Clean Technology (청정기술)

The Korean Society of Clean Technology (한국청정기술학회)
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Low Temperature CO Oxidation over Cu-Mn Mixed Oxides

Cu-Mn 혼합산화물 상에서 일산화탄소의 저온산화반응

  • Cho, Kyong-Ho (Department of Chemical Engineering, Chungbuk National University) ;
  • Park, Jung-Hyun (Department of Chemical Engineering, Chungbuk National University) ;
  • Shin, Chae-Ho (Department of Chemical Engineering, Chungbuk National University)
  • Received : 2010.05.27
  • Accepted : 2010.06.21
  • Published : 2010.06.30
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Abstract

The Cu-Mn mixed oxide catalysts with different molar ratios of Cu/(Cu+Mn) prepared by co-precipitation method have been investigated in CO oxidation at $30^{\circ}C$. The catalysts used in this study were characterized by X-ray Diffraction (XRD), $N_2$ sorption, X-ray photoelectron spectroscopy (XPS), and $H_2$-temperature programmed reduction $(H_2-TPR)$ to correlate with catalytic activities in CO oxidation. The $N_2$ adsorption-desorption isotherms of Cu-Mn mixed oxide catalysts showed a type 4 having pore range of 7-20 nm and BET surface area was increased from 17 to $205\;m^2{\cdot}g^{-1}$ with increasing of Mn content. The XPS analysis showed the surface oxidation state of Cu and Mn represented $Cu^{2+}$and the mixture of $Mn^{3+}$ and $Mn^{4+}$, respectively. Among the catalysts studied here, Cu/(Cu+Mn) = 0.5 catalyst showed the highest activity at $30^{\circ}C$ in CO oxidation and the catalytic activity showed a typical volcano-shape curve with respect to Cu/(Cu+Mn) molar ratios. The water vapor showed a prohibiting effect on the efficiency of the catalyst which is due to the competitive adsorption of carbon monoxide on the active sites of catalyst surface and finally the formation of hydroxyl group with active metals.

서로 다른 몰비의 Cu-Mn 혼합산화물을 공침법으로 제조하여 $30^{\circ}C$에서 CO 산화반응을 수행하였다. 제조된 촉매는 CO 산화반응에서 반응 활성과 연관시키기 위하여 XRD, $N_2$ 흡착 및 탈착, XPS, $H_2-TPR$ 등의 특성분석을 수행하였다. 제조된 촉매의 질소흡착 등온곡선은 4형태로 7-20 nm크기의 세공이 존재하며, Mn의 함량이 증가함에 따라 BET 표면적은 17에서 $205m^2{\cdot}g^{-1}$ 으로 증가하였다. XPS 분석으로 Cu-Mn 혼합산화물 상의 Cu는 주성분이 2+의 산화상태임을 확인하였고, Mn은 +3과 +4의 산화 상태를 나타냈다. Cu-Mn 촉매의 함량 및 비율에 따른 최적 활성을 실험 조사한 결과, $30^{\circ}C$의 반응온도에서 Cu/(Cu+Mn)의 몰비가 0.5일 때 가장 좋은 활성을 나타냈으며, 이를 기준으로 화산형 형태의 반응 곡선을 나타냈다. 수분 존재하의 CO 산화반응은 활성점에 수분과 CO의 경쟁흡착으로 촉매의 활성을 감소시켰으며 최종적으로는 활성금속 성분과 하이드록실 그룹을 형성하였기 때문이다.

Keywords

References

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