Korean Chemical Engineering Research

The Korean Institute of Chemical Engineers (한국화학공학회)
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Catalyst Carriers Preparation and Investigation of Catalytic Activities for Partial Oxidation of Methane to Hydrogen over Ru Impregnated on SPK and SPM Catalysts

메탄의 부분산화반응으로부터 수소제조를 위한 촉매담체(SPK, SPM) 제조 및 Ru 담지 촉매의 활성도 조사

  • Seo, Ho Joon (Division of Biotechnology and Chemical Engineering, Chonnam National University) ;
  • Fan, Shijian (Division of Biotechnology and Chemical Engineering, Chonnam National University) ;
  • Kim, Yong Sung (Division of Biotechnology and Chemical Engineering, Chonnam National University) ;
  • Jung, Do Sung (Faculty of Applied Chemical Engineering, Chonnam National University) ;
  • Kang, Ung Il (Faculty of Applied Chemical Engineering, Chonnam National University) ;
  • Cho, Yeong Bok (Faculty of Applied Chemical Engineering, Chonnam National University) ;
  • Kim, Sang Chai (Department of Environmental Education, Mokpo National University) ;
  • Kwon, Oh-Yun (Division of Biotechnology and Chemical Engineering, Chonnam National University) ;
  • Sunwoo, Chang Shin (School of Biological Sciences and Technology, Chonnam National University) ;
  • Yu, Eui Yeon (Faculty of Applied Chemical Engineering, Chonnam National University)
  • 서호준 (전남대학교 생명화학공학부) ;
  • 번세검 (전남대학교 생명화학공학부) ;
  • 김용성 (전남대학교 생명화학공학부) ;
  • 정도성 (전남대학교 응용화학공학부) ;
  • 강웅일 (전남대학교 응용화학공학부) ;
  • 조영복 (전남대학교 응용화학공학부) ;
  • 김상채 (목포대학교 환경교육과) ;
  • 권오윤 (전남대학교 생명화학공학부) ;
  • 선우창신 (전남대학교 생명과학기술학부) ;
  • 유의연 (전남대학교 응용화학공학부)
  • Received : 2007.12.03
  • Accepted : 2008.03.03
  • Published : 2008.06.30
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Abstract

The catalyst carriers of the mesoporous layer compounds were prepared to carry out the partial oxidation of methane(POM) to hydrogen. The catalytic activities of POM to hydrogen were investigated over Ru(3)/SPK and Ru(3)/SPM catalyst in a fixed bed flow reactor under atmosphere. In addition, the catalysts and carriers were characterized by BET, TEM, TPR. The BET surface areas of the silica-pillared $H^+-kenyaite$(SPK) and the silica-pillared $H^+-magadite$(SPM) were $760m^2/g$ and $810m^2/g$, repectively, and the average pore sizes were 3.0 nm and 2.6 nm, repectively. The nitrogen adsorption isotherms were type IV with developed hysteresis. The TEM showed that the mesoporous layer compounds were formed well. The Ru(3)/SPK and the Ru(3)/SPM catalyst were obtained high hydrogen yields(90%, 87%), and were kept constant high hydrogen yields even about 60 hours at 973 K, $CH_4/O_2=2$, $1.25{\times}10^{-5}g-Cat.hr/ml$. The TPR peaks of Ru(3)/SPK and the Ru(3)/SPM catalyst showed the similar reducibilities around 453 K and 413 K. It could be suggested that SPK and SPM had the physicochemical properties as oxidation catalyst carries from these analysis data.

중기공성 층상화합물의 촉매 담체를 제조하고, 메탄으로부터 수소를 제조하기 위한 활성도를 평가하기 위해서 고정층 상압 유통식 반응기를 사용하여 Ru(3)/SPK와 Ru(3)/SPM 촉매상에서 메탄의 부분산화반응를 수행하였다. 또한, BET, TEM, TPR를 사용하여 촉매 및 담체의 특성을 분석하였다. 촉매 담체인 실리카 지주 $H^+-kenyaite$(SPK) 와 $H^+-magadite$(SPM)의 BET 비 표면적은 각각 $760m^2/g$와 $810m^2/g$ 이었고, 평균기공크기는 각각 3.0 nm와 2.6 nm 이었다. $N_2$-흡착등온선은 히스테리시스가 잘 발달된 IV형이었으며, TEM으로 중기공성 층상화합물이 잘 만들어졌음을 확인할 수 있었다. Ru(3)/SPK와 Ru(3)/SPM 촉매는 973 K, $CH_4/O_2=2$, $1.25{\times}10^{-5}g-Cat.hr/ml$의 반응조건에서 각각 90%, 87%의 수소의 수율를 얻을 수 있었으며, 약 60시간 까지도 높은 수소 수율을 유지하였다. Ru(3)/SPK와 Ru(3)/SPM 촉매의 TPR 피크는 각각 453K와 413K의 근방에서 비슷한 환원도를 보여주었다. 이러한 분석자료로부터 SPK와 SPM은 산화반응의 촉매 담체로서 구비조건(비 표면적, 열안정성, 평균기공크기 등)를 갖추고 있음을 알 수 있었다.

Keywords

References

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