Korean Chemical Engineering Research

The Korean Institute of Chemical Engineers (한국화학공학회)
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Selective Oxidation of Hydrogen Sulfide Containing Ammonia and Water Using Fe2O3/SiO2 Catalyst

Fe2O3/SiO2 촉매 상에서 물과 암모니아가 함께 존재하는 황화수소의 선택적 산화 반응

  • Kim, Moon-Il (Division of Chemical and Biomolecular Engineering, Pusan National University) ;
  • Lee, Gu-Hwa (Division of Chemical and Biomolecular Engineering, Pusan National University) ;
  • Chun, Sung-Woo (Jeong Won Chemical Co., Ltd.) ;
  • Park, Dae-Won (Division of Chemical and Biomolecular Engineering, Pusan National University)
  • Received : 2011.10.10
  • Accepted : 2011.12.06
  • Published : 2012.06.01
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Abstract

The catalytic performance of some metal oxides in the vapor phase selective oxidation of $H_2S$ in the stream containing ammonia and water was investigated. Among the catalysts tested $Fe_2O_3/SiO_2$ was the most promising catalyst for practical application. It showed higher than 90% $H_2S$ conversion and very small amount of $SO_2$ emission over a temperature range of $240{\sim}280^{\circ}C$. The effects of reaction temperature, $O_2/H_2S$ ratio, amount of ammonia and water vapor on the catalytic activity of $Fe_2O_3/SiO_2$ were discussed to better understand the reaction mechanism. The $H_2S$ conversion showed a maximum at $260^{\circ}C$ and it decreased with increasing temperature over $280^{\circ}C$. With an increase of $O_2/H_2S$ ratio from 0.5 to 4, the conversion was slightly increased, but the selectivity to elemental sulfur was remarkably decreased. The increase of ammonia amount favored the conversion and the selectivity to elemental sulfur with a decrease in $SO_2$ production. The presence of water vapor decreased both the activity and the selectivity to sulfur, but increased the ATS selectivity.

본 연구는 암모니아와 물이 함께 존재하는 황화수소를 선택적 산화 반응을 통해 원소 황의 형태로 제거하는 기상 촉매 공정의 개발에 관한 것이다. 최적의 촉매를 개발하기 위해 여러 가지 금속산화물에 대한 반응성 실험 결과 $Fe_2O_3/SiO_2$ 촉매가 $240{\sim}280^{\circ}C$의 온도 범위에서 90% 이상의 $H_2S$ 전화율과 아주 낮은 $SO_2$ 방출을 나타내어 실제 공정에 적용하기에 가장 적합하였다. $Fe_2O_3/SiO_2$ 촉매 상에서 황화수소의 선택적 산화 반응에 대한 메커니즘 규명을 위하여 반응 온도, $O_2/H_2S$ 몰 비, 암모니아와 수증기의 분압이 촉매 활성에 미치는 영향에 관하여 고찰하였다. 전화율은 반응 온도가 $260^{\circ}C$에서 최대값을 보였고, $280^{\circ}C$ 이상에서는 전화율과 원소 황의 선택도가 모두 감소하는 경향을 나타내었다. $O_2/H_2S$ 비가 0.5에서 4로 증가하면 전화율이 증가하였으나 선택도는 크게 감소하였다. 암모니아 분압이 증가하면 전화율이 증가하고 $SO_2$ 발생은 감소하였으며 원소 황의 선택도가 증가하였다. 수증기가 함께 존재하면 전화율과 원소 황의 선택도는 감소하고, ATS의 선택도가 증가하였다.

Keywords

References

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