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Preferential CO oxidation in H2-rich stream over Au/CeO2 catalysts prepared via modified deposition-precipitation

机译:通过改进的沉积沉淀法在Au / CeO2催化剂上富H2物流中优先进行CO氧化

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摘要

Preferential CO oxidation in a H2-rich stream over Au/CeO2 catalysts prepared via modified deposition-precipitation by using different precipitating agents at various pH values was investigated in this research work. The prepared catalysts were characterized by XRD, TEM, XRF, BET, TPR, UV-vis, and FTIR. The experimental results showed that the Au/CeO2 catalysts prepared by using NaOH as a precipitating agent at pH 7 expressed the highest catalytic activities (complete conversion and 51% selectivity at 40 °C) due to its well-dispersed nano-size Au particles on the support surface with narrower particle size distribution. When adding CO2 to the feed stream, the catalytic performance was decreased dramatically due to the formation of the formate species. The co-addition of CO2 and H2O in the feedstream had a less negative effect on the CO oxidation compared to the effect of CO2 alone. Water can attack and decompose the carbonate intermediate; the accumulation of the formate species on the active sites of the catalysts is then decreased and the catalytic performance is improved. After in situ thermal regeneration under 5% oxygen in helium at 110 °C for 2 h, more active sites for the preferential CO oxidation reaction were recovered since the oxygen reacted with the formate species to form CO2. In addition, the Au/CeO2 catalysts exhibited good stability during the tested time in this study.
机译:在这项研究工作中,研究了通过使用不同的沉淀剂在各种pH值下通过改进的沉积沉淀法制备的Au / CeO2催化剂上富H2物流中的优选CO氧化。通过XRD,TEM,XRF,BET,TPR,UV-vis和FTIR对制备的催化剂进行表征。实验结果表明,以NaOH为沉淀剂在pH 7下制备的Au / CeO2催化剂表现出最高的催化活性(在40°C时完全转化和51%的选择性),这是由于其在纳米颗粒上分散得很好。具有较窄粒度分布的载体表面。当将CO 2添加到进料流中时,由于甲酸盐种类的形成,催化性能急剧下降。与单独的CO2影响相比,进料流中CO2和H2O的共添加对CO氧化的负面影响较小。水会侵蚀和分解碳酸盐中间体。然后减少了甲酸类在催化剂活性位点上的积累,并提高了催化性能。在110%的氦气中于5%的氧气中进行原位热再生2 h后,由于氧气与甲酸盐类物质反应生成CO2,因此回收了更多的优先CO氧化反应活性位点。此外,在这项研究中,Au / CeO2催化剂在测试时间内表现出良好的稳定性。

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