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NOx储存催化剂Pt/BaAl2O4-A12O3的XAFS研究

The Study of XAFS for the NOx Storage Catalyst Pt/BaAl2O4-Al2O3

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【作者】 李新刚孟明林培琰黄志坚伏义路谢亚宁胡天斗

【Author】 Li Xin-Gang,Meng Ming, Lin Pei-Yan,Huang Zhi-Jian, Fu Yi-Lu, Xie Ya-Ning, Hu Tian-Dou (Department of Chemical Physics, University of Science and Technology of China, Hefei 230026; Synchrotron Radiation Laboratory, Institute of High Energy Physics, Be

【机构】 中国科学技术大学化学物理系中国科学院高能物理研究所中国科学院高能物理研究所 合肥 230026合肥 230026合肥 2300

【摘要】 采用共沉淀-浸渍法在不同载体焙烧温度下,制备了不同Al/Ba原子比的Pt/BaAl2O4-A12O3系列样品。用XRD,XANES,EXAFS,以及NSC(NO_x storage capacity)测定等手段对样品的微观结构和NO_x储存性能进行了详细的表征.样品中Ba物种是以BaAl2O4和BaCO3两种混合物相的形式存在,且伴随着载体焙烧温度和Ba含量的降低,BaAl2O4物相的分散度变高,NO_x储存活性也随之提高,这表明BaAl2O4相的分散度与样品的NO_x储存性能密切相关,小颗粒的BaAl2O4相是NO_x的主要储存活性中心.在样品中,Pt物种以金属原子簇形式存在.分散度很高,其Pt—Pt壳层配位数较标样Pt粉有显著下降,Pt—Pt键长变短,出现了纳米收缩现象.高分散的小颗粒金属Pt原于簇为捕获和氧化NO_x的主要活性中心.

【Abstract】 A series of Pt/BaA12O4-A12O3 NOx trap samples were prepared by coprecipitation-impregnation method. The supports BaA12O4-Al2O3 were calcined at 800 ℃ and 1000 ℃, respectively. X-ray Diffraction (XRD), X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure(EXAFS) were used to characterize the microcosmic structure of barium and platinum species in the samples. It is shown that the barium exists in the forms of BaA12O4 and BaCO3 crystallites. With the decreasing of calcination temperature and barium content, the dispersion of BaA12O4 phase becomes higher. Platinum in the samples mainly exists as small atomic clusters, which possess very high dispersion. In comparison with the standard compound of platinum, the magnitude for Pt - Pt coordination shell is significantly decreased, and the coordination distance is also shortened about 0. 01 nm. All the results suggest that the BaAl2O4 crystallites should be the centers for NOx storage, while the fine-grained platinum species with high dispersion are deduced as the centers for the capture and oxidation of NOx species.

【关键词】 NO_xPt/BaAl2O4-Al2O3储存XAFS
【Key words】 NO_xPt/BaAl2O4-Al2O3StorageXAFS
【基金】 国家自然科学基金(29973037);教育部优秀青年教师资助计划;安徽省自然科学基金(99045429)资助项目
  • 【文献出处】 物理化学学报 ,Acta Physico-chimica Sinica , 编辑部邮箱 ,2001年12期
  • 【分类号】O643.3
  • 【被引频次】16
  • 【下载频次】142
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