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Received December 13, 2010
Accepted January 14, 2011
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AMnAl11O19(A=La, Sr, Ba) 및 CeO2/LaMnAl11O19를 이용한 메탄의 촉매 연소

Catalytic Combustion of Methane over AMnAl11O19(A=La, Sr, Ba) and CeO2/LaMnAl11O19

고려대학교 화공생명공학과, 136-791 서울시 성북구 안암동 5가 1SK에너지 기술원, 305-712 대전시 유성구 원촌동 140-1 2고려대학교 청정화공시스템연구소, 136-791 서울시 성북구 안암동 5가
Department of Chemical & Biological Engineering, Korea University, 5-ga, Anam-dong, Seongbuk-gu, Seoul 136-713, Korea 1Corporate R&D Center, SK Energy Instituted of Technology, 140-1, Wonchon-dong, Yuseong-gu, Daejeon 305-712, Korea 2Research Institute of Clean Chemical Engineering Systems, Korea University, 5-ga, Anam-dong, Seongbuk-gu, Seoul 136-713, Korea
Korean Chemical Engineering Research, October 2011, 49(5), 633-638(6), NONE Epub 30 September 2011
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Abstract

Mn이 치환된 헥사알루미네이트 촉매인 LaMnAl11O19, BaMnAl11O19, SrMnAl11O19을 (NH4)2CO3 공침법을 이용하여, 1,200 ℃ 5시간 소성을 통해 제조하였다. X-선 회절, 질소흡착을 통해 촉매의 결정구조와 비표면적을 분석한 결과, 결정 격자 내 거울면에 La이 존재하는 LaMnAl11O19이 BaMnAl11O19과 SrMnAl11O19보다 우수한 헥사알루미네이트 결정 구조를 가지는 동시에 13 m2/g의 높은 비표면적을 가지고 있었다. 또한 SEM 분석을 통해 LaMnAl11O19이 특유의 판상구조가 잘 발달함을 확인하였다. 메탄 연소 활성은 다음과 같은 차례로 증가하였고: LaMnAl11O19 > SrMnAl11O19 > BaMnAl11O19. 메탄 연소 활성은 비표면적에 의존하였다. LaMnAl11O19에 60 wt%의 CeO2를 첨가하고 700 ℃의 저온에서 소성한 경우 700 ℃의 저온에서 100% 전환율에 도달함으로써 ceria 첨가에 의한 메탄 연소 개선 효과를 확인할 수 있었으며, 이 촉매가 저온 및 중온 영역의 메탄 연소 촉매로 활용될 수 있음을 확인하였다. 그러나, 이 촉매의 경우 1,200 ℃의 고온에서 5시간 소성한 후에는 ceria입자 크기의 증가로 인해 메탄의 연소 활성 개선 효과를 잃게됨으로 고온용 연소 촉매로서의 사용은 한계가 있음을 확인하였다.
Mn substituted La, Sr or Ba- hexaaluminate were prepared by (NH4)2CO3 co-precipitate method and calcined at 1,200 ℃ for 5 h. Catalysts were characterized by X-ray diffraction and N2 physisorption and scanning electron microscope (SEM). Compared to SrMnAl11O19 and BaMnAl11O19, LaMnAl11O19 in which La located at mirror plane showed better crystallinity and high surface area, 13 m2/g. LaMnAl11O19 revealed well developed plate-like structure which is characteristic structure of hexaaluminate. The catalytic activity of methane combustion increased in the following order: LaMnAl11O19 > SrMnAl11O19 > BaMnAl11O19 and was dependent on surface area of catalysts. 60 wt% CeO2/LaMnAl11O19 calcined at 700 ℃ showed enhanced methane activity and methane was oxidized completely at low temperature (700 ℃). It was confirmed that addition of ceria seems to be effective for the low and middle temperature combustion of methane. But, after calcination at high temperature of 1,200 ℃, it lost the promoting effect of ceria due to increase of ceria particle size and it had a limit to applying to the high temperature catalytic combustion.

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