铈源对甲醇水蒸气重整制氢CuO/CeO2催化剂的影响

采用沉淀法合成了CeO_2载体,再经浸渍法负载活性组分得到CuO/CeO_2催化材料,探究了铈源(Ce(NO_3)_3·6H_2O、Ce Cl_3·6H_2O、Ce(NH_4)_2(NO_3)_6、Ce(SO_4)_2·4H_2O)对CuO/CeO_2催化性能的影响。通过采用XRD、SEM、N_2O滴定、BET和H_2-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/CeO_2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(NO_3)_3·6H_2O合成的CuO/CeO_2催化材料的Cu比表面积较大,CuO还原温度较低,CeO_2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(H_2O)/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%。

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

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%.