KR100488398B1 - Method for treating NOx using Mn oxide catalyst and ozone and the apparatus therefor - Google Patents
Method for treating NOx using Mn oxide catalyst and ozone and the apparatus therefor Download PDFInfo
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- KR100488398B1 KR100488398B1 KR10-2003-0037425A KR20030037425A KR100488398B1 KR 100488398 B1 KR100488398 B1 KR 100488398B1 KR 20030037425 A KR20030037425 A KR 20030037425A KR 100488398 B1 KR100488398 B1 KR 100488398B1
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- B—PERFORMING OPERATIONS; TRANSPORTING
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Abstract
본 발명은 오존과 산화망간계 촉매를 이용하여 일산화질소, 이산화질소 등 질소산화물을 처리하는 방법 및 장치에 관한 것이다.The present invention relates to a method and apparatus for treating nitrogen oxides such as nitrogen monoxide and nitrogen dioxide using ozone and manganese oxide catalysts.
본 발명에서는 과망간산칼륨 수용액에 담체를 함침시키고, 상기 함침된 담체를 상기 수용액으로부터 분리하여 건조시킨 후 상기 건조된 담체를 소성하여 얻어지는 산화망간계 촉매체와 오존을 동시에 이용하여 상온 내지 700℃에서 질소산화물을 제거하는 것을 특징으로 하는 산화망간계 촉매체 및 오존을 이용한 질소산화물의 처리방법을 제공한다.In the present invention, the aqueous solution of potassium permanganate is impregnated with a carrier, the impregnated carrier is separated from the aqueous solution, dried, and then dried using the manganese oxide catalyst body and ozone, which are obtained by firing nitrogen at room temperature to 700 ° C. Provided is a manganese oxide catalyst body and a method for treating nitrogen oxide using ozone, characterized in that the oxide is removed.
또한, 본 발명은 질소산화물을 포함하는 혼합가스가 유입되는 유입구와 연통되는 오존반응챔버에 오존을 주입하는 오존발생원과 상기 오존반응챔버와 접촉하여 위치하며, 과망간산칼륨 수용액에 담체를 함침시키고, 상기 함침된 담체를 상기 수용액으로부터 분리하여 건조시킨 후 상기 건조된 담체를 소성하여 얻어지는 산화망간계 촉매체를 저장하는 챔버로 구성된 것을 특징으로 하는 산화망간계 촉매체 및 오존을 이용한 질소산화물의 처리장치를 제공하는 것을 특징으로 한다.In addition, the present invention is located in contact with the ozone generating source for injecting ozone into the ozone reaction chamber in communication with the inlet port in which the mixed gas containing nitrogen oxide is introduced and the ozone reaction chamber, impregnated with a carrier in aqueous potassium permanganate solution, After the impregnated carrier is separated from the aqueous solution and dried, the manganese oxide catalyst body and nitrogen oxide processing apparatus using ozone are characterized by comprising a chamber for storing the manganese oxide catalyst body obtained by firing the dried carrier. It is characterized by providing.
Description
본 발명은 오존과 산화망간을 이용하여 일산화질소, 이산화질소 등 질소산화물을 처리하는 방법 및 장치에 관한 것이다.The present invention relates to a method and apparatus for treating nitrogen oxides such as nitrogen monoxide and nitrogen dioxide using ozone and manganese oxide.
질소산화물은 대기오염의 주 성분으로 환경법으로도 엄격히 규제하고 있으며, 질소 산화물을 그 발생원으로 분류하면 발전소, 소각로, 화학공장 등의 고정원에 의한 발생과 자동차 선박 등 이동원에 의한 발생이 있다. Nitrogen oxides are a major component of air pollution and are strictly regulated by the Environmental Law. When nitrogen oxides are classified as their sources, they are generated by stationary sources such as power plants, incinerators, chemical plants, and mobile sources such as automobiles and ships.
고정원에서 발생하는 질소산화물은 습식중화법, 촉매환원법 등이 많이 사용되고 있으며, 그 중에서 촉매환원법은 이산화망간을 주 촉매로 사용하여 150 ∼ 400℃구간에서 환원제로 우레아, 암모니아, 메탄올 등을 첨가하여 질소산화물을 제거하고 있다.Nitrogen oxides generated from fixed sources are frequently used in wet neutralization and catalytic reduction methods. Among them, the catalytic reduction method uses manganese dioxide as the main catalyst and adds urea, ammonia, methanol, etc. as a reducing agent in the range of 150 ~ 400 ℃. The oxide is being removed.
그러나, 기존의 촉매에 의한 질소산화물 처리방법에는 다음과 같은 문제점이 있었다.However, the conventional method for treating nitrogen oxides by catalysts has the following problems.
1) 고온에서 운영되므로 연료비의 부담이 크다.1) Fuel costs are high because it operates at high temperatures.
2) 망간촉매가 고가이다.2) Manganese catalyst is expensive.
3) 환원제인 우레아, 암모니아 등을 주입하므로 원료비의 부담이 크고 장치가 복잡하다.3) Injecting urea and ammonia, which are reducing agents, burden of raw material cost is high and the device is complicated.
4) 장치의 규모가 크고 고가라는 문제점이 있다.4) There is a problem that the device is large and expensive.
본 발명은 전술한 종래기술의 문제점을 해결하기 위하여 안출된 것으로서, 질소산화물의 처리효율이 탁월한 새로운 방법으로 제조된 이산화망간 촉매체와 오존을 동시에 이용하여 질소산화물을 처리하는 방법을 제공하며, 상온에서도 운전이 가능하며 간단하고 경제적인 질소산화물의 처리장치를 제공하는데 그 목적이 있다.The present invention has been made to solve the above-mentioned problems of the prior art, and provides a method for treating nitrogen oxides simultaneously using a manganese dioxide catalyst body and ozone prepared by a novel method with excellent treatment efficiency of nitrogen oxides, even at room temperature Its purpose is to provide a nitrogen oxide treatment device that is simple and economical to operate.
본 발명에서는 과망간산칼륨 수용액에 담체를 함침시키고, 상기 함침된 담체를 상기 수용액으로부터 분리하여 건조시킨 후 상기 건조된 담체를 소성하여 얻어지는 산화망간계 촉매체와 오존을 동시에 이용하여 상온 내지 700℃에서 질소산화물을 제거하는 것을 특징으로 하는 산화망간계 촉매체 및 오존을 이용한 질소산화물의 처리방법을 제공한다.In the present invention, the aqueous solution of potassium permanganate is impregnated with a carrier, the impregnated carrier is separated from the aqueous solution, dried, and then dried using the manganese oxide catalyst body and ozone, which are obtained by firing nitrogen at room temperature to 700 ° C. Provided is a manganese oxide catalyst body and a method for treating nitrogen oxide using ozone, characterized in that the oxide is removed.
또한, 본 발명에서는 상기 과망간산칼륨 수용액에 구리(Cu), 은(Ag), 크롬(Cr), 아연(Zn), 란타늄(La), 세륨(Ce), 네오듐(Nd) 중에서 선택된 어느 하나 이상의 금속의 질산염을 첨가하는 것을 특징으로 하는 산화망간계 촉매체 및 오존을 이용한 질소산화물의 처리방법을 제공한다. In the present invention, at least one selected from copper (Cu), silver (Ag), chromium (Cr), zinc (Zn), lanthanum (La), cerium (Ce), neodium (Nd) in the aqueous solution of potassium permanganate Provided is a manganese oxide catalyst body and a method for treating nitrogen oxides using ozone, comprising adding a metal nitrate.
또한, 본 발명에서는 질소산화물을 포함하는 혼합가스가 유입되는 유입구와 연통되는 오존반응챔버에 오존을 주입하는 오존발생원과 상기 오존반응챔버와 연통되며, 과망간산칼륨 수용액에 담체를 함침시키고, 상기 함침된 담체를 상기 수용액으로부터 분리하여 건조시킨 후 상기 건조된 담체를 소성하여 얻어지는 산화망간계 촉매체를 저장하는 챔버로 구성된 것을 특징으로 하는 산화망간계 촉매체 및 오존을 이용한 질소산화물의 처리장치를 제공한다.In addition, the present invention is in communication with the ozone generating source for injecting ozone into the ozone reaction chamber in communication with the inlet port in which the mixed gas containing nitrogen oxide is introduced and the ozone reaction chamber, impregnated with a carrier in the aqueous potassium permanganate solution, the impregnated Provided is a manganese oxide catalyst body and a nitrogen oxide processing apparatus using ozone comprising a chamber for storing the manganese oxide catalyst body obtained by firing the carrier separated from the aqueous solution after drying the carrier. .
또한, 본 발명에서는 상기 과망간산칼륨 수용액에 구리, 아연, 은, 크롬, 란타늄, 세륨, 네오듐 중에서 선택된 어느 하나 이상의 금속의 질산염을 더 첨가하는 것을 특징으로 하는 산화망간계 촉매체 및 오존을 이용한 질소산화물의 처리장치를 제공하는 것을 그 특징으로 한다.Further, in the present invention, the manganese oxide catalyst and nitrogen using ozone are further added to the potassium permanganate aqueous solution, further comprising a nitrate of at least one metal selected from copper, zinc, silver, chromium, lanthanum, cerium, and neodium. It is characterized by providing an apparatus for treating oxides.
이하, 본 발명에서의 질소산화물의 처리방법의 실시예를 설명한다. 우선 과망간산칼륨으로부터 산화망간계 촉매체를 제조한다. Hereinafter, the Example of the nitrogen oxide processing method in this invention is described. First, a manganese oxide catalyst body is prepared from potassium permanganate.
산화망간의 원료로서 과망간산칼륨의 수용액을 준비하고 그 수용액에 활성탄, 활성알루미나, 활성실리카, 제올라이트, 규조토, 일반필터 등의 담체를 함침하여 산화망간계 촉매체를 준비한다. An aqueous solution of potassium permanganate is prepared as a raw material of manganese oxide, and the manganese oxide catalyst body is prepared by impregnating the aqueous solution with activated carbon, activated alumina, activated silica, zeolite, diatomaceous earth, and a general filter.
이 때, 촉매의 성능을 높이기 위하여 선택적으로 첨가될 수 있는 금속첨가제로서 구리질산염, 은질산염, 크롬질산염, 세륨질산염, 아연질산염, 란타늄질산염 및 네오듐질산염 중 어느 하나 이상을 선택하여 사용할 수 있다.At this time, any one or more of copper nitrate, silver nitrate, chromium nitrate, cerium nitrate, zinc nitrate, lanthanum nitrate and neodium nitrate may be selected and used as a metal additive which may be selectively added to increase the performance of the catalyst.
함침이 끝난 담체는 50∼150℃에서 5∼10시간 건조하며, 건조후 150∼600℃ 구간에서까지 소성과정을 거쳐 최종 산화망간계 촉매체를 얻을 수 있다.The impregnated carrier is dried at 50 to 150 ° C. for 5 to 10 hours, and after drying, a final manganese oxide catalyst body can be obtained by baking to 150 to 600 ° C. section.
건조온도와 소성온도가 이와 같은 범위로 설정된 이유는 건조온도는 50℃이하에서는 건조시간이 너무 길어 부적절하고, 150℃ 이상에서는 과망간산칼륨이 분해되기 시작하기 때문에, 소성온도는 150℃ 이하에서는 과망간산칼륨이 산화망간과 산화칼륨으로 전환되지 않아 부적절하고, 600℃ 이상에서는 폭발적으로 분해되기 때문에 작업의 위험성이 있기 때문이다.The reason why the drying temperature and the firing temperature are set in such a range is that the drying temperature is inadequate because the drying time is too long at 50 ° C. or lower, and potassium permanganate starts to decompose at 150 ° C. or higher. This is because there is a risk of work because it is not converted to manganese oxide and potassium oxide and is inadequate.
과망간산칼륨은 소성과정을 거치면 다음 식(1)과 같은 분해 반응이 일어난다.Potassium permanganate undergoes a calcination process and a decomposition reaction occurs as shown in Equation (1).
2KMnO4 → K2O + 2MnO2 + 3/2O2 ---------------- (1)2KMnO 4 → K 2 O + 2MnO 2 + 3 / 2O 2 ---------------- (1)
이 분해과정은 과망간산칼륨이 원자규모에서 분해되기 때문에 미세한 산화망간을 얻을 수 있으며 담체상에서 균일하게 분포되며, 소성과정에서 생겨난 산화칼륨은 아주 강한 알칼리성을 나타내며 오존의 분해를 촉진시킨다.In this decomposition process, since potassium permanganate is decomposed at the atomic scale, fine manganese oxide can be obtained and distributed uniformly on the carrier. Potassium oxide generated during the firing process has a very strong alkalinity and promotes the decomposition of ozone.
한편, 상기와 같이 제조된 산화망간계 촉매체와 오존발생원으로부터발생한 오존을 동시에 이용하여 질소산화물을 제거한다. On the other hand, nitrogen oxides are removed by simultaneously using the manganese oxide catalyst body prepared as described above and ozone generated from the ozone generating source.
이 때 오존발생원은 자외선램프, 무성방전, 프라즈마 중 어느 하나중 에서 선택하여 사용할 수 있다. At this time, the ozone generating source can be selected from among ultraviolet lamp, silent discharge, and plasma.
본 발명에서 일어나는 질소산화물의 제거 방식은 다음과 같다.The nitrogen oxide removal method occurring in the present invention is as follows.
먼저 일산화질소(NO)가 오존과 반응하여 이산화질소(NO2)로 전환된다. 반응식은 다음 식 (2)와 같다.Nitrogen monoxide (NO) first reacts with ozone and is converted to nitrogen dioxide (NO 2 ). The reaction formula is shown in the following formula (2).
NO + O3 → NO2 + O2 ----------------------- (2)NO + O 3 → NO 2 + O 2 ----------------------- (2)
이렇게 일산화질소를 이산화질소를 전환시키는 이유는 일산화질소와 이산화질소가 동시에 존재할 경우에는 각각의 처리촉매가 필요하며, 또한 NO의 경우가 처리가 어려우므로 일산화질소를 오존과 반응하여 이산화질소로 먼저 전환한 다음, 이산화질소를 촉매로 처리하는 것이 유리하기 때문이다.The reason for converting nitrogen monoxide into nitrogen dioxide is that a treatment catalyst is required when both nitrogen monoxide and nitrogen dioxide are present at the same time. In addition, since NO is difficult to process, nitrogen monoxide is reacted with ozone to convert to nitrogen dioxide first. This is because it is advantageous to treat nitrogen dioxide with a catalyst.
기존에 존재하던 이산화질소(NO2)와 상기 반응 (2)에서 생성된 이산화질소는 망간촉매 하에서 환원제 없이 상온에서 분해가 가능하다. 그 반응식은 다음 식 (3)과 같다.Existing nitrogen dioxide (NO 2 ) and nitrogen dioxide produced in the reaction (2) can be decomposed at room temperature without a reducing agent under a manganese catalyst. The reaction formula is shown in the following formula (3).
NO2 → 1/2 N2 + O2 ------------------------ (3)NO 2 → 1/2 N 2 + O 2 ------------------------ (3)
이 때 과량으로 투입된 오존은 망간촉매에 의해 분해된다.At this time, the excess ozone is decomposed by manganese catalyst.
O3 → 3/2 O2 ------------------------------ (4)O 3 → 3/2 O 2 ------------------------------ (4)
이와 같이 오존처리된 망간촉매를 이용하여 질소산화물(NOx)을 완전하게 처리할 수 있다.The ozone-treated manganese catalyst can be used to completely treat nitrogen oxides (NOx).
상기 반응들은 재래식 방법에서 질소 산화물이 적어도 150℃ 이상에서 처리되지만 본 발명에서는 상온에서도 질소 산화물을 99%이상 처리할 수 있는 특징을 나타내고 있다. The reactions are characterized in that the nitrogen oxide is treated at least 150 ℃ or more in the conventional method, but in the present invention can process more than 99% nitrogen oxide even at room temperature.
다음은 본 발명의 장치를 실시예인 도면을 참조하여 설명한다.The following describes the apparatus of the present invention with reference to the accompanying drawings.
도 1은 본 발명 장치의 모식도이다.1 is a schematic view of the apparatus of the present invention.
본 발명의 장치는 질소산화물이 유입되는 유입구(10)와 유입구와 연통되도록 설치되는 오존반응챔버(20)와 그 오존반응챔버(20)에 오존을 주입할 수 있도록 연통된 오존발생원(30)과 산화망간계 촉매체(40)를 저장하며 상기 오존반응챔버(20)와 연통되는 챔버(50)로 이루어져 있다.The apparatus of the present invention includes an ozone generating source 30 in communication with the ozone reaction chamber 20 and the ozone reaction chamber 20 installed so as to communicate with the inlet 10 and the inlet 10 through which nitrogen oxide is introduced. The chamber 50 stores the manganese oxide catalyst body 40 and communicates with the ozone reaction chamber 20.
또한, 배출구(70) 측에 팬(60)을 설치하여 질소산화물이 제거된 청정공기를 흡입하여 배출하도록 하는 것도 가능하다. In addition, it is also possible to install a fan 60 on the outlet 70 side to inhale and discharge the clean air from which the nitrogen oxide has been removed.
이 때 챔버(50) 내의 산화망간계 촉매체(40)는 과망간산칼륨 수용액에 담체를 함침시키고, 상기 함침된 담체를 상기 수용액으로부터 분리하여 건조시킨 후 상기 건조된 담체를 소성하여 얻어지는 촉매체이다. 또한, 상기 과망간산칼륨 수용액에 구리, 아연, 은, 크롬, 란타늄, 세륨, 네오듐 중에서 선택된 어느 하나 이상의 금속의 질산염을 더 첨가하여 얻어지는 촉매체를 포함한다.At this time, the manganese oxide catalyst body 40 in the chamber 50 is a catalyst body obtained by impregnating a carrier in an aqueous solution of potassium permanganate, separating the impregnated carrier from the aqueous solution and drying the calcined carrier. In addition, a catalyst body obtained by further adding a nitrate of any one or more metals selected from copper, zinc, silver, chromium, lanthanum, cerium, and neodium to the aqueous potassium permanganate solution.
또한, 상기 오존발생원(30)은 자외선램프, 무성방전, 프라즈마 중에서 어느 하나를 선택하여 사용할 수 있다.In addition, the ozone generating source 30 may be used by selecting any one of the ultraviolet lamp, silent discharge, plasma.
산화망간 촉매층을 통과한 공기를 질량분석계, 검지관 등으로 NO, NO2, N2O의 배출농도를 측정한 결과, NOx의 처리 효율이 99%이상임을 확인하였다.As a result of measuring the concentration of NO, NO 2 and N 2 O through the mass spectrometer and detector tube, the air passing through the manganese oxide catalyst layer was found to be 99% or more.
이하, 본 발명의 장치와 방법에 대한 실시예를 설명한다.Hereinafter, examples of the apparatus and method of the present invention will be described.
[실시예]EXAMPLE
오존반응챔버(20)에 0.2g/min로 발생하는 오존발생원(30)으로부터 오존을 공급하고, 0.05%의 NO와 0.05%의 NO2와 나머지는 공기로 이루어지는 혼합가스를 유입구(10)로부터 주입하였다. 이 혼합가스를 산화망간촉매체(40)가 저장된 챔버(50)를 통과시켰으며 다음 후단에서 팬으로 공기를 흡입하여 배출하였다. 이 때 팬의 공기흡입량은 10m3/min로 고정하였다.Ozone is supplied to the ozone reaction chamber 20 from the ozone generating source 30 generated at 0.2 g / min, and a mixed gas composed of 0.05% NO, 0.05% NO 2 and the rest of the air is introduced from the inlet 10. It was. The mixed gas was passed through the chamber 50 in which the manganese oxide catalyst 40 was stored, and the air was sucked into the fan at the next stage and discharged. At this time, the air intake of the fan was fixed at 10 m 3 / min.
배출되는 공기내에서 오존, NO, NO2, N2O를 질량분석계(Mass spectrometer) 및 기체크로마토그래프(Gas Chromatograph)를 사용하여 분석하였으며, 이때에 NO농도는 검출되지 않았으며, N2O가 0.01ppm이하 NO2가 0.01ppm이하로 검출되어 질소산화물의 제거효율이 99%이상이었다.Ozone, NO, NO 2 and N 2 O in the exhaust air were analyzed by mass spectrometer and gas chromatograph. At this time, NO concentration was not detected and N 2 O was is less than 0.01ppm NO 2 are detected as less than 0.01ppm removal efficiency of nitrogen oxides was 99% or more.
이상에서는 본 발명의 바람직한 실시예에 관하여 설명하였으나, 이하 청구범위에서 청구하는 본 발명의 요지를 벗어나지 않고 당해 발명의 분야에서 통상의 지식을 가진 자라면 누구든지 다양한 변형실시가 가능함을 물론이며 이와 같은 변형은 청구범위의 기재 내에 있게 된다. In the above description of the preferred embodiment of the present invention, any one of ordinary skill in the art without departing from the gist of the present invention as claimed in the claims can be variously modified as well as such Modifications are intended to be within the scope of the claims.
이상에서 설명한 바와 같이 산화망간의 입자가 미세하고 균일하게 분포된 촉매상에 오존을 주입하여 질소산화물을 99%이상 처리할 수 있는 효율을 나타냄으로써 고온에서 작동하는 암모니아, 우레아 등의 환원제 주입에 의한 질소산화물 처리보다 처리효율이 높으며, 시설이 장치가 간단하여 경제적이며 효율적인 질소산화물 처리방법을 제공하는 효과가 있다.As described above, by injecting ozone onto a catalyst in which particles of manganese oxide are finely and uniformly distributed, the nitrogen oxide can be treated by 99% or more. The treatment efficiency is higher than nitrogen oxide treatment, and the facility has the effect of providing a simple and economical nitrogen oxide treatment method.
또한 본 발명은 고정원 발생의 질소산화물 처리뿐만 아니라 이동원 발생원인 자동차 배기가스에도 적용할 수 있어 그 사용범위가 넓다는 장점이 있다. In addition, the present invention has the advantage that it can be applied not only to the treatment of nitrogen oxide in the generation of the fixed source, but also to the automobile exhaust gas which is the moving source generating source.
도1은 본 발명 장치의 구조를 나타내는 모식도이다.1 is a schematic diagram showing the structure of the apparatus of the present invention.
♣도면의 주요부분에 대한 부호의 설명♣♣ Explanation of symbols for main part of drawing ♣
10 : 유입구 20 : 오존반응 챔버10: inlet 20: ozone reaction chamber
30 : 오존발생원 40 : 산화망간계 촉매체30: ozone generating source 40: manganese oxide catalyst
50 : 챔버 60 : 팬50: chamber 60: fan
70 : 배출구 70 outlet
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| KR100746704B1 (en) | 2006-09-14 | 2007-08-06 | 한국에너지기술연구원 | Manufacture of reacting media with carbon support impregrated metal catalyst and removing of nox using its media |
| US11441464B2 (en) | 2021-02-02 | 2022-09-13 | Saudi Arabian Oil Company | Use of ozone with LNT and MnO2 catalyst for the treatment of residual pollutant for the exhaust gas of an internal engine combustion |
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| KR101094672B1 (en) | 2009-03-17 | 2011-12-20 | 한국과학기술연구원 | Method and apparatus for the treatment of nitrogen oxides using an ozone and catalyst hybrid system |
| KR20200137216A (en) | 2019-05-29 | 2020-12-09 | 주식회사 퓨어스피어 | Adsorbents for Removing Acid Gases and Preparing Method Thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| KR100746704B1 (en) | 2006-09-14 | 2007-08-06 | 한국에너지기술연구원 | Manufacture of reacting media with carbon support impregrated metal catalyst and removing of nox using its media |
| US11441464B2 (en) | 2021-02-02 | 2022-09-13 | Saudi Arabian Oil Company | Use of ozone with LNT and MnO2 catalyst for the treatment of residual pollutant for the exhaust gas of an internal engine combustion |
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