中文摘要
本项目考察了多种制备方法对氧化铈形貌的影响。通过筛选,我们可控制备了零维、一维、三维结构的氧化铈。制备的零维、一维、三维结构的氧化铈结构稳定,经450 oC焙烧后结构仍然能够保持,而且具有较大的比表面积,高达200 m2/g以上。将该氧化铈担载铜后用于一氧化碳氧化催化反应,发现,三维和一维结构的氧化铈担载铜催化剂催化活性明显高于对应的零维催化剂。该结果证明了铈基纳米材料的形貌对催化活性是有影响的。. 在成功地制备了纳/微米氧化铈的基础上,我们又实现了氧化铈纳米线、纳米立方的可控制备。 得到的氧化铈纳米立方结构材料尺寸小于50 nm。将Zr引入该体系,得到了球形和六方的Ce-Zr-O,而将铜引入,分别得到了四方、球形的Ce-Cu-O复合材料,该系列催化剂在一氧化碳氧化反应中具有较高的催化活性。.采用共沉淀法、水热法、溶剂热法和络合燃烧法制备了CoOx-CeO2催化剂,并考察其一氧化碳催化活性。结果表明制备方法、制备条件对催化剂的结构和催化性能均有较大影响,Co3+含量及Ce与Co之间的协同还原是催化活性的关键。
英文摘要
In this project, our research focused on the controllable preparation of nanostructural ceria. A novel preparation of zero, one and three-dimensional (3D) CeO2 originating from single-crystal cerium formate by a surfactant-free route was used. The obtained sea urchin shaped crystal 3D CeO2 assembled from smooth rods with 1 to 5 μm in diameter and up to 50 μm in length, are composed of CeO2 nanocrystals as building units, giving rise to (3D) micro/nanocomposite structures with high BET surface area up to 234 m2 g-1. Raman spectroscopy, thermogravimetric analysis and temperature programmed reduction results indicated that the 3D structure improved the Oxygen Storage Capacity, in which OSC is 45% higher than that of conventional ceria and enhanced the reducibility of surface CeO2 is due to the increased oxygen vacancy. Both 3D CeO2 and 5 wt% CuO loaded on 3D CeO2 exhibit high catalytic activities for CO conversion, compared with zero or one-dimensional CeO2. The 3D micro/nanocomposite structure of CeO2 had the advantages of both microstructure and nanostructure, which could have great potential applications in many fields. . Ceria nanorod and nanocube were prepared in present project. The obtained ceria nanocube is about 50 nm in size. The redox property and catalytic activity were studied. Based on these researches, Zr was incorporated into the nanostructural ceria. nano sphere and nano hexagonal structure was found in the Ce-Zr-O. The incorporation of Zr improved the redox property of ceria. Cu was also incorporated into the nanostructural ceria, nano sphere and nanocube were obtained in Ce-Cu-O samples. The surface reduction of ceria was improved greatly and high CO oxidation activity was found in low Cu content samples, which was contributed to the high Cu dispersion and improved surface reudction property. .CoOx-CeO2 catalysts were preapred by different methods. CO catalytic reaction was performed. It was found that the preparation methods and condition had great influence on the structure of catalysis and their catalytic activity. Co3+ and the interaction between Co and Ce play important roles in the catalytic reaction.
结题摘要
本项目考察了多种制备方法对氧化铈形貌的影响。通过筛选,我们可控制备了零维、一维、三维结构的氧化铈。制备的零维、一维、三维结构的氧化铈结构稳定,经450 oC焙烧后结构仍然能够保持,而且具有较大的比表面积,高达200 m2/g以上。将该氧化铈担载铜后用于一氧化碳氧化催化反应,发现,三维和一维结构的氧化铈担载铜催化剂催化活性明显高于对应的零维催化剂。该结果证明了铈基纳米材料的形貌对催化活性是有影响的。 在成功地制备了纳/微米氧化铈的基础上,我们又实现了氧化铈纳米线、纳米立方的可控制备。 得到的氧化铈纳米立方结构材料尺寸小于50 nm。将Zr引入该体系,得到了球形和六方的Ce-Zr-O,而将铜引入,分别得到了四方、球形的Ce-Cu-O复合材料,该系列催化剂在一氧化碳氧化反应中具有较高的催化活性。采用共沉淀法、水热法、溶剂热法和络合燃烧法制备了CoOx-CeO2催化剂,并考察其一氧化碳催化活性。结果表明制备方法、制备条件对催化剂的结构和催化性能均有较大影响,Co3+含量及Ce与Co之间的协同还原是催化活性的关键。
