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Catalytic Recovery of Elemental Sulfur from Sulfur Dioxide-Laden Gas Streams

机译:从载有二氧化硫的气流中催化回收元素硫

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Single-stage catalytic reduction of SO_2 to elemental sulfur is a promising new technology better suited to treat SO_2-laden streams generated in power plants and certain industries than the conventional multi-stage Claus process. The catalytic reduction of SO_2 to elemental sulfur by CH_4 over ceria and metal-modified ceria was studied in this work at atmospheric pressure and with a feed gas mixture containing a molar ratio of CH_4/SO_2=0.5-3. These catalysts are active in the temperature range 550-750℃. At temperatures below ~550℃ the catalyst surface is capped by SO_2. Activation of CH_4 on these surfaces is initiated after sulfate decomposition. The catalyst structure was examined by XRD, STEM/EDS and XPS. The working catalyst surface was partially sulfated even under fuel-rich conditions. CH_4-TPR and isothermal CH_4 reduction of pre-sulfated catalysts suggest that the reaction light-off coincides with the threshold temperature for sulfate decomposition. The addition of five atomic metal percent (5 at%) of copper into La-doped ceria, Ce(La)Ox, improved dramatically both the wet activity of the latter as well as its selectivity to elemental sulfur under fuel-rich conditions. Nickel addition, on the other hand, favored the partial oxidation of methane, and decreased the selectivity to sulfur.
机译:将SO_2单段催化还原为元素硫是一种有前途的新技术,与常规的多段克劳斯工艺相比,它更适合处理发电厂和某些行业中产生的负载SO_2的物流。在这项工作中,在大气压下,使用摩尔比为CH_4 / SO_2 = 0.5-3的进料气体混合物,研究了CH_2在二氧化铈和金属改性的二氧化铈上将SO_2催化还原为元素硫。这些催化剂在550-750℃的温度范围内具有活性。在低于〜550℃的温度下,催化剂表面被SO_2覆盖。硫酸盐分解后,这些表面上的CH_4活化开始。通过XRD,STEM / EDS和XPS检查催化剂的结构。即使在富含燃料的条件下,工作催化剂表面也被部分硫酸化。预硫酸盐化催化剂的CH_4-TPR和等温CH_4还原表明,起燃反应与硫酸盐分解的阈值温度一致。在掺La的二氧化铈Ce(La)Ox中添加5个原子百分比的金属(5%原子)可显着提高后者的湿活性以及在富燃料条件下对元素硫的选择性。另一方面,添加镍有利于甲烷的部分氧化,并降低了对硫的选择性。

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