ZrO2和La2O3助剂对Cu催化剂甲醇水蒸气重整反应的促进作用.docVIP

ZrO2和La2O3助剂对Cu催化剂甲醇水蒸气重整反应的促进作用 摘要：以活性碳为载体，制备出用于甲醇水蒸气重整制氢的新型高效Cu/Zr/C，Cu/Ce/C，Cu/La/C催化剂，并详细比较Zr，Ce，La元素对催化性能的影响。结果表明，添加适量的Zr，Ce，La可显著提高催化活性和制氢选择性，同时有效降低产物中CO的含量。采用XRD图谱及TPR图谱分析方法证实添加适量稀土元素La、Ce对催化剂的微结构性质可产生重要的调控作用，从而大大提高催化活性和制氢选择性,其中Ce的催化活性和制氢选择性优于其它稀土元素。采用XPS谱图表明加入Zr可使铜系催化剂的活性提高，但催化活性的提高仅仅保持在小范围内。另外TPR结果表明催化剂的还原行为和ZrO2含量存在很大的关系。5276 关键词: 制氢；甲醇重整；Cu/Zr/C催化剂；Cu/Ce/C催化剂；Cu/La/C催化剂 The promoting role of ZrO2 and La2O3 on Cu catalysts for Methanol Steam Reforming Abstract: The catalysts of Cu/Zr/C,Cu/Ce/C,Cu/La/C with high catalytic activities for hydrogen production by methanol steam reforming were prepared with the active carbon as supporters, and the promoting roles of Zr, Ce, La promoters to catalytic performance were compared in detail. The results displayed that the proper loadings of Zr,Ce,La can improve the catalytic activity and selectivity of H2, and depress the production of CO effectively. The results of XRD and TPR illustrated the high activity and selectivity of catalysts with Ce and La are accounted for the structure modification of rare earth promoters. The catalysts promoted by Ce are superior to other ones in catalytic activity and selectivity of hydrogen. The results of XPS confirmed that the introduction of Zr can make copper catalyst activity increased, but only keep on a small scale. In addition the TPR results showed that the reduction behavior of catalyst depends much on the content of ZrO2. KeyWords: Hydrogen Production; Steam Reforming of Methanol; Cu/ Zr/ C; Cu/ Ce/C ; Cu/ La/C 3.2.2 ZrO2对催化剂表面电子性质的影响17 3.2.3 ZrO2助剂对催化剂还原行为的影响22 3.2.4 ZrO2对催化剂甲醇水蒸气重整反应性能的影响23 4 结论25 致谢26 参考文献27 1引言 1.1 前言 由于汽车尾气污染日益加剧, 传统汽车不仅消耗了大量的石油资源，而且汽车尾气中的氮氧化物，碳氢化物，一氧化碳等造成了大气的严重污染。燃料电池[1-2]作为一种无污染，高效率的能源设备正在势不可挡地进入汽车工业，电动车取代目前的内燃机汽车，将从根本上解决汽车工业排污问题，实现ldquo;零排放rdquo;。世界各国争相研发ldquo;零排放rdquo;的燃料电池电动车( FCEV) 。甲醇[3]作为液体燃料因具有高能量密度、低碳含量以及运输和贮存方便等优势成为车载制氢的理想燃料，解决由于世界石油储量的持续减少、地球生态环境不断恶化所带来的能源与环境问题，目前已经成为研究的热点之一。 现在制氢的工艺方法是电解水，烃类水蒸汽重整制氢方法及重油（或渣油）部分氧化重整制氢方法。电解水方法制氢是目前应用较广