A Study of $Ce_{1-x}Zr_xO_2$ Catalytic Reaction for the Recovery of Elemental Sulfur from $SO_2$

$SO_2$로부터 원소 황 회수를 위한 $Ce_{1-x}Zr_xO_2$ 촉매반응연구

Kim, Bong-Suk;Lee, Jong-Dae;Park, No-Kuk;Ryu, Si-Ok;Lee, Tae-Jin;Kim, Jae-Chang
김봉석;이종대;박노국;류시옥;이태진;김재창

  • Published : 2003.10.31

Abstract

The catalytic reduction of $SO_2$ to elemental sulfur with CO over $Ce_{1-x}Zr_xO_2$ was studied. The $Ce_{1-x}Zr_xO_2$ catalysts were prepared by changing the Ce/Zr mole ratio (x=1, 0.8, 0.5, 0.2, 0). The reactivity of $Ce_{1-x}Zr_xO_2$ in accordance with experimental conditions, such as reaction temperature ($400-450^{\circ}C$), space velocity ($GHSV:\;10,000-70,000\;h^{-1}$) were investigated. The conversion of $SO_2$ and the selectivity to elemental sulfur in the recovery of elemental sulfur from $SO_2$ using $Ce_{0.8}Zr_{0.2}O_2\;and\;Ce_{0.5}Zr_{0.5}O_2$ catalysts were respectively about 93% and 98% at temperature about $425^{\circ}C$, which were superior to other catalysts. It seems that the reactivity is influenced by the Ce/Zr mole ratio. From these results, it was concluded that the oxygen mobility of catalysts was increased with inserting the Zr. Because the reduction of lattice oxygen and reoxidation of Ce-based catalysts was improved by the adding Zr, it is possible to improve the redox characteristic.

$Ce_{1-x}Zr_xO_2$ 촉매상에서 CO에 의한 $SO_2$의 촉매환원으로부터 원소 황 회수 반응에 대하여 연구하였다. $Ce_{1-x}Zr_xO_2$ 촉매는 Ce/Zr 조성비를 x=1, 0.8, 0.5, 0.2, 0과 같이 조절하여 제조하였으며 반응온도($400-450^{\circ}C$), 공간속도($10,000-70,000\;h^{-1}$)변화에 따른 $SO_2$전화율과 원소 황(S)선택도를 조사하였다. $Ce_{1-x}Zr_xO_2$촉매의 최적반응온도는 $425^{\circ}C$ 이었으며 공간속도 $50,000\;h^{-1}$에서 $Ce_{0.8}Zr_{0.2}O_2$$Ce_{0.5}Zr_{0.5}O_2$ 촉매의 $SO_2$ 전환율이 93%, 원소 황 선택도 98%로 $CeO_2,\;Ce_{0.2}Zr_{0.8}O_2$ 촉매보다 반응성이 높았다. $Ce_{1-x}Zr_xO_2$촉매에 Zr의 첨가량이 증가할수록 $CeO_2$의 환원률이 증가되었으며, 이러한 결과는 산소 저장성이 우수한 $CeO_2$에 Zr를 첨가함으로써 산소이동성이 증가되었기 때문인 것으로 판단된다. 본 연구에서는 Zr의 첨가로부터 Ce-based 촉매의 격자산소 환원과 비어있는 격자산소 자리의 재산화에 영향을 주어 redox 반응특성을 개선할 수 있음을 확인하였다.

Keywords

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