KR20170099615A - Electrochemical Process for high concentration of nitrate containing wastewater treatment, and Apparatus therefor - Google Patents
Electrochemical Process for high concentration of nitrate containing wastewater treatment, and Apparatus therefor Download PDFInfo
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Abstract
Description
본 발명은 고농도의 질산성 질소를 함유하고 있는 폐수로부터 전기화학적 방법에 의해 질산성 질소를 제거함으로써 폐수를 정화처리하는 방법과 장치에 관한 것이다. The present invention relates to a method and apparatus for purifying wastewater by removing nitrate nitrogen from wastewater containing nitrate nitrogen at a high concentration by an electrochemical method.
질산성 질소를 함유하고 폐수에서 질산성 질소를 제거하는 종래의 방법으로는 생물학적 탈질, 역삼투막을 이용한 여과 등의 방법이 이용되었다. As a conventional method for removing nitrate nitrogen from wastewater containing nitrate nitrogen, biological denitrification and filtration using a reverse osmosis membrane have been used.
대한민국 공개특허공보 제10-2012-0135746호에는 아질산화균이나 질산화균 등의 미생물을 이용하여 폐수로부터 질소를 제거하는 기술이 개시되어 있다. Korean Patent Laid-Open Publication No. 10-2012-0135746 discloses a technique for removing nitrogen from wastewater by using microorganisms such as nitrifying bacteria or nitrifying bacteria.
그러나 이러한 종래의 방법은 고비용이 소요되거나 운전이 어렵다는 단점이 있는 바, 종래 기술보다 더 효율적이고 경제적으로 질산성 질소를 제거할 수 있는 기술의 제시가 매우 시급한 실정이다. However, such a conventional method has disadvantages such as high cost and difficult operation, and it is very urgent to present a technology capable of removing nitrate nitrogen more efficiently and economically than the prior art.
본 발명은 위와 같은 종래 기술의 한계를 극복하기 위하여 개발된 것으로서, 저렴한 비용과 쉬운 운전방식을 이용하여 경제적이고 매우 효율적으로 폐수로부터 질산성 질소를 제거할 수 있는 기술을 제공하는 것을 목적으로 한다. SUMMARY OF THE INVENTION It is an object of the present invention to provide a technique for economically and efficiently removing nitrate nitrogen from wastewater using a low cost and an easy operation method.
위와 같은 과제를 달성하기 위하여 본 발명에서는, 양이온의 이동을 위한 양이온 교환막에 의해 양극실과 음극실로 구분되어 있으며, 질산성 질소 제거를 위한 전기분해가 일어나는 전기분해조(반응조); 양극(anode); 음극(cathode); 및 암모니아제거용 혼화조를 포함하는 구성을 가지며, 고농도의 질산성 질소를 함유하고 있는 폐수로부터 전기화학적 방법에 의해 질산성 질소를 제거함으로써 폐수를 정화처리하는 방법과 이를 위한 장치가 제공된다. According to an aspect of the present invention, there is provided an electrolytic cell comprising: an electrolytic cell (a reaction tank) divided into an anode chamber and a cathode chamber by a cation exchange membrane for transferring cations, in which electrolysis for removing nitrate nitrogen occurs; Anode; A cathode; And an ammonia-removing admixture tank for removing nitrate nitrogen from the wastewater containing nitrate nitrogen at a high concentration by an electrochemical method to purify wastewater, and an apparatus therefor.
본 발명의 폐수처리 방법에 의하면, 저렴한 비용과 쉬운 운전방식을 이용하여 경제적이고 매우 효율적으로 폐수로부터 질산성 질소를 제거할 수 있게 된다. According to the wastewater treatment method of the present invention, it is possible to economically and highly efficiently remove nitrate nitrogen from wastewater by using a low cost and an easy operation method.
본 발명에 의하면, 농축액 대상 전해 탈질 반응기(전기분해조)의 용량을 획기적으로 감소시킬 수 있게 되면, 에너지 사용 효율 역시 크게 향상시킬 수 있게 되는 효과가 발휘된다. According to the present invention, when the capacity of the electrolytic denitrification reactor (electrolysis tank) for concentrate can be drastically reduced, the energy use efficiency can be greatly improved.
도 1은 본 발명에 따른 폐수처리방법이 적용되는 폐수처리장치에 대한 개략적인 구성도이다.
도 2는 본 발명에 따라 만들어진 용액 속에 존재하는 암모니아 함유량과 용액의 pH 간의 상관관계에 대한 그래프도이다.
도 3은 본 발명에서 용액내에 하이포아염소산과 하이포아염소산 이온이 pH에 따라 공존하는 것을 보여주는 그래프도이다. 1 is a schematic configuration diagram of a wastewater treatment apparatus to which a wastewater treatment method according to the present invention is applied.
FIG. 2 is a graph showing the correlation between the ammonia content in the solution prepared according to the present invention and the pH of the solution. FIG.
FIG. 3 is a graph showing that hypochlorous acid and hypochlorous acid ions coexist in pH in the solution according to the present invention. FIG.
이하, 본 발명의 바람직한 실시예를 첨부한 도면을 참조하여 설명한다. 본 발명은 도면에 도시된 실시예를 참고로 설명되었으나 이는 하나의 실시예로서 설명되는 것이며, 이것에 의해 본 발명의 기술적 사상과 그 핵심 구성 및 작용이 제한되지 않는다. Hereinafter, preferred embodiments of the present invention will be described with reference to the accompanying drawings. Although the present invention has been described with reference to the embodiments shown in the drawings, it is to be understood that the technical idea of the present invention and its essential structure and operation are not limited thereby.
도 1에는 본 발명에 따른 폐수처리방법이 적용되는 본 발명의 폐수처리장치에 대한 개략적인 구성도가 도시되어 있다. Fig. 1 shows a schematic configuration diagram of a wastewater treatment apparatus of the present invention to which the wastewater treatment method according to the present invention is applied.
본 발명에 따른 폐수처리장치에는, 질산성 질소 제거를 위한 전기분해가 일어나는 전기분해조(반응조)가 구비되어 있다. 전기분해조는, 양이온의 이동을 위한 양이온 교환막에 의해 양극실과 음극실로 구분되는데, 양극실에는 불용성 전극으로서 양극(anode)((+)극)이 배치되고, 음극실에는 불용성 전극으로서 음극(cathode)((-)극)이 배치된다. 양극과 음극에는 각각 전원(power supply)를 통해서 전기가 공급된다. The waste water treatment apparatus according to the present invention is provided with an electrolysis tank (reaction tank) in which electrolysis for removing nitrate nitrogen is performed. The electrolysis tank is divided into an anode chamber and a cathode chamber by a cation exchange membrane for the movement of cations. An anode ((+) electrode) is disposed as an insoluble electrode in the anode chamber, ((-) pole). The anode and cathode are supplied with power through a power supply, respectively.
NaCl 용액이 담겨있는 NaCl 용액 저장조로부터 NaCL 용액이 양이온 교환막과 양극 사이에 형성된 양극실로 공급되며, 폐수 저장조에 담겨 있던 처리 대상 폐수(고농도의 질산성 질소를 포함하고 있는 폐수)는 양이온 교환막과 음극 사이에 형성된 음극실로 공급된다. From the NaCl solution storage tank containing the NaCl solution, NaCl solution is supplied to the anode chamber formed between the cation exchange membrane and the anode. The wastewater to be treated (wastewater containing high concentration of nitrate nitrogen) contained in the wastewater storage tank is supplied between the cation exchange membrane and the cathode As shown in Fig.
위와 같은 구성에 있어서, 전기분해조에서는 다음의 화학식 1 내지 5의 반응이 진행된다. In the above constitution, in the electrolytic bath, the reaction of the following formulas (1) to (5) proceeds.
[화학식 1] [ Chemical Formula 1 ]
NO3 - + H2O + 2e- ■ NO2 - + 2OH- NO 3 - + H 2 O + 2e - NO 2 - + 2OH -
[화학식 2] [Formula 2]
NO3 - + 6H2O + 8e- ■ NH3 + 9OH- NO 3 - + 6H 2 O + 8e - NH 3 + 9OH -
[화학식 3] [Formula 3]
NO3 - + 3H2O + 5e- ■ 1/2 N2(g) + 6OH- NO 3 - + 3H 2 O + 5e -? 1/2 N 2 (g) + 6OH -
[화학식 4] [ Chemical Formula 4 ]
NO2 - + 5H2O + 6e- ■ NH3 + 7OH- NO 2 - + 5H 2 O + 6e - NH 3 + 7OH -
[화학식 5] [ Chemical Formula 5 ]
NO2 - + 2H2O + 3e- ■ 1/2 N2(g) + 4OH- NO 2 - + 2H 2 O + 3e -? 1/2 N 2 (g) + 4OH -
상기한 화학식 1 내지 5에 따른 반응식을 통해서 발생된 암모니아는, 용액의 pH에 따라 도 2에 도시된 그래프와 같이 암모늄 이온(NH4 +) 형태로 존재할 수 있으나, 위 화학식 1 내지 5에서 알 수 있듯이, 수산화기(OH-)의 발생으로 인하여 pH가 상승하게 되어 암모니아(NH3)의 형태로 존재하게 되는 양이 많으며, 음극에 이끌려서 양이온교환막을 통하여 양극실로 이동하는 암모늄 이온(NH4 +)은 미량에 불과하다. The ammonia generated through the reaction formula (1) to (5) may exist in the form of ammonium ion (NH 4 + ) according to the pH of the solution as shown in the graph of FIG. 2, as shown, a hydroxyl group (OH -) ammonium ions (NH 4 +) to generate the result is the pH rises often the amount by which it is in the form of ammonia (NH 3), yikkeulryeoseo the cathode move indeed positive electrode through the cation exchange membrane of the It is only a trace amount.
음극실로부터의 유출수는 높은 pH로 인한 다량의 암모니아(NH3)와 미량의 아질산성 질소 이온(NO2 -)을 함유하고 있으므로, 이들의 제거를 위하여 암모니아제거용 혼화조로 이송된다. 즉, 음극실로부터 배출되는 유출수는 암모니아 제거용 혼화조로 보내지는 것이다. The effluent from the cathode chamber contains a large amount of ammonia (NH 3 ) and a small amount of nitrite nitrogen ions (NO 2 - ) due to the high pH, and is transported to the ammonia removal mixing tank for removal thereof. That is, the effluent discharged from the cathode chamber is sent to the mixing tank for removing ammonia.
한편, 전해질 용액(NaCl 용액)이 유입되는 양극실에서는 NaCl 용액의 염소이온으로부터 아래의 화학식 6 내지 화학식 8의 반응식에 따라 강력한 산화제인 하이포아염소산(HClO)이 생성되며, 음극실로부터 양이온 교환막을 통과하여 넘어온 미량의 암모늄 이온(NH4 +)과 아래의 화학식 9와 같이 반응하여 질소가스로 산화된다. On the other hand, hypochlorous acid (HClO), which is a strong oxidizing agent, is produced from the chloride ion of the NaCl solution in the anode chamber into which the electrolytic solution (NaCl solution) flows, according to the following reaction formulas (6) (NH 4 + ), which is passed through the reactor, and is oxidized to nitrogen gas by reacting as shown in the following chemical formula (9).
[화학식 6] [ Chemical Formula 6 ]
2Cl- ⇒ Cl2 + 2e- 2Cl - ⇒ Cl 2 + 2e -
[화학식 7] [Chemical Formula 7]
Cl2 + H2O ⇒ HClO + H+ + Cl- Cl 2 + H 2 O ⇒ HClO + H + + Cl -
[화학식 8] [ Chemical Formula 8 ]
HClO ⇒ OCl- + H+ HClO ⇒ OCl - + H +
[화학식 9] [ Chemical Formula 9 ]
NH4 + + 1.5HOCl ⇒ 0.5N2 + 1.5H2O + 2.5H+ + 1.5Cl- NH 4 + + 1.5HOCl? 0.5N 2 + 1.5H 2 O + 2.5H + + 1.5Cl -
상기한 화학식 8에서 하이포아염소산(HClO)과 하이포아염소산 이온(OCl-)은 도 3에 도시된 것처럼 용액의 pH에 따라 공존한다.In the above formula (8), hypochlorous acid (HClO) and hypochlorite ion (OCl - ) coexist according to the pH of the solution as shown in FIG.
미량의 암모늄 이온의 질소가스로의 전환 반응이 끝난 전해질 용액에는 유리염소인 하이포아염소산이 고농도로 잔류하고 있으며, 이들은 추가적인 암모니아 제거를 위하여 암모니아 제거용 혼화조로 이송된다. 즉, 암모니아 제거용 혼화조로부터 배출되는 용액 중 일부는 다시 NaCl 용액 저장조로 반송되며, 나머지는 처리수로서 배출되는 것이다. After the conversion of the trace amount of ammonium ions into nitrogen gas, the free electrolyte solution contains a high concentration of free chlorine hypochlorous acid, which is transferred to the ammonia-removing admixture for further ammonia removal. That is, a part of the solution discharged from the mixing tank for removing ammonia is returned to the NaCl solution storage tank, and the remainder is discharged as treated water.
암모니아제거용 혼화조로 이송된 암모니아(NH3) 함유 음극실 유출수와 다량의 하이포아염소산(HClO) 함유 양극실 유출수는 아래의 화학식 10 및 화학식 11에 따라 반응하며, 수중의 암모니아는 질소 형태로 전환되어 대기 중으로 방출됨으로써 수중으로부터 제거된다. The anode-outlet water containing ammonia (NH 3 ) transferred to the ammonia-removing admixture and the anode effluent containing a large amount of hypochlorous acid (HClO) react according to the following
[화학식 10] [ Chemical formula 10 ]
2NH3 + 3OCl- ⇒ N2 + Cl- + 3H2O 2NH 3 + 3OCl -> N 2 + Cl - + 3H 2 O
[화학식 11] [Chemical Formula 11]
NO2 - + OCl- ⇒ NO3 - + Cl- NO 2 - + OCl - ⇒ NO 3 - + Cl -
이 때 암모니아를 산화시켜 질소가스로 전환시키기 위해서는 과량의 하이포아염소산(HClO)이 필요한데, 여기에서 과량이라 함은 염소와 암모니아의 질량비를 7.5:1 이상이 되도록 함을 의미한다. To convert ammonia to nitrogen gas, excess hypochlorous acid (HClO) is required, which means that the mass ratio of chlorine and ammonia is at least 7.5: 1.
양극실의 전해질 용액(NaCl 용액) 농도는 양극실에서 암모늄 이온(NH4 +)과의 반응이 끝난 후 암모니아제거용 혼화조에서 음극실 유출수 중의 암모니아를 완전히 제거할 수 있도록 하는 수준에서 결정한다. The concentration of the electrolyte solution (NaCl solution) in the anode chamber is determined at a level that allows complete removal of ammonia in the cathode outlet water in the mixing chamber for removing ammonia after the reaction with ammonium ions (NH 4 + ) in the anode chamber is completed.
암모니아제거용 혼화조 유출수에는 산화제인 하이포아염소산(HClO) 생성에 필요한 염소 이온(Cl-)이 다량 존재하므로 양극실 유출수량 만큼 NaCl 용액 저장조로 반송시켜 NaCl 사용량을 극소화한다. Since there is a large amount of chlorine ion (Cl - ) necessary for the production of hypochlorous acid (HClO), which is an oxidizing agent, the mixing tank effluent for ammonia removal is returned to the NaCl solution storage tank by the amount of the anode chamber distillate to minimize the use of NaCl.
이와 같은 본 발명에 의하면, 농축액 대상 전해 탈질 반응기(전기분해조)의 용량을 획기적으로 감소시킬 수 있게 되면, 에너지 사용 효율 역시 크게 향상시킬 수 있게 된다. According to the present invention, when the capacity of the electrolytic denitrification reactor (electrolytic tank) for concentrate can be drastically reduced, the energy use efficiency can be greatly improved.
또한 본 발명에서는 양극실의 전해질 용액으로서 NaCl 용액을 사용하므로, 소독효과를 가지는 차아염소산(hypochlorous acid, HOCl)이나 차아염소산 이온(hypochlorite, OCl-)을 생성하게 된다. 전기분해시에 양극에서의 반응은 물의 산화에 의한 산소와 수소 이온의 생성이며, 양극 표면에서의 염소이온은 염소가스로 전환된다. 이 때, 염소수율을 높이기 위해서는 산소 발생을 최소화할 필요가 있는데, 이를 위하여 MMO(Mixed Metal Oxide) 전극에 Ruthenium, Iridium 과 같은 촉매물질을 코팅함으로써 염소 발생에 필요한 전압을 낮춤과 동시에 반응속도를 빠르게 하여 산소 발생을 최소화하여 염소발생을 더욱 활성화시키게 된다. In the present invention, hypochlorous acid (HOCl) and hypochlorite ions (hypochlorite, OCl - ) are produced using a NaCl solution as an electrolyte solution in the anode chamber. In the electrolysis, the reaction at the anode is the production of oxygen and hydrogen ions by the oxidation of water, and the chloride ion at the anode surface is converted into chlorine gas. In order to increase the chlorine yield, it is necessary to minimize the generation of oxygen. To this end, a catalyst material such as ruthenium and iridium is coated on a mixed metal oxide (MMO) electrode to lower the voltage required for chlorine generation and to accelerate the reaction rate Thereby minimizing oxygen generation and further activating chlorine generation.
염소가스는 수중의 수산기와 반응하여 차아염소산이온이나 차아염소산을 발생시킨다. 부가적인 방응으로 차아염소산과 차아염소산이온은 서로 반응하여 염소산염을 형성하며, 염소산염의 분해 반응에 의해 산소를 발생시킬 수도 있다. 이와 같은 반영에서 존재하는 염소산화물에 의해 소독이 일어나게 된다. Chlorine gas reacts with hydroxyl groups in water to generate hypochlorite ions and hypochlorous acid. As an additional stimulus, hypochlorous acid and hypochlorite ion react with each other to form chlorate, and oxygen can be generated by the decomposition reaction of chlorate. In such a reflection, disinfection occurs due to the presence of chlorine oxide.
본 발명에서는 이와 같이 전기농축이 일어나는 이온교환막 여과장치를 거친 전해액 내에 소독효과를 가지는 물질들이 다량으로 존재하므로, 이를 별도로 저장해두었다가 이온교환막 여과를 거친 처리수를 필요에 따라 간헐적으로 희석하여 주입함으로써, 일반 세균과 총대장균군을 제거할 수 있다. In the present invention, since there are a large amount of substances having an effect of disinfecting in the electrolytic solution which has passed through the ion exchange membrane filtration apparatus in which electric enrichment takes place, it is separately stored, and the treated water after the ion exchange membrane filtration is intermittently diluted and injected, General bacteria and total coliforms can be removed.
본 발명에 따른 이와 같은 전기분해에 의한 소독(Electro-disinfection) 과정은 소독을 위한 별도의 약품 투입을 필요없게 한다는 점에서 매우 유리한 장점을 가진다. 특히, 처리수에 이들 소독 물질 즉, 산화제를 주입할 경우에는 이온 교환막 여과에서 제거되지 못한 비소를 5가의 비소로 산화시키게 되어 음용수의 안전성을 향상시키게 되는 효과가 발휘된다. The electrolytic disinfection process according to the present invention has a very advantageous advantage in that it does not require the addition of a separate chemical for disinfection. In particular, when these disinfecting substances, that is, oxidizing agents, are injected into the treated water, arsenic which has not been removed by the ion exchange membrane filtration is oxidized to arsenic of pentavalent, and the safety of the drinking water is improved.
Claims (2)
양극(anode);
음극(cathode); 및
암모니아제거용 혼화조를 포함하는 구성을 가지며,
고농도의 질산성 질소를 함유하고 있는 폐수로부터 전기화학적 방법에 의해 질산성 질소를 제거함으로써 고농도 질산성 질소 함유 폐수를 정화처리하는 방법.
An electrolysis tank (electrolysis tank) which is divided into an anode chamber and a cathode chamber by a cation exchange membrane for the movement of cations and in which electrolysis for removing nitrate nitrogen occurs;
Anode;
A cathode; And
And a mixing tank for removing ammonia,
A method for purifying nitrate-containing wastewater with high concentration by removing nitrate nitrogen from an effluent containing high nitrate nitrogen by an electrochemical method.
양극(anode);
음극(cathode); 및
암모니아제거용 혼화조를 포함하는 구성을 가지며,
고농도의 질산성 질소를 함유하고 있는 폐수로부터 전기화학적 방법에 의해 질산성 질소를 제거함으로써 고농도 질산성 질소 함유 폐수를 정화처리하는 장치. An electrolysis tank (electrolysis tank) which is divided into an anode chamber and a cathode chamber by a cation exchange membrane for the movement of cations and in which electrolysis for removing nitrate nitrogen occurs;
Anode;
A cathode; And
And a mixing tank for removing ammonia,
An apparatus for purifying nitrate-containing wastewater with high concentration by removing nitrate nitrogen from an effluent containing nitrate nitrogen at a high concentration by an electrochemical method.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2020032312A1 (en) * | 2018-08-07 | 2020-02-13 | (주) 테크로스 | Method for treating nitrate nitrogen in water |
| CN115403114A (en) * | 2022-08-11 | 2022-11-29 | 江苏泰源环保科技股份有限公司 | Nitrate wastewater treatment method based on double-chamber electrolytic reaction tank |
-
2016
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2020032312A1 (en) * | 2018-08-07 | 2020-02-13 | (주) 테크로스 | Method for treating nitrate nitrogen in water |
| CN115403114A (en) * | 2022-08-11 | 2022-11-29 | 江苏泰源环保科技股份有限公司 | Nitrate wastewater treatment method based on double-chamber electrolytic reaction tank |
| CN115403114B (en) * | 2022-08-11 | 2024-01-05 | 江苏泰源环保科技股份有限公司 | Nitrate wastewater treatment method based on double-chamber electrolytic reaction tank |
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