Abstract
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.
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