载体焙烧气氛对甲醇水蒸气重整制氢CuO/CeO_2催化剂的影响

Effect of support calcination atmospheres on the activity of CuO/CeO_2 catalysts for methanol steam reforming

采用沉淀法和浸渍法制备了具有氧空位的CeO_2纳米材料和甲醇水蒸气重整制氢CuO/CeO_2催化剂,探索不同焙烧气氛对CeO_2纳米材料结构、性质和甲醇水蒸气重整制氢性能的影响。采用SEM、XRD、BET、H2-TPR、N2O滴定和XPS等手段对催化剂进行了表征。结果表明,CuO/CeO_2催化剂的催化活性与催化剂的Cu比表面积大小、Cu-Ce的相互作用强弱、表面缺陷和表面氧空位的多少有关。其中,在氢气气氛下焙烧所得的CeO_2负载CuO后的CuO/CeO_2-H催化剂催化活性最佳。在反应温度为250℃,水醇物质的量比为1.2时,甲醇气体空速为800 h-1,甲醇转化率达到了100%,重整尾气中CO含量为0.87%。

In this paper,CeO2 nanomaterials with oxygen vacancies and CuO/CeO2 catalysts for hydrogen production from methanol steam reforming were prepared by precipitation and impregnation methods. The influence of different calcination atmosphere on the structure and properties of CeO2 nanomaterials and the hydrogen production performance of methanol steam reforming was investigated. SEM,XRD,BET,H2-TPR,N2 O titration and XPS were adopted to characterize the catalyst materials. The results showed that the catalytic activity of CuO/CeO2 catalyst was closely related to the surface area of copper, the strength of Cu-Ce interaction,the number of surface defects and surface oxygen vacancies. When the reaction temperature was250 ℃,the molar ratio of water to methanol was 1.2 and the gas hourly space velocity was 800 h-1,the methanol conversion was 100% and the CO concentration in the offgas was 0.87%.