JP4111858B2 - Underwater discharge plasma method and liquid treatment apparatus - Google Patents
Underwater discharge plasma method and liquid treatment apparatus Download PDFInfo
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- JP4111858B2 JP4111858B2 JP2003105852A JP2003105852A JP4111858B2 JP 4111858 B2 JP4111858 B2 JP 4111858B2 JP 2003105852 A JP2003105852 A JP 2003105852A JP 2003105852 A JP2003105852 A JP 2003105852A JP 4111858 B2 JP4111858 B2 JP 4111858B2
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【０００１】
【発明が属する技術分野】
本発明は、化学工場排水、薬品工場排水、食品工場排水、油脂工場排水、パルプ工場排水、その他の産業排水、河川水、上水道、などに含まれる有害有機物及びダイオキシン類のような生物難分解性有機物処理を行うための水中放電プラズマ法及び液体処理装置に関するものである。
【０００２】
【従来の技術】
従来の有機物を含む排水処理では微生物を含む活性汚泥を用いた生物処理法が広く実用化されている。しかし、生物処理では芳香族化合物、難生物分解性有機物等が除去できないとの問題が発生している。また、窒素、燐の除去を目的とした従来の高度処理に加えて、脱臭、脱色、殺菌、微量汚染物質、ダイオキシン類や内分泌攪乱物質除去等を目的とした処理方法の導入が進められるようとしている。
【０００３】
そこで、生物難分解性物質等の除去法や水を再利用可能とする処理法として、促進酸化法が提案され、紫外線処理法、オゾン処理法、水中放電プラズマ処理法等の実用化が進められている。
【０００４】
しかし、上記の紫外線処理法は汚染有機物質を除去、殺菌可能であるが、水中では紫外線の透過距離が小さいため、処理効率が悪い。オゾン処理法は脱臭、脱色、殺菌、有機物質の除去に優れているが、オゾンガスは不安定で加圧、熱により分解され易いため、オゾンガスは現場で放電式オゾナイザーにより製造し、送配管を通して処理すべき水に混合させる。したがって、設備全体の効率が悪い。
【０００５】
これらの処理法に対して水中プラズマ放電法は水中にプラズマの発生に伴って生じるラジカル、紫外線、衝撃波、また、急激な電界の変化によって、有機物質を分解除去する方法であり、脱臭、脱色、殺菌作用も優れている。また、二次的な廃棄物も生じず、好ましい処理方法である。尚この様な水中放電プラズマ処理法としては、例えば、特開２０００−９３９７２号に記載されている様な放電容器内の水に平行平板電極の間に微***を有する電気絶縁性隔離壁を設け、両電極に高電圧パルスを印加すると、微***において電界が集中して水中放電プラズマが生ずる。これは金属の溶出が少ないが、プラズマ領域が限られるため実用上の障害となっている。さらに、特開２００１−９４６３号には放電容器内の水に非接触状態で対向した電極に交流パルス電圧を印加し、放電容器内に発生する電場により微細気泡中で水中放電プラズマを起こす方法がある。この方法では電極金属の溶出は押さえられるが、絶縁物を介して水と接しているため、電気エネルギーの注入量が少なく、従って実用上大きな問題となる。
【０００６】
【発明が解決しようとする課題】
水中にプラズマを発生させるためには高電圧を印加して電界密度を高める必要がある。針対平板電極を用いることにより、電界を針電極に集中し、水中放電プラズマを発生させる方法が一般に用いられる。しかし、この方法では放電プラズマが針電極の近傍にしか発生しないため、広域の放電プラズマが得られない。また、電極は直接に水と接するため、針電極の溶出を避けることができない。したがって、針対平板電極は実用化が困難であり、全体的な処理効率が悪い。
【０００７】
本発明においては、高いエネルギー効率で有機物質の分解ができ、さらに金属電極の溶出を防止することができる、高効率液体処理方法及び液体処理装置を提供する。
【０００８】
【課題を解決するための手段】
上記課題を解決するために、本発明の水中放電プラズマ装置では、多孔質誘電体パイプの内側にスパイラル電極（高電圧側）を貼り付けて、多孔質誘電体パイプ及びスパイラル電極の内部にガス通路を形成する。多孔質誘電体パイプの外部を囲んだ接地電極との間に水通路を形成する。ガスは多孔質誘電体パイプを通して微細気泡の形で水に供給される。そこで、両電極に高電圧高周波電源又は高電圧パルス電源を接続することで、電界は多孔質パイプの外部に集中し、微細気泡の存在により水中放電プラズマを発生させることを特徴とする。
【０００９】
この場合、多孔質誘電体としてはポーラスセラミック製或いは合成樹脂製あるいは電気絶縁体よりなるパイプあるいはそれらよりなる平板を用いる。多孔質誘電体はガスと処理水を介しており、ガス圧を水圧より高く保つておくと、ガスは微細気泡として処理水に供給される。
【００１０】
ここでは、微細気泡の存在により、低いエネルギーで水中放電プラズマの生成ができる。また、微細気泡は多孔質パイプの外部に広い範囲で生成されるため、広い範囲の水中放電プラズマを生成することができる。
【００１１】
ガスは空気、酸素、アルゴン等を用いることができる。放電により、ＯＨ、Ｏ、Ｈラジカル等と共にオゾンや過酸化水素が生成され、特に酸素ガスの場合はラジカルの他に多量のオゾンも生成できる。
【００１２】
さらに、本発明は高圧側のスパイラル電極は水と接触していないので、電極の溶出を防止できる。
【００１３】
これらの結果、本発明は低いエネルギーで水中放電プラズマが広く生成できるうえに、オゾンも生成できるため、高効率な液体処理装置となる。
【発明の実施の形態】
以下、本発明について実施例に基づき図面を参照して詳細に説明する。
【００１４】
【実施例】
図１は本発明の実施例を示す水中放電プラズマ装置である。セラミックで形成された多孔質誘電体パイプ６の内側にスパイラル電極（高電圧電極側）５を配している。また、多孔質誘電体パイプ６の外側に網状、円筒状などに成型された接地電極９が置かれている。
【００１５】
高電圧電極５はブッシング１６を、また、接地電極９は電流導入端子１３をそれぞれ介して電源１８に接続されている。電源１８としては高電圧パルス電源や高周波高電圧電源を用いる。
【００１６】
処理すべき水は入口２より多孔質誘電体パイプ６と容器１０の間に形成された水の通路８を通って水出口３から排水される。
【００１７】
空気、アルゴン、酸素ガス等をガス入口１より多孔質誘電体パイプ６と高電圧電極５の内部４に供給する。ガスは多孔質誘電体パイプ６を通過して処理すべき水に微細気泡１９として供給する。高電圧パルスや高周波高電圧を印加すると電界が発生し、集中された電界が多孔質誘電体パイプ６の細孔を微細気泡とともに通過することにより、放電プラズマが発生する。この放電プラズマは、電子温度は高いがガス温度が低い、低温非平衡放電プラズマとなる。水中では低温非平衡放電プラズマにより水分子がＯＨラジカルとＨラジカルに効率的に解離する。また、原料ガスが酸素ガスの場合は、低温非平衡放電プラズマ中では酸素分子が解離することにより酸素原子が発生しオゾンが生成する。
【００１８】
その結果、処理水中の有機物はＯＨラジカルおよびオゾンにより分解される。また、酸素ガスを原料ガスとした場合、処理すべき水が純水であれば、オゾンガス及びオゾン水が水出口３から排水される。
【００１９】
図２に示したのは水処理システムに本水中放電プラズマ水処理装置を組み込んだ一実施例であり、処理槽２０は図１示した水中放電プラズマ装置を用いる。
【００２０】
貯留槽内の被処理液２３は、ポンプ２４によって被処理水導入経路２２を経由して処理槽２０に導入される。同時に、ガスボンベ２５からガス導入経路２６を経由して、図１における多孔質誘電体パイプ６内に導入される。そして、ガスと被処理液２３は処理済排出経路２１を経て、貯留槽３０に返送される。
【００２１】
この際、図１における電極５，９間に高電圧電源１８によりパルス状の高電圧が印加され、プラズマが発生し、上記被処理液２３がプラズマ処理される。
【００２２】
＜プラズマ発生に必要な最低電圧＞上記装置Ｎｏ．１〜５についてプラズマ発生に必要な最低の印加電圧に関する実験を行った。尚比較として、装置Ｎｏ．１はガスを導入しないときのプラズマの発生について示す。
【００２３】
【表−１】
＜プラズマ処理に要するエネルギー量＞本発明においてプラズマ処理に要するエネルギー量に関する比較として、表１中の装置条件１と３と５について実験を行った。
【００２５】
被処理液２３として、蒸留水にオレンジＩＩ染料を１０ｐｐｍ添加し、更にＫＣｌを添加して導電率を１．０×１０−４Ｓ／ｃｍに調整した試料液２００ｍｌを使用し、ピーク電圧が１５ｋＶの直流パルス電圧を印加してオレンジＩＩの脱色を行った。その結果を図３に示す。尚図３は、電気パルスの印加投入エネルギーと、被処理液のオレンジＩＩ濃度との関係を表すグラフである。
【００２６】
【発明の効果】
以上に説明した通り、本発明による水中放電プラズマ処理装置は、電界を多孔質誘電体の細孔に集中し、微細気泡の存在により、低いエネルギーで水中放電プラズマを生成できる。さらに、放電プラズマが多孔質誘電体パイプの細孔に発生するため、電極金属の溶出を防止できる。また、多孔質誘電体パイプ全体にわたって放電が発生するため、広範囲な水中放電プラズマが可能である。
【図面の簡単な説明】
【図１】本発明の実施例における水中放電プラズマ処理装置の構成図の断面図である。
【図２】本発明の一実施例に係る液体処理装置を示す。
【図３】電気パルスの印加投入エネルギーと、被処理液の染料オレンジＩＩ濃度との関係を示すグラフ。
【符号の説明】
１１ 容器フランジ（水入口部）
１２ 容器フランジ（水出口部）
１４ 接地側配線
１５ 配線
１７ 高圧側配線
１８ 電源[0001]
[Technical field to which the invention belongs]
The present invention relates to biodegradability such as harmful organic matter and dioxins contained in chemical factory effluent, chemical factory effluent, food factory effluent, fat factory effluent, pulp factory effluent, other industrial effluent, river water, waterworks, etc. The present invention relates to an underwater discharge plasma method and a liquid processing apparatus for treating organic substances.
[0002]
[Prior art]
In conventional wastewater treatment containing organic matter, biological treatment methods using activated sludge containing microorganisms have been widely put into practical use. However, there is a problem that biological treatment cannot remove aromatic compounds, hardly biodegradable organic substances, and the like. In addition to conventional advanced treatments aimed at removing nitrogen and phosphorus, the introduction of treatment methods aimed at deodorizing, decolorizing, sterilizing, removing trace pollutants, dioxins and endocrine disrupting substances will be promoted. Yes.
[0003]
Therefore, an accelerated oxidation method has been proposed as a method for removing biologically degradable substances, etc., and a treatment method that makes water reusable, and an ultraviolet treatment method, an ozone treatment method, an underwater discharge plasma treatment method, etc. are being put to practical use. ing.
[0004]
However, although the above-mentioned ultraviolet treatment method can remove and sterilize contaminating organic substances, the treatment efficiency is poor because the ultraviolet ray transmission distance is short in water. The ozone treatment method is excellent for deodorization, decolorization, sterilization, and removal of organic substances, but ozone gas is unstable and easily decomposed by pressure and heat, so ozone gas is manufactured on site with a discharge-type ozonizer and processed through a pipe. Mix in the water to be. Therefore, the efficiency of the entire facility is poor.
[0005]
In contrast to these treatment methods, the underwater plasma discharge method is a method of decomposing and removing organic substances by radicals, ultraviolet rays, shock waves, and abrupt changes in the electric field generated by the generation of plasma in water. Bactericidal action is also excellent. In addition, secondary waste does not occur, which is a preferable treatment method. In addition, as such an underwater discharge plasma treatment method, for example, an electrically insulating isolation wall having a minute hole between parallel plate electrodes is provided in water in a discharge vessel as described in JP-A-2000-93972. When a high voltage pulse is applied to both electrodes, the electric field concentrates in the minute holes and underwater discharge plasma is generated. This is a practical impediment due to the limited plasma region, although there is little metal elution. Furthermore, Japanese Patent Laid-Open No. 2001-9463 discloses a method in which an AC pulse voltage is applied to an electrode facing the water in the discharge vessel in a non-contact state, and an underwater discharge plasma is generated in the fine bubbles by the electric field generated in the discharge vessel. is there. In this method, the elution of the electrode metal can be suppressed, but since it is in contact with water through an insulator, the amount of injected electric energy is small, and therefore, it becomes a large practical problem.
[0006]
[Problems to be solved by the invention]
In order to generate plasma in water, it is necessary to increase the electric field density by applying a high voltage. Generally, a method of concentrating an electric field on the needle electrode and generating an underwater discharge plasma by using a needle-to-plate electrode is generally used. However, in this method, since discharge plasma is generated only in the vicinity of the needle electrode, a wide range of discharge plasma cannot be obtained. Further, since the electrode is in direct contact with water, elution of the needle electrode cannot be avoided. Therefore, it is difficult to put the needle-to-plate electrode into practical use, and the overall processing efficiency is poor.
[0007]
The present invention provides a high-efficiency liquid processing method and liquid processing apparatus that can decompose organic substances with high energy efficiency and can prevent elution of metal electrodes.
[0008]
[Means for Solving the Problems]
In order to solve the above problems, in the underwater discharge plasma apparatus of the present invention, a spiral electrode (high voltage side) is attached to the inside of a porous dielectric pipe, and a gas passage is formed inside the porous dielectric pipe and the spiral electrode. Form. A water passage is formed between the porous dielectric pipe and the ground electrode surrounding the outside. Gas is supplied to the water in the form of fine bubbles through a porous dielectric pipe. Therefore, by connecting a high-voltage high-frequency power source or a high-voltage pulse power source to both electrodes, the electric field is concentrated outside the porous pipe, and underwater discharge plasma is generated by the presence of fine bubbles.
[0009]
In this case, as the porous dielectric, a pipe made of porous ceramic, synthetic resin, or an electrical insulator or a flat plate made of them is used. The porous dielectric material passes through gas and treated water. If the gas pressure is kept higher than the water pressure, the gas is supplied to the treated water as fine bubbles.
[0010]
Here, underwater discharge plasma can be generated with low energy due to the presence of fine bubbles. In addition, since the fine bubbles are generated in a wide range outside the porous pipe, a wide range of underwater discharge plasma can be generated.
[0011]
As the gas, air, oxygen, argon or the like can be used. By discharge, ozone and hydrogen peroxide are generated together with OH, O, H radicals and the like, and particularly in the case of oxygen gas, a large amount of ozone can be generated in addition to the radicals.
[0012]
Furthermore, in the present invention, since the high-pressure side spiral electrode is not in contact with water, it is possible to prevent electrode elution.
[0013]
As a result, the present invention can generate a wide variety of underwater discharge plasmas with low energy, and can also generate ozone, so that it becomes a highly efficient liquid processing apparatus.
DETAILED DESCRIPTION OF THE INVENTION
Hereinafter, the present invention will be described in detail based on examples with reference to the drawings.
[0014]
【Example】
FIG. 1 shows an underwater discharge plasma apparatus according to an embodiment of the present invention. A spiral electrode (high voltage electrode side) 5 is disposed inside a porous dielectric pipe 6 made of ceramic. In addition, a ground electrode 9 formed in a net shape, a cylindrical shape, or the like is placed outside the porous dielectric pipe 6.
[0015]
The high voltage electrode 5 is connected to the power supply 18 via the bushing 16 and the ground electrode 9 is connected to the power supply 18 via the current introduction terminal 13. As the power source 18, a high voltage pulse power source or a high frequency high voltage power source is used.
[0016]
Water to be treated is drained from the water outlet 3 through the water passage 8 formed between the porous dielectric pipe 6 and the
[0017]
Air, argon, oxygen gas or the like is supplied from the gas inlet 1 to the porous dielectric pipe 6 and the inside 4 of the high voltage electrode 5. The gas passes through the porous dielectric pipe 6 and is supplied as fine bubbles 19 to the water to be treated. When a high voltage pulse or a high frequency high voltage is applied, an electric field is generated, and the concentrated electric field passes through the pores of the porous dielectric pipe 6 together with fine bubbles, thereby generating discharge plasma. This discharge plasma is a low temperature non-equilibrium discharge plasma having a high electron temperature but a low gas temperature. In water, water molecules are efficiently dissociated into OH radicals and H radicals by low-temperature nonequilibrium discharge plasma. When the source gas is oxygen gas, oxygen atoms are generated by the dissociation of oxygen molecules in the low temperature non-equilibrium discharge plasma, and ozone is generated.
[0018]
As a result, organic substances in the treated water are decomposed by OH radicals and ozone. When oxygen gas is used as the raw material gas, if the water to be treated is pure water, ozone gas and ozone water are drained from the water outlet 3.
[0019]
FIG. 2 shows an embodiment in which the present underwater discharge plasma water treatment apparatus is incorporated in the water treatment system, and the
[0020]
The liquid to be treated 23 in the storage tank is introduced into the
[0021]
At this time, a pulsed high voltage is applied between the electrodes 5 and 9 in FIG. 1 by the high voltage power source 18 to generate plasma, and the liquid to be processed 23 is plasma processed.
[0022]
<Minimum voltage required for plasma generation> Experiments on the minimum applied voltage required for plasma generation were conducted for 1-5. For comparison, the device No. Reference numeral 1 denotes plasma generation when no gas is introduced.
[0023]
[Table-1]
<Energy Amount Required for Plasma Treatment> As a comparison regarding the energy amount required for the plasma treatment in the present invention, an experiment was conducted with respect to apparatus conditions 1, 3 and 5 in Table 1.
[0025]
As the liquid to be treated 23, 200 ml of a sample liquid prepared by adding 10 ppm of Orange II dye to distilled water and further adding KCl to adjust the conductivity to 1.0 × 10 −4 S / cm is used, and the peak voltage is 15 kV. The DC pulse voltage was applied to decolorize Orange II. The result is shown in FIG. FIG. 3 is a graph showing the relationship between the applied energy of electric pulses and the orange II concentration of the liquid to be treated.
[0026]
【The invention's effect】
As described above, the underwater discharge plasma processing apparatus according to the present invention concentrates the electric field on the pores of the porous dielectric and can generate underwater discharge plasma with low energy due to the presence of fine bubbles. Furthermore, since discharge plasma is generated in the pores of the porous dielectric pipe, it is possible to prevent electrode metal from eluting. In addition, since discharge is generated over the entire porous dielectric pipe, a wide range of underwater discharge plasma is possible.
[Brief description of the drawings]
FIG. 1 is a cross-sectional view of a configuration diagram of an underwater discharge plasma processing apparatus in an embodiment of the present invention.
FIG. 2 shows a liquid processing apparatus according to an embodiment of the present invention.
FIG. 3 is a graph showing the relationship between the electric pulse application energy and the concentration of dye orange II in the liquid to be treated.
[Explanation of symbols]
11 Container flange (water inlet)
12 Container flange (water outlet)
14 Grounding side wiring 15
Claims (5)
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| JP2003105852A JP4111858B2 (en) | 2003-03-06 | 2003-03-06 | Underwater discharge plasma method and liquid treatment apparatus |
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| JP2003105852A JP4111858B2 (en) | 2003-03-06 | 2003-03-06 | Underwater discharge plasma method and liquid treatment apparatus |
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| JP2004268003A JP2004268003A (en) | 2004-09-30 |
| JP4111858B2 true JP4111858B2 (en) | 2008-07-02 |
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| KR100938323B1 (en) * | 2005-03-25 | 2010-01-22 | 미츠비시 레이온 가부시키가이샤 | Method of surface treatment and surface-treated article |
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