催化学报

催化学报 ›› 2013, Vol. 34 ›› Issue (2): 305-312.DOI: 10.1016/S1872-2067(11)60466-X

• 研究论文 • 上一篇    下一篇

Ni 掺杂对纳米结构牡丹花状 CeO2 材料催化特性的影响

仙存妮 1, 王少飞 1, 孙春文 1, 李泓 1,*, 陈晓惠 2, 陈立泉 1   

  1. 1中国科学院物理研究所清洁能源重点实验室, 北京 100190; 2哥伦比亚大学应用物理与应用数学学院, 美国纽约
  • 收稿日期:2012-08-13 修回日期:2012-10-12 出版日期:2013-02-05 发布日期:2013-02-05

Effect of Ni Doping on the Catalytic Properties of Nanostructured Peony-Like CeO2

XIAN Cunni1, WANG Shaofei1, SUN Chunwen1, LI Hong1,*, CHAN Suiwai2, CHEN Liquan1   

  1. 1Key Laboratory for Renewable Energy, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China; 2Department of Applied Physics and Applied Mathematics, Columbia University, New York, USA
  • Received:2012-08-13 Revised:2012-10-12 Online:2013-02-05 Published:2013-02-05

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摘要： 制备了一种新型 Ni 掺杂多层纳米结构牡丹花状 CeO2 材料, 研究了其催化性能, 同时与 Ni 负载牡丹花状 CeO2 样品进行了比较. 结果表明, Ni 掺杂 CeO2 样品具有纳米晶粒和开放的介孔结构, 特殊的形貌使其在 CO 氧化和甲烷部分氧化反应中具有独特的催化特性. Ni 掺杂后, CeO2 中产生了多余氧空位, 同时其氧化还原活性也增强, 其在 CO 氧化反应中的催化活性明显高于纯 CeO2 和 Ni 负载 CeO2 样品; 在甲烷部分氧化反应中, 牡丹花状 CeO2 负载 3 atm% Ni 催化剂样品上甲烷转化率高于所有 Ni 掺杂的催化剂样品. 但是在 Ni 负载型催化剂和花状 CeO2 催化剂上, 甲烷的起始转化温度为 400 oC, 而 5.7 atm%Ni 的掺杂使其降至 340 oC.

关键词: 纳米结构氧化铈, 镍, 一氧化碳氧化, 甲烷部分氧化

Abstract: Nanostructured ceria materials have attracted wide attention as catalysts, and the doping of these materials with rare earth elements to modify their catalytic activity has been comprehensively investigated. A novel type of Ni-doped hierarchical nanostructured peony-like ceria (PCO) has been prepared and its catalytic activity is investigated and compared with that of Ni-loaded samples. The prepared Ni-doped ceria have nanoscale grain sizes and open mesopores. This unique morphology endows it with superior catalytic activity for the oxidation of CO and the partial oxidation of methane. It is found that extra oxygen vacancies are generated in the ceria, and the reducibility of the ceria is highly enhanced after Ni-doping. The catalytic activity for CO oxidation is improved after Ni-doping, compared with that of pure ceria and Ni-loaded ceria. In the reaction for the partial oxidation of methane, the 3.8 atm% Ni-loaded PCO sample realizes a higher CH4 conversion than the Ni-doped ceria. However, it is found that the onset temperature for CH4 conversion decreases from 400 °C for the pure PCO and 3.8 atm% Ni-loaded PCO sample, to 340 °C for the 5.7 atm% Ni-doped PCO sample.

Key words: nanostructured ceria, nickel, carbon monoxide oxidation, partial oxidation of methane