청정기술 (Clean Technology)

  • 제17권2호
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  • Pages.166-174
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  • 2011
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  • 1598-9712(pISSN)
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  • 2288-0690(eISSN)
한국청정기술학회 (The Korean Society of Clean Technology)
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서로 다른 몰비의 Al/(Al+Ce)를 가진 Al-Ce 혼합산화물에 담지된 Pt 촉매 상에서의 일산화탄소 산화반응

CO Oxidation Over Pt Supported on Al-Ce Mixed Oxide Catalysts with Different Mole Ratios of Al/(Al+Ce)

  • Park, Jung-Hyun (Department of Chemical Engineering, Chungbuk National University) ;
  • Cho, Kyung-Ho (Department of Chemical Engineering, Chungbuk National University) ;
  • Kim, Yun-Jung (Department of Chemical Engineering, Chungbuk National University) ;
  • Shin, Chae-Ho (Department of Chemical Engineering, Chungbuk National University)
  • 투고 : 2011.04.14
  • 심사 : 2011.05.25
  • 발행 : 2011.06.30
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초록

지지체의 구성비가 일산화탄소 산화반응에 미치는 영향을 조사하기 위하여 다양한 몰 비의 Al/(Al+Ce) 산화물을 공침법으로 제조하고 백금을 담지한 촉매를 함침법으로 제조하였다. 제조한 촉매의 물리 화학적 특성을 알아보고 반응 활성과 연관시키기 위하여 X-선 회절분석(XRD), 질소 흡착 탈착분석($N_2$ sorption), 수소/일산화탄소-승온환원분석($H_2$/CO-TPR)의 특성분석을 수행하였다. Pt/xAl-yCe 촉매에서 지지체의 몰 비에 따른 최적 활성을 조사한 결과, 건식 및 습식 반응조건에서 Pt/1Al-9Ce 촉매가 가장 좋은 활성을 나타냈으며, 이를 기준으로 회산형 형태의 반응 곡선을 나타냈다. 반응물에 5%의 수분이 존재 할 때, 50%의 전환율 온도가 건조 반응조건에서의 활성보다 약 $30^{\circ}C$ 저온으로 이동하였다. CO-TPR 분석에서Pt/1Al-9Ce 촉매 상의 이산화탄소 탈착피크가 가장 크게 관찰되었고, CO-TPR 결과는 반응결과와 잘 일치하였다. 이는 다른 촉매에 비해 Pt/1Al-9Ce 촉매의 표면 흡착점이 가장 많고 지지체로부터 산소공급이 용이함을 의미한다. 또한 $^{27}Al$ NMR 분석에서 오면체로 배위된 $Al^{3+}$ 점의 양과 반응 활성이 비례관계에 있음을 확인하였다.

The xAl-yCe oxide catalysts with different mol ratios of Al/(Al+Ce) were prepared by a co-precipitation method and Pt supported on xAl-yCe oxide catalysts were synthesized by an incipient wetness impregnation method. The catalysts were characterized by X-ray Diffraction (XRD), $N_2$ sorption, and $H_2$/CO-temperature programmed reduction ($H_2$/CO-TPR) to correlate with catalytic activities in co oxidation. Among the catalysts studied here, Pt/1Al-9Ce oxide catalyst showed the highest activity in dry and wet reaction conditions and the catalytic activity showed a typical volcano-shape curve with respect to Al/(Al+Ce) mol ratio. When the presence of 5% water vapor in the feed, the temperature of $T_{50%}$ was shifted ca. $30^{\circ}C$ to lower temperature region than that in dry condition. From CO-TPR, the desorption peak of $CO_2$ on Pt/1Al-9Ce oxide catalyst showed the highest value and well correlated the catalytic performance. It indicates that the Pt/1Al-9Ce oxide catalyst has a large amount of active sites which can be adsorbed by co and easy to supplies the needed oxygen. In addition, the amount of pentacoordinated $Al^{3+}$ sites obtained through $^{27}Al$ NMR analysis is well correlated the catalytic performance.

키워드

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