공업화학 (Applied Chemistry for Engineering)

  • 제26권2호
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  • Pages.138-144
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  • 2015
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  • 1225-0112(pISSN)
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  • 2288-4505(eISSN)
한국공업화학회 (The Korean Society of Industrial and Engineering Chemistry)
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CoAPSO-34 촉매상에서 DTO (Dimethyl Ether to Olefins) 반응에 미치는 Co/Al 및 Si/Al 몰 비의 영향

Effects of Co/Al and Si/Al Molar Ratios on DTO (Dimethyl Ether to Olefins) Reaction over CoAPSO-34 Catalyst

  • 김효섭 (충남대학교 정밀응용화학과) ;
  • 이수경 (충남대학교 정밀응용화학과) ;
  • 최기환 (충남대학교 정밀응용화학과) ;
  • 이동희 (충남대학교 정밀응용화학과) ;
  • 박주식 (한국에너지기술연구원 수소연료전지연구단) ;
  • 김영호 (충남대학교 정밀응용화학과)
  • Kim, Hyo-Sub (Department of Fine Chemical Engineering and Applied Chemistry, Chungnam National University) ;
  • Lee, Su-Gyung (Department of Fine Chemical Engineering and Applied Chemistry, Chungnam National University) ;
  • Choi, Ki-Hwan (Department of Fine Chemical Engineering and Applied Chemistry, Chungnam National University) ;
  • Lee, Dong-Hee (Department of Fine Chemical Engineering and Applied Chemistry, Chungnam National University) ;
  • Park, Chu-Sik (Hydrogen and fuel cell department, Korea Institute of Energy Research) ;
  • Kim, Young-Ho (Department of Fine Chemical Engineering and Applied Chemistry, Chungnam National University)
  • 투고 : 2014.12.08
  • 심사 : 2015.01.23
  • 발행 : 2015.04.10
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초록

Co가 첨가된 SAPO-34 촉매(CoAPSO-34)상의 DTO 반응에서 촉매의 수명 향상에 미치는 Co/Al 및 Si/Al 몰 비의 영향을 연구했다. 제조된 CoAPSO-34 촉매들의 특성은 XRD, SEM, $^{29}Si$ MAS NMR 및 $NH_3$-TPD 기법에 의해 확인했다. 먼저 Co/Al 몰 비를 변화시키며 제조한 CoAPSO-34 촉매들의 수명은 SAPO-34와 비교하여 향상된 것으로 나타났으며, 가장 높은 수명을 갖는 촉매의 Co/Al 몰 비는 0.0025로 나타났다. Co/Al 몰 비를 0.0025로 고정하고 Si/Al 몰 비를 0.05에서 0.20으로 증가시킴에 따라 총 산점량은 0.432에서 1.111 mmol/g까지 증가하였다. 그러나 총 산점량이 너무 큰 촉매들은 둥지 내 다환 방향족 화합물들의 급속한 축척으로 인한 기공 막힘으로 빠르게 비활성화되었다. 따라서 0.1의 적절한 Si/Al 몰 비를 갖는 CoAPSO-34 촉매가 수명이 가장 우수한 것으로 나타났으며, SAPO-34 촉매의 수명과 비교하여 약 87% 향상되었다.

Effects of Co/Al and Si/Al molar ratios of cobalt incorporated SAPO-34 catalysts (CoAPSO-34) on their catalytic lifetime were investigated in dimethyl to olefin (DTO) reaction. The property of CoAPSO-34 catalysts was characterized using XRD, SEM, $^{29}Si$ MAS NMR, and $NH_3$-TPD techniques. First, the lifetime of CoAPSO-34 prepared by varying Co/Al molar ratios was improved than that of using the SAPO-34 catalyst, and the optimal Co/Al molar ratio was 0.0025. The total acid site amounts increased from 0.432 to 1.111 mmol/g with increasing Si/Al molar ratios from 0.05 to 0.20 while fixing a Co/Al molar ratio of 0.0025. However, the catalysts with too high acid site amounts were deactivated rapidly with blockages of the pores due to the fast accumulation of polycyclic aromatic hydrocarbons in the cage. Therefore, the CoAPSO-34 catalyst with a proper Si/Al molar ratio of 0.10 was the most superior in terms of the lifetime, which was improved by about 87% as compared with that of the SAPO-34 catalyst.

키워드

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