JP3770077B2 - Method and apparatus for removing manganese from raw water - Google Patents
Method and apparatus for removing manganese from raw water Download PDFInfo
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- JP3770077B2 JP3770077B2 JP2000357613A JP2000357613A JP3770077B2 JP 3770077 B2 JP3770077 B2 JP 3770077B2 JP 2000357613 A JP2000357613 A JP 2000357613A JP 2000357613 A JP2000357613 A JP 2000357613A JP 3770077 B2 JP3770077 B2 JP 3770077B2
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Description
【0001】
【発明の属する技術分野】
本発明は、上水原水からマンガンを除去する方法及びその装置に係わる。
【0002】
【従来の技術】
上水原水には0.1〜0.1mg/Lのマンガンが含まれている。このマンガンは微生物により酸化されて不溶性の二酸化マンガン(MnO2)として浄水処理槽や配管の内壁に付着し、ときおり“黒水”として流出したり、ろ過障害を惹き起こす。このため、着水井から出た原水に予め塩素を注入して二酸化マンガンへ酸化し、後段の凝集沈殿及び砂ろ過により除去している。しかし、トリハロメタン,臭素酸など発ガン性物質の生成を抑える観点から、最近では殺菌用の塩素も含めて塩素の使用量を抑える方向にある。このため、最近ではアミドキシム樹脂によりマンガンを吸着除去する試みがなされている。
【0003】
例えばD.Baralkiewiczらは、文献「D.Baralkiewicz and J.Siepak:Chem.Anal.(Warsaw),40(2) 195-200 (1995)」に記載のように、水溶液中のFe3+,Mn2+,Mo6+の分離(吸着除去)を試みており、0.1mg/L のMn2+はpH6以上で50%以上分離できる、すなわち残留液のMn2+ の濃度は規制値である0.05mg/L以下になると報告している。しかし、吸着除去時の樹脂と溶液の接触時間は5時間、吸着したMn2+の回収(酸洗)には1時間を要しており、浄水処理するには時間がかかりすぎ、浄水処理への適用は困難である。また、上水原水にはマンガン以外にも濁度1〜10程度の濁質やTOC(全有機炭素)として1〜10mg/L程度の有機物(フミン質)が共存しており、マンガンの吸着に対するこれらの影響は考慮されていない。
【0004】
さらに、アミドキシム樹脂は鉄,マンガン,モリブデン以外の重金属,ウラン,アクチニドを吸着するため、核燃料の再処理,排水処理,海水ウラン捕集の分野でも注目され、特公平3−2011号公報,特開平9−113681号公報,特開平2000−176279号公報などでも紹介されている。
【0005】
【発明が解決しようとする課題】
本発明は上記従来技術の欠点を鑑みてなされたものであり、本発明の目的は、アミドキシム樹脂による好適な上水原水中のマンガンの除去方法及びその装置を提供することにある。
【0006】
【課題を解決するための手段】
本発明は、凝集沈殿池及びろ過池を有する浄水処理システムの上水原水からマンガンを除去する方法において、該凝集沈澱池またはろ過池からの流出水をアミドキシム樹脂に接触させることを特徴とする。
【0007】
【発明の実施の形態】
本発明の実施の形態では、特に、凝集沈澱またはろ過処理後の上水原水を、アミドキシム樹脂に接触させてマンガンを吸着除去し、吸着除去に使用後の該樹脂を再生して再使用することについて説明する。上記以外にも、凝集沈殿及びろ過処理の前段で前塩素処理された上水原水でもよい。これらの上水原水中のマンガン濃度は一般的に0.1mg/L 程度以下であり、吸着反応は樹脂表面へのマンガンの拡散が律速となる。
【0008】
したがって、樹脂を攪拌,流動,回転させて上水原水と十分に接触させることで、吸着反応を促進し、時間短縮がはかれる。
【0009】
上記上水原水を連続的に処理する場合、樹脂1m2 当りの処理量はおよそ1〜10m3/hである。また、凝集沈殿またはろ過処理により発生する汚泥やろ過及び活性炭吸着池の逆洗水から回収した循環水中のマンガンも、本発明の実施の形態を適用できる。この場合、マンガンは高濃度(1mg/L以上)であり、回分処理が適する。原水1m3当り50〜500cm2の樹脂に5〜30分程度の短時間接触させればよい。
【0010】
アミドキシム樹脂は、前記した特開平2000−176279号公報に記載されているように、ポリエチレン,ポリプロピレンなどの樹脂の素材の表面に電子線を照射したのち、アクリロニトリル及びヒドロキシルアミンを作用させてアミドキシム基を導入したものが代表的である。
【0011】
アミドキシム樹脂の素材の形状としては、球状,粒状,円柱状,円筒状,布状,平板状,波板状のいずれか、またはこれらを組み合わせた構造体が本発明に適用できる。
【0012】
簡便な使用法としては、布状または板状のアミドキシム樹脂を、攪拌機の翼に貼り付けて使用すればよい。つまり、アミドキシム樹脂を布状または板状として、攪拌手段の攪拌部に取り付けることで、簡易に短時間でマンガン除去が可能である。
【0013】
攪拌機等の回転は速いほどよいが、浄水処理における通常の回転数、すなわち50〜150rpm で十分に攪拌効果が現れる。
【0014】
球状,粒状のアミドキシム樹脂は、網,布袋,カゴ等に入れて処理する水と接触させればよい。このとき、網,布袋,カゴ等を強制的に移動または回転させると、樹脂同志がお互いに接触しながら上水原水と接触するので、共存している濁質や有機物が付着するのを防止しながら吸着及び後記する再生を効果的に進めることができる。
【0015】
また、布状の樹脂は、上水原水の流速の速い越流部に自由に流動する吹き流しのように設置し、再生時に引き上げて処理してもよい。流速は0.1 から1m/s程度が望ましい。
【0016】
次に、マンガン吸着性能の低下したアミドキシム樹脂は、マンガンの錯化剤を含む塩酸,硝酸,硫酸などの酸溶液で処理して再生する事が可能であり、効果的である。錯化剤としては、特にクエン酸が好ましいが、シュウ酸,酒石酸,コハク酸,酢酸なども添加効果を発揮する。その添加量は10%以下で十分である。
【0017】
再生処理のときの溶液を30〜50℃に加熱するとさらに再生効果が増大する。
【0018】
以下、本発明をより具体的に説明する。
(実施例1)
まず、河川表流水を凝集沈殿処理して得た汚泥を脱水して、マンガン濃度8.1mg/L,TOC5.3mg/Lのろ過液を得る。そのろ過液の100Lの中に、5cm四方に裁断した布状のアミドキシム樹脂20枚を木綿布の袋の中に入れて沈め、60rpm で液を攪拌しながら室温で処理したところ、マンガン濃度は、10分後に0.03mg/Lまで減少した。
【0019】
つまり、上水原水から簡易な設備で短時間でマンガンを十分に除去することが出来る。
(実施例2)
次に実施例2を図1を用い説明する。図1は、本発明の実施の形態の一つであるアミドキシム樹脂を備えた処理装置の断面図である。この処理装置は、ろ過液4の供給口を備え、ろ過液4を導入する吸着槽3と、攪拌手段であり、攪拌の回転翼を備えた攪拌機2とを備えている。本実施例では攪拌機2の攪拌部である回転翼にアミドキシム樹脂1を貼り付けている。つまり、実施例1と同じ種類のアミドキシム樹脂1を、幅2.5cm ,長さ10cmに裁断し、その40枚を攪拌機2の翼に貼りつけ。それを液滞留量100Lの吸着槽3の中に設置している。
【0020】
攪拌機2の攪拌部である回転翼を、60rpm で回転させた。そこへ、実施例1と同じ表流水をさらに砂ろ過して得たマンガン濃度0.06〜0.07mg/L,TOC2.9〜4.0mg/Lのろ過液4を入れ、流量10L/min で流通させた。
【0021】
その結果、吸着槽3出口のマンガン濃度は、0.01mg/L以下まで短時間で低下した。但し、アミドキシム樹脂1のマンガンの吸着能力が一時間後にはおちてしまい、1h後には0.01mg/Lまで上昇した。
【0022】
そこで、攪拌機2を吸着槽3から取り出し、クエン酸ナトリウム1%を添加した0.1N の塩酸溶液10Lに攪拌部である翼を浸漬して5分洗浄し、さらにpH7で5分水洗した。このような再生処理後に、再び攪拌部である翼を吸着に使用したところ、吸着槽3出口のマンガン濃度は0.01mg/L まで低下した。以上のように、アミドキシム樹脂1のマンガン吸着能力は、簡易に再生することが可能である。
(実施例3)
次に、実施例1と同じ樹脂の布を50cm四方に裁断し、その2枚を5cm隔てて端部を固定し、布がアコーデオンのように動くような構造体を作製した。この構造体を図1に示すような実施例2と同じ吸着槽3内に設置し、1分間に50回の頻度でアコーデオンを操作するように構造体を往復運動させ、ろ過液を処理した。
【0023】
その結果、吸着槽3出口のマンガン濃度は、0.01mg/L 以下まで短時間で低下させることが出来た。しかし、実施例2と同様に、1h後には0.01mg/Lまで上昇した。そこで、再生処理のため、構造体を吸着槽から取り出し、0.1Nの硫酸溶液10Lに構造体を往復運動させながら浸漬して5分洗浄し、さらにpH7で5分水洗した。そして、再生処理後に、再び吸着処理に使用したところ、吸着槽出口のマンガン濃度は、0.01 mg/L以下まで減少させることができた。
(実施例4)
次に、図2を用いて他の例を説明する。図2は、本発明の実施の形態の一つであるアミドキシム樹脂を備えた処理装置の断面図である。一辺が約10mmの立方体状のアミドキシム樹脂5(約100L)を、直径50cm,高さ1m,最大網目間5mmのステンレス製網カゴ6に入れ、それを吸着槽3内で回転させながら、前塩素及び凝集沈澱処理して得たマンガン濃度0.04〜0.05mg/L,TOC4.0〜5.2mg/Lの上水原水7を10L/min で接触させた。その結果、吸着槽3出口のマンガン濃度を0.01mg/L 以下に更に短時間で減少させることが出来た。但し、12分後には0.01mg/Lまで上昇した。
【0024】
そこで、再生処理のため、網カゴ6を吸着槽3から取り出し、クエン酸1%を含む0.1N の塩酸溶液内で浸漬、回転させながら5分間樹脂を洗浄し、さらに水洗した後、再び吸着処理に使用したところ、吸着槽3出口のマンガン濃度は0.01 mg/L以下であり、簡易に再生処理でき、マンガンを除去することができた。
(実施例5)
凝集沈殿池の汚泥が流入する排泥池とろ過池及び活性炭吸着池の逆洗水が流入する排水池から回収した循環水を対象として、処理を実施した。実施例4と同じ方法で処理したところ、循環水中のマンガン濃度は、処理前に7.0〜11.2mg/Lであったが、流通開始5分後に0.2〜0.3mg/Lとすることができた。つまり、短時間で所望するマンガン濃度に減少でき、この処理水は凝集沈殿池の前段にある着水池へ返送し、循環系統を形成することができた。
【0025】
本実施の形態によれば、塩素を注入せず、アミドキシム樹脂に上水原水を接触させるだけマンガンを除去できるので、マンガン由来の“黒水”の発生やろ過障害を回避できるばかりでなく、塩素に由来する発ガン性物質の生成量を低減できる。
【0026】
【発明の効果】
本発明によると、アミドキシム樹脂による好適な上水原水中のマンガンの除去方法及びその装置を提供することができるという効果を奏する。
【図面の簡単な説明】
【図1】本発明の実施の形態の一つであるアミドキシム樹脂を備えた処理装置の断面図である。
【図2】本発明の実施の形態の一つであるアミドキシム樹脂を備えた処理装置の断面図である。
【符号の説明】
1…アミドキシム樹脂、2…攪拌機、3…吸着槽、4…ろ過液、5…アミドキシム樹脂、6…網カゴ、7…原水。[0001]
BACKGROUND OF THE INVENTION
The present invention relates to a method and apparatus for removing manganese from raw water.
[0002]
[Prior art]
The raw water contains 0.1 to 0.1 mg / L of manganese. This manganese is oxidized by microorganisms and becomes insoluble manganese dioxide (MnO 2 ) and adheres to the inner wall of the water purification tank or piping, and sometimes flows out as “black water” or causes filtration trouble. For this reason, chlorine is previously injected into the raw water discharged from the landing well to oxidize to manganese dioxide, and is removed by subsequent aggregation and sand filtration. However, from the viewpoint of suppressing the generation of carcinogenic substances such as trihalomethane and bromic acid, recently, the amount of chlorine including sterilizing chlorine is being reduced. Therefore, recently, attempts have been made to adsorb and remove manganese with an amidoxime resin.
[0003]
For example D.Baralkiewicz et al article "D.Baralkiewicz and J.Siepak:. Chem.Anal (Warsaw ), 40 (2) 195-200 (1995) " as described in, Fe 3+ in aqueous solution, Mn We are trying to separate (adsorb and remove) 2+ and Mo 6+ , and 0.1 mg / L of Mn 2+ can be separated by 50% or more at pH 6 or higher, that is, the concentration of Mn 2+ in the residual liquid is a regulated value. Reported to be 0.05 mg / L or less. However, the contact time between the resin and the solution at the time of adsorption removal is 5 hours, and it takes 1 hour to recover the adsorbed Mn 2+ (pickling). Application is difficult. In addition to manganese, turbidity with a turbidity of about 1 to 10 and organic substances (humic substances) of about 1 to 10 mg / L as TOC (total organic carbon) coexist in manganese water. These effects are not considered.
[0004]
Furthermore, since amidoxime resins adsorb heavy metals other than iron, manganese, and molybdenum, uranium, and actinides, they are also attracting attention in the fields of nuclear fuel reprocessing, wastewater treatment, and seawater uranium collection. It is also introduced in Japanese Patent Laid-Open No. 9-113681 and Japanese Patent Laid-Open No. 2000-176279.
[0005]
[Problems to be solved by the invention]
This invention is made | formed in view of the fault of the said prior art, and the objective of this invention is providing the removal method and the apparatus of the suitable manganese in raw | natural water raw water by an amidoxime resin.
[0006]
[Means for Solving the Problems]
The present invention is characterized in that, in a method for removing manganese from clean water in a water purification system having a coagulation sedimentation basin and a filtration basin, effluent water from the coagulation sedimentation basin or filtration basin is brought into contact with an amidoxime resin.
[0007]
DETAILED DESCRIPTION OF THE INVENTION
In the embodiment of the present invention, in particular, the raw water after the coagulation precipitation or filtration treatment is brought into contact with the amidoxime resin to adsorb and remove manganese, and the resin after use for adsorption removal is regenerated and reused. Will be described. In addition to the above, it is also possible to use raw water raw water that has been pre-chlorinated in the previous stage of coagulation sedimentation and filtration treatment. The manganese concentration in these raw water raw water is generally about 0.1 mg / L or less, and the diffusion of manganese to the resin surface is rate-limiting in the adsorption reaction.
[0008]
Therefore, the agitation reaction is promoted and the time is shortened by sufficiently agitating, flowing, and rotating the resin and bringing it into sufficient contact with the raw water.
[0009]
When the above raw water is continuously treated, the treatment amount per 1 m 2 of the resin is about 1 to 10 m 3 / h. The embodiment of the present invention can also be applied to sludge generated by coagulation sedimentation or filtration treatment and manganese in circulating water collected from filtration and backwash water of an activated carbon adsorption pond. In this case, manganese has a high concentration (1 mg / L or more), and batch processing is suitable. What is necessary is just to contact 50-500 cm < 2 > resin per 1 m < 3 > of raw | natural water for a short time of about 5 to 30 minutes.
[0010]
As described in JP-A-2000-176279, the amidoxime resin irradiates the surface of a resin material such as polyethylene and polypropylene with an electron beam, and then acts on acrylonitrile and hydroxylamine to form amidoxime groups. The ones introduced are typical.
[0011]
As the shape of the material of the amidoxime resin, any of spherical, granular, columnar, cylindrical, cloth, flat, corrugated, or a combination thereof can be applied to the present invention.
[0012]
As a simple method of use, cloth-like or plate-like amidoxime resin may be attached to the blades of a stirrer. That is, manganese can be easily removed in a short time by attaching the amidoxime resin in the form of cloth or plate to the stirring part of the stirring means.
[0013]
Faster rotation of the stirrer and the like is better, but a sufficient stirring effect appears at a normal rotation speed in water purification treatment, ie, 50 to 150 rpm.
[0014]
The spherical and granular amidoxime resin may be brought into contact with water to be treated in a net, a cloth bag, a basket or the like. At this time, if the net, cloth bag, basket, etc. are forcibly moved or rotated, the resins will come into contact with the raw water while being in contact with each other, thus preventing the adhering turbidity and organic matter from adhering. However, the adsorption and the regeneration described later can be effectively advanced.
[0015]
In addition, the cloth-like resin may be installed like a windsock that freely flows in the overflow portion where the flow rate of the raw water is high, and may be pulled up during the regeneration. The flow rate is preferably about 0.1 to 1 m / s.
[0016]
Next, the amidoxime resin having reduced manganese adsorption performance can be regenerated by treatment with an acid solution such as hydrochloric acid, nitric acid or sulfuric acid containing a complexing agent of manganese, which is effective. As the complexing agent, citric acid is particularly preferable, but oxalic acid, tartaric acid, succinic acid, acetic acid and the like also exert the effect of addition. An amount of addition of 10% or less is sufficient.
[0017]
When the solution during the regeneration treatment is heated to 30 to 50 ° C., the regeneration effect is further increased.
[0018]
Hereinafter, the present invention will be described more specifically.
Example 1
First, sludge obtained by coagulating and precipitating river surface water is dehydrated to obtain a filtrate having a manganese concentration of 8.1 mg / L and a TOC of 5.3 mg / L. In 100 liters of the filtrate, 20 pieces of cloth-like amidoxime resin cut into 5 cm square were placed in a cotton cloth bag and submerged, and treated at room temperature while stirring the solution at 60 rpm. After 10 minutes, it decreased to 0.03 mg / L.
[0019]
That is, manganese can be sufficiently removed from the raw water source water in a short time with simple equipment.
(Example 2)
Next, Example 2 will be described with reference to FIG. FIG. 1 is a cross-sectional view of a processing apparatus including an amidoxime resin which is one embodiment of the present invention. The processing apparatus includes a supply port for the
[0020]
The rotary blade which is a stirring part of the stirrer 2 was rotated at 60 rpm. Thereto,
[0021]
As a result, the manganese concentration at the outlet of the adsorption tank 3 decreased to 0.01 mg / L or less in a short time. However, the adsorption capacity of manganese of the amidoxime resin 1 dropped after 1 hour, and increased to 0.01 mg / L after 1 hour.
[0022]
Then, the stirrer 2 was taken out from the adsorption tank 3, and the wing | blade which was a stirring part was immersed in 10 L of 0.1N hydrochloric acid solution which added sodium citrate 1%, and it wash | cleaned for 5 minutes, and also water-washed at pH 7 for 5 minutes. After such regeneration treatment, when the blade as the stirring unit was used again for adsorption, the manganese concentration at the outlet of the adsorption tank 3 decreased to 0.01 mg / L. As described above, the manganese adsorption ability of the amidoxime resin 1 can be easily regenerated.
Example 3
Next, the same resin cloth as in Example 1 was cut into a 50 cm square, the two pieces were separated by 5 cm, and the ends were fixed, to produce a structure in which the cloth moved like an accordion. This structure was placed in the same adsorption tank 3 as in Example 2 as shown in FIG. 1, and the structure was reciprocated so as to operate the accordion at a frequency of 50 times per minute to process the filtrate.
[0023]
As a result, the manganese concentration at the outlet of the adsorption tank 3 could be reduced to 0.01 mg / L or less in a short time. However, as in Example 2, it increased to 0.01 mg / L after 1 h. Therefore, for the regeneration treatment, the structure was taken out of the adsorption tank, immersed in 10 L of 0.1 N sulfuric acid solution while reciprocating the structure, washed for 5 minutes, and further washed with water at pH 7 for 5 minutes. Then, after the regeneration treatment, when used again for the adsorption treatment, the manganese concentration at the adsorption tank outlet could be reduced to 0.01 mg / L or less.
(Example 4)
Next, another example will be described with reference to FIG. FIG. 2 is a cross-sectional view of a processing apparatus including an amidoxime resin which is one embodiment of the present invention. Cubic amidoxime resin 5 (about 100 L) with a side of about 10 mm is placed in a stainless steel basket 6 having a diameter of 50 cm, a height of 1 m, and a maximum mesh size of 5 mm. Then, the raw water 7 in a concentration of 0.04 to 0.05 mg / L and TOC 4.0 to 5.2 mg / L obtained by coagulation precipitation was brought into contact at 10 L / min. As a result, the manganese concentration at the outlet of the adsorption tank 3 could be further reduced to 0.01 mg / L or less in a shorter time. However, it rose to 0.01 mg / L after 12 minutes.
[0024]
Therefore, for the regeneration treatment, the net basket 6 is taken out from the adsorption tank 3, immersed in a 0.1N hydrochloric acid solution containing 1% citric acid, washed for 5 minutes while rotating, further washed with water, and again adsorbed. When used in the treatment, the manganese concentration at the outlet of the adsorption tank 3 was 0.01 mg / L or less, which could be easily regenerated and removed.
(Example 5)
The treatment was carried out on the circulating water collected from the drainage pond into which the sludge of the coagulation sedimentation basin flows, the drainage basin of the filtration basin and the backwash water from the activated carbon adsorption pond. When treated in the same manner as in Example 4, the manganese concentration in the circulating water was 7.0 to 11.2 mg / L before treatment, but 0.2 to 0.3 mg /
[0025]
According to the present embodiment, manganese can be removed only by bringing raw water into contact with the amidoxime resin without injecting chlorine, so that not only generation of “black water” derived from manganese and filtration troubles can be avoided, but also chlorine. The amount of carcinogenic substances derived from can be reduced.
[0026]
【The invention's effect】
If according to the invention, an effect that it is possible to provide a removal method and apparatus of the preferred upper Suwon water manganese by A Midokishimu resin.
[Brief description of the drawings]
FIG. 1 is a cross-sectional view of a processing apparatus provided with an amidoxime resin which is one embodiment of the present invention.
FIG. 2 is a cross-sectional view of a processing apparatus including an amidoxime resin which is one embodiment of the present invention.
[Explanation of symbols]
DESCRIPTION OF SYMBOLS 1 ... Amidoxime resin, 2 ... Stirrer, 3 ... Adsorption tank, 4 ... Filtrate, 5 ... Amidoxime resin, 6 ... Net basket, 7 ... Raw water.
Claims (7)
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CN105016505A (en) * | 2015-07-14 | 2015-11-04 | 合肥科启环保科技有限公司 | Stirring type water purification device |
CN112121522B (en) * | 2020-09-21 | 2022-03-22 | 潢川县鹏升畜产品有限公司 | A collect belt cleaning device for heparin sodium draws resin |
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