the present invention will be described more specifically with reference to examples and comparative examples.
［実施例１］
本発明に従って、以下の水質の模擬海水を処理した。
＜模擬海水水質＞
導電率：４４２０ｍＳ／ｍ
Ｃａ：４１７ｍｇ／Ｌ
Ｍｇ：１２６０ｍｇ／Ｌ
Ｓｒ：４．２８ｍｇ／Ｌ
ｐＨ：８．２
[Example 1]
In accordance with the present invention, simulated seawater of the following water quality was treated:
<Simulated seawater quality>
Conductivity: 4420 mS / m
Ca: 417 mg / L
Mg: 1260mg / L
Sr: 4.28 mg / L
pH: 8.2
模擬海水に炭酸塩としてＮａ２ＣＯ３を１２００ｍｇ／Ｌ添加すると共にＮａＯＨを添加してｐＨ１２に調整して１０分間反応させた後、凝集槽２にてアニオンポリマー（栗田工業（株）製「クリフロックＰＡ８２３」（アクリル酸系ポリマー））を３ｍｇ／Ｌ添加して５分間凝集処理し、その後３０分間静置して沈降分離した。上澄水を孔径０．４５μｍのフィルターで濾過し、濾液を分析し、結果を表１に示した。 After adding 1200 mg / L of Na 2 CO 3 as carbonate to simulated seawater and adding NaOH to adjust the pH to 12 and reacting for 10 minutes, anionic polymer (“Cliff” manufactured by Kurita Kogyo Co., Ltd.) 3 mg / L of Rock PA823 ”(acrylic acid polymer)) was added, and the mixture was agglomerated for 5 minutes, and then allowed to stand for 30 minutes for sedimentation. The supernatant water was filtered through a filter having a pore size of 0.45 μm, the filtrate was analyzed, and the results are shown in Table 1.
［比較例１］
実施例１において、模擬海水にＮａＣＯ３を添加しなかったこと以外は同様にして処理を行い、結果を表１に示した。
[Comparative Example 1]
In Example 1, treatment was performed in the same manner except that NaCO 3 was not added to the simulated seawater, and the results are shown in Table 1.
表１より、本発明によれば、模擬海水中のＳｒをＣａ，Ｍｇと共に効率的に除去することができることが分かる。一方、炭酸塩を添加していない比較例１では、ｐＨ１２としたことにより、Ｍｇが除去され、またＣａについても一部除去されたが、Ｓｒは殆ど除去されなかった。 From Table 1, it can be seen that according to the present invention, Sr in the simulated seawater can be efficiently removed together with Ca and Mg. On the other hand, in Comparative Example 1 to which no carbonate was added, Mg was removed and Ca was partially removed by adjusting the pH to 12, but Sr was hardly removed.
実施例１で得られた処理水は、これをイオン交換樹脂やオルトチタン酸などの吸着材で処理することにより、更にＳｒを高度に除去することができ、この場合において、被吸着処理水のＳｒ濃度が十分に低減されており、また、他の陽イオン濃度も低いため、吸着材を頻繁に交換することなく、効率的な高度処理が可能となる。 The treated water obtained in Example 1 can be further removed with a high degree of Sr by treating it with an adsorbent such as an ion exchange resin or orthotitanic acid. Since the Sr concentration is sufficiently reduced and the concentration of other cations is also low, efficient advanced processing can be performed without frequently changing the adsorbent.
１ 反応槽
２ 凝集槽
３ 沈殿槽
４ 濾過器
1 Reaction tank 2 Coagulation tank 3 Precipitation tank 4 Filter
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