铈源对甲醇水蒸气重整制氢CuO/CeO2催化剂的影响

Influence of cerium sources on CuO/CeO2 catalysts for hydrogen production from steam reforming of methanol

    摘要
  • 摘要: 采用沉淀法合成了CeO2载体，再经浸渍法负载活性组分得到CuO/CeO2催化材料，探究了铈源（Ce（NO3）3·6H2O、CeCl3·6H2O、Ce（NH4）2（NO3）6、Ce（SO4）2·4H2O）对CuO/CeO2催化性能的影响。通过采用XRD、SEM、N2O滴定、BET和H2-TPR等表征手段对催化材料的结构和性质研究发现，四种铈源合成的CuO/CeO2催化材料在Cu比表面积、还原性能以及活性组分和载体间的相互作用方面存在着明显差别。其中，由Ce（NO3）3·6H2O合成的CuO/CeO2催化材料的Cu比表面积较大，CuO还原温度较低，CeO2载体与CuO之间相互作用较强，在甲醇水蒸气重整反应过程中，表现出较佳的催化活性，在反应温度为553 K，水醇比n（H2O）/n（MeOH）为1.2，甲醇水蒸气气体空速（GHSV）为1760 h-1时，甲醇的转化率为100%，重整气中CO摩尔含量为0.84%。

     

    Abstract: CeO2 support was synthesized by precipitation method and used to prepare CuO/CeO2 catalyst using impregnation method. The effects of cerium sources (Ce(NO3)3·6H2O, CeCl3·6H2O, Ce(NH4)2(NO3)6 and Ce(SO4)2·4H2O) on the catalytic performance of CuO/CeO2 catalyst were investigated. XRD, SEM, N2O titration, BET and H2-TPR were used to study the structure and properties of the catalysts. The CuO/CeO2 catalysts with different cerium sources have obvious differences in Cu specific surface area, reduction performance and interaction between active component and support. Moreover, CuO/CeO2 catalyst prepared with Ce(NO3)3·6H2O has large Cu specific surface area, low reduction temperature and strong interaction between CeO2 support and CuO and shows better catalytic activity in methanol steam reforming. The methanol conversion is 100% at reaction temperature of 553 K, water/methanol ratio in feed of 1.2 and methanol water gas hourly space velocity of 1760 h-1. Besides, the CO molar content in reformed gas is 0.84%.

     

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