KR100401996B1 - Improved method of wet scrubbing of nitrogen oxides from flue gas - Google Patents

Improved method of wet scrubbing of nitrogen oxides from flue gas Download PDF

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KR100401996B1
KR100401996B1 KR10-1998-0058101A KR19980058101A KR100401996B1 KR 100401996 B1 KR100401996 B1 KR 100401996B1 KR 19980058101 A KR19980058101 A KR 19980058101A KR 100401996 B1 KR100401996 B1 KR 100401996B1
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nitrogen oxides
naoh
nox
exhaust gas
hydrogen peroxide
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KR20000042033A (en
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고동준
사영삼
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주식회사 포스코
재단법인 포항산업과학연구원
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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/04—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust using liquids
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2370/00—Selection of materials for exhaust purification
    • F01N2370/22—Selection of materials for exhaust purification used in non-catalytic purification apparatus
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2570/00—Exhaust treating apparatus eliminating, absorbing or adsorbing specific elements or compounds
    • F01N2570/14—Nitrogen oxides

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Treating Waste Gases (AREA)

Abstract

본 발명은 배기가스에 함유된 질소산화물(NOx)의 개선된 습식 제거 방법에 관한 것으로,The present invention relates to an improved wet removal method of NOx contained in exhaust gas.

NaOH 또는 Na2S와 같은 알칼리 용액을 사용하는 습식 세정공정에서 질소산화물을 제거함에 있어서, 산화제로서 세정용액의 중량을 기준으로 과산화수소를 0.5 ~ 2% 첨가함을 특징으로 하는 배기가스내에 함유된 질소산화물 제거방법이 제공된다.In removing nitrogen oxides in a wet cleaning process using an alkaline solution such as NaOH or Na 2 S, nitrogen is contained in the exhaust gas, which is characterized by adding 0.5 to 2% hydrogen peroxide based on the weight of the cleaning solution as an oxidizing agent. An oxide removal method is provided.

본 발명의 방법을 사용함으로써 고형물질을 발생시키지 않고 배기가스내의 질소산화물을 보다 효율적으로 제거할 수 있다.By using the method of the present invention, it is possible to more efficiently remove nitrogen oxides in the exhaust gas without generating solid substances.

Description

배기가스에 함유된 질소산화물의 개선된 습식 제거방법{IMPROVED METHOD OF WET SCRUBBING OF NITROGEN OXIDES FROM FLUE GAS}IMPROVED METHOD OF WET SCRUBBING OF NITROGEN OXIDES FROM FLUE GAS

본 발명은 배기가스에 함유된 질소산화물(NOx)의 개선된 습식 제거 방법에 관한 것으로, 보다 상세하게는 질소산화물의 습식 세정공정에서 산화제로서 과산화수소를 주입하여 질소산화물의 제거효율을 증진시키는 개선된 방법에 관한 것이다.The present invention relates to an improved wet removal method of nitrogen oxides (NOx) contained in exhaust gas, and more particularly, to improve the removal efficiency of nitrogen oxides by injecting hydrogen peroxide as an oxidant in the wet cleaning process of nitrogen oxides. It is about a method.

일반적으로 배기가스내에 함유된 NOx를 제거하는 방법으로는 크게 건식공정과 습식공정이 있다. 이중 습식공정은 질산 제조설비나 금속의 산세 공정 등에서 발생하는 배기가스내의 NOx를 제거하는데 주로 사용되는데, 이들 공정에서 발생하는 NOx는 물에 잘 용해되어 쉽게 제거되는 이산화질소(NO2)가 많이 포함되어 있기 때문이다.Generally, there are largely a dry process and a wet process to remove NOx contained in exhaust gas. The double wet process is mainly used to remove NOx in the exhaust gas from nitric acid manufacturing facilities or metal pickling processes, and the NOx generated in these processes contains a lot of nitrogen dioxide (NO 2 ) that is easily dissolved in water and easily removed. Because there is.

이와같은 습식 세정공정에서는 주로 NaOH 또는 Na2S와 같은 알칼리 용액을 사용하여 다음과 같은 반응들에 의해 NOx가 제거된다.In such a wet cleaning process, NOx is removed mainly by using an alkali solution such as NaOH or Na 2 S by the following reactions.

2NaOH + 2NO2→NaNO2+ NaNO3+ H2O2NaOH + 2NO 2 → NaNO 2 + NaNO 3 + H 2 O

Na2S + 2NO2→ Na2SO3+ N2+ 1/2O2 Na 2 S + 2 NO 2 → Na 2 SO 3 + N 2 + 1/2 O 2

4Na2SO3+ 2NO2→ 4Na2SO4+ N2 4Na 2 SO 3 + 2NO 2 → 4Na 2 SO 4 + N 2

NO + 1/2O2→ NO2 NO + 1 / 2O 2 → NO 2

그러나, NOx중 많은 부분을 차지하는 일산화질소(NO)의 경우 물에 잘 용해되지 않고, 산소와의 산화반응에 의해 NO2로 산화되는 정도가 매우 낮기 때문에 NOx중 NO의 함량이 높을 경우 제거효율이 떨어지게 된다.However, since nitrogen monoxide (NO), which occupies a large portion of NOx, does not dissolve well in water, and the oxidation rate with NO 2 is very low by oxidation with oxygen, the removal efficiency is high when the NO content is high Will fall.

이와같은 습식 세정 공정의 문제점을 해결하기 위한 방법들이 고안되어 왔다. 예를들어, 산화제로서 KMnO4를 NaOH 용액에 사용하여 NO를 물에 대한 용해도가 높은 NO2또는 NO3로 산화시킴으로써 NOx의 제거효율을 증대시킬 수 있다고 개시되어 있다〔Industrial & Engineering Chemistry : Process Design and Development, Vol.22, No.2, pp 323 ~ 329(1983)〕. 그러나, 이 방법에서는 반응 과정에서 MnO2고형분이 일부 생성되기 때문에 세정탑이 막히는 문제점이 있다.Methods have been devised to solve this problem of wet cleaning processes. For example, it has been disclosed that the removal efficiency of NOx can be increased by oxidizing NO to NO 2 or NO 3 having high solubility in water by using KMnO 4 in NaOH solution as an oxidizing agent [Industrial & Engineering Chemistry: Process Design and Development, Vol. 22, No. 2, pp 323-329 (1983)]. However, this method has a problem that the washing tower is clogged because some MnO 2 solids are generated during the reaction.

이에 본 발명의 목적은 질소산화물의 습식 세정공정에 과산화수소를 산화제로서 사용함으로써 고형물질을 발생시키지 않고 질소산화물의 제거효율을 증대시키는 개선된 질소산화물 제거 방법을 제공하는 것이다.Accordingly, an object of the present invention is to provide an improved method for removing nitrogen oxides by using hydrogen peroxide as an oxidant in the wet cleaning process of nitrogen oxides, thereby increasing the removal efficiency of nitrogen oxides without generating solid materials.

본 발명에 의하면,According to the invention,

NaOH 또는 Na2S와 같은 알칼리 용액을 사용하는 습식 세정공정에서 질소산화물을 제거하는데 있어서,In the removal of nitrogen oxides in a wet cleaning process using an alkaline solution such as NaOH or Na 2 S,

산화제로서 세정용액의 중량을 기준으로 과산화수소를 0.5 ~ 2% 첨가함을 특징으로 하는 배기가스내에 함유된 질소산화물 제거 방법이 제공된다.Provided is a method for removing nitrogen oxide contained in exhaust gas, wherein 0.5 to 2% of hydrogen peroxide is added based on the weight of the cleaning solution as an oxidizing agent.

이하, 본 발명에 대하여 상세히 설명한다.EMBODIMENT OF THE INVENTION Hereinafter, this invention is demonstrated in detail.

본 발명에서는 종래 NaOH 또는 Na2S와 같은 알칼리 용액을 사용하는 배가스중의 질소산화물 제거시, 과산화수소를 첨가함으로써 질소산화물의 제거 효율이 증대된다는 것이다.In the present invention, the removal efficiency of nitrogen oxides is increased by adding hydrogen peroxide when removing nitrogen oxides in the exhaust gas using an alkaline solution such as NaOH or Na 2 S.

이와같이 종래 질소산화물의 습식 세정공정에 산화제로 과산화수소를 첨가함으로써, 습식공정에서는 다음과 같은 2가지 작용에 의하여 NOx의 제거효율을 증대시킨다.Thus, by adding hydrogen peroxide as an oxidant to the conventional wet cleaning process of nitrogen oxides, the wet process increases the removal efficiency of NOx by the following two actions.

첫째, 과산화수소는 강력한 산화제로서 NO를 NO2로 산화시키면서 물로 전환되기 때문에 물에 대한 용해도가 높은 NO2의 양이 증가하여 NOx의 제거효율이 향상된다.First, since hydrogen peroxide is a powerful oxidant and is converted into water while oxidizing NO into NO 2 , the amount of NO 2 having high solubility in water is increased to improve the NOx removal efficiency.

둘째, 세정용액에 흡수된 NOx는 다음과 같이 물과 반응하여 HNO2를 생성하게 되는데, 이 HNO2는 매우 불안정하기 때문에 NO와 NO2로 쉽게 다시 분해된다.Second, NOx absorbed in the washing solution reacts with water to produce HNO 2 , which is easily decomposed into NO and NO 2 because HNO 2 is very unstable.

NO + NO2+ H2O → 2HNO2 NO + NO 2 + H 2 O → 2HNO 2

NO + OH → HNO2 NO + OH → HNO 2

NO2+ OH → HNO3 NO 2 + OH → HNO 3

그러나, 여기에 과산화수소가 첨가되면 하기식과 같은 반응에 의해 불안정한 HNO2가 안정하고 물에 잘 용해되는 HNO3로 산화되기 때문에 NOx 제거효율이 증대된다.However, when hydrogen peroxide is added thereto, the NOx removal efficiency is increased because unstable HNO 2 is oxidized to HNO 3 that is stable and soluble in water by a reaction such as the following formula.

HNO2+ H2O2→ HNO3+ H2OHNO 2 + H 2 O 2 → HNO 3 + H 2 O

본 발명의 방법에서 산화제로서 사용되는 과산화수소의 첨가량은 세정용액의 중량을 기준으로 0.1% 이상이며, 보다 바람직하게는 0.5 ~ 2%이다. 과산화수소의 투입량이 0.1% 미만일 경우에는 약품의 효과가 너무 적게 나타나며, 2% 이상 투입할 경우에는 투입량에 비해 제거효율이 낮아 경제적이지 않다.The amount of hydrogen peroxide used as the oxidizing agent in the method of the present invention is 0.1% or more based on the weight of the washing solution, more preferably 0.5 to 2%. When the amount of hydrogen peroxide is less than 0.1%, the effect of the drug is too small, and when more than 2% is added, the removal efficiency is not economical because it is lower than the amount.

이하, 실시예를 통하여 본 발명을 상세히 설명한다.Hereinafter, the present invention will be described in detail through examples.

비교예 1 : 습식 세정 방법을 사용한 질소산화물의 제거Comparative Example 1 Removal of Nitrogen Oxide Using Wet Cleaning Method

2단의 세정탑으로 이루어진 장치에서 세정용액으로서 NaOH 단독으로, 그리고 NaOH와 Na2S를 혼합하여 사용한 경우 각각에 있어, 금속 산세정 공정에서 발생된 배기가스에 함유된 NOx의 제거율을 측정하였다. 본 실험에서는 세정용액으로 NaOH와 Na2S가 함께 사용되는데, 배기가스중에 함께 배출되는 HF를 제거하기 위해 NaOH가 사용되어야 한다. 상기 배출된 배기가스의 유량은 약 350Nm3/min이었으며, 세정 용액의 투입량은 각각 NaOH는 1.9kg/hr이며, Na2S는 18.7kg/hr였다. 세정용액으로 NaOH 단독으로 사용한 경우와 NaOH와 Na2S를 함께 사용한 경우에 있어, NOx 제거율의 차이를 표 1에 나타내었다.In the apparatus consisting of a two-stage washing tower, the removal rate of NOx contained in the exhaust gas generated in the metal pickling process was measured for each of NaOH alone and NaOH and Na 2 S as a washing solution. In this experiment, NaOH and Na 2 S are used together as a cleaning solution. NaOH must be used to remove HF that is discharged together in the exhaust gas. The flow rate of the discharged exhaust gas was about 350 Nm 3 / min, the input amount of the cleaning solution was 1.9 kg / hr NaOH, respectively, 18.7 kg / hr Na 2 S. In the case of using NaOH alone and NaOH and Na 2 S together as a washing solution, the difference in NOx removal rate is shown in Table 1.

세정 용액의 성분에 따른 질소산화물의 제거율Removal rate of nitrogen oxides according to the components of the cleaning solution 입구 농도(ppm)Inlet concentration (ppm) 출구 농도(ppm)Outlet concentration (ppm) 총 NOx제거율(%)Total NOx Removal Rate (%) NONO NO2 NO 2 NOxNOx NONO NO2 NO 2 NOxNOx NaOH 단독투입NaOH alone 453453 230230 683683 199199 113113 312312 54.354.3 NaOH+Na2S 투입NaOH + Na 2 S input 453453 230230 683683 188188 7676 264264 61.361.3

실시예 1 : HExample 1: H 22 OO 22 첨가에 의한 질소산화물 제거율의 향상Improvement of NOx Removal Rate by Addition

세정용액으로서 NaOH 용액만을 사용하고, 이 용액에 세정용액의 중량을 기준으로 과산화수소 1%를 투입한 것을 제외하고는, 비교예 1에서와 동일한 장치 및 조건을 사용하여 배기가스내에 함유된 NOx의 제거율을 측정하였다. 출구쪽의 NOx의 농도는 각각 NO가 150ppm, NO2가 81ppm으로 총 231ppm이었으며, NOx의 총 제거율은 66.2%였다. 이와같이, 과산화수소를 첨가하지 않고 NaOH 단독으로, 또는 NaOH와 Na2S의 혼합물을 세정액으로 사용한 경우에 비해 NOx의 제거율이 높다는 것을 알 수 있다.Removal rate of NOx contained in exhaust gas using the same apparatus and conditions as in Comparative Example 1, except that only NaOH solution was used as the cleaning solution and 1% hydrogen peroxide was added to the solution based on the weight of the cleaning solution. Was measured. The concentration of NOx at the exit was 150 ppm NO and 81 ppm NO 2 , respectively, totaling 231 ppm. The total removal rate of NOx was 66.2%. As described above, it can be seen that the removal rate of NOx is higher than that in the case where NaOH alone or a mixture of NaOH and Na 2 S is used as the washing liquid without adding hydrogen peroxide.

실시예 2 : HExample 2: H 22 OO 22 첨가량 변화에 따른 질소산화물 제거율의 변화Changes in the Removal Rate of Nitrogen Oxide with Changes in Addition Amount

실시예 1에 기술된 방법을 사용하여 과산화수소의 첨가량을 변화시키면서 NOx 제거율의 변화를 측정하였다. 결과는 표 2에 나타내었다.The change in NOx removal rate was measured while varying the amount of hydrogen peroxide added using the method described in Example 1. The results are shown in Table 2.

H2O2첨가량 변화에 따른 NOx 제거율NOx removal rate according to the amount of H 2 O 2 addition 입구 농도(ppm)Inlet concentration (ppm) 출구 농도(ppm)Outlet concentration (ppm) 총 NOx제거율(%)Total NOx Removal Rate (%) NONO NO2 NO 2 NOxNOx NONO NO2 NO 2 NOxNOx NaOH 단독 투입NaOH alone 342342 143143 485485 211211 104104 315315 35.135.1 NaOH + 0.5% H2O2투입NaOH + 0.5% H 2 O 2 input 342342 143143 485485 167167 8080 247247 49.149.1 NaOH + 1.0% H2O2투입NaOH + 1.0% H 2 O 2 input 342342 143143 485485 156156 6969 225225 53.653.6 NaOH + 1.5% H2O2투입NaOH + 1.5% H 2 O 2 input 342342 143143 485485 154154 6767 221221 54.454.4 NaOH + 2.0% H2O2투입NaOH + 2.0% H 2 O 2 input 342342 143143 485485 149149 6767 216216 55.555.5

표 2에 나타난 바와 같이, NaOH 세정용액에 첨가한 과산화수소의 양이 증가할수록 질소산화물의 제거율이 향상되었음을 알 수 있다.As shown in Table 2, it can be seen that the removal rate of nitrogen oxide was improved as the amount of hydrogen peroxide added to the NaOH cleaning solution increased.

본 발명에 의하면, 알칼리 용액을 사용하는 습식 세정공정에서 질소산화물을 제거하는데 있어 산화제로서 과산화수소를 주입함으로써 보다 효율적으로 질소산화물을 제거할 수 있다.According to the present invention, nitrogen oxide can be removed more efficiently by injecting hydrogen peroxide as an oxidizing agent in removing nitrogen oxide in a wet cleaning process using an alkaline solution.

Claims (1)

NaOH 또는 Na2S와 같은 알칼리 용액을 사용하는 습식 세정공정에서 질소산화물을 제거함에 있어서, 산화제로서 세정용액의 중량을 기준으로 과산화수소를 0.5 ~ 2% 첨가함을 특징으로 하는 배기가스내에 함유된 질소산화물 제거방법.In removing nitrogen oxides in a wet cleaning process using an alkaline solution such as NaOH or Na 2 S, nitrogen is contained in the exhaust gas, which is characterized by adding 0.5 to 2% hydrogen peroxide based on the weight of the cleaning solution as an oxidizing agent. Oxide removal method.
KR10-1998-0058101A 1998-12-24 1998-12-24 Improved method of wet scrubbing of nitrogen oxides from flue gas KR100401996B1 (en)

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KR20020050991A (en) * 2000-12-22 2002-06-28 신현준 Method for wet scrubbing of nitrogen oxides from flue gas
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KR970073702A (en) * 1996-05-21 1997-12-10 송재준 A reforming reductant for flue gas denitrification and a method for removing nitrogen oxides using the same

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US5366711A (en) * 1991-11-02 1994-11-22 Degussa Aktiengesellschaft Process for the oxidative purification of waste gases containing nitrogen oxides
WO1994012429A1 (en) * 1992-11-23 1994-06-09 Olin Corporation PROCESS FOR REMOVING NOx/SOx OXIDES FROM GASES ______________
JPH09103642A (en) * 1995-09-08 1997-04-22 Commiss Energ Atom Exhaust gas wet purification method
KR970073702A (en) * 1996-05-21 1997-12-10 송재준 A reforming reductant for flue gas denitrification and a method for removing nitrogen oxides using the same

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