以钙钛矿型复合氧化物为前驱体构筑La-Ce氧化物修饰的Pt-Co纳米双金属催化剂及其对CO氧化的性能

Preparation of La-Ce oxide-modified platinum-cobalt nano-bimetallic catalysts with perovskite-type composite oxides as precursors and their performance in CO oxidation

  • 摘要: 利用钙钛矿型复合氧化物(PTO)可以将多种金属离子限域并均匀混合于钙钛矿晶格中的特点,提出了一种构筑氧化物修饰的纳米双金属催化剂团簇的新构想。以担载于大比表面积SiO2上的钙钛矿型复合氧化物La1-yCeyCo0.87Pt0.13O3/SiO2作为前驱体,将La、Ce、Co和Pt多种金属离子均匀混合并限域于PTO晶粒中,还原后得到Pt-Co/La-Ce-O/SiO2催化剂;通过氮气吸附-脱附、XRD、H2-TPR和TEM等手段对Pt-Co/La-Ce-O/SiO2催化剂进行了表征,考察了其对CO氧化的催化性能,研究了构效关系。结果发现,La-Ce-O-Pt-Co构成了纳米团簇,担载于SiO2表面,形成了Pt-Co纳米双金属颗粒;Co修饰Pt提高了其催化活性,而添加Ce进一步改善了其催化性能。当Ce含量(y)为0.2时,催化剂La0.8Ce0.2Co0.87Pt0.13O3/SiO2的活性最佳,在120℃下即可实现CO完全转化,且在含体积分数15% H2O及12.5% CO2的气氛中仍具有较好的催化性能。稳定性测试表明,所制得的Pt-Co/La-Ce-O/SiO2催化剂具有良好的稳定性和抗烧结性能。

     

    Abstract: A new scheme for constructing composite catalyst composed of oxide-modified bimetallic nanoparticles was proposed, where perovskite-type oxide (PTO) is utilized to confine multifold metal ions in the perovskite crystal lattice. With a perovskite-type oxide (PTO) of La1-yCeyCo0.87Pt0.13O3 loaded on large surface area SiO2 as the precursor, where the La, Ce, Co and Pt ions were uniformly mixed and confined in the PTO crystallites, a series of Pt-Co/La-Ce-O/SiO2 catalysts were prepared through reduction. The Pt-Co/La-Ce-O/SiO2 catalysts were characterized by nitrogen physisorption, XRD, H2-TPR and TEM; their catalytic performance in CO oxidation was investigated. The results indicate that La-Ce-O-Pt-Co clusters are constructed on the SiO2 surface, forming platinum-cobalt nano-bimetallic particles after reduction; the modification of Pt with Co can enhance the catalytic activity and the addition of Ce can further improve the catalytic performance in CO oxidation. The La0.8Ce0.2Co0.87Pt0.13O3/SiO2 catalyst with y=0.2 (representing the Ce content) exhibits high activity in CO oxidation; over it, a complete conversion of CO can be achieved at 120℃. The La0.8Ce0.2Co0.87Pt0.13O3/SiO2 catalyst performs well for CO oxidation even in the presence of 15% (volume ratio) H2O and 12.5% (volume ratio) CO2. Moreover, the oxide-modified platinum-cobalt nano-bimetallic catalysts display excellent stability with high resistance against sintering.

     

/

返回文章
返回