Korean Chemical Engineering Research

The Korean Institute of Chemical Engineers (한국화학공학회)
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Catalytic Combustion of Methane over $AMnAl_{11}O_{19}$(A=La, Sr, Ba) and $CeO_2/LaAMnAl_{11}O_{19}$

$AMnAl_{11}O_{19}$(A=La, Sr, Ba) 및 $CeO_2/LaAMnAl_{11}O_{19}$를 이용한 메탄의 촉매 연소

  • Kim, Seongmin (Department of Chemical & Biological Engineering, Korea University) ;
  • Lee, Joon Yeob (Department of Chemical & Biological Engineering, Korea University) ;
  • Cho, In-Ho (Corporate R&D Center, SK Energy Instituted of Technology) ;
  • Lee, Dae-Won (Research Institute of Clean Chemical Engineering Systems, Korea University) ;
  • Lee, Kwan-Young (Department of Chemical & Biological Engineering, Korea University)
  • 김성민 (고려대학교 화공생명공학과) ;
  • 이준엽 (고려대학교 화공생명공학과) ;
  • 조인호 (SK에너지 기술원) ;
  • 이대원 (고려대학교 청정화공시스템연구소) ;
  • 이관영 (고려대학교 화공생명공학과)
  • Published : 2011.10.01
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Abstract

Mn substituted La, Sr or Ba-hexaaluminate were prepared by $(NH_4)_2CO_3$ co-precipitate method and calcined at $1,200^{\circ}C$ for 5 h. Catalysts were characterized by X-ray diffraction and $N_2$ physisorption and scanning electron microscope (SEM). Compared to $SrMnAl_{11}O_{19}$ and $BaMnAl_{11}O_{19}$, $LaMnAl_{11}O_{19}$ in which La located at mirror plane showed better crystallinity and high surface area, 13 $m^2/g$. $LaMnAl_{11}O_{19}$ revealed well developed plate-like structure which is characteristic structure of hexaaluminate. The catalytic activity of methane combustion increased in the following order: $LaMnAl_{11}O_{19}$ > $SrMnAl_{11}O_{19}$ > $BaMnAl_{11}O_{19}$ and was dependent on surface area of catalysts. 60 wt% $CeO_2/LaMnAl_{11}O_{19}$ calcined at $700^{\circ}C$ showed enhanced methane activity and methane was oxidized completely at low temperature ($700^{\circ}C$). 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 $1,200^{\circ}C$, 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.

Mn이 치환된 헥사알루미네이트 촉매인 $LaMnAl_{11}O_{19}$, $BaMnAl_{11}O_{19}$, $SrMnAl_{11}O_{19}$을 $(NH_4)_2CO_3$ 공침법을 이용하여, $1,200^{\circ}C$ 5시간 소성을 통해 제조하였다. X-선 회절, 질소흡착을 통해 촉매의 결정구조와 비표면적을 분석한 결과, 결정 격자 내 거울면에 La이 존재하는 $LaMnAl_{11}O_{19}$이 $BaMnAl_{11}O_{19}$과 $SrMnAl_{11}O_{19}$보다 우수한 헥사알루미네이트 결정 구조를 가지는 동시에 13 $m^2/g$의 높은 비표면적을 가지고 있었다. 또한 SEM 분석을 통해 $LaMnAl_{11}O_{19}$이 특유의 판상구조가 잘 발달함을 확인하였다. 메탄 연소 활성은 다음과 같은 차례로 증가하였고: $LaMnAl_{11}O_{19}$ > $SrMnAl_{11}O_{19}$ > $BaMnAl_{11}O_{19}$. 메탄 연소 활성은 비표면적에 의존하였다. $LaMnAl_{11}O_{19}$에 60 wt%의 $CeO_2$를 첨가하고 $700^{\circ}C$의 저온에서 소성한 경우 $700^{\circ}C$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 $1,200^{\circ}C$의 고온에서 5시간 소성한 후에는 ceria입자 크기의 증가로 인해 메탄의 연소 활성 개선 효과를 잃게됨으로 고온용 연소 촉매로서의 사용은 한계가 있음을 확인하였다.

Keywords

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