KR960010900B1 - Method for producing catalyst for exhaust gas purification - Google Patents

Method for producing catalyst for exhaust gas purification Download PDF

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KR960010900B1
KR960010900B1 KR1019930001693A KR930001693A KR960010900B1 KR 960010900 B1 KR960010900 B1 KR 960010900B1 KR 1019930001693 A KR1019930001693 A KR 1019930001693A KR 930001693 A KR930001693 A KR 930001693A KR 960010900 B1 KR960010900 B1 KR 960010900B1
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catalyst
ceo
weight
zro
gas purification
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박명석
김명수
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구자홍
엘지전자주식회사
정형한
한국엥겔하드주식회사
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Abstract

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Description

배기가스 정화용 촉매의 제조방법Method for producing catalyst for exhaust gas purification

제1도는 배기가스의 산화반응을 나타낸 상태의 흐름도.1 is a flowchart showing a state of oxidation of exhaust gas.

제2도는 종래의 담체위에 촉매 형태를 나타낸 상태도로서,2 is a state diagram showing the form of a catalyst on a conventional carrier,

(a)도는 하니컴(Honey-comb)형 세라믹 촉매 상태도.(a) is a honey-comb type ceramic catalyst state diagram.

(b)도는 (a)도의 점선부분을 확대한 단면도.(b) is sectional drawing which expanded the dotted line part of (a) figure.

제3도는 종래의 위쉬코트 슬러리 제조공정도.3 is a conventional process for preparing a wish coat slurry.

제4도는 본 발명의 위쉬코트 슬러리 제조공정도.Figure 4 is a process for producing a wish coat slurry of the present invention.

제5도는 촉매의 내열화 가스 정화특성을 나타낸 그래프.5 is a graph showing the purification characteristics of the heat-resistant gas of the catalyst.

제6도는 촉매의 경시변화 가스 정화특성을 나타낸 그래프.6 is a graph showing the gas purification characteristics of the catalyst over time.

본 발명은 각종 연소기기의 배기가스 정화용 촉매에 관한 것으로, 특히 위쉬코트 재료에 CeO2, ZrO2-CeO2를 혼합함으로서 고온에서의 내열안정성을 도모함은 물론 비표면적이 감소되지 않고 촉매의 확산에 의한 소결을 방지함으로서 가스정화성능 열화가 일어나지 않는데 적합한 배기가스 정화용 촉매의 제조방법에 관한 것이다.The present invention relates to a catalyst for purifying exhaust gases of various combustion apparatuses. In particular, by mixing CeO 2 and ZrO 2 -CeO 2 in a wish coat material, the thermal stability at high temperatures is not only reduced, but also the specific surface area is not reduced and the catalyst is diffused. The present invention relates to a method for producing an exhaust gas purification catalyst suitable for preventing deterioration of gas purification performance by preventing sintering.

일반적으로 석유연소기기 사용시 배출되는 불안전 연소에 따른 유해 및 냄새성분(CO, HC)는 제1도에 도시한 바와 같이 공기중 O2와 반응하여 CO2와 H2O로 산화분해된다.In general, as shown in FIG. 1, harmful and odorous components (CO, HC) caused by unsafe combustion emitted from petroleum combustion equipment are oxidized to CO 2 and H 2 O by reacting with O 2 in air.

이와 같은 유해 및 냄새성분가스는 점화 및 소화시에 가장 많이 배출되는데, 이련 유해가스를 제거하는 산화반응은 촉매를 사용하지 않은 상태에서는 고온(약 1,000℃)에서 가능하지만, 촉매를 사용할 경우는 실제 석유연소기기의 점화, 연소시의 배기가스 배출온도인 비교적 저온(약 200℃)에서 산화반응이 활성화되어 가스(CO, HC)가 제거된다.Such toxic and odorous component gases are most emitted during ignition and extinguishing. Oxidation reactions to remove the harmful toxic gases are possible at high temperatures (about 1,000 ° C) without using a catalyst. Oxidation reaction is activated at relatively low temperature (about 200 ° C), which is the exhaust gas discharge temperature during ignition and combustion of petroleum combustion equipment, to remove gases (CO, HC).

이와 같이 CO2와 H2O로로 완전산화시키는 촉매는 MgO, SiO2, Al2O3의 분말을 성형, 소형하여 만든 제2도의 (a)와 같은 세라믹 하니컴 담체(cordierite : 2MgO. 2Al2O3, 5SiO2) 위에 (b)도와 같은 귀금속(Pd, Pt) 등을 담지시키는 것이 일반적이다.The catalyst which completely oxidizes to CO 2 and H 2 O is a ceramic honeycomb carrier (cordierite: 2MgO. 2Al 2 O 3 , 5SiO 2 ) as shown in FIG. 2 (a) formed by molding and compacting MgO, SiO 2 , and Al 2 O 3 powder. ) It is common to support precious metals (Pd, Pt) and the like (b) above.

또한 최근에는 귀금속 대신에 ABO3로 표현되는(여기에서 A는 La, Ce 등의 회토류금속, 또는 Mg, Ca 등의 알카리 토류금속, B는 Co, Mn 등의 천이금속) 페로프스카이트 복합 산화물에 귀금속을 소량 담지한 것을 담체에 담지하고 있다.Also recently, ABO 3 instead of precious metals (where A is a rare earth metal such as La, Ce, or alkaline earth metals such as Mg, Ca, and B is a transition metal such as Co, Mn) perovskite complex A small amount of precious metal supported on the oxide is supported on the carrier.

상기한 두 방법의 촉매물질의 담지는 비표면적을 넓혀 촉매의 담지성을 높이고 분산성을 좋게하기 위해 γ-Al2O3로 워쉬코트 슬러리(wash coat slurry)를 만들고, 위쉬코트층 내부에 촉매를 담지하여 코디어라이트(cordierite) 담체 위에 워쉬코트 슬러리를 코팅한다.In order to increase the specific surface area of the catalyst materials of the two methods described above, the catalyst is supported and a wash coat slurry is made of γ-Al 2 O 3 to improve the dispersibility. The washcoat slurry is coated on a cordierite carrier by carrying a.

제3도는 상기한 워쉬코트 슬러리 제조를 나타낸 공정도로서, γ-Al2O3(비교적 : 150m2/g)와 귀금속(Pd, Pt) 촉매 또는 페로프스카이트 복합산화물에 귀금속 담지한 것을 혼합하여 촉매를 함침하고 평균입경이 10∼15μ이 되게 밀링(Milling)하여 위쉬코트 슬러리를 얻게 된다.Figure 3 is a process chart showing the washcoat slurry described above, γ-Al 2 O 3 (comparative: 150m2 / g) and a noble metal (Pd, Pt) catalyst or a mixture of the precious metal supported on the perovskite composite oxide catalyst Impregnated and milled to an average particle diameter of 10 to 15 μm to obtain a wish coat slurry.

이렇게 하여 얻어진 워쉬코트 슬러리를 담체에 코팅하게 된다.The washcoat slurry thus obtained is coated on the carrier.

그러나 실제 유해 및 냄새성분가스를 배출하는 점화 및 소화시에는 200℃ 정도의 저온이지만 연소시에는 1000℃γ 정도의 고온에 이르러 촉매체의 위쉬코트된 -Al2O3가α-Al2O3로 상변태하여 비표면적이 줄고(γ-Al2O3150m2/g, α-Al2O33∼5m2/g), 균일분산되어 있던 귀금속 촉매가 확산(diffusion)에 의해 소결(sintering)되어 큰 입자 성산을 이름으로서 상능 열화가 일어나는 문제점이 있다.However, in case of ignition and extinguishing, which emits harmful and odorous gas, the low temperature of about 200 ℃ but the high temperature of about 1000 ℃ γ causes combustion of the catalyst coated -Al 2 O 3 to α-Al 2 O 3 Phase transformation to reduce specific surface area (γ-Al 2 O 3 150m2 / g, α-Al 2 O 3 3 to 5m2 / g), and the uniformly dispersed noble metal catalyst is sintered by diffusion There is a problem in that deterioration of performance occurs under the name of particulate acid.

이에 본 발명은 상기한 문제점을 해결하기 위해 안출한 것으로, 워쉬코트 재료인 γ-Al2O3에 CeO2, ZrO2-CeO2를 혼합한 워쉬코트 슬러리를 이용함으로서 고온에서의 내열안정성을 비롯한 비표면적이 감소되지 않고, 촉매의 확산에 의한 소결을 방지하여 성능 열화가 일어나지 않는 배기가스 정화용 촉매를 제공하고자 하는데 목적이 있다.Accordingly, the present invention has been made to solve the above problems, by using a washcoat slurry of CeO 2 , ZrO 2 -CeO 2 mixed with γ-Al 2 O 3 which is a washcoat material, including thermal stability at high temperature It is an object of the present invention to provide a catalyst for purifying exhaust gases in which the specific surface area is not reduced and the sintering caused by diffusion of the catalyst is prevented so that performance deterioration does not occur.

이하 본 발명을 설명한다.Hereinafter, the present invention will be described.

본 발명은 코디어라이트(cordierite : 2MgO, 2Al2O3, 5SiO2) 담체 위에귀금속(Pd, Pt) 또는 페로프스카이트(perovskite) 복합산화물(Pd, Pt) 성분을 담지한 워쉬코트 슬러리(wash coat slurry)를 코팅하는 것에 있어서, γ-Al2O3에 CeO2및 ZrO2-CeO2혼합물을 첨가한 워쉬코트 슬러리로 함을 특징으로 하는 연소기기의 배기가스 정화용 촉매 재조방법으로 이루어진다.The present invention is a washcoat slurry supporting a precious metal (Pd, Pt) or a perovskite composite oxide (Pd, Pt) component on a cordierite (cordierite: 2MgO, 2Al 2 O 3 , 5SiO 2 ) carrier ( In the coating of the wash coat slurry), a method of preparing a catalyst for purifying exhaust gas of a combustion apparatus, characterized in that the washcoat slurry is added with a mixture of CeO 2 and ZrO 2 -CeO 2 to γ-Al 2 O 3 .

상기한 워쉬코트 슬러리 재료는 γ-Al2O3100중량부에 대하여 CeO2가 25∼35중량부이고, ZrO2-CeO2가 15∼30중량부 첨가하에서 된 것으로, ZrO2-CeO2혼합물중에는 ZrO2가 70∼90중량%이고, CeO가 30∼10중량% 비율로 한 것을 γ-Al2O3 100증량부에 대하여 15∼30중량부 첨가한 것이다.The washcoat slurry material is 25 to 35 parts by weight of CeO 2 and 15 to 30 parts by weight of ZrO 2 -CeO 2 with respect to 100 parts by weight of γ-Al 2 O 3 , and a ZrO 2 -CeO 2 mixture. Among them, 15 to 30 parts by weight of ZrO2 and 70 to 90% by weight of CeO were added to 100 parts by weight of γ-Al2O3.

제4도는 본 발명의 워쉬코트 슬러리 제조구성도로서 이에 따라 구체적으로 설명한다.Figure 4 is a washcoat slurry production configuration of the present invention will be described in detail accordingly.

워쉬코트 재료인 γ-Al2O3에 분말상태인 귀금속(Pd, Pt 등 ) 촉매 또는 페로프스카이트 복합산화물에 귀금속 촉매를 담지한 것을 혼합하여 촉매를 함침하고 평균 10∼15μ 정도로 1차 밀링(Milling) 한 후, γ-Al2O3에 대하여 CeO2(상온에서 비표면적이 약 170m2/g)를 25∼35중량부, ZrO2-CeO2(ZrO2 : 70∼90중량%, CeO2: 30∼10중량%)를 15∼30중량부 첨가하여 평균입경이 4∼10μ까지 2차 밀링한다.Γ-Al 2 O 3 , a washcoat material, mixed with a precious metal catalyst (Pd, Pt, etc.) or a perovskite composite oxide loaded with a precious metal catalyst was impregnated with the catalyst, and milled first to an average of 10 to 15 μ. (Milling) after, γ-Al 2 O 3 with respect to the CeO2 25~35 parts by weight of the (a specific surface area of at room temperature of about 170m2 / g), ZrO 2 -CeO 2 (ZrO2: 70~90% by weight, CeO 2: 30 to 10% by weight) is added to 15 to 30 parts by weight, and secondary milling is carried out to an average particle diameter of 4 to 10 mu.

그리고 PH를 5∼6 정도 맞추고 점도는 400∼500cps로 조절한다.Adjust the pH to 5-6 and adjust the viscosity to 400-500 cps.

이렇게 함으로서 담체에 코팅될 워쉬코트 슬러리가 완성된다.This completes the washcoat slurry to be coated on the carrier.

(표 1)은 비표면적 변화특성을 나타낸 것으로, 본 발명이 종래에 비해 중진된 비표면적으로 나타났다Table 1 shows the specific surface area change characteristics, and the present invention showed a specific surface area which is more advanced than in the prior art.

제5도는 전기로에서 1000℃, 100Hr 열처리 한 후 촉매의 가스 정화성능 실험을 한 결과로서 이때 시험 조건은 SV=40,000(h-1), CO 농도는 120±10PPm으로 하였다.5 is a result of gas purification performance of the catalyst after the heat treatment at 1000 ℃, 100Hr in an electric furnace, the test conditions were SV = 40,000 (h-1), CO concentration was 120 ± 10ppm.

이와 같은 시험조건에서 600℃를 기준하여 CO가스 정화성능(%)를 비교한 바, 본 발명이나 종래의 경우 초기 CO가스 정화율은 공히 95%로서 차이가 없었으나, 상기 열처리 후 본 발명은 90%인데 반해 종래의 경우는 약 55%로서, 본 발명의 경우는 성능 열화가 거의 없으나 종래는 성능 열화가 심한 현상을 나타내었다.Compared to the CO gas purification performance (%) based on 600 ℃ under such test conditions, the initial CO gas purification rate in the present invention or in the prior art was no difference as 95%, the present invention after the heat treatment 90 In contrast to the%, the conventional case is about 55%. In the present invention, there is almost no performance deterioration, but the conventional art shows a severe performance deterioration.

또한 제6도는 실제 석유 연소기기에 본 발명의 워쉬코트 슬러리를 코팅한 촉매를 장착하여 연소기기의 작용시간별 촉매의 가스정화 특성의 경시변화를 실험한 결과로서, 이때 시험조건인 SV=40,000(h-1), CO 농도 120±10PPm, HC(C3H8)농도 : 1000PPm, 온도 : 600℃ 하에서 2000시간 경과후 CO 및 HC의 가스 정화율 특성은 초기성능(종래 및 본 발명 공히 CO 및 HC 정화율은 각각 95%와 85%) 대비하여 종래의 것은 CO 및 HC의 정화율이 각각 50%와 30%로 성능열화가 심한 반면 본 발명은 각각 90%와 80%로서 성능열화가 거의 없었다.In addition, Figure 6 is a test result of the time-dependent change in the gas purification characteristics of the catalyst according to the operating time of the combustion apparatus equipped with a catalyst coated with the washcoat slurry of the present invention in the actual petroleum combustion equipment, SV = 40,000 (h -1), CO concentration 120 ± 10PPm, HC (C3H8) concentration: 1000PPm, temperature: after 2000 hours under 600 ℃, the gas purification rate characteristics of CO and HC are initial performance (both CO and HC purification rate Compared to 95% and 85%, respectively, the conventional ones have a severe performance deterioration of 50% and 30% of CO and HC, respectively, while the present invention has almost no performance deterioration as 90% and 80%, respectively.

이상에서와 같이 조성된 본 발명의 워쉬코트 슬러리를 이용함에 따라 고온에서의 내열안정성을 도모함은 물론 비표면적이 감소되지 않고 촉매의 확산에 의한 소결이 방지됨으로서 성능약화가 일어나지 않는 배기가스 정화용 촉매를 얻게 된다.By using the washcoat slurry of the present invention as described above, the catalyst for exhaust gas purification which does not reduce performance by achieving thermal stability at high temperature and of not reducing specific surface area and preventing sintering by diffusion of the catalyst. You get

Claims (3)

코디어라이트(cordierite : 2MgO. 2Al2O3, 5SiO2) 담체 위에 워쉬코트(γ-Al|2O3)에 귀금속(Pd, Pt) 또는 페로프스카이트(Perovskite) 복합산화물에 귀금속(Pd, Pt) 성분을 담지한 워쉬코트 슬러리(Wash coat slurry)를 코팅하는 것에 있어서, γ-Al2O3에 CeO2와 ZrO2-CeO2의 혼합물을 첨가한 워쉬코트 슬러리로 함을 특징으로 하는 연소기기의 배기가스 정화용 촉매의 제조방법.Precious metals (Pd, Pt) or perovskite composite oxides in washcoat (γ-Al | 2 O 3 ) on cordierite (cordierite: 2MgO. 2Al 2 O 3 , 5SiO 2 ) carrier , In coating a wash coat slurry carrying a Pt) component, comprising a washcoat slurry obtained by adding a mixture of CeO 2 and ZrO 2 -CeO 2 to γ-Al 2 O 3 . A method for producing a catalyst for purifying exhaust gas of a combustion device. 제1항에 있어서, γ-Al2O3100중량부에 대하여 CeO2가 25∼35중량부, ZrO2-CeO2가 15∼30중량부 첨가한 것을 특징으로 한는 연소기기의 배기가스 정화용 촉매의 제조방법.The catalyst for purifying exhaust gases of a combustion apparatus according to claim 1, wherein 25 to 35 parts by weight of CeO 2 and 15 to 30 parts by weight of ZrO 2 -CeO 2 are added to 100 parts by weight of γ-Al 2 O 3. Manufacturing method. 제2항에 있어서, ZrO2-CeO2혼합물 중 ZrO2가 70∼90중량%, CeO2가 30∼10중량% 비율로 혼합되어 이루어짐을 특징으로 하는 연소기기의 배기가스 정화용 촉매의 제조방법.The method according to claim 2, wherein ZrO 2 is mixed in an amount of 70 to 90% by weight and CeO 2 is in an amount of 30 to 10% by weight in the ZrO 2 -CeO 2 mixture.
KR1019930001693A 1993-02-08 1993-02-08 Method for producing catalyst for exhaust gas purification Expired - Fee Related KR960010900B1 (en)

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KR1019930001693A KR960010900B1 (en) 1993-02-08 1993-02-08 Method for producing catalyst for exhaust gas purification
CN 94101583 CN1092697A (en) 1993-02-08 1994-02-08 The preparation method of exhaust gas purifying catalyst
JP6035296A JP2625640B2 (en) 1993-02-08 1994-02-08 Method for producing exhaust gas purifying catalyst

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