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• 作者：Stan Harding ; Terry Wall ; Fraser Wigley ; Fleming Fr ; sen ; Miko Hupa ; Dave Tillman
• 关键词：Ce-based catalysts ; Desulfurization ; Claus reaction ; Redox ; Coal gas cleanup
• 刊名：Fuel Processing Technology
• 出版年：2007
• 出版时间：December 2007
• 年：2007
• 卷：88
• 期：11-12
• 页码：1009
• 全文大小：62 K

文摘

Claus reaction (2H₂S + SO₂ ↔ 3/nS_n + 2H₂O) was used to clean the gasified coal gas and the reactivity of several metal oxide-based catalysts on Claus reaction was investigated at various operating conditions. In order to convert H₂S contained in the gasified coal gas to elemental sulfur during Claus reaction, the catalysts having the high activity under the highly reducing condition with the moisture should be developed. CeO₂, ZrO₂, and Ce_1−xZr_xO₂ catalysts were prepared for Claus reaction and their reactivity changes due to the existence of the reducing gases and H₂O in the fuel gas was investigated in this study. The Ce-based catalysts shows that their activity was deteriorated by the reduction of the catalyst due to the reducing gases at higher than 220 °C. Meanwhile, the effect of the reducing gases on the catalytic activity was not considerable at low temperature. The activities of all three catalysts were degraded on the condition that the moisture existed in the test gas. Specifically, the Ce-based catalysts were remarkably deactivated by their sulfation. The Ce–Zr-based catalyst had a high catalytic activity when the reducing gases and the moisture co-existed in the simulated fuel gas. The deactivation of the Ce–Zr-based catalyst was not observed in this study. The lattice oxygen of the Ce-based catalyst was used for the oxidation of H₂S and the lattice oxygen vacancy on the catalyst was contributed to the reduction of SO₂. ZrO₂ added to the Ce–Zr-based catalyst improved the redox properties of the catalyst in Claus reaction by increasing the mobility of the lattice oxygen of CeO₂.