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Purification of chemical feedstocks by the removal of aerial carbonyl sulfide by hydrolysis using rare earth promoted alumina catalysts

机译:通过使用稀土促进的氧化铝催化剂进行水解以去除空中的羰基硫,从而纯化化学原料

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The effect of rare earth doping of alumina catalysts is investigated for the carbonyl sulfide ( COS) hydrolysis reaction ( COS + H2O = CO2 + H2S). The effect of the catalyst preparation method is described and discussed, and three methods are compared, namely: impregnation by incipient wetness, coprecipitation and deposition precipitation. The most effective catalysts are prepared using the incipient wetness impregnation method. The addition of rare earth oxides, namely Y2O3, Gd2O3, Nd2O3, La2O3, increases the basicity of the material as shown by pulsed CO2 chemisorption and the basicity increases with the amount of rare earth oxide added. CO2 TPD shows that the La2O3- doped alumina has the strongest basic sites. The promoted catalysts are all effective for the COS hydrolysis reaction and the best results are obtained with Y2O3- doped materials, as these have the most pronounced promotion of activity over the reaction timescale we have examined. The combination of the results for COS conversion with the H2S selectivity data and the effects of H2S pre- treatment shows that a highly active catalyst also has a high H2S selectivity. The La2O3- doped materials deactivate rapidly and have poor H2S selectivities, and we propose that the higher basicity of this material leads to reaction with the acidic COS and H2S leading to the formation of the less basic lanthanum sulfide. This study has presented results for the first time showing that an alumina catalyst for COS hydrolysis can be promoted by the addition of rare earth oxides, and this is related to the enhanced basicity of the promoted catalyst.
机译:研究了稀土掺杂对氧化铝催化剂对羰基硫(COS)水解反应(COS + H2O = CO2 + H2S)的影响。描述并讨论了催化剂制备方法的效果,并比较了三种方法:初湿浸渍,共沉淀和沉积沉淀。最有效的催化剂是使用初期湿润浸渍法制备的。如脉冲CO2化学吸附所示,添加稀土氧化物(即Y2O3,Gd2O3,Nd2O3,La2O3)会增加材料的碱度,并且碱度随添加的稀土氧化物量而增加。 CO2 TPD表明,掺杂La2O3的氧化铝具有最强的碱性位。助催化剂对COS水解反应都是有效的,使用Y2O3掺杂的材料可获得最佳结果,因为这些材料在我们研究的反应时间范围内具有最明显的活性提升。 COS转换结果与H2S选择性数据以及H2S预处理的效果的结合表明,高活性催化剂还具有较高的H2S选择性。掺杂La2O3的材料会迅速失活,并具有很差的H2S选择性,我们认为该材料的较高碱度会导致与酸性COS和H2S反应,从而导致碱性较低的硫化镧的形成。该研究首次给出结果,表明通过添加稀土氧化物可以促进用于COS水解的氧化铝催化剂,这与增强的碱度有关。

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